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Urea Decomposition and SCR Performance at Low Temperature
Urea Decomposition and SCR Performance at Low Temperature Scott Sluder, John Storey, Sam Lewis, Linda Lewis, Oak Ridge National Laboratory 10th Annual DEER Workshop Coronado, CA September 2, 2004 Sponsors: DOE-OFCVT, Steve Goguen and Kevin Stork OAK RIDGE NATIONAL LABORATORY U. S. DEPARTMENT OF ENERGY 1 Why study urea decomposition? • Under light-duty conditions (< 250 °C), there is negligible urea decomposition in the gas phase. Current models assume NH3 as input to catalyst. • It appears that urea decomposition kinetics on catalyst surfaces has to be understood. This will affect the length of the catalyst that is used for urea decomposition. OAK RIDGE NATIONAL LABORATORY U. S. DEPARTMENT OF ENERGY 2 Urea/SCR Chemistry Ideally, injected urea decomposes to NH3 O Heat NH3 + HCNO H2O, O2 isocyanic acid H 2N NH2 Heat HCNO NH3 + CO2 isocyanic acid H2O then reacts with NOX to form N2. 2 NH3 + NO + NO2 ⇔ 2 N2 + 3 H2O OAK RIDGE NATIONAL LABORATORY U. S. DEPARTMENT OF ENERGY 3 Unusual things can happen, such as ammonium nitrate formation and decomposition at T < 200 °C. 2NH3 + 2NO2 →NH4NO3 + N2 + 3 H2O NH4NO3 ⇔ NH3 + HNO3 2HNO3 + NO → 3 NO2 + H2O M. Koebel et al. in Ind.Eng.Chem.Res.: 39,p. 4120; 40, p. 52; 41, p.4008; 42, p.2093 Also in Catal.Today, 73, p.239 OAK RIDGE NATIONAL LABORATORY U. S. DEPARTMENT OF ENERGY 4 Experimental Approach • Use engine controls to: − Vary temperature − Keep constant: NOX and exhaust flow. • Investigate urea decomposition (if any) upstream of SCR catalyst. • Analyze exhaust products exiting undersized monoliths to elucidate urea decomposition − 3” and 6” monoliths = space velocities of 25K and 50K − const. -
) (51) International Patent Classification: A01N 43/58
) ( 0 (51) International Patent Classification: Declarations under Rule 4.17: A01N 43/58 (2006.01) A01P 15/00 (2006.01) — as to applicant's entitlement to apply for and be granted a (21) International Application Number: patent (Rule 4.17(H)) PCT/EP20 19/055007 — of inventorship (Rule 4.17(iv)) (22) International Filing Date: Published: 28 February 2019 (28.02.2019) — with international search report (Art. 21(3)) (25) Filing Language: English (26) Publication Language: English (30) Priority Data: 18159322.9 28 February 2018 (28.02.2018) EP (71) Applicant: BASF SE [DE/DE]; Carl-Bosch-Str. 38, 67056 Ludwigshafen am Rhein (DE). (72) Inventors: NESVADBA, Peter; Klybeckstrasse 141, 4002 Basel (CH). CUNNINGHAM, Allan Francis; Klybeck¬ strasse 141, 4002 Basel (CH). NAVE, Barbara; Speyerer Strasse 2, 67 117 Limburgerhof (DE). WALLQUIST, Olof; Klybeckstrasse 141, 4002 Basel (CH). WISSEMEIER, Alexander; Speyerer Strasse 2, 671 17 Limburgerhof (DE). HINDALEKAR, Shirang; 1st Floor, VIBGYOR Towers, Plot C62, 40005 1 Mumbai (IN). POTHI, Tejas; G Block, Bandra Kurla Complex, 40005 1 Mumbai (IN). (74) Agent: MAIWALD PATENTANWALTS- UND RECHTSANWALTSGESELLSCHAFT MBH; Eva Dbrner, Postfach 33 05 23, 80065 Mtinchen (DE). (81) Designated States (unless otherwise indicated, for every kind of national protection available) : AE, AG, AL, AM, AO, AT, AU, AZ, BA, BB, BG, BH, BN, BR, BW, BY, BZ, CA, CH, CL, CN, CO, CR, CU, CZ, DE, DJ, DK, DM, DO, DZ, EC, EE, EG, ES, FI, GB, GD, GE, GH, GM, GT, HN, HR, HU, ID, IL, IN, IR, IS, JO, JP, KE, KG, KH, KN, KP, KR, KW, KZ, LA, LC, LK, LR, LS, LU, LY, MA, MD, ME, MG, MK, MN, MW, MX, MY, MZ, NA, NG, NI, NO, NZ, OM, PA, PE, PG, PH, PL, PT, QA, RO, RS, RU, RW, SA, SC, SD, SE, SG, SK, SL, SM, ST, SV, SY, TH, TJ, TM, TN, TR, TT, TZ, UA, UG, US, UZ, VC, VN, ZA, ZM, ZW. -
