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Atmospheric oxidation capacity sustained by a tropical forest (2008)

J. Lelieveld ; T. M. Butler ; J. N. Crowley ; [et al.]

Nature Publishing Group (NPG)

In: Nature. 452(7188): 737-40. doi: 10.1038/nature06870.

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Publication Date: 2008-04-11

Description: Terrestrial vegetation, especially tropical rain forest, releases vast quantities of volatile organic compounds (VOCs) to the atmosphere, which are removed by oxidation reactions and deposition of reaction products. The oxidation is mainly initiated by hydroxyl radicals (OH), primarily formed through the photodissociation of ozone. Previously it was thought that, in unpolluted air, biogenic VOCs deplete OH and reduce the atmospheric oxidation capacity. Conversely, in polluted air VOC oxidation leads to noxious oxidant build-up by the catalytic action of nitrogen oxides (NO(x) = NO + NO2). Here we report aircraft measurements of atmospheric trace gases performed over the pristine Amazon forest. Our data reveal unexpectedly high OH concentrations. We propose that natural VOC oxidation, notably of isoprene, recycles OH efficiently in low-NO(x) air through reactions of organic peroxy radicals. Computations with an atmospheric chemistry model and the results of laboratory experiments suggest that an OH recycling efficiency of 40-80 per cent in isoprene oxidation may be able to explain the high OH levels we observed in the field. Although further laboratory studies are necessary to explore the chemical mechanism responsible for OH recycling in more detail, our results demonstrate that the biosphere maintains a remarkable balance with the atmospheric environment.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Lelieveld, J -- Butler, T M -- Crowley, J N -- Dillon, T J -- Fischer, H -- Ganzeveld, L -- Harder, H -- Lawrence, M G -- Martinez, M -- Taraborrelli, D -- Williams, J -- England -- Nature. 2008 Apr 10;452(7188):737-40. doi: 10.1038/nature06870.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Max Planck Institute for Chemistry, 27 Becherweg, 55128 Mainz, Germany. lelieveld@mpch-mainz.mpg.de〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/18401407" target="_blank"〉PubMed〈/a〉

Keywords: Animals ; Atlantic Ocean ; Atmosphere/*chemistry ; Butadienes/metabolism ; French Guiana ; Guyana ; Hemiterpenes/metabolism ; Hydroxyl Radical/metabolism ; Nitric Oxide/metabolism ; Oxidation-Reduction ; Ozone/analysis ; Pentanes/metabolism ; Suriname ; Trees/*metabolism ; *Tropical Climate

Print ISSN: 0028-0836

Electronic ISSN: 1476-4687

Topics: Biology , Chemistry and Pharmacology , Medicine , Natural Sciences in General , Physics

Published by Nature Publishing Group (NPG)

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Atmospheric chemistry: A missing sink for radicals (2010)

J. Lelieveld

Nature Publishing Group (NPG)

In: Nature. 466(7309): 925-6. doi: 10.1038/466925a.

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Publication Date: 2010-08-21

Description: 〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Lelieveld, Jos -- England -- Nature. 2010 Aug 19;466(7309):925-6. doi: 10.1038/466925a.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/20725025" target="_blank"〉PubMed〈/a〉

Print ISSN: 0028-0836

Electronic ISSN: 1476-4687

Topics: Biology , Chemistry and Pharmacology , Medicine , Natural Sciences in General , Physics

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The contribution of outdoor air pollution sources to premature mortality on a global scale (2015)

J. Lelieveld ; J. S. Evans ; M. Fnais ; [et al.]

Nature Publishing Group (NPG)

In: Nature. 525(7569): 367-71. doi: 10.1038/nature15371.

