Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , 6 , J. Wildt 1 , and 5 , K. Block 5 , R. Grote 2 , K. Butterbach-Bahl 8 23006 23005 , Y. Wang 2 , M. Hallquist 7 , X. Zheng 2,3,4,* 1 , J. Xie 1,* , A. Kiendler-Scharr 7 This discussion paper is/has beenand under Physics review (ACP). for Please the refer journal to Atmospheric the Chemistry corresponding final paper in ACP if available. Department of Chemistry and Molecular Biology, University of Gothenburg, 41296 Helmholtz Zentrum München, Research Unit Environmental Simulation (EUS) at theState Institute Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, University of Chinese Academy ofBeijing Sciences, Institute Beijing of 100049, Landscape China Architecture,Institute Beijing of 100102, Meteorology China and Climate Research, Atmospheric Environmental Research Institute of Bio- and GeosciencesInstitute (IBG-2), for Forschungszentrum, Energy 52425 and Jülich, Climate Germany Research (IEK-8), Forschungszentrum, 52425 Jülich, These authors contributed equally to this work. 8 Gothenburg, Sweden * Received: 6 July 2015 – Accepted: 11Correspondence August to: 2015 A. – Ghirardo Published: ([email protected]) 27 August 2015 Published by Copernicus Publications on behalf of the European Geosciences Union. T. Mentel J.-P. Schnitzler 1 of Biochemical Plant2 Pathology (BIOP), 85764 Neuherberg, Germany Institute of Atmospheric Physics, ChineseChina Academy of3 Sciences (IAP-CAS), Beijing 100029, 4 5 (IMK-IFU), Karlsruhe Institute6 of Technology (KIT), 82467 Garmisch-Partenkirchen,7 Germany Germany Urban stress-induced biogenic VOC emissions impact secondary aerosol formation in Beijing A. Ghirardo Atmos. Chem. Phys. Discuss., 15, 23005–23049,www.atmos-chem-phys-discuss.net/15/23005/2015/ 2015 doi:10.5194/acpd-15-23005-2015 © Author(s) 2015. CC Attribution 3.0 License. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 3 − ) and/or 3 in 2005 to 1 − gCyear 9 10 × 3.6 ∼ 23008 23007 ), altering the concentrations of hydroxyl radicals, the x in 2010. This study demonstrates that biogenic and, in partic- in 2010 due to the increase in urban greens, while at the same 3 ects on urban air quality. 40 %) to the formation of total secondary organic aerosol (SOA) 1 − ff − ∼ gCyear 9 10 15 %) of the total annual BVOC emissions, and we estimated that the over- × ∼ Plant BVOC emissions are species-specific, whereby the terpenoids isoprene and 7.1 biotic (e.g. herbivores) stresses (Behnke2012; et al., Heiden 2009; et Fäldt al., et 1999,Kleist al., 2003; 2003; et Ghirardo Holopainen et and al., al., Gershenzon,Staudt, 2012; 2010; 2010; Joó Loreto Toome et et and al.,and al., 2011; Schnitzler, 1,8-cineole; 2010). the 2010; For class Mentel of instance,late sesquiterpenes the et (MeSa), (SQT); monoterpenes and benzenoids al., such volatile linalool, lipoxygenase as 2013; ocimene green products methyl salicy- foliage Peñuelas are after typically and exposure induced to andHeiden emitted ozone et from (Behnke al., et 1999; al., Kiendler-Scharret 2009; et Bourtsoukidis al., al., 2013; et 2012; al., Arimura Niinemets, 2012; 2010)respect et or to al., herbivores air 2005; (Amo chemistry, Holopainen SQT and and MeSa Gershenzon, can 2010). significantly Important contribute with to the SOA forma- (Niinemets, 2010) as a“constitutive” function emissions, of significant light,(Niinemets, quantities temperature, 2010) can of and be “stress-induced” seasonality. emitted into In BVOCs the addition atmosphere (sBVOCs) following to abiotic (e.g. O monoterpenes normally dominate theet overall al., BVOC 2013; profile Kesselmeier of andthat woody Staudt, are 1999). plants predominantly Isoprene (Harrison and emitted monoterpenes from are plant volatiles foliage in a “constitutive” (cBVOC) manner 1 Introduction Plants are the(Guenther dominant et source al.,those of 2012). of On biogenic anthropogenic a volatile VOCsreactivity, BVOCs global (AVOCs) organic play by important scale, compounds an roles thesecondary in order (BVOCs) determining organic source of atmospheric aerosol strengths magnitude. processes, (SOA) Due suchpogenic of and as to nitrogen ozone BVOC formation, their oxides exceed or high (NO in the presence of anthro- tial impacts on climate. main atmospheric oxidants (Claeys etGoldstein al., et 2004; al., Ehn 2009; et Pun al.,troposphere, et 2014; BVOCs al., can Fuentes 2002). influence Thus, et the in al., local changing 2000; and the regional oxidative air capacity composition of with the substan- Abstract Trees can significantly impactreactive the biogenic urban air volatile chemistry organicand by compounds particle the (BVOCs), formation. uptake which Here andVOCs) are we emission and involved present of “stress-induced” in the ozone BVOCsplant emission potentials species (sBVOCs) of in from “constitutive” the theand (cB- megacity the dominant of tree broadleaf census, Beijing. woody ticulate we Based matter assessed on the formation an potential intree-planting inventory impact program 2005 of of for and BVOC BVOCs the emissions 2010, onfatty 2008 i.e., secondary acid Olympic before par- Games. derivatives, We and benzenoidstion found after and that ( realizing sesquiterpenes, sBVOCs, such the constitutedall as large a annual significant BVOC frac- budget may have doubled from formation in Beijing. Compared5 to %) AVOCs, for the secondary contribution particulate oficantly matter biogenic in contribute precursors Beijing ( (2– was low. However, sBVOCs can signif- time, the emission of anthropogenicon VOCs our (AVOCs) BVOC could emission be assessment, lowered we by estimated 24 the %. biological Based impact on SOA mass ∼ from biogenic sources; apparently,in their 2005 annual to emission 2.05 increased µgmular, sBVOC from emissions 1.05 µgm contribute toproblems SOA regarding formation in air megacities. qualityNevertheless, However, the the in main present Beijing survey stilllection suggests that of originate in plant from urban species anthropogenicpossible plantation with beneficial activities. programs, e low the cBVOC se- and sBVOC emission potentials have some 5 5 20 25 15 10 10 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , an 3 concentrations x ects on air quality. ff uptake and the deposi- 2 ects on SOA formation range ff e ect plant performance and further x ff 23010 23009 ect and increasing CO ff and AVOCs. However, the possible impacts of BVOC on SOA formation is not fully understood and depends x x ect”, air temperatures in large cities are oftentimes much ff ect of NO ff C) than those that are recorded in surrounding suburban and rural ◦ ratio and specific VOC mixture. NO ect of multiple stress factors, which frequently co-occur in nature, on ff x NO / ect is also associated with higher radiation, increased air pollution levels, and ff er from a chronic multi-stress environment (Calfapietra et al., 2013b). For exam- ff Over the past two decades, large tree-planting programs have been initiated to im- In the present work, we investigated whether BVOC emissions from green areas in tion/detoxification of ozone, NO emissions on ground-level ozone formation andsidered. SOA formation are oftentimes not con- Beijing contribute to the formation21 of million particulate matter. (2013) With and a heavyideal population air of location pollution more for than (Chan assessing andin the Yao, a 2008), megacity. importance Beijing Before represents of theaimed an summer BVOC to Olympic improve emissions the Games from air in qualitythe plants 2008, by number the growing a of large-tree municipality urban plantation of program,were trees Beijing more used, and than shrubs risking doubling (Table high 1).all emissions For of with planting, the progress the strong that cBVOC consequencesthe has emitters year. outlined been Additionally, above. air made, Despite the pollution airinduce may of quality sBVOC negatively emissions, a in which Beijing have ister a still (Mentel high poor et potential throughout al., to 2013; formemissions Bergström organic for particulate et our al., mat- evaluation, 2014). studiednificantly We whether therefore contribute cBVOC also to and considered sBVOC air sBVOC emissionsFor pollution may this and sig- evaluation compared we their conductedwoody contribution broadleaf an to plant extensive species that BVOC of of inventoryplant the AVOCs. of species administrative districts with the of high most Beijing. sBVOC abundant these We emission found potentials emissions. some and We estimated furthermore SOAnomic constructed formation data from a that phylogenetic might tree beurban based of greening” on use (Churkina for the et future taxo- al., planting 2015) programs. has “Picking potential the beneficial right e tree for prove the livelihoods ofis city dwelling increasing residents. in Consequently,2013). the America, Increasing urban Europe the green and urban space including “green Asia decreasing lung” the but by heat most planting island e trees notably results in in China diverse benefits, (Zhao et al., tion even at relatively