Thermodynamics and Reaction Mechanism of Urea Decomposition† Cite This: Phys
PCCP View Article Online PAPER View Journal | View Issue Thermodynamics and reaction mechanism of urea decomposition† Cite this: Phys. Chem. Chem. Phys., 2019, 21,16785 a b b b Steffen Tischer, * Marion Bo¨rnhorst, Jonas Amsler, Gu¨nter Schoch and Olaf Deutschmann ab The selective catalytic reduction technique for automotive applications depends on ammonia production from a urea–water solution via thermolysis and hydrolysis. In this process, undesired liquid and solid by-products are formed in the exhaust pipe. The formation and decomposition of these Received 18th March 2019, by-products have been studied by thermogravimetric analysis and differential scanning calorimetry. Accepted 5th July 2019 A new reaction scheme is proposed that emphasizes the role of thermodynamic equilibrium of the DOI: 10.1039/c9cp01529a reactants in liquid and solid phases. Thermodynamic data for triuret have been refined. The observed phenomenon of liquefaction and re-solidification of biuret in the temperature range of 193–230 1Cis rsc.li/pccp explained by formation of a eutectic mixture with urea. Creative Commons Attribution-NonCommercial 3.0 Unported Licence. 1 Introduction and ammonium ISE (ion-selective electrode) measurements. Concluding from experimental results and literature data, 23 Air pollution by nitrogen oxides from Diesel engines is a major possible reactions including urea and its by-products biuret, problem concerning the environment and society. Therefore, cyanuric acid, ammelide, ammeline and melamine are presented. governments follow the need to regulate emissions by law (e.g., Further, cyanate and cyanurate salts and cyanamide are 715/2007/EG, ‘‘Euro 5 and Euro 6’’).1 The favored method to proposed as possible intermediates of high temperature urea reduce nitrogen oxides is selective catalytic reduction (SCR) decomposition. -
United States Patent Office E
Unitede States- Patent- Office 3,845,059E. 1. 2 The reaction of biuret with diethanolamine to form PREPARATION OF N,N'-DIETHANOL3,845,059 PIPERAZINE N,N'-diethanol piperazine can be illustrated as follows: Alvin F. Beale, Jr., Lake Jackson, Tex., assignor to The Dow Chemical Company, Midland, Mich. 2(HOCH)NH -- NH2CONHCONH --> No Drawing. Filed June 19, 1972, Ser. No. 264,704 5 CHO Int, C. C07d51/70 U.S. C. 260-268. SY 8 Claims /N al-woman-mamm CH, CH, ABSTRACT OF THE DISCLOSURE + 2CO. 1 + 8NHat Diethanolamine is reacted with urea or a urea pyrol- lo Y yzate (e.g. biuret, triuret, or cyanuric acid) to form N,N'-diethanol piperazine. The following chart illustrates the balanced stoichiom BACKGROUND OF THE INVENTION la etry for reacting diethanolamine with urea, biuret, triuret, N,N'-diethanol piperazine has been previously prepared and cyanuric acid. Reaction products Moles of Empirical Moles N,N'- Moles of formula of of diethanol Moles Moles (HOCH)NH Name of reactant reactant reactant piperazine of Co2 of NH3 2---------------------- Urea------------------------ CHNO 2 2 4. 2- ---. Biuret---. C2HNO2 2 3 6-- --- Triuret.----- ... C3HNO3 2 3. 6 8 6.----- ... Cyanuric aci - C3H3NO3 2 3. 6 6 by the condensation of piperazine with ethylene chloro- The reaction has been found to be specific for dieth hydrin as reported in J. Am. Chem. Soc., Vol. 55, p. 3823 anolamine since analogous dialkanolamines do not give (1933). The compound has been reported to have phar- corresponding dialkanol-substituted cyclic structures con macological properties as an anesthetic or sedative in 30 taining nitrogens within a carbon ring. -
