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Ambient Formaldehyde Measurements Made at A Ambient formaldehyde measurements made at a remote marine boundary layer site during the NAMBLEX campaign ? a comparison of data from chromatographic and modified Hantzsch techniques T. J. Still, S. Al-Haider, P. W. Seakins, R. Sommariva, J. C. Stanton, G. Mills, S. A. Penkett To cite this version: T. J. Still, S. Al-Haider, P. W. Seakins, R. Sommariva, J. C. Stanton, et al.. Ambient formaldehyde measurements made at a remote marine boundary layer site during the NAMBLEX campaign ? a comparison of data from chromatographic and modified Hantzsch techniques. Atmospheric Chemistry and Physics, European Geosciences Union, 2006, 6 (9), pp.2711-2726. hal-00295970 HAL Id: hal-00295970 https://hal.archives-ouvertes.fr/hal-00295970 Submitted on 6 Jul 2006 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. Atmos. Chem. Phys., 6, 2711–2726, 2006 www.atmos-chem-phys.net/6/2711/2006/ Atmospheric © Author(s) 2006. This work is licensed Chemistry under a Creative Commons License. and Physics Ambient formaldehyde measurements made at a remote marine boundary layer site during the NAMBLEX campaign – a comparison of data from chromatographic and modified Hantzsch techniques T. J. Still1, S. Al-Haider1, P. W. Seakins1, R. Sommariva1, J. C. Stanton1, G. Mills2, and S. A. Penkett2 1School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK 2School of Environmental Sciences, University of East Anglia, Norwich, NR4 7TJ, UK Received: 9 August 2005 – Published in Atmos. Chem. Phys. Discuss.: 6 December 2005 Revised: 13 June 2006 – Accepted: 13 June 2006 – Published: 6 July 2006 Abstract. Ambient formaldehyde concentrations are re- that oxygenated VOCs such as ethanal and methanol are very ported from the North Atlantic Marine Boundary Layer Ex- significant sources of formaldehyde in the air masses reach- periment (NAMBLEX) campaign at Mace Head on the west ing Mace Head. coast of Eire during August 2002. The results from two techniques, using direct determination via gas chromatogra- phy and the Hantzsch technique, show similar trends but a significant off set in concentrations. For westerly air flows 1 Introduction characteristic of the marine boundary layer, formaldehyde concentrations from the gas chromatographic and Hantzsch technique ranged from 0.78–1.15 ppb and 0.13–0.43 ppb, re- The North Atlantic Boundary Layer Experiment, NAM- spectively. Possible reasons for the discrepancy have been BLEX, took place at Mace Head, Eire, during July and Au- investigated and are discussed, however, no satisfactory ex- gust 2002 to help quantify our understanding of photochem- planation has yet been found. In a subsequent laboratory in- ical oxidation processes in clean and moderately polluted tercomparison the two techniques were in good agreement. environments. Objectives included quantifying the role of The observed concentrations have been compared with halogen species in the marine boundary layer (MBL), study- previous formaldehyde measurements in the North Atlantic ing the reactive nitrogen budget and formation of new par- marine boundary layer and with other measurements from ticles. Objectives particularly relevant for our formaldehyde the NAMBLEX campaign. The measurements from the (HCHO), measurements included model/measurement com- Hantzsch technique and the GC results lie at the lower and parisons for radical species and the role of reactive hydro- upper ends respectively of previous measurements. In con- carbons in the MBL. Formaldehyde plays an important role trast to some previous measurements, both techniques show in determining radical concentrations, influencing both HOx distinct diurnal profiles with day maxima and with an ampli- formation and removal. Due to its importance and difficulties tude of approximately 0.15 ppb. Strong correlations were ob- in determining accurate concentrations (Gilpin et al., 1997) served with ethanal concentrations measured during NAM- formaldehyde concentrations were measured using two dif- BLEX and the ratio of ethanal to formaldehyde determined ferent techniques. The University of Leeds (UoL) used a by the gas chromatographic technique is in good agreement chromatographic method based on the detection of separated with previous measurements. HCHO with a helium ionization detector (Hunter et al., 1998, Some simple box modelling has been undertaken to inves- 1999; Hopkins et al., 2003). The University of East Anglia, tigate possible sources of formaldehyde. Such models are UEA, used a version of the Hantzsch reaction (Cardenas et not able to predict absolute formaldehyde concentrations as al., 2000) where ambient HCHO was scrubbed into solutions they do not include transport processes, but the results show and derivitized by reaction with 2,4 pentadione and ammo- nia. The adduct was then detected via fluorescence at 510 nm Correspondence to: P. W. Seakins following UV excitation by a mercury lamp. The two sys- ([email protected]) tems were located at sites approximately 200 m apart. Published by Copernicus GmbH on behalf of the European Geosciences Union. 