low concentrationspared due to to the isoprene higher and SOA-forming2008). potential monoterpenes However, despite com- (Mentel their potential etfluxes to al., are influence rarely 2013; ozone considered and Sakulyanontvittaya in SOA etBergström the formation, et context al., sBVOC al., of 2014). atmospheric Both chemistry fieldfactors, (Berg and such et laboratory as al., studies 2013; heat, have shownmation water that limitation, and single stress salinization, change and the2012; ozone, Loreto overall can and BVOC alter Schnitzler, emission sBVOCsless, 2010; for- rates Pellegrini the (Joó et net al., et e sBVOC 2012; al., emission Wu remains 2011; et still Kleist al., poorlyPerennial understood 2015). et plants, (Holopainen Neverthe- al., such and as Gershenzon, trees 2010). su growing in largely populated urbanple, habitats, due constantly to the “heathigher island e (up to 10 areas (Chen et al., 2006;island Peng e et al., 2012). Inmore addition frequent to drought high episodes. temperatures,enhance These the sBVOC heat factors emissions. Furthermore, together because negatively anthropogenic impair NO plants and in urban environments are high,tion BVOC and emissions thus can directly leadet contribute to to enhanced al., ozone formation 2013b; forma- ofet Churkina ozone al., and et 2013). particle The al., matter e on 2015; (Calfapietra BVOC Hellén et al., 2012; Papiez et al., 2009; Wang from the suppression ofor new decrease particle of formation SOAPandis (Wildt et yields et al., (e.g. 1991; al., Kim Presto 2014), et et an al., al., 2005; enhancement Zhang 2012; et Kroll al., et 2012) to al., the 2006; formation of Ng NO et al., 2007; important night time oxidant2011; of Rollins BVOC et with al., considerable 2009). SOA yields (Fry et al., 2009, 5 5 10 15 20 25 10 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | - ffi (1) 40 cm) ) is an 40 ppb, × 40 > ] 3 was calculated 40 for a short period erent branch. Ap- ff 3 (tobacco) were used Gossypium hirsutum (not available in the park) were 40 ppb and unity for [O < (Gray poplar), ] 3 Nicotiana tabacum values exceeding 40 ppb. The sum was de- 23011 23012 3 Salix babylonica canescens data over the threshold value of 40 ppb (AOT h. × · 3 and 40 (tomato), and t ∆ SE) were used as biological replicates. data were continuously collected at an 8 m height from Populus ek and Yakir, 2002; Geron et al., 2006; Harley et al., 1998; ± h to ppm 1 h) from the beginning of July until the end of the sampling ff 3 · 3 and AOT = 3 40ppb) = t n ∆ − ,O ] 3 is zero for hourly averaged [O x , and O erent deciduous and one evergreen woody plant species (see Table 1) 2 ([O max ff Populus tomentosa R max R Solanum lycopersicum = Σ 40 exposure plant index that is set by the US-Environmental Protection Agency and from the trees. Immediately, a second cut of 2–4 cm was done under water to re- ect benzenoid compound emissions neither (Misztal et al., 2015), conversely to in- To take into account the high variability in emission rates, which is due to analytical The accumulated amount of O 3 ff ff 2.2 Climate, NO Climate (light, temperature, precipitation, relative humiditysure), (RH), wind NO, speed, and NO pres- the 325 m-tall meteorologicalAcademy tower of at Sciences, the Beijing. Instituteaveraged into The of daily data Atmospheric means. were Physics, collected Chinese at a 1 h time resolution and approaches (Ortega and Helmig,variability 2007; in Tholl cBVOC et andbacher al., sBVOC et 2006) emissions al., and (Kesselmeier 2015),and intra-species and leaves plant from specific Staudt, averages ( the 1999; same Nieder- plant were treated as technical replicates AOT O the United Nations Economic Commission forusing Europe the (UNECE). following AOT equation: 2 Materials and methods 2.1 Plant material We used 21 di that are commonly found in thepark urban of area of the Beijing. Beijing Treesconditions. were Institute naturally Tree grown age of in ranged the Landscapedetails). between Architecture Only 8 under and ambient 25 years environmental (see Table S6 for age and size The function two-years old, originating from a local plant nursery, and were potted (40 cm in standard soil and grownthree under trees ambient were conditions. independently Twoto fully measured developed for mid-October leaves each in from species 2011.proximately in Each the 30–60 min measured period prior from leafo August to originated from analysis, a healthy di whole plants or branches were cut surements allows measurements underminimizes more foliage controlled perturbation. and This procedure standardlarge is conditions commonly and and used tall when natural accessibility trees to with the cuvette system without branch disturbance is di meaning that the sum only includes O move embolisms and theBVOC branches measurements were (see transferred to Sect. the 2.4). lab Cutting for branches gas-exchange followed and by laboratory mea- experiences, measuring cut brunches dorardo not et alter al., terpene 2011; for Welterin several et hours distant al., (e.g., 2012) Ghi- foliage and (e.g.,They lipoxygenase-derived Ghirardo compound show emissions et that al., exceptted 2011). a from This broadleaf small plant agrees amountlocated. species with of Furthermore, when Loreto acetaldehyde, the a et no mechanical verya wounding al. other recent (cutting) (2006). report VOCs is were showed remotely sect that emit- damaged mechanical plants wounding (Ghirardo do et al., not 2012; Holopainen and Gershenzon, 2010). termined over time ( Helmig et al., 1999; Klinger et al., 1998; Monson et al., 2007). On the basis of own cult or impossible (e.g. A period (beginning of Octoberthen 2011) converted and from for ppb daytime only (6 a.m.–8 p.m.). Values were 2.3 Laboratory study of ozone-induced BVOCThe emissions model plant species (cotton), in the laboratory experiments and exposed to elevated levels of O 5 5 10 15 10 15 25 20 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | C ◦ 0.1 ± erent con- ff concentration of erent concentra- ff 2 PPFD, 30 VOC-free synthetic PPFD, with a cham- 1 ). The net photosyn- 1 − 1 1 − s − − 2 s s − 2 2 0.9997). In addition, a de- − − = for 1–2 h. BVOCs were col- 2 1 , depending on the size of the erent experiments and an RH − R to a final CO 1 ff − )( 2 O analysis using an infra-red gas 1 ). The calibration procedures are 2 1 − − eltrich, Germany; volume 40 mL, sur- ff and H erent BVOCs were achieved by thermo- ff 2 . All of the flows were controlled using mass 1 23014 23013 − C during the di ◦ C for approximately two weeks prior to chemical ◦ -2-carene resolved in hexane at di 20 (standards solvent δ − 1 ; standards solvent − 1 − exposure and were analyzed using GC-MS as described previ- ) that was mixed with pure CO 2 3 -2-carene was added to each sample as an internal standard to take δ . The air exiting the cuvette was diverted into a T-piece, from where 3 L 1 fumigation, plants were allowed to reach steady-state photosynthetic ac- − , 21 % O 3 2 ) after allowing them to acclimate (30–45 min, until photosynthetic gas ex- 2 The identification and quantification of di Prior to O tivities under constant chamber temperature and 800 µmolm ber temperature between 20 and 25 between 50 and 80was %, then depending applied on at the a concentration size of of 8–900 the nmolmol plants and the air flow. Ozone analyzer (IRGA, GFS-3000, Walz GmbH).EUS The (Germany) sample and tubes stored wereanalysis. then at sent to BIOP- desorption (Gerstel) and gas7890A; chromatography-mass MS spectrometry type: (GC-MS; 5975C; both GCviously from described type: Agilent (Ghirardo et Technologies, Palo al., Alto, 2012).sured CA, Each for USA), day, a background as control subtraction. pre- (emptytute cuvette) BVOC was were of mea- identified Standards with and(v.275, the USA) Technology 2011 and Mass National by Spectral comparing Insti- liquid the Library standards retention (NIST, (Sigma-Aldrich). time USA), and Forwas Wiley spectra the diluted library with calibration at those of of finaland isoprene, authentic concentration sampled 10 ppm of in of 10–250 GC-MS ppb,tion standard tubes. curves passed The that through other were thethe obtained volatiles GC-MS whole by were after system, being injecting calibrated diluted pure basedcentrations in liquid hexane on (1–1000 (HPLC-grade, pmolµL standards Sigma-Aldrich) calibra- (Sigma-Aldrich) at di described into elsewhere (Kreuzwieser etstandards were al., calibrated 2014). using Volatiles that were not available as mass flow meter (ADM-3000, Agilentexiting Technologies, Palo the Alto, cuvette USA). was The sub-sampled remaining air for CO tions between 1–1000 pmolµL fined amount of into account the changingrates of MSD BVOC sensitivities were calculated during on each a leaf-area GC-MS basis run. (nmolm The emission thesis and transpiration ratesequations were of calculated von by Caemmerer the and GFS-3000 Farquhar (1981). system based on the of time. Plants wereat placed the individually Institute in ofet continuously Bio- al., stirred 1997) and and tank Geosciences flushedplants). reactors (IBG-2) with Details (CSTR) purified in of air Jülich (15–40 the(Behnke (Mentel Lmin et experimental et al., procedures 2009). al., and 2009; Wildt set-up can be found elsewhere lected continuously by trappingsorbents (Tenax online TA/Carbotrap, Grace-Alltech, at Rottenburg-Hailfingen, Germany) anand for 20 approx. 