United States Patent (19) 11 Patent Number: 4,822,624 Young (45) Date of Patent: Apr
United States Patent (19) 11 Patent Number: 4,822,624 Young (45) Date of Patent: Apr. 18, 1989 54 PRESERVATIVE FOR HARVESTED CROPS 4,033,747 7/1977 Young ................................... 426/69 (75) Inventor: Donald C. Young, Fullerton, Calif. 4,426,396 l/1984 Young .... ... 426/69 73 Assignee: Union Oil Company of California, FOREIGN PATENT DOCUMENTS Los Angeles, Calif. 117171 1/1976 German Democratic Rep. ... 426/69 Appl. No.: 1191470 5/1970 United Kingdom.................. 426/69 (21) 79,347 Primary Examiner-R. B. Penland 22 Filed: Jul. 30, 1987 Attorney, Agent, or Firm-Michael H. Laird; G. Wirzbicki Related U.S. Application Data (57) ABSTRACT 60 Continuation of Ser. No. 568,067, Jan. 4, 1984, aban doned, which is a division of Ser. No. 272,687, Jun. 11, The growth of microorganisms in stored crops, and 1981, Pat. No. 4,426,396. especially in animal feedstuffs, is inhibited by the appli (51) Int. C.'................................................ A23K 1/22 cation of a preservative composition which comprises (52) U.S. C. ........................................ 426/53; 426/69; ammonia, urease enzyme urea and/or urea polymers in 426/332; 426/532; 426/623; 426/630; 426/636; . a fluid medium. Urea polymers which are useful include 426/807 biuret, triuret, cyanuric acid, urea cyanurate and other (58) Field of Search ................... 426/53, 69,332, 532, compounds which decompose to form ammonia. The 426/623, 630, 807, 636 effect of treatment with the preservative composition is to provide an immediate microorganism-inhibiting am 56) References Cited monia level, which, due to delayed decomposition of U.S. PATENT DOCUMENTS the urea and urea polymers, is sustained to some signifi 1,702,735 2/1929 Legendre ........................... -
Sources of Isocyanic Acid (HNCO) Indoors: a Focus on Cigarette Smoke
TSpace Research Repository tspace.library.utoronto.ca Sources of isocyanic acid (HNCO) indoors: a focus on cigarette smoke Rachel F. Hems, Chen Wang, Douglas B. Collins, Shouming Zhou, Nadine Borduas-Dedekind, Jeffrey A. Siegel, Jonathan P.D. Abbatt Version Post-print/Accepted Manuscript Citation Hems, R.F., Wang, C., Collins, D.B., Zhou, S., Borduas-Dedekind, N., (published version) Siegel, J.A., Abbatt, J.P.D., 2019. Sources of isocyanic acid (HNCO) indoors: a focus on cigarette smoke. Environ. Sci.: Processes Impacts, 21, 1334. https://doi.org/10.1039/C9EM00107G. How to cite TSpace items Always cite the published version, so the author(s) will receive recognition through services that track citation counts, e.g. Scopus. If you need to cite the page number of the author manuscript from TSpace because you cannot access the published version, then cite the TSpace version in addition to the published version using the permanent URI (handle) found on the record page. This article was made openly accessible by U of T Faculty. Please tell us how this access benefits you. Your story matters. 1 Sources of isocyanic acid (HNCO) indoors: a focus on cigarette smoke 2 Rachel F. Hems,† Chen Wang,† Douglas B. Collins,ǂ Shouming Zhou,† Nadine Borduas- 3 Dedekind,† Jeffrey A. Siegel,‡ Jonathan P.D. Abbatt*† 4 †Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, Ontario M5S 5 3H6, Canada. 6 ‡Department of Civil and Mineral Engineering, University of Toronto, 35 Street George Street, 7 Toronto, Ontario M5S 1A4, Canada. 8 ǂDepartment of Chemistry, Bucknell University, 1 Dent Drive, Lewisburg, PA 17837, USA. -
