Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks (Alaska), the Northern Hemisphere, and the Contiguous United States.

IF 5.2 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES
Atmospheric Chemistry and Physics Pub Date : 2025-03-01 Epub Date: 2025-03-18 DOI:10.5194/acp-25-3287-2025
Sara L Farrell, Havala O T Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, Fengkui Duan, Tao Ma, Shuping Zhang, Kathleen Fahey
{"title":"Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks (Alaska), the Northern Hemisphere, and the Contiguous United States.","authors":"Sara L Farrell, Havala O T Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, Fengkui Duan, Tao Ma, Shuping Zhang, Kathleen Fahey","doi":"10.5194/acp-25-3287-2025","DOIUrl":null,"url":null,"abstract":"<p><p>A portion of Alaska's Fairbanks North Star Borough was designated as nonattainment for the 2006 24 h fine particulate matter 2.5 μm or less in diameter (PM<sub>2.5</sub>) National Ambient Air Quality Standards (NAAQS) in 2009. PM<sub>2.5</sub> NAAQS exceedances in Fairbanks mainly occur during dark and cold winters, when temperature inversions form and trap high emissions at the surface. Sulfate ( <math> <mrow><msubsup><mtext>SO</mtext> <mn>4</mn> <mrow><mn>2</mn> <mo>-</mo></mrow> </msubsup> </mrow> </math> ), often the second-largest contributor to PM<sub>2.5</sub> mass during these wintertime PM episodes, is underpredicted by atmospheric chemical transport models (CTMs). Most CTMs account for primary <math> <mrow><msubsup><mtext>SO</mtext> <mn>4</mn> <mrow><mn>2</mn> <mo>-</mo></mrow> </msubsup> </mrow> </math> and secondary <math> <mrow><msubsup><mtext>SO</mtext> <mn>4</mn> <mrow><mn>2</mn> <mo>-</mo></mrow> </msubsup> </mrow> </math> formed via gas-phase oxidation of sulfur dioxide ( <math> <mrow><msub><mtext>SO</mtext> <mn>2</mn></msub> </mrow> </math> ) and in-cloud aqueous oxidation of dissolved S(IV). Dissolution and reaction of <math> <mrow><msub><mtext>SO</mtext> <mn>2</mn></msub> </mrow> </math> in aqueous aerosols are generally not included in CTMs but can be represented as heterogeneous reactive uptake and may help better represent the high <math> <mrow><msubsup><mtext>SO</mtext> <mn>4</mn> <mrow><mn>2</mn> <mo>-</mo></mrow> </msubsup> </mrow> </math> concentrations observed during Fairbanks winters. In addition, hydroxymethanesulfonate (HMS), a particulate sulfur species sometimes misidentified as <math> <mrow><msubsup><mtext>SO</mtext> <mn>4</mn> <mrow><mn>2</mn> <mo>-</mo></mrow> </msubsup> </mrow> </math> , is known to form during Fairbanks winters. Heterogeneous formation of <math> <mrow><msubsup><mtext>SO</mtext> <mn>4</mn> <mrow><mn>2</mn> <mo>-</mo></mrow> </msubsup> </mrow> </math> and HMS in aerosol liquid water (ALW) was implemented in the Community Multiscale Air Quality (CMAQ) modeling system. CMAQ simulations were performed for wintertime PM episodes in Fairbanks (2008) as well as over the Northern Hemisphere and Contiguous United States (CONUS) for 2015-2016. The added heterogeneous sulfur chemistry reduced model mean sulfate bias by ~0.6 μg m<sup>-3</sup> during a cold winter PM episode in Fairbanks, AK. Improvements in model performance are also seen in Beijing during wintertime haze events (reducing model mean sulfate bias by ~2.9 μgS m<sup>-3</sup>). This additional sulfur chemistry also improves modeled summertime <math> <mrow><msubsup><mtext>SO</mtext> <mn>4</mn> <mrow><mn>2</mn> <mo>-</mo></mrow> </msubsup> </mrow> </math> bias in the southeastern US, with implications for future modeling of biogenic organosulfates.</p>","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"25 5","pages":"3287-3312"},"PeriodicalIF":5.2000,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12181941/pdf/","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Atmospheric Chemistry and Physics","FirstCategoryId":"89","ListUrlMain":"https://doi.org/10.5194/acp-25-3287-2025","RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/3/18 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
引用次数: 0