2712 T. J. Still et al.: Ambient HCHO at NAMBLEX Table 1. Some previous measurements of formaldehyde in the marine environment. Reference Campaign and Date Location Platform Technique [HCHO] in Notes clean air/pptv Harris et al. (1992) “Polarstern” 1988 North Atlantic Ship TDLS 650 Measurement is mean value over 40–45◦ N. No diurnal variation Tanner et al. (1996) NARE 1993 Nova Scotia Coastal site DNPH 200–400 Summer measure- ment Solberg et al. (1996) EMEP 1994-5 Mace Head Coastal site DNPH 200–500 Winter measurement. Measurements at other sites show summer maxima. Cardenas et al. (2000) ACSOE 1996 Mace Head Coastal site Hantzsch 200–450 Summer measure- ment. Weller et al. (2000) ALBATROSS 1996 North Atlantic Ship Hantzsch 400–500 No diurnal variation observed. Fried et al. (2002) NARE 1997 Newfoundland Plane TDLS 410±150 Wagner et al. (2001) INDOEX 1999 Indian Ocean Ship TDLS 430±100 Diurnal variation with amplitude of ∼200 pptv observed. In the very remote environment, methane is the major In a modelling study of formaldehyde production in the re- source of formaldehyde via the reactions: mote Indian Ocean, Wagner et al. (2002) showed that in the presence of only 2 pptv of NO approximately 50% of CH3O2 O2 OH + CH4 −→ H2O + CH3O2 (R1) reacts via Reaction (R9). There are two major chemical removal processes for CH3O2 + HO2 → CH3OOH + O2 (R2) formaldehyde. Firstly, reaction with OH (Reaction R10) which, via the subsequent rapid reaction of HCO with oxy- CH O + CH O → 2CH O + O (R3) 3 2 3 2 3 2 gen (Reaction R11), is a major route for conversion of OH to HO . CH3O2 + CH3O2 → HCHO + CH3OH + O2 (R4) 2 OH + HCHO → H O + HCO (R10) CH OOH + hν → CH O + OH (R5) 2 3 3 −8 HCO + O2 → HO2 + CO(τ=4 × 10 s) (R11) OH + CH OOH → HCHO + H O + OH (R6) 3 2 Secondly, photolysis, which can act as a significant free rad- OH + CH3OOH → CH3O2 + H2O (R7) ical source. The efficiency of HCHO as a radical source de- pends on the branching ratio between the molecular and rad- CH3O + O2 → HO2 + HCHO (R8) ical channels (Pope et al., 2005): + → + Under such low NOx conditions, the methyl peroxy radical HCHO hν H2 CO (R12) (CH3O2) formed from the reaction of OH with CH4 pre- HCHO + hν → H + HCO (R13) dominantly reacts with other peroxy radicals. Reaction with Formaldehyde, and carbonyls in general, have been shown HO2 leads to CH3OOH which effectively acts as a reser- voir species on route to HCHO formation (although it can to be major sources of HOx radicals in the urban winter at- be rained out). Self reaction leads more directly to HCHO mosphere (Heard et al., 2004), but formaldehyde is also an formation. Reaction (R8) is very rapid and other reactions important HO2 source in the remote free troposphere. Frost of methoxy radicals do not need to be considered. Addi- et al. noted that the importance of formaldehyde as a radi- tional sources of formaldehyde include higher hydrocarbons cal source will increase at higher, increasingly drier altitudes and oxygenated VOCs such as methanol or acetaldehyde. (Frost et al., 2002). Table 1 lists some previous formaldehyde measurements In the presence of sufficient NO, CH3O2 radicals react di- rectly with NO to form methoxy radicals and subsequently in remote MBL environments, focusing particularly on stud- formaldehyde via Reaction (R8). ies in the North Atlantic environment. Measurements have been with a variety of techniques and from airborne, ship- CH3O2 + NO → CH3O + NO2 (R9) borne and coastal platforms. Average values range from Atmos. Chem. Phys., 6, 2711–2726, 2006 www.atmos-chem-phys.net/6/2711/2006/ T. J. Still et al.: Ambient HCHO at NAMBLEX 2713 ∼200–1000 pptv. A seasonal dependence has been observed 2.2 UoL apparatus for formaldehyde measurements in the EMEP programme (Solberg et al., 1996) peaking during the summer months. The UoL instrument used during the NAMBLEX campaign There is conflicting evidence on meridional variations with was based on a gas chromatographic (GC) system as de- measurements in the North Atlantic showing both positive scribed by Hopkins et al. (2003). The sampling inlet was and negative variations with increasing latitude (Harris et al., placed 2 m above the ground and consisted of ∼12 m 1/400 1992; Weller et al., 2000). Fried and co-workers have carried PFA tubing, and was pumped at a speed of 1 slm. The sam- out several airborne campaigns, their measurements show a ple passed through a 6.4 ml sample loop (Silco Steel).
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