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Publication Date: 2015-09-19

Description: Assessment of the global burden of disease is based on epidemiological cohort studies that connect premature mortality to a wide range of causes, including the long-term health impacts of ozone and fine particulate matter with a diameter smaller than 2.5 micrometres (PM2.5). It has proved difficult to quantify premature mortality related to air pollution, notably in regions where air quality is not monitored, and also because the toxicity of particles from various sources may vary. Here we use a global atmospheric chemistry model to investigate the link between premature mortality and seven emission source categories in urban and rural environments. In accord with the global burden of disease for 2010 (ref. 5), we calculate that outdoor air pollution, mostly by PM2.5, leads to 3.3 (95 per cent confidence interval 1.61-4.81) million premature deaths per year worldwide, predominantly in Asia. We primarily assume that all particles are equally toxic, but also include a sensitivity study that accounts for differential toxicity. We find that emissions from residential energy use such as heating and cooking, prevalent in India and China, have the largest impact on premature mortality globally, being even more dominant if carbonaceous particles are assumed to be most toxic. Whereas in much of the USA and in a few other countries emissions from traffic and power generation are important, in eastern USA, Europe, Russia and East Asia agricultural emissions make the largest relative contribution to PM2.5, with the estimate of overall health impact depending on assumptions regarding particle toxicity. Model projections based on a business-as-usual emission scenario indicate that the contribution of outdoor air pollution to premature mortality could double by 2050.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Lelieveld, J -- Evans, J S -- Fnais, M -- Giannadaki, D -- Pozzer, A -- England -- Nature. 2015 Sep 17;525(7569):367-71. doi: 10.1038/nature15371.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Max Planck Institute for Chemistry, Atmospheric Chemistry Department, 55128 Mainz, Germany. ; The Cyprus Institute, Energy, Environment and Water Research Center, 1645 Nicosia, Cyprus. ; Harvard School of Public Health, Boston, Massachusetts 02215, USA. ; Cyprus International Institute for Environment and Public Health, Cyprus University of Technology, 3041 Limassol, Cyprus. ; King Saud University, College of Science, Riyadh 11451, Saudi Arabia.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/26381985" target="_blank"〉PubMed〈/a〉

Keywords: Adult ; Agriculture/statistics & numerical data ; Air Pollutants/*adverse effects/poisoning ; Air Pollution/*adverse effects ; Atmosphere/chemistry ; Biomass ; Child, Preschool ; China/epidemiology ; Cooking/statistics & numerical data ; Environmental Exposure/*adverse effects ; Environmental Monitoring ; Europe/epidemiology ; Far East/epidemiology ; Fires/statistics & numerical data ; Heating/statistics & numerical data ; Humans ; India/epidemiology ; Infant ; *Internationality ; Middle Aged ; *Mortality, Premature/trends ; Ozone/adverse effects/analysis/poisoning ; Particulate Matter/*adverse effects/poisoning ; Power Plants/statistics & numerical data ; Rural Health/statistics & numerical data ; Russia/epidemiology ; United States/epidemiology ; Urban Health/statistics & numerical data ; Vehicle Emissions/poisoning

Print ISSN: 0028-0836

Electronic ISSN: 1476-4687

Topics: Biology , Chemistry and Pharmacology , Medicine , Natural Sciences in General , Physics

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In Situ Trace Gas and Particle Measurements in the Summer Lower Stratosphere during STREAM II: Implications for O3 Production (1997)

Bregman, A. ; Arnold, F. ; Bürger, V. ; [et al.]

Springer

Journal of atmospheric chemistry 26 (1997), S. 275-310

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ISSN: 1573-0662

Keywords: trace gas and particle distributions ; ozone production ; aircraft measurements ; tropopause region

