Atmosphere II: Perturbations and Chemical Reactions. Topics. Photodissociation NO 2. h NO O( 3 P) O( 3 P) O 2 M O 3

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1 Atmosphere II: Perturbations and Chemical Reactions Parts of Chapters 5 and 13 (H&H) Brasseur et al., Chapters 3 and 5 Topics Chemical and photochemical processes OH snd O 3 Aerosols and clouds C, N, S, and halogen compounds Photodissociation The most common photochemical event of relevance to atmospheric chemistry (see table 3.1, Brasseur et al.) E.g. photolysis of NO 2 is the dominant source of tropospheric ozone NO 2 h NO O( 3 P) O( 3 P) O 2 M O 3 M 1

2 OH radicals Determines the oxidation efficiency of the atmosphere: detergent of the atmosphere Produced through photolysis of ozone followed by reaction between excited oxygen and water vapour O 3 h O( 1 D) O 2 O( 1 D) H 2 O 2OH Importance of the OH radical Compoun d CH 4 CO N 2 O 120 yr 0 NO x 1 day 100 NH 3 5 days < 2 (CH 3 ) 2 S H 2 S Residence time 9 yr 60 days 1 day 4 days % of sink due to OH COS 5 yr 22 SO 2 3 days 50 Ozone (O 3 ) Central importance in atmospheric chemistry Role in producing OH Produced and destroyed in large amounts in the troposphere 2

3 Chapman mechanism O 2 uv O O O O 2 M O 3 M (M = inert third body) O 3 uv O 2 O O O 3 2O 2 Tropospheric Ozone (O 3 ) Concentration varies from place to place ( = few days) Tropospheric O 3 is the main gas in photochemical smog 2NO O 2 2NO 2 NO 2 h NO O O O 2 M O 3 M Tropospheric O 3 Gradually increasing because of increasing emissions of NOx and hydrocarbons Could enhance greenhouse warming but the effect is strongly dependent on its concentration distribution in the troposphere 3

4 Stratospheric Ozone (O 3 ) Stratospheric O 3 is declining due to attacks by chlorine and bromine released by CFCs and halons, and attacks by N 2 O Low stratospheric O 3 has resulted in cooling which has offset some of the expected greenhouse warming O 3 destruction by Cl, Br, NO, OH, H X O 3 XO O 2 XO O X O 2 O O 3 O 2 O 2 Antarctic O 3 hole HCl ClONO 2 Cl 2 HNO 3 ice gas gas ice H 2 O ClONO 2 HOCl HNO 3 Cl 2 hv Cl Cl Cl O 3 ClO O 2 4

5 Clouds Global mean cloud cover ~ 60% Most in lower atmosphere (~ 10% of tropospheric mass is contained in cloud systems) Influence tropospheric chemistry by Modifying incoming UV radiation Carrying trace gases from boundary layer into free troposphere Remove soluble species from gas phase Cause precipitation Polar Stratospheric Clouds (PSC) Sparse clouds that form in the cold temperatures in polar regions Composed of water-ice or nitric acid trihydrate (NAT) Surfaces of PSC particles used for reactions that convert HCl to Cl 2 (active Cl) Particulate matter Any dispersed matter, solid or liquid, with particle size ranging from m to 100 m Aerosol is the general term used to describe all particulate matter Category of atmospheric pollutant based on: Size Composition Concentration 5

6 Types of aerosols Dust Particles caused by grinding or crushing operations Mist or fog liquid particles formed when vapours condense Smoke and soot Particles of carbon resulting from incomplete combustion Sources of aerosols Anthropogenic Primary: industrial dust, soot, biomass burning, windblown dust Gas-particle conversion of: SO 2 (smelters, power plants), NO x (vehicles, power plants) VOCs Natural Primary: windblown dust, forest fires, sea salt, volcanoes, organics Gas-particle conversion of: DMS, H 2 S, volcanic SO 2, biogenic NO x, VOCs, NH 3 -NH 4 + salts PM 10 and PM 2.5 Atmospheric particulate matter with aerodynamic diameter < 10 and 2.5 m respectively Small enough to penetrate beyond upper airways 6

7 Smog smoke + fog = smog Smog can be the result of primary pollutants as in the case of London smog Or it can be a consequence of chemical reactions in the atmosphere producing secondary pollutants as in the case of Los Angeles smog London Smog (primary) Fuel-rich combustion (insufficient oxygen) produces CO and water instead of CO 2 and water Low temperature combustion favours pyrolysis producing polycyclic aromatic hydrocarbons (PAH) E.g.: benzo( )pyrene, B( )P, a carcinogen Los Angeles Smog (photochemical) Results when hydrocarbons (primarily NMHC such as isoprene) react with nitric oxide to form aldehydes (eg. RCHO where R is an alkyl group) Process disrupts the equilibrium between other nitrogen oxides and ozone causing an increase in the production of tropospheric ozone, formaldehyde (HCHO), and peroxyacetyl nitrate (PAN, CH 3 C(O)O 2 NO 2 ) 7