Surface Chemistry and Kinetics of the Hydrolysis of Isocyanic Acid on Anatase
Technische Universität München Lehrstuhl 2 für Technische Chemie Surface chemistry and kinetics of the hydrolysis of isocyanic acid on TiO2 anatase Philipp Christian Dino Patrick Hauck Vollständiger Abdruck der von der Fakultät für Chemie der Technischen Universität München zur Erlangung des akademischen Grades eines Doktors der Naturwissenschaften (Dr.rer.nat.) genehmigten Dissertation. Vorsitzender: Univ.-Prof. Dr. Klaus Köhler Prüfer der Dissertation: 1. Univ.-Prof. Dr. Johannes A. Lercher 2. Univ.-Prof. Dr. Kai-Olaf Hinrichsen Die Dissertation wurde am 14.02.2007 bei der Technischen Universität München eingereicht und durch die Fakultät für Chemie am 16.04.2007 angenommen. Gott sei Dank! Nun ist’s vorbei mit der Übertäterei! Meine Damen und Herren, vielleicht hat niemand mehr damit gerechnet. Um so größer wird die Überraschung sein: Ich komme jetzt zum Ende. Wilhelm Busch (1832-1908) Acknowledgements Finally the PhD time has drawn to its close and the tamer of the isocyanic acid would like to say a few words of thank to a bunch of people who made a substantial contribution to the ultimate thesis. First of all I would like to thank Johannes (Prof. J.A. Lercher) for inviting me into his group and thus giving me the opportunity to work in a fairly international team on an adventurous project. Thank you for all the guidance, trust, fruitful, but also sharp- tongued discussions during the last three years three months and the sufficient freedom and independence with regard to structuring my work. The time at TC 2 has been an important and joyful part of my life for sure. -
Arxiv:1510.07052V1 [Astro-Ph.EP] 23 Oct 2015 99 Lae Ta.20,Adrfrne Therein)
A Chemical Kinetics Network for Lightning and Life in Planetary Atmospheres P. B. Rimmer1 and Ch Helling School of Physics and Astronomy, University of St Andrews, St Andrews, KY16 9SS, United Kingdom ABSTRACT There are many open questions about prebiotic chemistry in both planetary and exoplane- tary environments. The increasing number of known exoplanets and other ultra-cool, substellar objects has propelled the desire to detect life and prebiotic chemistry outside the solar system. We present an ion-neutral chemical network constructed from scratch, Stand2015, that treats hydrogen, nitrogen, carbon and oxygen chemistry accurately within a temperature range between 100 K and 30000 K. Formation pathways for glycine and other organic molecules are included. The network is complete up to H6C2N2O3. Stand2015 is successfully tested against atmo- spheric chemistry models for HD209458b, Jupiter and the present-day Earth using a simple 1D photochemistry/diffusion code. Our results for the early Earth agree with those of Kasting (1993) for CO2, H2, CO and O2, but do not agree for water and atomic oxygen. We use the network to simulate an experiment where varied chemical initial conditions are irradiated by UV light. The result from our simulation is that more glycine is produced when more ammonia and methane is present. Very little glycine is produced in the absence of any molecular nitrogen and oxygen. This suggests that production of glycine is inhibited if a gas is too strongly reducing. Possible applications and limitations of the chemical kinetics network are also discussed. Subject headings: astrobiology — atmospheric effects — molecular processes — planetary systems 1. Introduction The input energy source and the initial chem- istry have been varied across these different ex- The potential connection between a focused periments. -