10 h 76 following min O time resolution on solid The leaf emissionleaves potentials in of BVOCs aexchange were cuvette system determined GFS-3000, system by Walz (standard enclosing GmbH, measuring fully E mature head 3010-S of a portable gas ously (Behnke et al., 2009; Wildt et al., 1997). 2.4 BVOC and gas-exchange analyses face 8 cm Germany) at a flowflow rate controllers (MKS, of Andover, USA) 100 mLmin and the flow rates were verified using a calibrated of air was sampled with(Gerstel, two adsorbents Mülheim in an series der containing Ruhr, polydimethylsiloxane Germany) foam and 50 mg of CarboPack B (Sigma-Aldrich, change became stable) to standard conditions (1000 µmolm air (79 % N 380 µmolmol leaf temperature, 40 % RH). Cuvettes were flushed with 1 Lmin 5 5 10 15 20 25 10 15 25 20 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | - β ) for isoprene 1 concentrations − 3 h 1 − concentration during 2011, C), had been defined to give ◦ 3 is the only plant species that was not cov- 23016 23015 (see Fig. 1). The relative contribution of sMT to 3 concentration (Mid-April to Mid-October). Robinia 3 ), literature estimates of emission factors were used ) and a reference temperature (48 1 concentrations; and (iii) the parameters of the Guenther/Tingey − 3 Robinia pseudoacacia “constitutive” (cBVOCs) Actual emissions were calculated in hourly resolution from daily emission factors (ii) the determinedparallel emission with rates the were O algorithm related describing to storage the emissionrameter temperature beta as (0.12 as K a measured function in of temperature, the scaling pa- for isoprene and light inducedfrom storage monoterpenes were emissions. calculated The using monoterpene aFor phenomenological emissions sBVOC model emissions, (Guenther we et applied al.,ally 1995). the used temperature-dependent to equation describe that emissionstion is from have gener- been storage modified structures. to The reflectas parameters the of described response this of in SQT equa- emissionssponse Bourtsoukidis to was O et described al., in 2012 response in to the the following measured way: O (i) the emission re- the least overall deviation2012, method. from All the of values thescaled emissions determined to the that with whole were city the determinedtree of per Bourtsoukidis number Beijing gram per by et of species, multiplying dry corrected al., withderived by weight the from phenological were leaf measured development. biomass diameters The per usingsidering leaf tree the a biomass and equation species-specific is the from shading Nowak factor for (Nowak,described 1996). urban by Phenological trees an development con- is empiricalof function based seven on dominant repeated treeno leaf species emission area rates (Fig. index were measurements S2,ble available in (another 1 the 12 plus tree Supplement). and For shrub species species for are which listed in Ta- (Table S5B, in theered Supplement). by the currentin inventory, Beijing although in it 2002 was (Yangcreased one et it al., of for 2005). 2010 the We by most used the abundant the factor of tree given 2.45 tree species (the number average for increase 2005 of and all in- other species). For non-induced monoterpene emissions fall into thiset fraction al., (Ghirardo et 2014). al., 2010; Forduring Harley all the period stress-induced of BVOCs substantial we O assumed a constant emission factor ocimene, linalool and 1,8-cineol (sMT), allgreen sesquiterpenes leaves (SQT), volatiles benzenoids (GLV) (BZ) while and pene constitutive isoprene BVOCs (cBVOC) (IS) included andincluded the hemiter- all as constitutively sMT emitted (Tablethe S1, monoterpenes BVOC in (cMT) emission the pattern thatplant Supplement). that were models This that was not were classification obtained exposedthe fully in to overall agreed O the MT with laboratory emissionand study was 4. using However, small; we the considered thus the four formation the sMT potentials, separately sMT for multivariate and sBVOC analysis emission cMTsBVOCs and scaling, vs. were SOA- when total combined calculating BVOCs (see in the sections Fig. overall below). fraction 3 of 2.6 BVOC emission budget The measured potentialchanges in emission enzyme rates activitieslight, in for as relation calculated isoprene to withDepending were the the on annual “Seasonal-Isoprenoid-Model” corrected the fluctuation SIM calculated for of (Lehningleaf activity temperature mass et seasonal for and per al., the area 2001). date (LMA), of the potential measurement emission and factors the (gCgDW measured 2.5 Classification of BVOCs into “stress-induced” (sBVOCs) and The classification of volatilesview as of “stress-induced” and/or Niinemets “constitutive” (2010)literature followed and the search was re- (Beauchamp based on et2012; the al., Fäldt et generalized 2005; al., findings Behnke 2003; of2003; et Ghirardo an Holopainen et al., extensive al., and 2010; 2012; Gershenzon, Hakola Bourtsoukidiset 2010; et al., et Joó al., 2010). et Stress-induced al., 2006; BVOCs al., Heiden included et 2011; the al., Pinto stress-induced 1999, monoterpenes et (E)- al., 2010; Toome were derived (Table S5A, independent the monoterpene Supplement). emission Similarly, thesuming (i.e. emission that de factors for deciduous novo for species light- biosynthesis) all were and for determined, evergreen species as- half, of the measured 5 5 10 15 20 25 10 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ) ), A Weigela (Kiendler- ), centered | 1 ) − and X 0.03, Hamilton ∼ ), we obtained the log( | τ · = Q ) for particulate organic 0.02 µgµg X = Q = C ( τ ). The height of the box was 2 ect of GLV on particle mass formation and lifetime 1 %). At such low levels, the suppressing ff Q < Jasminum, Kerria, Sorbaria, 23017 23018 0.06 (Mentel et al., 2009), benzenoids and SQT = erent VOC classes (Mentel et al., 2013). Accounting for ff , source strengths as data pre-processing. In addition, the phylogenetic data were C 1 ’ variables, logarithmically transformed ( − X ect of suppression of new particle formation by isoprene (Kiendler- ff 2 year, these numbers were multiplied by 2 to obtain the average emis- / 1 ∼ ect is marginal (Mentel et al., 2013). A potential contribution of GLVs to particle mass Average flux densities for VOCs were obtained from the data given in Table 2 by divid- To obtain the mass of organic matter on particles originating from BVOCs, we as- As postulates for this procedure, we assumed that (i) the load of particulate matter in 0.22 (Mentel et al., 2013)) to obtain the source strengths for particulate matter. ff sions over a day. Thewere results then for the multiplied average by flux the densities over particle the mass vegetation period yields (isoprene ing the total annual emissionsperiod by of the surface area of Beijing. Considering a vegetation and scaled with 1 SD mass. rics, Umeå, Sweden).scribed This (Ghirardo analysis et conceptuallyof al., follows the BVOC 2012; groups method Kreuzwieser (i.e., previously et de- IS, al., cMT, 2014), sMT, where SQT, the BZ, emission GLV) rates andnumerically converted the (Table assimilation S8,“full rates in cross ( validation” the and Supplement). significant at The the results 95 % were2.8 confidence validated level. by SOA- formation potentials from biogenicFor and estimates anthropogenic VOC of SOA-formationwas potentials equal we defined to a the box area with of a surface the area city that of Beijing (1434 km anthropogenic VOCs entering the volumethat of was the determined box for were the multiplied di by the mass yield Scharr et al., 2012), monoterpenes The taxonomic data oflogenetic the 22 tree woody using species the2011) analyzed web (Table were S7). tool used The iTOL torates correlation generate) (http://itol.embl.de/ (Table S2) a between (Letunic and phy- plant-specific and taxonomic BVOCsis data Bork, were (PCA) profiles, 2006, evaluated statistical assimilation using methods principal from component the analy- software package “SIMCA-P” (v13.0.0.0, Umet- the height of the assumed box,particle the mass transformation enabled of the the estimation flux of density the from source VOC strengths mass ( to we used an average emission(Table factor S5B, that in was the derived from Supplement).isoprene all Because and of constitutive literature the monoterpene values deciduous emissions,measured could shrubs a emissions only and ratio be those was based obtained calculated onfrom between for literature the total”). values (Table All 2: “percent ofthe measured the total induced emissions. However, sBVOCwere the emissions between percentages increased 84 of and by measured 96covered this %, in emissions indicating ratio this over that analysis to the (see the estimate also total majority Table of 2). emissions2.7 were likely to Phylogenetic be tree, multivariate data and statistical analyses were used as the ‘ fixed to 2 km, as a typical proxy for the height of an inversion layer. The biogenic or sumed that the atmospheric lifetime ofbetween concentration particles is approx. 