Source: Springer Online Journal Archives 1860-2000

Topics: Chemistry and Pharmacology , Geosciences

Notes: Abstract In situ aircraft measurements of O3, CO,HNO3, and aerosol particles are presented,performed over the North Sea region in the summerlower stratosphere during the STREAM II campaign(Stratosphere Troposphere Experiments by AircraftMeasurements) in July 1994. Occasionally, high COconcentrations of 200-300 pbbv were measured in thelowermost stratosphere, together with relatively highHNO3 concentrations up to 1.6 ppbv. The particlenumber concentration (at standard pressure andtemperature) between 0.018-1 μm decreased acrossthe tropopause, from 〉1000 cm-3 in the uppertroposphere to 〈500 cm-3 in the lowermoststratosphere. Since the CO sources are found in thetroposphere, the elevated CO mixing ratios areattributed to mixing of polluted tropospheric air intothe lowermost extratropical stratosphere. Further wehave used a chemical model to illustrate that nitrogenoxide reservoir species (mainly HNO3) determinethe availability of NOx (=NO + NO2) andtherefore largely control the total net O3production in the lower kilometers of thestratosphere. Model simulations, applying additionalNOx perturbations from aircraft, show that theO3 production efficiency of NOx is smallerthan previously assumed, under conditions withrelatively high HNO3 mixing ratios, as observedduring STREAM II. The model simulations furthersuggest a relatively high O3 productionefficiency from CO oxidation, as a result of therelatively high ambient HNO3 and NOxconcentrations, implying that upward transport of COrich air enhances O3 production in the lowermoststratosphere. Analysis of the measurements and themodel calculations suggest that the lowermoststratosphere is a transition region in which thechemistry deviates from both the upper troposphere andlower stratosphere.

Type of Medium: Electronic Resource

URL: http://dx.doi.org/10.1023/A:1005763023538

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The role of clouds in tropospheric photochemistry (1991)

Lelieveld, J. ; Crutzen, P. J.

Springer

Journal of atmospheric chemistry 12 (1991), S. 229-267

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ISSN: 1573-0662

Keywords: Troposphere ; photochemistry ; clouds ; ozone

Source: Springer Online Journal Archives 1860-2000

Topics: Chemistry and Pharmacology , Geosciences

Notes: Abstract We show that photochemical processes in the lower half of the troposphere are strongly affected by the presence of liquid water clouds. Especially CH2O, an important intermediate of CH4 (and of other hydrocarbon) oxidation, is subject to enhanced breakdown in the aqueous phase. This reduces the formation of HO x -radicals via photodissociation of CH2O in the gas phase. In the droplets, the hydrated form of CH2O, its oxidation product HCO2 −, and H2O2 recycle O2 − radicals which, in turn, react with ozone. We show that the latter reaction is a significant sink for O3. Further O3 concentrations are reduced as a result of decreased formation of O3 during periods with clouds. Additionally, NO x , which acts as a catalyst in the photochemical formation of O3, is depleted by clouds during the night via scavenging of N2O5. This significantly reduces NO x -concentrations during subsequent daylight hours, so that less NO x is available for O3 production. Clouds thus directly reduce the concentrations of O3, CH2O, NO x , and HO x . Indirectly, this also affects the budgets of other trace gases, such as H2O2, CO, and H2.

Type of Medium: Electronic Resource

URL: http://dx.doi.org/10.1007/BF00048075

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The calculation of transboundary and deposition fluxes of SO2 and sulfate by means of aircraft measurements (1988)

Lelieveld, J.

Springer

Water, air & soil pollution 38 (1988), S. 199-209

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ISSN: 1573-2932

Source: Springer Online Journal Archives 1860-2000

Topics: Energy, Environment Protection, Nuclear Power Engineering

Notes: Abstract Aircraft measurements of the air pollutants SO2 and sulfate (SOx is defined as SO2 plus sulfate), plus data on wind velocity, wind direction and depth of the planetary boundary layer, enable the calculation of transboundary mass fluxes of SOx. When emission data are available, an emission-deposition balance of SOx can be determined. The results of a measurement flight, carried out on 12 February, 1986, are presented. Two tracks were flown, along the eastern and along the western border of the Netherlands, respectively. The wind was easterly. The calculated deposition flux of SOx is converted to an area-averaged dry deposition velocity (ν d ). The result, ν d = 1.2 × 10−2 m s−1, seems to be in good agreement with literature data.

Type of Medium: Electronic Resource

URL: http://dx.doi.org/10.1007/BF00279598

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