Investigating Diesel Engines As an Atmospheric Source of Isocyanic Acid in Urban Areas
Atmos. Chem. Phys., 17, 8959–8970, 2017 https://doi.org/10.5194/acp-17-8959-2017 © Author(s) 2017. This work is distributed under the Creative Commons Attribution 3.0 License. Investigating diesel engines as an atmospheric source of isocyanic acid in urban areas Shantanu H. Jathar1, Christopher Heppding1, Michael F. Link2, Delphine K. Farmer2, Ali Akherati1, Michael J. Kleeman3, Joost A. de Gouw4,5, Patrick R. Veres4,5, and James M. Roberts4 1Department of Mechanical Engineering, Colorado State University, Fort Collins, CO 80523, USA 2Department of Chemistry, Colorado State University, Fort Collins, CO 80523, USA 3Department of Civil and Environmental Engineering, University of California Davis, Davis, CA 95616, USA 4NOAA Earth System Research Laboratory, Chemical Sciences Division, Boulder, CO 80305, USA 5Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80305, USA Correspondence to: Shantanu H. Jathar ([email protected]) Received: 20 January 2017 – Discussion started: 22 February 2017 Revised: 18 May 2017 – Accepted: 19 May 2017 – Published: 26 July 2017 Abstract. Isocyanic acid (HNCO), an acidic gas found in implied that diesel-powered engines were the largest source tobacco smoke, urban environments, and biomass-burning- of HNCO in urban areas. The CTM also predicted that daily- affected regions, has been linked to adverse health outcomes. averaged concentrations of HNCO reached a maximum of Gasoline- and diesel-powered engines and biomass burning ∼ 110 pptv but were an order of magnitude lower than the are known to emit HNCO and hypothesized to emit pre- 1 ppbv level that could be associated with physiological ef- cursors such as amides that can photochemically react to fects in humans. -
Evaluation of Chemical and Particle Exposures During Vehicle Fire Suppression Training
This Health Hazard Evaluation (HHE) report and any recommendations made herein are for the specific facility evaluated and may not be universally applicable. Any recommendations made are not to be considered as final statements of NIOSH policy or of any agency or individual involved. Additional HHE reports are available at http://www.cdc.gov/niosh/hhe/ Workplace Safety and Health Evaluation of Chemical and Particle Exposures During Vehicle Fire Suppression Training Kenneth W. Fent, PhD Douglas E. Evans, PhD James Couch, MS, CIH Health Hazard Evaluation Report HETA 2008-0241-3113 Miami Township Fire and Rescue Yellow Springs, Ohio July 2010 Department of Health and Human Services Centers for Disease Control and Prevention National Institute for Occupational Safety and Health The employer shall post a copy of this report for a period of 30 calendar days at or near the workplace(s) of affected employees. The employer shall take steps to insure that the posted determinations are not altered, defaced, or covered by other material during such period. [37 FR 23640, November 7, 1972, as amended at 45 FR 2653, January 14, 1980]. CONTENTS REPO R T Abbreviations .......................................................................ii Highlights of the NIOSH Health Hazard Evaluation ............iv Summary ............................................................................vi Introduction ..........................................................................1 Assessment .........................................................................3 -
Isocyanic Acid and Ammonia in Vehicle Emissions ⇑ ⇑ R