4 days. With the relationship Scharr et al., 2009). (ii) The suppressing e = neglecting the e (Mentel et al., 2013) isand negligible. even GLVs less contribute to to thee 6 total % VOC of emissions the ( totalformation BVOC was emissions also neglected becauseet the al., mass 2009). yields are (iii)independent also All of low each other ( other, VOC i.e.,nation contributions the of total to individual SOA SOA contributions mass from formation can AVOC were be and described BVOC. assumed as to linear be combi- data listed in Tables S3–S4. the air of Beijing isportant high, compared and to hence, the nucleation addition of and organic new matter particle to formation the are existing not particles. im- This allows species with no known emission factors ( 5 5 20 15 10 10 25 25 15 20 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | and x (based . 1 3 − s 2 − erent plant ff Sophora japon- Populus tomen- fumigation under and average rates Berberis thunbergii 3 1 − s 2 (Lu et al., 2013) and the − 3 (Sb) and − (Pa) and ; these species are thus classified as 1 ) were measured for the cBVOC iso- − acerifolia 1 moleculecm s − × 6 s 2 − 2 10 − Salix babylonica × exposure, and their emission strengths were 23020 23019 values (the accumulated amount of ozone over 3 exposure (Fig. 1b). The emissions of sBVOC ap- Platanus 40 3 data indicated that plant leaves may have frequently ). BZ, GLV and SQTs were emitted at rates that were 3 (Ej), 1 − s . 3 2 − − cients (Atkinson, 1990). The SOA yields were taken from the ) were also observed from the plant species 24 h after O 1 ffi − flux density into the plant foliage (data not shown), which agrees 1 s − 3 (Fig. 1a). In contrast, sBVOCs were apparent when plants expe- 2 s − 2 1 − − s 2 − stress, reaching emission rates of up to 50 nmolm stress for the entire summer period. 3 3 Euonymus japonicus h), relatively constant AOT · models (Pt), two well-known strong isoprene-emitters. Significant isoprene emission rates levels (Fig. 2a–c). The ozone concentrations measured at an 8 m height from (Sj), We analyzed the BVOC emission potentials (“standard emission factors”) of the most To compare the contribution of BVOC to AVOC emissions to the organic particu- Importantly, we detected a diverse chemical spectrum of sBVOCs from most of the 3 recent study by Emanuelsson etconcentration al., of 2013, 10 corresponding µgCm to 0.14 at an organic aerosol 3 Results 3.1 Laboratory study of stress-induced BVOC emissions from di corresponding rate coe To classify plant BVOC emissions(Table into the S1, categories “constitutive” in ormodel “stress-induced” the plants Supplement), (poplar, we cotton, analyzed tomato, the and leaf tobacco) BVOC following emissions O from four controlled conditions inchamber continuously (Mentel stirred et tankemission al., reactors 2009; of (CSTR) Wildt sBVOCsvolatiles et inside such (GLVs) and al., a some as 1997). monoterpenes, climate was benzenoidssions Under negligible. The (BZ), from unstressed sum unstressed sesquiterpenes of conditions, all plants the sBVOC (SQT), emis- was green consistently leaf lower than 0.05 nmolm rienced O on the projected0.005 leaf nmolm area) in any model plant,of ca. and 3.3 nmolm the averages were asdependent low on as the O peared directly following pulses of O well with previous studies (Beauchamp et al., 2005; Behnke et al., 2009). Together, the 325 m-tall meteorological towerAcademy at of the Sciences Institute of (IAP-CAS)maxima Atmospheric of were Physics 60–100 from ppb. – 10–40 The Chinese ppb O (daily mean), reaching daily 3.2 Urban trees in Beijing releaseDuring large the quantities measurement of campaign stress-induced inwarm BVOCs Beijing and (August–October 2011), characterized the by climateO relatively was high light intensities, air temperatures, NO experienced oxidative stress during summer,40 but ppm more importantly, the high (from 30– the threshold value ofchronic O 40 ppb) suggest that all ofabundant the urban woody plants broadleaf wereand tree exposed Table species to 1), coveringBVOC observing the emission urban potentials highly area (20–35 plant nmolm of species-specific Beijing BVOC (Fig. profiles. 3 The highest (Bt). As notable monoterpene-emittinging plant a BVOC species, potential we of detected approx. 3–5 Ej nmolm and Bt, exhibit- these data suggest thatgreen foliage sBVOCs under are unstressed virtuallylarge conditions; amounts however, absent they following from acute can stress be the episodes, induced volatile here in simulated fingerprint relatively by applying of O both isoprene- and monoterpene-emitting species. woody broadleaf planthigh species rates (Fig. (0.1–10 nmolm 3a–c), which were also emitted at significantly prene originating fromtosa the tree species (range 3–5 nmolm ica late matter, we used benzene,pounds. toluene The and source xylenes strengths data forthe as benzene, ambient main toluene summer anthropogenic and measurements com- xylenesusing at were an an calculated average urban from OH background concentration site of (Wang 5 et al., 2015) 5 5 10 15 25 20 10 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , 1 − (Pp), Berberis Sophora sBVOCs). (Kp) were gCyear 9 + (Ej), Berberis thun- 10 (Sb), the contri- Populus tomen- × assimilation rates 2 Prunus persica ), accounting for 63– to 7.1 9 (Aa), 10 (Sb) (Fig. 5). × Euonymus Salix babylonica Koelreuteria paniculata Euonymus japonicus and Kp, from the respective families (13 %). The total annual BVOC emission (Ms), (Pt) and (Pa) and Salix babylonica Ailanthus altissima Salix 23022 23021 ected the total BVOC budgets, we based our calcula- (Pc) and acerifolia ff × Ailanthus altissima (26 %), and Malus spectabilis (Pt and Sb) from the family Salicaceae (Fig. 5, depicted in Populus tomentosa , as member of the family Ginkgoaceae is not closely related Platanus Sophora and Pa showed a much weaker correlation with cBVOC emissions. ) and monoterpenes (dominated by (Gb), Prunus cerasifera Salix (38 %), (Bt), followed by Ginkgo biloba Salix babylonica (Sj), and belongs to the family Berberidaceae, evolving from the stem Eudicotyledons. taxa and We also observed that the tree species 100–1000 times higher than those that were detected from unstressed plants in lab- 65 % and 21–22 %significantly of contributed the to total the BVOC, overall respectively BVOCEuonymus (Table budget 2). (15–16 %), Importantly, originating the mainly sBVOCs from might have therefore doubled from 2005 to 2010 (from 3.6 tosa tions on the tree inventories ofof 2005 the and year 2010 and whenis used the in independent measurements each from case were the climate performedment). weather condition (2011), data Overall (Table the so 2, total that Fig.Populus BVOC the S1 emissions comparison and were always Table S3, dominated in by isoprene the (mainly Supple- cyan). 3.4 BVOC emissions in Beijing beforeTo and understand how after increases the in 2008 the Olympics greening area the of Beijing Olympic in Games the have years before a and follow- not correlated with sBVOCs,or indicating low-emitters that of these sBVOCs. Simaroubaceae species and can Sapindaceae, belong be toin classified the white). as order of non- Sapindalesto (Fig. any 5, other depicted plant speciesTable S2, (yellow). Isoprene in emission the (and Supplement) net was strongly CO correlated with the species Ginkgo biloba see Table 1–2) as a consequenceimpacts of of the plant increased stress number onplant of the stress trees, sBVOC in emissions assuming 2010. in that 2005 the were similar to the impacts of the clade Asterids (Fig.green) 5, were low-to-moderate depicted sBVOCs in emitters and orange) low-to-moderate and cBVOC from emitters. the family Magnoliaceae (in ∼ oratory studies (Fig. 1),sBVOCs were clearly emitted from indicating plants plantprofile in stress. Beijing based compared We on to estimated the eachVOCs dominated plant’s to classification specific the what from cBVOC overall emission extent theof profile laboratory 83 for %; two-thirds survey. Fig. of The the 4b,were proportion species GLV see compounds (mean of black (Fig. value points). sB- 4b),cBVOC The followed emitters, by major such BZ as contributors and to SQT the compounds. Even fraction for of strong sBVOCs The PCA further indicated that the plant species that were phylogenetically related to Sophora japonica bergii In contrast, Ms, Ej,Eudicotyledons Sj, throughout Gunneridae/Pentapetalae/Rosids Pc (Fig. and 5,Thus, depicted Sb, it in all appears blue). that members the ofBt, trait Ej to the and emit Fabids Sb sBVOCs is clade, werecan phylogenetically also originated related. correlated be Furthermore, from with generally cBVOC emissions, classified