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Chapter 12, Part 2 Fundamentals of Atmospheric Modeling

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Chapter 12, Part 2 Fundamentals of Atmospheric Modeling Overhead Slides for Chapter 12, Part 2 of Fundamentals of Atmospheric Modeling by Mark Z. Jacobson Department of Civil & Environmental Engineering Stanford University Stanford, CA 94305-4020 January 30, 2002 Alkene Reaction With Ozone Ethene H H O 37% C O + C O H H H H O C C + O Formaldehyde Criegee biradical 3 O O H H H H O* H2C CH2 63% C O + C O Ethene Ethene molozonide H H Formaldehyde Excited Criegee biradical (12.89) Criegee biradical reaction + NO H O H C O C O H H NO2 Criegee biradical Formaldehyde (12.90) Excited criegee biradical decomposition 60% CO + H2O H O* H C O C O 21% CO2 + H2 H H O * + O2 Excited Criegee Excited formic 19% CO + OH + HO2 biradical acid (12.91) Alkene Reaction With Ozone Propene H H3C O 7.5% C O + C O H H Formaldehyde Methyl criegee biradical H H3C O* C O + C O 42.5% H H O H O O Formaldehyde Excited methyl criegee C CH + O biradical 2 3 H3C CH CH2 H3C H O H3C C O + C O 18.5% H H Propene Propene molozonide Acetaldehyde Criegee biradical H3C H O* 33.5% C O + C O H H Acetaldehyde Excited criegee biradical (12.92) Alkene Reaction With Ozone Methylcriegee biradical reaction + NO H3C O H3C C O C O H H NO2 Methyl criegee Acetaldehyde biradical (12.93) Excited methylcriegee biradical decomposition 16% CH4 + CO2 H3C O* H3C C O C O 64% CH3 + CO + OH H H O * 20% CH3O + HO2 + CO Excited methyl criegee Excited acetic biradical acid (12.94) Alkene Reaction With Nitrate Ethene --> nitrated organic radicals O O O + NO O H H + NO3 O N + O2 O O N O O N C C H H H O O O H H C CH2 C CH2 C CH2 H H NO2 H Ethene Ethyl nitrate radical Ethylperoxy nitrate Ethoxy nitrate radical radical (12.95) Propene --> nitrated organic radicals O O O O + NO H H O O N O O N + NO3 H O N + O2 H H C C O C CH O C CH O C CH2 2 2 H3C H H C H3C H3C 3 NO2 Propene Propyl nitrate radical Propylperoxy nitrate Propoxy nitrate radical radical (12.96) Aromatic Reaction With Hydroxyl Radical Toluene oxidation CH2 H2C O O + OH + O2 Benzylperoxy 8% radical H2O Benzyl O CH3 radical O CH3 H OH CH3 + O Toluene-hydroxyl- + OH H 2 radical adduct Toluene 92% OH CH3 OH o-Hydroxytoluene + HO2 o-Cresol (12.97) Aromatic Reaction With Hydroxyl Radical Benzylperoxy radical reaction with NO H2C O O CH + NO + O2 H C O O NO2 HO2 2 Benzoxy Benzaldehyde radical O H C O N + NO 2 O Benzylperoxy radical Benzyl nitrate (12.98) Toluene-hydroxyl radical adduct reaction O CH3 CH3 O O + NO H H OH OH NO2 Toluene-hydroxyl radical adduct (12.99) Fate of Cresol Cresol --> methylphenylperoxy radical and nitrocresol CH3 + OH, 2O 2 O O CH 3 2HO2 OH Methylphenylperoxy radical CH3 CH3 + OH OH o-Cresol O + NO2 O N H2O O Methylphenoxy m-Nitrocresol radical (12.100) Terpene Reaction With OH HO HO CH3 CH3 H CH C C C (1) O (4) O O C H2C C O 16.4% CH2 23.6% H2 H2 O O O H CH3 + OH, O O CH 2 (2) CH3 (5) H 3 C C 21.2% C C 12.3% CH C OH H C CH HO 2 2 C H2C C CH2 H2 H2 Isoprene CH3 CH (3) H (6) H 3 HO C C 14.1% O C C 12.3% O O O OH C C C C H2 H H2 2 H2 Isoprene peroxy radicals (12.101) All six products convert NO to NO2 Terpene Reaction With OH Methacrolein production via second product (12.102) O O + NO + O2 CH CH3 H 3 H C C + C O HO CH C C CH O CH2 H H 2 2 NO2 HO2 Isoprene peroxy radical Methacrolein Formaldehyde Methylvinylketone production via fifth product (12.103) O + NO + O O 2 CH3 H H CH3 H C C C C + C O OH H C H H2C C 2 O H2 NO2 HO2 Isoprene peroxy radical Methylvinylketone Formaldehyde Terpene Reaction With Ozone H CH3 H C C O + C O H2C O H Methylvinylketone Criegee biradical CH H 3 H O C C + C O O CH H CH 2 H 3 + O3 C C Methacrolein Criegee biradical H C CH 2 CH2 H 3 H C C C O Isoprene + H2C O O H Ozonide product Formaldehyde CH H 3 H C C C O O O + CH2 H Ozonide product Formaldehyde (12.104) Alcohol Reactions Hydroxyl radical scavenges methanol (36-hour lifetime) H + O2 O 85% H C O H C + OH H H H HO H 2 Formaldehyde H C O H H H2O 15% H C O Methanol H Methoxy radical (12.105) Hydroxyl radical scavenges ethanol (10-hour lifetime) H H 5% H C C O H H H + O H O H H + OH H 2 H 90% H C C O H C C H C C O H H H H H H H O HO2 2 H H Acetaldehyde Ethanol 5% H C C O H H Ethoxy radical (12.106) Carbon Bond Lumping Organic gases lumped into surrogate groups. PAR (paraffins) -- Single carbon atoms with a single-bond between them OLE (olefins) -- Terminal carbon atom pair with a double-bond between the two atoms ALD2 -- Non-terminal carbon atom pairs with a double bond attached to one of the carbons and terminal two-carbon carbonyl groups [C-C(=O)H] KET -- Single carbon ketone groups (C=O) TOL (toluene) -- 7-carbon aromatics XYL (m-xylene) -- 8-carbon aromatics ISOP (isoprene) -- Terpenes UNR -- Unreactive Carbon Bond Lumping (Table 12.7) Chemical Name Chemical Name Chemical Name Chemical Name Carbon Bond Group Carbon Bond Group Carbon Bond Group Carbon Bond Group Chemical Structure Chemical Structure Chemical Structure Chemical Structure Ethane n-Butane 2,2,4-Trimethylpentane Cyclopentane 0.4 PAR +1.6 4 PAR 8 PAR 5 PAR UNR H2 H H H H CH3 CH3 H C C H H 2 H C C C C H H C C C C CH CH2 3 3 H C H C C H H H2 2 C H H H H CH3 H2 H H Ethene Trans 2-butene Propene Ethyne 1 ETH 2 ALD2 1 PAR + 1 OLE 1 PAR + 1 UNR H H H H H H C C C CH H C C C C H 2 H C C H H H H3C H H H Formaldehyde Acetaldehyde Propionaldehyde Benzaldehyde 1 FORM 1 ALD2 1 PAR + 1 ALD2 1 ALD2 + 5 UNR O CH O H O H C CH2 H C H C C O CH3 H H H Toluene Ethylbenzene m-Xylene 1,2,3- 1 TOL 1 PAR + 1 TOL 1 XYL Trimethylbenzene 1 PAR + 1 XYL H3C CH CH CH 3 2 3 CH3 CH3 CH 3 CH3 Stratospheric Chemistry Ozone mixing ratios stratosphere » 10 ppmv free troposphere » 40 ppbv urban air » 0.1 - 0.3 ppmv Ozone production in the stratosphere Oxygen photolysis 1 O2 + hn O( D) + O l < 175 nm (12.107) O2 + hn O + O 175 < l < 245 nm (12.108) Ozone formation M 1 O( D) O (12.109) O + O2 + M O3 + M (12.110) Ozone photodissociation O + hn 1 l < 310 nm 3 O2 + O( D) (12.111) O3 + hn O2 + O l > 310 nm (12.112) Ozone Destruction by NOx Nitrous oxide reaction: 10% of N2O destruction 64% 2NO 1 N2O + O( D) 36% N2 + O2 (12.113) Nitrous oxide photolysis: 90% of N2O destruction (12.114) 1 N2O + hn N2 + O( D) l < 240 nm NO catalytically destroys ozone in the upper stratosphere NO + O3 NO2 + O2 (12.115) NO2 + O NO + O2 (12.116) ---------------------------- O + O3 2O2 (12.117) Ozone Destruction by HOx Hydroxyl radical formation in stratosphere H2O 2OH 1 O( D) + CH4 CH3 + OH H2 H + OH (12.118) OH catalytically destroys ozone in the lower stratosphere OH + O3 HO2 + O2 (12.119) HO2 + O3 OH + 2O2 (12.120) ---------------------------- 2O3 3O2 (12.121) Removal of HOx and NOx Removal reactions HO2 + OH H2O + O2 (12.122) M NO2 + OH HNO3 (12.123) M HO2 + NO2 HO2NO2 (12.124) Nitric acid and peroxynitric acid photodissociation is slow Source of Water Vapor CH4 + OH CH3 + H2O (12.125) Methane and carbon monoxide reactions in the stratosphere are similar to those in the free troposphere Chlorine Emissions to Stratosphere Table 12.8. WMO (1994) Chemical Trade Name Chemical Name Percent Formula Contribution to Stratospheric Emissions Anthropogenic Sources CF2Cl2 CFC-12 Dichlorodifluoromethane 28 CFCl3 CFC-11 Trichlorofluoromethane 23 CCl4 Carbon tetrachloride 12 CH3CCl3 Methyl chloroform 10 CFCl2CF2Cl CFC-113 1-Fluorodichloro,2- 6 difluorochloroethane CF2ClH HCFC-22 Chlorodifluoromethane 3 Natural Sources CH3Cl --- Methyl chloride 15 HCl --- Hydrochloric acid 3 Total 100% Ozone Destruction by Chlorine Photolysis of chlorinated compounds above 20 km Cl Cl F C Cl + hn F C + Cl l < 250 nm Cl Cl (12.126) Cl Cl F C Cl + hn F C + Cl l < 230 nm F F (12.127) Cl Cl Cl C Cl + hn Cl C + Cl l < 250 nm Cl Cl (12.129) H H H C Cl + hn H C + Cl l < 220 nm H H (12.130) Methyl chloride scavenging by hydroxyl radical H + OH H C Cl H C Cl H H H2O (12.128) Ozone Destruction by Chlorine Catalytic ozone destruction by chlorine Cl + O3 ClO + O2 (12.131) ClO + O Cl + O2 (12.132) ----------------------------- O + O3 2O2 (12.133) Only 1% of chlorine is typically active as Cl or ClO.
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