8 Reactions CH 4 2O 2 2NO h H 2 O HCHO 2NO Vehicle emissions are the largest source of NO x 2NO O 2 2NO 2 NO 2 h NO O O O 2 M O 3 M O 3 NO O 2 NO 2 VOCs (volatile organic compounds) and PAN (peroxyacetyl nitrate) make effective catalysts (M) Trace gases Produced by biological and geochemical processes on the continents and in the oceans Described in terms of reservoirs and exchange fluxes between the reservoirs Challenge is to distinguish natural fluctuations from anthropogenically induced changes Carbon dioxide Well mixed in lower atmosphere ( = 3 years) Annual average values in 1995 ~ 360 ppmv (increasing by 1.6 ppm per year) Pre-industrial value ~ 280 ppmv 8

9 CO 2 Changes in atmospheric CO 2 have been measured with considerable accuracy Average change is 3.3 ± 0.2 GtC/yr When this value is compared with known sources and sinks a net imbalance of 1.3 ± 1.5 GtC/yr results (sources > sinks) Methane (CH 4 ) Naturally occurring gas increasing as a result of human activities Produced by bacterial fermentation in swamps, rice paddies, landfills Released during production, transport and consumption of fossil fuels Removed from atmosphere by reaction with the OH radical Effects of reaction with OH Produces water vapour Produces ozone Reduces [OH] 2CH 4 2OH 18O 2 2CO 2 H 2 4 H 2 O 10O 3 9

10 Reactions involving C compounds Oxidation of CH 4 by OH produces formaldehyde, CO and, in the presence of NO x, O 3 CO reacts with OH and in many areas concentrations of OH are controlled by CO levels Atmospheric concentrations of both CH 4 and CO declined in the early 1990 s Sulphur compounds: SO 2, DMS, COS, H 2 S, CS 2 SO 2 is a common intermediate in the oxidation of all reduced sulphur compounds COS is the most abundant sulphur gas in the atmosphere (residence time ~ 1.5 years) COS is photolyzed in the stratosphere to produce SO 2 H 2 S is rapidly oxidized by OH CS 2 reacts with OH to form COS Oxides of sulphur Primarily the result of fossil fuel combustion in stationary sources such as power plants Only significant non-combustion sources are petroleum refining and smelting Small proportion from vehicles Most emissions are in the form of sulphur dioxide (SO 2 ) React with OH to form sulphuric acid 10

11 Oxidation of SO 2 OH + SO 2 + M HOSO 2 + M HOSO 2 + O 2 HO 2 + SO 3 SO 3 + H 2 O H 2 SO 4 SO 2 (aq) H + + HSO - 3 HSO - 3 H + + SO 2-3 HSO 3- + H 2 O 2 HSO 4- + H 2 O HSO 4- + H + H 2 SO 4 Oxidation of DMS CH 3 SCH 3 or dimethyl sulphide (DMS) is the largest single reduced sulphur emission It is released by marine algae Oxidized by OH to SO 2 and CH 3 SO 3 H or methane sulphonic acid (MSA) Nitrogen compounds: NH 3, N 2 O, NO x NH 3 is the only natural alkaline gas in the atmosphere so is an important neutralizer of anthropogenic acidity Major sink for NH 3 is conversion to ammonium containing aerosols 2NH 3 H 2 SO 4 NH 4 2 SO 4 11

12 Nitrous Oxide N 2 O is removed from the atmosphere primarily by photolysis Provides a source of reactive nitrogen oxides in the stratosphere because of its long residence time ( years) Contributes to the radiative forcing of the climate system (greenhouse gas) Nitrous Oxide (N 2 O) Released to the atmosphere during the nitrification portion of the N cycle NH 4 N 2 N 2 O 60% from natural sources, 40% anthropogenic (agriculture) = 120 years NO 2 NO 3 Halocarbons (CFC s, etc) CFCs (CFCl 3, CF 2 Cl 2, CF 2 ClCFCl 2 )used as refrigerants, aerosol propellants, foaming agents entirely due to human activities, no natural sources years Halons (CF 3 Br and CF 2 ClBr) are used as fire extinguishers = years 12

13 Halogens Ubiquitous source of tropospheric halogens is sea salt aerosol NaCl, CH 3 Cl, CH 3 Br, CH 3 I Halogens: NaCl, HCl, CH 3 (Cl, Br, I) CH 3 Cl produced by photochemical reactions in seawater involving phytoplankton Largest natural source of Cl in the stratosphere with residence time ~ 1.5 years Reacts with OH and is photolyzed Halogens (cont d) CH 3 Br destroyed by reaction with OH but penetrates into the stratosphere because of its residence time of ~ 1-2 years CH 3 I also reacts with OH but has a much shorter residence time ~ 5 days so is unlikely to reach the stratosphere As with other halides in the stratosphere, these compounds act to destroy ozone 13

14 This document was created with Win2PDF available at The unregistered version of Win2PDF is for evaluation or non-commercial use only.

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