indicating that as both overall species strong BVOC emitters (cBVOCs bution of sBVOCs to theof total the BVOC total budget moles was of significant, BVOC,of respectively. accounting Together, the the for BVOC plant 7 profiles species and suggest that that 20contribution % most are of found sBVOCs in is a Beijing significantare grow fraction under emitted of stress in the conditions the total and air amount that of of plant the Beijing. volatiles that 3.3 The stress-induced BVOC response is phylogenetically related to plant We further examined correlationsing between a BVOC principal emissiontionships. component rates The analysis and most (PCA), plant positivelythunbergii aiming taxa correlated plant us- to species analyze tojaponica the emit phylogenetic sBVOCs rela- was 5 5 20 10 15 25 25 20 10 15 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 2 ∼ erent bio- ff 83 %) of two- 40 %) (Fig. 6a ∼ fumigation. The ∼ 3 ) to significantly elevated 1 − s 2 − 23023 23024 erent model plant species via O ff ) following stress. The emission rates are quite similar between 1 − s 2 − 4 % in 2010 (Fig. 6c). as an abiotic stressor by generating an oxidative burst is a common pro- ∼ 3 emissions The estimated average SOA mass formation from all of the BVOCs was approx. The sBVOCs are biosynthetically formed in response to stress from di to exist in nature(Table (reviewed S1, in in Niinemets, the 2010). Supplement) Theoretically,pending are stress-induced on elicited BVOCs the after severity of exceedingvalidated the a this stress, stress are threshold concept emitted and, utilizing in de- relatively di large amounts. We have use of O cedure in plant sciencewounding and (Heiden mimics plant et responses al.,2005; following 2003). pathogen Behnke In attack et accordance or with al.,the leaf other 2009; degree studies Heiden of (Beauchamp et sBVOCunder et al., emissions unstressed al., 1999, (or can plant-optimal) 2003), change conditions these dramatically (pmolm data from demonstrate negligible that emissions VOCs constituted a considerable portion of the total biogenic SOA ( 1.05 µg in 2005 and 2.05 µg in 2010, respectively. The SOA production rates from sB- 3.5 Impacts of stress-induced BVOCs onBased SOA formation on in the the annual airof BVOC of BVOC budget Beijing emissions calculation, for wetion secondary analyzed via aerosol the anthropogenic (SOA) putative formation VOCs importance the (AVOCs). compared We contribution to were of SOA particularly forma- sBVOCsmated interested to the in potential the contribution quantifying overall of biogenic cBVOC,mass sBVOC SOA-formation in and AVOC the potential. emissions air to We the forprograms esti- particle 2005 (Fig. and 6a 2010, and i.e. Table S3, before in and the after Supplement). the realized large-tree planting Plants are constantlyenvironments, exposed including to heat, a wind,bial variety attacks. intensive of As sun such, abiotic light, unstressed and and trees biotic growing herbivorous under stresses and optimal in micro- conditions natural are unlikely emissions (nmolm laboratory-grown plants that are grownappears that in sBVOC the emissions dominated urban the environment overall emission of pattern Beijing. ( Overall, it 4.1 Multiple urban stresses cause strong taxa-related stress-induced BVOC and Table S3). Therefore,62 neglecting % lower the estimates of sBVOC organicBeijing, emissions particulate respectively, for would matter 2005 originating lead and fromorganic to 2010. biogenic sources aerosol The a in AVOCs production 64 were (Fig. the and accounts 6b dominant for precursors and less of than Table S4), 5emissions % where increased of between SOA the 2005 total formation and (Fig. 2010, viaThe while 6c contribution BVOCs in and of contrast, Table the S4). VOCs AVOCs from Nevertheless, decreased. in the biogenic 2005 BVOC sources to to SOA formation increased from 4 Discussion thirds of the analyzed species,to indicating severe levels that of plants multiple in stresses,2013b). Beijing typically Thus, are of commonly urban it environments exposed isand (Calfapietra et their imperative al., impact that on future chemical processes research in also the considers troposphere. chemical sBVOC pathways emissions (Laothawornkitkul etplants. al., Green 2009) leaf that volatiles originate areduces from commonly oxylipins (i.e., the found jasmonic lipoxygenase in acid (LOX) derivatives) green age, pathway, as which a fatty pro- defense acids response. Upon thatzymes leaf are dam- and are stored partially inmate converted the pathway, into and lipids GLV. the Benzenoids become are mostsignaling available common produced (e.g., substrate BZ from Liu for methyl the et salicylate LOX shiki- al.,spectively, is from en- 2011). required the The for cytosolic volatile plant-stress isoprenoids mevalonate(MEP) and SQTs pathways, and the and MTs plastidic both originate, methylerythritolsects classes re- phosphate (e.g., are Ghirardo crucial etduction infochemicals al., of between 2012). sBVOCs plants require Although further and the examination, in- exact oxidative mechanisms stress generally leading causes to dra- the in- 5 5 10 25 10 15 20 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 3 erent ff ect, the use of purified ff erent plant species under stress can ff 23026 23025 for the actual production pathwaysemissions (Grote of isoprene et and al., monoterpene 2013). might(Behnke also et Fourth, increase al., the under 2009; constitutive stressed Blande conditions et BVOC xylenes al., have 2007; been Niinemets, 2010). assumed Fifth, toa toluene, originate benzene very and solely recent from study anthropogenic sources, supports although biogenic sources (Misztal et al., 2015). Sixth, emission synthetic air in combination withdeterminating an the real enclosure plant cuvette species-specific measurementup, sBVOC was emission many potential. essential species Using for this that set- to are their commonly “constitutive” classified emissionnificant as emission potentials) “non-emitting rates. actually species” Thus, emit (according “non-emitting” our several traditional BVOC view hydrocarbons species of at –potentials classifying sig- based plants – as only should “emitting” on bemodels or revised. isoprene (i.e., The and MEGAN implementation and monoterpeneoverall of BEIS) BVOC emission sBVOCs emissions. paves the into way BVOC for emission a more4.3 realistic representation of Modeling BVOCs A number of constraints andeling uncertainties and should measuring be approaches. noted First, thattions phenological are in development related and emission to seasonal factors the varia- have mod- tion. been This lumped grouping for was all necessaryof deciduous because species all measuring in plant the this species BVOCinstantaneous investiga- emission weather was conditions potentials not and continuous feasible.emissions seasonal Second, development, occurring for we instance, during neglected2012). budbreak any Third, (Aalto impacts we et other usedtion, al., than the although 2014) conventional the calculation or underlying methods assumptions flowering for of (Baghi emission these et algorithms determina- al., might be very di and/or other reactive oxygenready species be (i.e., oxidized before OH being radicals), detected. With and respect sBVOCs to might this thus e al- that of cBVOCs (Bergström etVOCs al., such 2014; as Mentel et SQT al., in 2013). ambient However, measuring air sB- is challenging due to their high reactivity with O emit a large spectrumwhich and in turn high can amounts potentiallyported of influence air very stress-induced quality recently VOCs in that (Niinemets, urbanare sBVOCs environments. 2010), compose It emitted has a into been substantial re- the partronmental atmosphere conditions of and is the urgently that total needed their BVOCs2009; (Bergström that Guenther, quantification et 2013; in al., Mentel 2014; et dependenceshown Bouvier-Brown al., on et that 2013). envi- al., Online significant above-canopy amounts measurementsexist of have benzenoids in (e.g., the MeSa), atmospherefrom SQT products, biogenic (e.g., and sources Karl GLVs have etpogenic been sources al., estimated (Misztal to 2008). et be al., Verycompounds in 2015). recently, has the Moreover, global increased the same as scientific BZ range itnificant interest emissions as has in roles from been BZ in shown anthro- and that SQT SOA these formation compounds due may play to sig- their higher formation potential compared to The present study supports the hypothesis that di matic changes in the chemical-physical propertiesKanchiswamy of et the plant al., cell 2015) (Arimura and etVOC al., can emissions 2011; therefore (within activate minutes enzymes toof that hours) the are following related gene respective to activation proteinsplant sB- and species, (hours the but translation to the days).