View metadata, citation and similar papers at core.ac.uk brought to you by CORE provided by Elsevier - Publisher Connector Transportation Research Part D 49 (2016) 259–270 Contents lists available at ScienceDirect Transportation Research Part D journal homepage: www.elsevier.com/locate/trd Isocyanic acid and ammonia in vehicle emissions ⇑ ⇑ R. Suarez-Bertoa , C. Astorga European Commission Joint Research Centre Ispra, Institute for Energy and Transport, Sustainable Transport Unit, 21027 Ispra, VA Italy article info abstract Article history: Vehicles are considered to be an important source of ammonia (NH3) and isocyanic acid Available online 22 October 2016 (HNCO). HNCO and NH3 have been shown to be toxic compounds. Moreover, NH3 is also a precursor in the formation of atmospheric secondary aerosols. For that reason, real- Keywords: time vehicular emissions from a series of Euro 5 and Euro 6 light-duty vehicles, including Vehicle emissions spark ignition (gasoline and flex-fuel), compression ignition (diesel) and a plug-in electric HNCO hybrid, were investigated at 23 and À7 °C over the new World harmonized Light-duty NH 3 vehicle Test Cycle (WLTC) in the Vehicle Emission Laboratory at the European WLTC Commission Joint Research Centre Ispra, Italy. The median HNCO emissions obtained for DeNOx the studied fleet over the WLTC were 1.4 mg kmÀ1 at 23 °C and 6 mg kmÀ1 at À7 °C. The À1 À1 fleet median NH3 emission factors were 10 mg km and 21 mg km at 23 and À7 °C, respectively. The obtained results show that even though three-way catalyst (TWC), selec- tive catalytic reduction (SCR), and NOx storage catalyst (NSC) are effective systems to reduce NOx vehicular emissions, they also lead to considerable emissions of the byproducts NH3 and/or HNCO. -
Applied As Nitrogen Slow-Release Fertilizer
Uncorretced Proof Facile Synthesis of Poly(Carbonyl Urea) Oligomer (Pcuo) from Urea and Dipropyl Carbonate (Dprc) Applied as Nitrogen Slow-Release Fertilizer 1,2JIANCHAO CHEN, 2YAQING LIU*, 1HONGFANG JIU, 2PEIHUA ZHAO AND 2FUTIAN ZHU 1 Department of Chemistry, School of Science, North University of China, Taiyuan 030051, P. R. China 2 Research Center for Engineering Technology of Polymeric Composites of Shanxi Province, North University of China, Taiyuan 030051, P. R. China. * [email protected] (Received on 19th September 2011, accepted in revised form 15th February 2012) Summary: A novel slow-release nitrogen fertilizer poly(carbonyl urea)oligomer (PCUO) was prepared by the condensation polymerization of urea and dipropyl carbonate (DPrC) at normal pressure, in which anhydrous potassium carbonate was as a catalyst. The oligomer was characterized by FT-IR, 1H- NMR, and 13C-NMR spectroscopy, which showed that the number average degree of PCUO was 1 to 5. The effects of the molar ratio of urea to DPrC, reaction time as well as the temperature on the yields were investigated and optimized. In addition, the slow-release behaviour of PCUO was evaluated in distilled water and the results showed that the product with good slow-release properties could be expected to have wide potential applications in modern agriculture and horticulture. Introduction The consumption of synthetic nitrogen methods for poly(carbonyl urea)oligomer have some fertilizer in agriculture has increased over the past drawbacks: the raw materials (e.g. sulfurisocyanatidic several decades, and it might continue to rise in order chloride, phosgene) and by-products (e.g. to meet the food demand of the growing global chlorinegas, hydrogen chloride and so forth) were population [1].