Abstract

A portion of Alaska's Fairbanks North Star Borough was designated as nonattainment for the 2006 24 h fine particulate matter 2.5 μm or less in diameter (PM2.5) National Ambient Air Quality Standards (NAAQS) in 2009. PM2.5 NAAQS exceedances in Fairbanks mainly occur during dark and cold winters, when temperature inversions form and trap high emissions at the surface. Sulfate ( SO 4 2 - ), often the second-largest contributor to PM2.5 mass during these wintertime PM episodes, is underpredicted by atmospheric chemical transport models (CTMs). Most CTMs account for primary SO 4 2 - and secondary SO 4 2 - formed via gas-phase oxidation of sulfur dioxide ( SO 2 ) and in-cloud aqueous oxidation of dissolved S(IV). Dissolution and reaction of SO 2 in aqueous aerosols are generally not included in CTMs but can be represented as heterogeneous reactive uptake and may help better represent the high SO 4 2 - concentrations observed during Fairbanks winters. In addition, hydroxymethanesulfonate (HMS), a particulate sulfur species sometimes misidentified as SO 4 2 - , is known to form during Fairbanks winters. Heterogeneous formation of SO 4 2 - and HMS in aerosol liquid water (ALW) was implemented in the Community Multiscale Air Quality (CMAQ) modeling system. CMAQ simulations were performed for wintertime PM episodes in Fairbanks (2008) as well as over the Northern Hemisphere and Contiguous United States (CONUS) for 2015-2016. The added heterogeneous sulfur chemistry reduced model mean sulfate bias by ~0.6 μg m-3 during a cold winter PM episode in Fairbanks, AK. Improvements in model performance are also seen in Beijing during wintertime haze events (reducing model mean sulfate bias by ~2.9 μgS m-3). This additional sulfur chemistry also improves modeled summertime SO 4 2 - bias in the southeastern US, with implications for future modeling of biogenic organosulfates.

非均质化学途径对费尔班克斯(阿拉斯加)、北半球和美国本土颗粒硫的预测影响。
2009年,阿拉斯加州费尔班克斯北星区的一部分地区被指定为2006年24小时直径小于2.5 μm的细颗粒物(PM2.5)不达标国家环境空气质量标准(NAAQS)。费尔班克斯的PM2.5超标主要发生在黑暗和寒冷的冬季,当逆温形成并在地表捕获高排放时。在这些冬季PM事件中,硫酸盐(so42 -)通常是PM2.5质量的第二大贡献者,但大气化学输送模式(CTMs)对其预测不足。大多数CTMs是由二氧化硫(so2)的气相氧化和云内溶解S(IV)的水氧化形成的初级so42 -和次级so42 -组成的。so2在含水气溶胶中的溶解和反应通常不包括在CTMs中,但可以表示为非均质反应性吸收,并可能有助于更好地表示费尔班克斯冬季观察到的高so42 -浓度。此外,费尔班克斯冬季还会形成羟基甲磺酸盐(HMS),这是一种微粒硫,有时会被误认为是so42 -。在社区多尺度空气质量(CMAQ)模拟系统中实现了气溶胶液态水(ALW)中so42 -和HMS的非均相形成。CMAQ模拟了费尔班克斯(2008年)以及北半球和美国本土(2015-2016年)的冬季PM事件。在费尔班克斯,AK寒冷的冬季PM事件中,添加的非均相硫化学减少模型平均硫酸盐偏差约0.6 μg m-3。在冬季雾霾事件期间,北京的模式性能也有所改善(将模式平均硫酸盐偏差降低了约2.9 μgS m-3)。这种额外的硫化学反应也改善了美国东南部夏季模拟的so42 -偏差,这对未来生物源有机硫酸盐的模拟具有重要意义。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
Atmospheric Chemistry and Physics
Atmospheric Chemistry and Physics 地学-气象与大气科学
CiteScore
10.70
自引率
20.60%
发文量
702
审稿时长
6 months
期刊介绍: Atmospheric Chemistry and Physics (ACP) is a not-for-profit international scientific journal dedicated to the publication and public discussion of high-quality studies investigating the Earth''s atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere, and mesosphere. The main subject areas comprise atmospheric modelling, field measurements, remote sensing, and laboratory studies of gases, aerosols, clouds and precipitation, isotopes, radiation, dynamics, biosphere interactions, and hydrosphere interactions. The journal scope is focused on studies with general implications for atmospheric science rather than investigations that are primarily of local or technical interest.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信