(Fig. emission 5). Thus, strengths Because sBVOCs the (rarely can sBVOCsome investigated) emission plant be are families potentials activated might plant-taxa-specific are be in genus-ing more most and area. suitable While species-dependent, than comparison others with foranalysis literature expanding of is the not cBVOCs urban agrees possible green- for wellfamily sBVOCs, with the Salicaceae previous phylogenetic studies, and indicating Fagaceae thatspecies are species within from strong the the cBVOC emitters,VOCs Oleaceae (Benjamin in and et contrast al., Rosaceae to 1996;to families, the Karlik maintain which plant et plant al., are fitness 2002).stress non-emitters Whether in conditions these of remains the cBVOCs to cB- analyzed are be tree needed elucidated. species and4.2 to cope with The severe importance urban of measuring stress-induced BVOC emissions 5 5 25 10 15 20 20 25 10 15 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ects, increase ff erent biogenic and anthropogenic VOC ff orts (e.g., “the million tree-planting”) have ff 23027 23028 . This is somewhat less than the mass loading in ort to reduce urban heat island e 3 , e.g. Sun et al., 2010) but still in a realistic range ff − 3 formation potential of sBVOC such as BZs or some − 3 stress) cover only a small range of species and are quite 3 20–200 µgm ∼ ort to improve air quality issues. This initiative more than doubled the number of ff erent in magnitude (Calfapietra et al., 2013a). Taken together, considerable uncer- In the present analysis, we investigated some impacts of a large greening initiative, The yields used here for the formation of organic SOA mass from the oxidation of ff an e trees between 2005 and 2010of in fast Beijing growth species and selectionsion previous and experiences potentials. was on performed Using in development thewith favor rather tree our than coverage BVOC on emission before BVOCsions survey, and emis- we on after quantified the this the air activitythe impact ozone- quality in of and in the combination SOA-formation Beijing. potentials altered of Theoretically, BVOC di this emis- impact can be characterized as emissions. However, neither the O thus been initiated worldwide in an e SQT nor the partitioning ofor their pre-existing oxidation particulate products matter in areperimental pre-existing well data matter characterized. and of Due in high to absence mass mation, the of we a present use model lack the that in results exactly ex- for of considers a recent all rough laboratory facets estimate experiments of (Mentel of SOAsured et for- SOA the al., formation SOA 2009, formation from 2013) potentials BVOC of infor constitutive masses Beijing. and in stress-induced Mentel the BVOC et range emissions of al.,the 8–40 2013 µgm air mea- over Beijing ( 4.4 Impacts of the enlargement ofAir urban pollution greening in is Beijing costlylost work to days, human health problems healthagricultural and and yields. hospital Large-scale well-being, costs, damage greening resulting to e in buildings, and premature reduced death, namely the tree plantation action that occurred before the summer 2008 Olympics, in potentials of constitutive BVOCs based onthan cut those plants/branches may from be uncut somehow1999; lower branches Ghirardo due et to al., disturbancemation 2011). in of Consequently carbon those to allocation stress-related pointstive (Funk BVOC 4th–6th, importance et in the of al., possible the biogeniclarger. underesti- emissions, actual Seventh, compared analysis other to may BVOCs anthropogenic,non-specific mean other might storages that actually than or the be terpenes be rela- A might synthetized specific originate de emission novo from function underserved specific responses stress for and (i.e., (Iriti sBVOC to and has O Faoro, not 2009). yet beentainties reported about because the the absoluteincreasing ob- BVOC knowledge estimates about are productionThis apparent estimate pathways and is, and may however, environmentaltance conservative, be dependencies. making of reduced it the with more sBVOCBeijing likely over has that cBVOC been the underestimated and rather relative biogenic than impor- vs. overvalued. anthropogenic VOC emissions in carbon sequestration, remove pollutants,the increase aesthetic space value of for cities recreation, (McPhersonurban and et green al., increase area 2011; Morani by et plantingHowever, al., while trees 2011). the improves Enlarging air benefits the quality ofterms by planting of actively trees the removing are pollution. contribution clear,into the of account possible BVOCs) (Churkina disadvantages of et (in planting al., 2015). the “wrong trees” are often not taken di for moderately polluted atmospheres. Furthermore,formation from a sBVOC model emissions study demonstrated that implementingcontribute these to SOA emissions the can formation substantially ofet particulate al., organic 2014). matter Our on calculations apotential for regional the originating scale megacity (Bergström from Beijing revealed BVOCthat that sources the the might SOA-formation contribution have of sBVOC doubled emission from to 2005 SOA to formation fromBVOC 2010 BVOC were and is determined substantial. for conditionsparable to where that the of surface moderately of pollutedmass particulate atmospheres formation but matter from less is the than oxidation com- mass that of in of volatile megacities. organic pre-existing As compounds matterof also (Odum BVOC depends Jay on to et the SOAabove. al., mass 1996; formation Pankow, in 1994), Beijing the may contribution be somewhat higher than estimated 5 5 10 15 15 25 10 20 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , and x ). This 1 − , NO 3 Ailanthus al- -caryophyllene β cient way to optimize ffi 23030 23029 ectively removes pollutants such as O ff in 2010). 3 (Guo et al., 2012) compared with our estimation of − ), the carbon reduction in terms of BVOCs would have been from xylenes). Despite the likely overestimation, the atmo- 3 3 − − (Table 2), equivalent to 1.5 million cars (assuming 115 mg AVOC The authors thank Amy Trowbridge for critical reading the manuscript and 1 − 0.18 µgm ± for the sum of all SQT and for BZ. Thus, the extent of SOA production (Ho et al., 2009) and the typical car being driven 20 000 km year Prunus persica 3 1 − gCyear − 9 and car 10 1 × − orts to reduce anthropogenic pollution in the megacity of Beijing were generally suc- ects arising from BVOC emissions. The landscape planning of megacity urban ar- While BVOC emissions from plants still contribute only to a minor amount of the Another way to visualize the relevance of BVOC emissions in urban air chemistry The SOA production from the sBVOCs as estimated here agrees with recent esti- Nevertheless, in the heavily polluted area of Beijing the relative importance of or- ff ff 5 Conclusion E cessful and ledless, to pollution a in reduction thisalthough of megacity the is AVOC vegetated still of areaareas doubled dominated 25–30 % from by in 2005 from anthropogenic megacities to trace 2005 doestrast, 2010. compounds, considering Hence, not to that a lead 2010. vegetation plantation to e Neverthe- of an large unacceptable increase in pollution. In con- VOC load in Beijing, decreasingof anthropogenic BVOCs. pollution The may more increasebution successful the of importance AVOC emissions BVOCs will are be. reduced, However, the there higher is the an contri- easy and cost-e The Supplement related to thisdoi:10.5194/acpd-15-23005-2015-supplement. article is available online at Acknowledgements. the Helmholtz-CAS joint laboratoryunder project predicted ENvironmental climate TRANsition change of (ENTRANCE). China’s Ecosystems formaldehyde, from the atmosphere, a plantationadvantages. of large areas in megacities has many e eas should consider the species-specific“stress-induced” emission BVOCs potentials to of mitigate the bothscale BVOC “constitutive” load tree and in planting urban operations areas. shouldand In choose “stress-induced” particular, non-emitting BVOCs. large- We plants conclude ofing” that both (Churkina “picking “constitutive” the et right al., treeof 2015) for megacities. has urban potentially green- beneficial consequences on the air quality is to compare theming with that anthropogenic the car2010 emissions enlargement was (Curtis hypothetically of managed et using the al., only urban 2014). “non-emitting Suppos- plants” vegetation (e.g., cover in Beijing from 2005 and more SOA from tolueneservation than on from toluene SQT being and aever, BZ). the major This precursor relative is of importance further Beijingbecause of supported SOA anthropogenic stress-induced by pollution (Guo the decreased BSOA et and ob- al., increased, the 2012). from vegetated How- 2005 area was to increased. 