Global S&T Development Trend Analysis Platform of Resources and Environment
DOI | 10.5194/acp-18-12765-2018 |
Understanding nitrate formation in a world with less sulfate | |
Vasilakos, Petros1; Russell, Armistead2; Weber, Rodney3; Nenes, Athanasios1,3,4,5,6 | |
2018-09-05 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2018 |
卷号 | 18期号:17页码:12765-12775 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Greece; Switzerland |
英文摘要 | SO2 emission controls, combined with modestly increasing ammonia, have been thought to generate aerosol with significantly reduced acidity for cases in which sulfate is partially substituted by nitrate. However, neither expectation agrees with decadal observations in the southeastern USA, suggesting that a fundamentally different response of aerosol pH to emissions changes is occurring. We postulate that this nitrate substitution paradox arises from a positive bias in aerosol pH in model simulations. This bias can elevate pH to a level at which nitrate partitioning is readily promoted, leading to behavior consistent with nitrate substitution. CMAQ simulations are used to investigate this hypothesis; modeled PM2.5 pH using 2001 emissions compare favorably with pH inferred from observed species concentrations. Using 2011 emissions, however, leads to simulated pH increases of one unit, which is inconsistent with observations from that year. Nonvolatile cations (K+, Na+, Ca+2, and Mg+2) in the fine mode are found to be responsible for the erroneous predicted increase in aerosol pH of about 1 unit on average over the USA. Such an increase can induce a nitrate bias of 1-2 mu g m(-3), which may further increase in future projections, reaffirming an otherwise incorrect expectation of a significant nitrate substitution. Evaluation of predicted aerosol pH against thermodynamic analysis of observations is therefore a critically important, but overlooked, aspect of model evaluation for a robust emissions policy. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000443874100001 |
WOS关键词 | EASTERN UNITED-STATES ; FINE-PARTICLE PH ; SOUTHEASTERN AEROSOL RESEARCH ; CHARACTERIZATION SEARCH ; PARTICULATE MATTER ; ORGANIC AEROSOL ; HAZE EPISODES ; MINERAL DUST ; AMMONIA ; ACIDITY |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/24955 |
专题 | 地球科学 |
作者单位 | 1.Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA; 2.Georgia Inst Technol, Sch Civil & Environm Engn, Atlanta, GA 30332 USA; 3.Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA; 4.Fdn Res & Technol Hellas, Inst Chem Engn Sci, Patras 26504, Greece; 5.Natl Observ Athens, Inst Environm Res & Sustainable Dev, Palea Penteli 15236, Greece; 6.Ecole Polytech Fed Lausanne, Sch Architecture Civil & Environm Engn, CH-1015 Lausanne, Switzerland |
推荐引用方式 GB/T 7714 | Vasilakos, Petros,Russell, Armistead,Weber, Rodney,et al. Understanding nitrate formation in a world with less sulfate[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(17):12765-12775. |
APA | Vasilakos, Petros,Russell, Armistead,Weber, Rodney,&Nenes, Athanasios.(2018).Understanding nitrate formation in a world with less sulfate.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(17),12765-12775. |
MLA | Vasilakos, Petros,et al."Understanding nitrate formation in a world with less sulfate".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.17(2018):12765-12775. |
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