Global S&T Development Trend Analysis Platform of Resources and Environment
DOI | 10.1073/pnas.1803295115 |
Chemical feedbacks weaken the wintertime response of particulate sulfate and nitrate to emissions reductions over the eastern United States | |
Shah, Viral1; Jaegle, Lyatt1; Thornton, Joel A.1; Lopez-Hilfiker, Felipe D.1,12; Lee, Ben H.1; Schroder, Jason C.2,3; Campuzano-Jost, Pedro2,3; Jimenez, Jose L.2,3; Guo, Hongyu4; Sullivan, Amy P.5; Weber, Rodney J.4; Green, Jaime R.6; Fiddler, Marc N.7; Bililign, Solomon7,8; Campos, Teresa L.9,10; Stell, Meghan10,13; Weinheimer, Andrew J.9; Montzka, Denise D.9; Brown, Steven S.2,11 | |
2018-08-07 | |
发表期刊 | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA |
ISSN | 0027-8424 |
出版年 | 2018 |
卷号 | 115期号:32页码:8110-8115 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Switzerland |
英文摘要 | Sulfate (SO42- and nitrate (NO3-) account for half of the fine particulate matter mass over the eastern United States. Their wintertime concentrations have changed little in the past decade despite considerable precursor emissions reductions. The reasons for this have remained unclear because detailed observations to constrain the wintertime gas-particle chemical system have been lacking. We use extensive airborne observations over the eastern United States from the 2015 Wintertime Investigation of Transport, Emissions, and Reactivity (WINTER) campaign; ground-based observations; and the GEOS-Chem chemical transport model to determine the controls on winter SO42- and NO3-. GEOS-Chem reproduces observed SO42--NO3--NH4+ particulate concentrations (2.45 mu g sm(-3)) and composition (SO42-: 47%; NO3-: 32%; NH4+: 21%) during WINTER. Only 18% of SO2 emissions were regionally oxidized to SO42- during WINTER, limited by low [H2O2 ] and [OH]. Relatively acidic fine particulates (pH similar to 1.3) allow 45% of nitrate to partition to the particle phase. Using GEOS-Chem, we examine the impact of the 58% decrease in winter SO2 emissions from 2007 to 2015 and find that the H2O2 limitation on SO2 oxidation weakened, which increased the fraction of SO2 emissions oxidizing to SO42-. Simultaneously, NOx emissions decreased by 35%, but the modeled NO3- particle fraction increased as fine particle acidity decreased. These feedbacks resulted in a 40% decrease of modeled [SO42-] and no change in [NO3-], as observed. Wintertime [SO42-] and [NO3-] are expected to change slowly between 2015 and 2023, unless SO2 and NOx emissions decrease faster in the future than in the recent past. |
英文关键词 | sulfate nitrate winter anthropogenic emissions PM2.5 |
领域 | 地球科学 ; 气候变化 ; 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000440982000038 |
WOS关键词 | AIR-QUALITY TRENDS ; HIGH-RESOLUTION ; POLLUTION ; AEROSOLS ; NITROGEN ; MATTER ; DEPOSITION ; AMMONIA ; SURFACE ; SO2 |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
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/204961 |
专题 | 地球科学 资源环境科学 气候变化 |
作者单位 | 1.Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA; 2.Univ Colorado, Dept Chem, Boulder, CO 80309 USA; 3.Univ Colorado, CIRES, Boulder, CO 80309 USA; 4.Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA; 5.Colorado State Univ, Dept Atmospher Sci, Ft Collins, CO 80523 USA; 6.North Carolina A&T State Univ, Dept Energy & Environm Syst, Greensboro, NC 27411 USA; 7.North Carolina A&T State Univ, NOAA, ISET Cooperat Sci Ctr, Greensboro, NC 27411 USA; 8.North Carolina A&T State Univ, Dept Phys, Greensboro, NC 27411 USA; 9.Natl Ctr Atmospher Res, Atmospher Chem Observat & Modeling Lab, Boulder, CO 80305 USA; 10.Natl Ctr Atmospher Res, Earth Observing Lab, Boulder, CO 80305 USA; 11.NOAA, Chem Sci Div, Earth Syst Res Lab, Boulder, CO 80305 USA; 12.TOFWERK AG, CH-3600 Thun, Switzerland; 13.Calif State Univ, Undergrad Res Opportun Ctr, Monterey, CA 93955 USA |
推荐引用方式 GB/T 7714 | Shah, Viral,Jaegle, Lyatt,Thornton, Joel A.,et al. Chemical feedbacks weaken the wintertime response of particulate sulfate and nitrate to emissions reductions over the eastern United States[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2018,115(32):8110-8115. |
APA | Shah, Viral.,Jaegle, Lyatt.,Thornton, Joel A..,Lopez-Hilfiker, Felipe D..,Lee, Ben H..,...&Brown, Steven S..(2018).Chemical feedbacks weaken the wintertime response of particulate sulfate and nitrate to emissions reductions over the eastern United States.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,115(32),8110-8115. |
MLA | Shah, Viral,et al."Chemical feedbacks weaken the wintertime response of particulate sulfate and nitrate to emissions reductions over the eastern United States".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 115.32(2018):8110-8115. |
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