2010, tissima 3.5 km comparison is rather conservativeare because less it reactive does thanSOA not than BVOCs, consider can i.e., the AVOC vehicles. in fact the that same AVOCs amount, BVOCs can produce more spheric concentrations of particulate organicare matter by from far anthropogenic larger VOC than sources those that can be derived from BVOC emission (e.g., 17 times count for less thanmade 10 %. for anthropogenic However, it VOCs seem should to(i.e., be result more noted in than that an unrealistically 30 our µgm high simplified SOA assumptions production mations using a tracer method in which the0.78 µgm contribution of therates SQT derived from sBVOC emissionstions in this of work BVOC agrees tracers withto and the the could observed BSOA concentra- contribute (total to 2.05 µgm a considerable portion ofganic approx. SOA 40 mass % from BVOCCompared oxidation is to still SOA rather potential small, at from least anthropogenic on VOC an annual sources, basis. it is estimated to ac- yielded 0.21 5 5 10 25 15 20 20 25 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ) clones under am- tremuloides × Populus tremula 23032 23031 and air pollution, in: Biology, Controls and Models of Tree 2 Hartz, K. E., Hallar, A. G., Meddens, A. J. H., Hicke, J. A., Lamar- ff ek, H. P.and Yakir, D.: Protection by isoprene against singlet oxygen in leaves, Plant Physiol., que, J.-F., and Tilmes, S.: Theand impact secondary of organic bark aerosol beetle13, infestations formation 3149–3161, on doi:10.5194/acp-13-3149-2013, in monoterpene 2013. western emissions North America, Atmos.icant Chem. Phys., contributor todoi:10.5194/acp-14-13643-2014, organic 2014. aerosol in Europe?, Atmos. 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Phys., 14, 2789– x Pissard Plum 20.01 37.92 quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic and its hybrid quality for 2008 the Olympic quality for 2008 the Olympic quality for 2008 the Olympic mann, T., Andres, S., Ehn, M., Kleist, E., Müs- ff Laxm. Golden Rain Tree 17.64 31.10 x tulipikera Chinese Tulip Tree 0.25 0.4 n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and of area 2010 in urban the n 2005 and of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and n 2005 and 2010 in the urban area of of area 2010 in urban the n 2005 and Thunb. 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Winter Jasmine 97.45 194.73 (L.) Franco Chinese Arborvitae 142.324 471.26 (Thunb.) Vahl Weeping Forsythia 64.93 168.61 L. Crape Myrtle 35.85 57.24 Carr. Chinese White Poplar 125.75 201.96 (Ait) Willd. London Plane 7.62 23.43 DC. Japanese Barberry 154.45 82.77 Rupr. Broad-leaved Lilac 32.64 76.01 (Mill.) Swingle Tree of Heaven 15.77 22.69 Desr. Yulan Magnolia 7.89 14.05 23041 23042 Carr. Wax Leaf Privet 139.71 267.26 (L.) Antoine Chinese Juniper 118.114 257.14 Carr. Chinese Pine 58.14 129.28 Ehrh. L. Japanese Pagoda Tree 80.38 192.98 (Ait) Borkh. Chinese Flowering Crabapple 9.10 40.3076 s Oliv. Hardy Rubber Tree 4.32 9.51 Torr. Velvet Ash 22.84 63.88 (Rupr.) Maxim. Amur Honeysuckle 21.86 62.93 Sieb.et Zucc var. Korean Box 169.66 257.23 L. Weeping Willow 101.24 260.20 Durazz. Silk Tree 4.24 6.88 (Regel) Maxim. False Spirea 28.54 52.07 Nakai Korean Spruce 3.76 7.51 cv. Duplex Flowering Peach 20.02 47.99 Zucc.ex Endl. Lacebark Pine 9.24 28.34 (Roxb.) G.Don Himalayan Cedar 12.72 37.86 C.A.Mey. Manchurian Catalpa 1.07 10.07 L.f. Japanese Persimmon 9.59 12.63 Ant. Savin Juniper 327.93 808.80 Bunge Shantung Maple 15.65 26.79 L. Maidenhair Tree 46.34 166.02 (L.) DC. Corchorus 58.35 140.38 L. Siberian Elm 18.94 43.82 Lindl. Flowering Almond 20.73 46.11 L. Tatarian Dogwood 24.51 78.16 acerifolia × Nakai florida (Bunge) A. DC. Old-fashioned Weigela 10.67 52.73 to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air to improve environment air

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Sorbaria kirilowii Lagerstroemia indica Acer truncatum Sabina vulgaris Buxus microphylla koreana Kerria japonica Weigela Jasminum nudiflorum Prunus triloba Picea koraiensis Eucommia ulmoide Albizia julibrissin cv. “Atropurpurea” Cornus alba Juniperus chinensis Cedrus deodara Pinus tabulaeformis Platycladus orientalis Pinus bungeana level, relative humidity and aerosol acidity, Environ. Chem., 9,

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Quercus suber Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody

Tables Tables Table 1 plant species found of i abundance Absolute woody Table 1 plant species found of i abundance Absolute woody Games. Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the I city. Beijing 2005 between 2010and in order text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody

Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody

Tables Table 1 plant species found of i abundance Absolute woody Tables Table 1 plant species found of i abundance Absolute woody Games. Games. Games. Tables Table 1 plant species found of i abundance Absolute woody I city. Beijing I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order 2005 between 2010and in order I city. Beijing of based in on space the inventory censusgreen Beijing data from 2005 and 2010. of based in on space the inventory censusgreen Beijing data from 2005 and 2010. text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody

Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody Tables Table 1 Tables plant species found of i abundance Absolute woody Table 1 plant species found of i abundance Absolute woody Games. Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the of based in on space the inventory censusgreen Beijing data from 2005 and 2010. 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Games. Tables Table 1 plant species found of i abundance Absolute woody I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Games. Tables Table 1 plant species found of i abundance Absolute woody I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Games. Games. Beijing city. I city. Beijing Tables text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order Table 1 plant species found of i abundance Absolute woody of based in on space the inventory censusgreen Beijing data from 2005 and 2010. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody

Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody

Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Games. Games. Games. Tables Table 1 I city. Beijing plant species found of i abundance Absolute woody text for each species. thus trees increased and vegetation The of was cover number urban the I city. Beijing 2005 between 2010and in order I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 Tables plant species found of i abundance Absolute woody Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Games. Tables Table 1 plant species found of i abundance Absolute woody I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody

Games. Tables Table 1 plant species found of i abundance Absolute woody I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Tables Table 1 plant species found of i abundance Absolute woody

Games. Tables Table 1 plant species found of i abundance Absolute woody I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Games. Tables Table 1 plant species found of i abundance Absolute woody I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010.

Tables Table 1 plant species found of i abundance Absolute woody Games. Beijing city. I city. Beijing text for each species. thus trees increased and vegetation The of was cover number urban the 2005 between 2010and in order of based in on space the inventory censusgreen Beijing data from 2005 and 2010. Deciduous trees Evergreen shrubs Deciduous shrubs Plant typeEvergreen Species Abr. Latin name English name 2005 2010 trees 6 9 3 4 5 7 8 2 1 2 2 6 6 9 9 1 1 3 4 3 5 4 5 7 8 7 8 6 9 3 4 5 7 8 2 1 2 6 9 1 3 4 5 7 8 6 9 3 4 5 7 8 2 1 2 2 6 6 6 9 9 9 1 1 2 3 3 1 4 4 5 5 3 7 7 4 8 8 5 7 8 6 9 3 4 5 7 8 2 1 2 6 9 1 3 4 5 7 8 2 6 9 1 3 4 5 7 8 6 9 3 4 5 7 8 2 1 2 2 6 6 9 9 1 1 3 4 5 3 4 7 5 8 7 8 2 6 9 1 3 4 5 7 8 6 9 1 2 3 4 5 7 8 6 9 1 2 3 4 5 7 8 6 6 9 9 3 4 1 5 2 7 3 8 4 5 7 8 2 1 2 6 9 1 3 4 5 7 8 6 9 3 4 5 7 8 2 1 2 6 9 1 3 4 5 7 8 2 6 9 1 3 4 5 7 8 Absolute abundance of woody plant species found in 2005 and 2010 in the urban 6 9 3 4 5 7 8 2 1 2 6 9 1 3 4 5 7 8 6 6 6 9 9 9 1 3 2 4 3 5 3 4 4 5 7 5 8 7 7 8 8 2 2 1 1 6 9 3 4 5 7 8 2 1 6 9 3 4 5 7 8 2 1 2 6 9 1 3 4 5 7 8 6 9 1 2 3 4 5 7 8 6 9 3 4 5 7 8 2 1 6 9 1 2 3 4 5 7 8 6 9 3 4 5 7 8 2 1 6 9 1 2 3 4 5 7 8 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 2 6 9 1 3 4 5 7 8 6 9 1 2 3 4 5 7 8 2 6 9 1 3 4 5 7 8 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 10 247–262, doi:10.1071/EN12004, 2012. space coverage in ChinaSci. and Total Environ., its 442, 455–65, relationship, doi:10.1016/j.scitotenv.2012.10.014 with 2013. urbanization over the last two decades, 2804, doi:10.5194/acp-14-2789-2014 , 2014. Kiendler-Scharr, A., Kleist,pacts E., of soil Paoletti, moisture E., onScots de pine, Wahner, and novo Norway monoterpene A., spruce, emissions Biogeosciences,2015. Wildt, 12, from 177–191, European doi:10.5194/bg-12-177-2015, J., beech, Holm and oak, Mentel, T. F.:reduction, Im- Urban For. Urban Gree., 3, 65–78, doi:10.1016/j.ufug.2004.09.001, 2005. Kamens, R. M., andphotooxidation: Surratt, roles J. of D.: NO Secondary organic aerosol formation from methacrolein gen, P., Rohrer, F., Rudich,new Y., particle Springer, formation M., from monoterpene Tillmann, oxidation R., by NO and Wahner, A.: Suppression of 32, 1082–1091,, doi:10.1093/treephys/tps069 2012. higher plant species, J. Geophys. Res., 102, 5919–5927, doi:10.1029/96JD02968, 1997. H., and Chang, C.-C.: Biogenicquality, isoprene Atmos. in Environ., subtropical 79, urban 369–379, settings, doi:10.1016/j.atmosenv.2013.06.055 and 2013. implications for air C., Wang, B.,bons Zeng, (NMHC) emissions L., in Beijing Hu,,doi:10.5194/acp-15-1489-2015 during 2015. 2002–2013, M., Atmos. Chem. Yang, Phys., Y., 15, and 1489–1502, Li,and Y.: Staudt, M.: Trends The of diversification ofa non-methane terpene study emissions of hydrocar- in Mediterranean oaks: lessons from Zhao, J., Chen, S., Jiang, B., Ren, Y., Wang, H., Vause, J., and Yu, H.: Temporal trend of green Wu, C., Pullinen, I., Andres, S., Carriero, G., Fares, S., Goldbach, H., Hacker, L., Kasal, T., Yang, J., McBride, J., Zhou, J., and Sun, Z.: The urban forest inZhang, Beijing H., and Lin, its Y. role H., in Zhang, air Z., pollution Zhang, X., Shaw, S. L., Knipping, E. M., Weber, R. J., Gold, A., Table 1. area of Beijing city. Inin bold, the the text 22 for broadleafincreased species each between studied species. 2005 and The andOlympic the number abbreviation 2010 Games. (Abr.) of in used The treesforestry, order data inventory and to of were the thus improve green derived the environment space from urban in air Beijing vegetation quality Beijing based cover for on Municipal census was the Bureau data 2008 from of 2005 and Landscape 2010. and Wildt, J., Kley, D., Rockel, A., Rockel, P., and Segschneider, H.Wildt, J.: Emission J., of Mentel, NO T. from F., Kiendler-Scharr, several A., Ho Wang, J.-L., Chew, C., Chang, C.-Y., Liao, W.-C., Lung, S.-C. C., Chen, W.-N., Lee, P.-J., Lin, P.- Wang, M., Shao, M., Chen, W., Lu, S., Liu, Y., Yuan, B., Zhang, Q.,Welter, S., Zhang, Bracho-Nuñez, A., Q., Mir, C., Chang, Zimmer, I., C.- Kesselmeier, J., Lumaret, R., Schnitzler, J.-P., 5 30 25 20 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 3 based canescens benzenoids; benzenoids; × = = Gossypium hir- total [%] total [%] sum (all) sum (all) = one day after O G constitutive monoter- Populus (b) = = P ) were: n 7); Robinia pseudoacacia stress-induced. Meas.: BVOC = = n before and sesquiterpenes; BZ monoterpenes. (a) 27). Abbr. of VOC: BZ = = = ] vs Total [%] vs Total [%] group vs. group vs. 1 − n (Tomato, erent times with similar results. The plant ff gCyr 6 constitutive; s erences of BVOC between pre-Olympic (2005) ff = ] [10 23044 23043 1 − (Tobacco, gCyr 6 ] [10 1 − green leaf volatiles; MT = gCyr 6 Solanum lycopersicum = ] [10 S 1 − Nicotiana tabacum 4); = gCyr 6 = N n stress-induced monoterpenes, SQT erent plant model species from the laboratory study. Measurements were per- ff = 17); s 3314 6470 3558 7062 100 100 + Example of stress-induced BVOC emissions = Annual BVOC emission estimates in Beijing for the year 2005 and 2010, modeled n (Cotton, sesquiterpenes; GLVs green leaves volatiles; BVOC class: c = = erence 3156 3504 ff SumSumSum (all) cDi c s 2870 444 5593 877 3049 509 6013 1049 86 14 85 15 BVOCgroup BVOC 2005 (Meas.) class 2010Isoprene (Meas.) [10 cMT 2005 c (Total)sMT 2010 (Total)SQT 2005 Meas. cBZ 2010 Meas.GLV s 2005 BVOC s 2219 2010 BVOC s s 651 4281(2005–2010) 122 3 1312 119 200 2302 223 6 747 4445 236 412 140 1568 137 96 3 229 267 87 282 96 493 7 87 84 64.7 87 87 87 84 21.0 62.9 84 84 84 22.2 3.9 3.9 6.4 0.1 3.8 4.0 7.0 0.1 (Poplar, SQT and post-Olympic (2010) are2010 reported measured and below total, the respectively. estimations of the total BVOC for the years on data provided in Yang et al. (2005). The di estimates based on thetions 22 from plant plant species species measured. not Total: BVOC measured estimates (see including Table 1) estima- as well as exposure in di sutum formed continuously throughoutcate the daily day means. with Experimentsspecies a were that time replicated were resolution used di of and approx. the 76 number min. of Bars biological indi- replicates ( Figure 1. Table 2. as described in the text in hourly resolution. Abbr. BVOC groups: cMT penes; sMT GLV Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ), daily 2 axis. x NO + sesquiterpenes; = (NO x SQT NO (c) (d) air temperature, daily means (white circles), green leaf volatiles; (b) = 23046 23045 GLVs ozone, daily means (white circles), daily maximum (black (b) (c) isoprene. For the sBVOC in panels A-C, the red lines indicate the (e) benzenoids; = BZ (calculated from beginning July, black rectangles); 40 (a) Light, daily means (black circles); Climate data during the BVOC field campaign (August–October 2011) at an 8 m BVOC emission rates from 22 broadleaf tree species that are commonly found in the monoterpenes; (a) = MT (d) double maximum emission rates betweensBVOC all group. of For the graph unstressedstress-induced, model clearness, the plants the latter of MT being Fig. marginal emissions 1a compared to were to each not the total divided MT into emissions. constitutive and Figure 3. urban area of Beijing. The speciesdata were sorted (Fig. by 5). the phylogenetic tree based on the taxonomic Figure 2. height. triangles) AOT means (white triangles). The sampling time of each plant species is given along the daily maximum (black triangles);

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) Phylogenetic) tree based on the taxonomic of 22 data the plant species A A ) Phylogenetic) tree based on the taxonomic of 22 data the plant species Asterids, ( Asterids, Color code in score plot of panel code reflects panel Color B improve To A. assimilation. net in loading plot: shown the ( the parameters are mostvisualization, significant only ( assimilation, (Explained X - stress = sMT emission rates, net assimilation and numerically taxonconverted omic data assimilation net numerically (Tableemission and rates, S8, Supporting (left=score plot;Information) plot). Abbreviations plant right=loading of are given in Table 1. according to iTOL ( be can notes internal with all tree phylogenetic complete (the points main branching the for in Supportingfound Table S7). ( Information ( Fig.5 Asterids, ( Asterids, Color code in score plot of panel code reflects panel Color B improve To A. assimilation. net in loading plot: shown the ( the parameters are mostvisualization, significant only ( assimilation, (Explained X - stress = sMT emission rates, net assimilation and numerically taxonconverted omic data assimilation net numerically (Tableemission and rates, S8, Supporting (left=score plot;Information) plot). Abbreviations plant right=loading of are given in Table 1. according to iTOL ( be can notes internal with all tree phylogenetic complete (the points main branching the for in Supportingfound Table S7). ( Information ( Fig.5 A ) Phylogenetic) tree based on the taxonomic of 22 data the plant species A

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Asterids, ( Asterids, (Explained X emission rates, net assimilation and numerically taxonconverted omic data assimilation net numerically (Tableemission and rates, S8, Supporting (left=score plot;Information) plot). Abbreviations plant right=loading of Color code in score plot of panel code reflects panel Color B improve To A. assimilation. net in loading plot: shown the ( the parameters are mostvisualization, significant only ( assimilation, - stress = sMT according to iTOL ( be can notes internal with all tree phylogenetic complete (the points main branching the for in Supportingfound Table S7). ( Information are given in Table 1. ( Fig.5 A

according to iTOL ( ( Fig.5 Fig.5 Asterids, ( Asterids, emission rates, net assimilation and numerically taxonconverted omic data assimilation net numerically (Tableemission and rates, S8, Supporting (left=score plot;Information) plot). Abbreviations plant right=loading of - stress = sMT in score plot of panel code reflects panel Color B improve To A. assimilation. net in loading plot: shown the ( the parameters are mostvisualization, significant only ( assimilation, confidence 95% (ExplainedPC1 PC2at X-variation): significance 15.1%, 8.6%; = = for the main branching points (the complete phylogenetic tree with all internal notes can be can notes internal with all tree phylogenetic complete (the points main branching the for in Supportingfound Table S7). ( Information are given in Table 1. BZ = benzenoids 9 8 5 6 7 2 3 4 1 9 8 5 6 7 2 3 4 1 12 15 16 10 11 13 14 12 15 16 10 11 13 14 5 6 9 8 2 3 4 7 1 5 6 9 8 2 3 4 7 1 15 16 12 13 14 10 11 15 16 12 13 14 10 11 2 1 5 6 8 9 3 4 7 15 16 12 10 11 13 14 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | the percentages (c) 23049 anthropogenic VOC (AVOC) and (b) biogenic VOC (BVOC), Atmospheric concentrations of secondary organic particulate matter (SOA) originat- (a) Figure 6. ing from to total SOA expected atdenote a data 2 km for height 2005“constitutive” of and and the “stress-induced” in planetary BVOCs, boundary dark respectively. layer gray in data Beijing. for Bars 2010. in gray In panels A and C, “c” and “s” denote