Hannah S. Kenagy, Colette L. Heald, Nadia Tahsini, Matthew B. Goss, Jesse H. Kroll
{"title":"我们能否在实验室中实现大气化学环境?室内 SOA 研究的综合模型测量方法","authors":"Hannah S. Kenagy, Colette L. Heald, Nadia Tahsini, Matthew B. Goss, Jesse H. Kroll","doi":"10.1126/sciadv.ado1482","DOIUrl":null,"url":null,"abstract":"<div >Secondary organic aerosol (SOA), atmospheric particulate matter formed from low-volatility products of volatile organic compound (VOC) oxidation, affects both air quality and climate. Current 3D models, however, cannot reproduce the observed variability in atmospheric organic aerosol. Because many SOA model descriptions are derived from environmental chamber experiments, our ability to represent atmospheric conditions in chambers directly affects our ability to assess the air quality and climate impacts of SOA. Here, we develop an approach that leverages global modeling and detailed mechanisms to design chamber experiments that mimic the atmospheric chemistry of organic peroxy radicals (RO<sub>2</sub>), a key intermediate in VOC oxidation. Drawing on decades of laboratory experiments, we develop a framework for quantitatively describing RO<sub>2</sub> chemistry and show that no previous experimental approaches to studying SOA formation have accessed the relevant atmospheric RO<sub>2</sub> fate distribution. We show proof-of-concept experiments that demonstrate how SOA experiments can access a range of atmospheric chemical environments and propose several directions for future studies.</div>","PeriodicalId":21609,"journal":{"name":"Science Advances","volume":null,"pages":null},"PeriodicalIF":11.7000,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.science.org/doi/reader/10.1126/sciadv.ado1482","citationCount":"0","resultStr":"{\"title\":\"Can we achieve atmospheric chemical environments in the laboratory? An integrated model-measurement approach to chamber SOA studies\",\"authors\":\"Hannah S. Kenagy, Colette L. Heald, Nadia Tahsini, Matthew B. Goss, Jesse H. Kroll\",\"doi\":\"10.1126/sciadv.ado1482\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div >Secondary organic aerosol (SOA), atmospheric particulate matter formed from low-volatility products of volatile organic compound (VOC) oxidation, affects both air quality and climate. Current 3D models, however, cannot reproduce the observed variability in atmospheric organic aerosol. Because many SOA model descriptions are derived from environmental chamber experiments, our ability to represent atmospheric conditions in chambers directly affects our ability to assess the air quality and climate impacts of SOA. Here, we develop an approach that leverages global modeling and detailed mechanisms to design chamber experiments that mimic the atmospheric chemistry of organic peroxy radicals (RO<sub>2</sub>), a key intermediate in VOC oxidation. Drawing on decades of laboratory experiments, we develop a framework for quantitatively describing RO<sub>2</sub> chemistry and show that no previous experimental approaches to studying SOA formation have accessed the relevant atmospheric RO<sub>2</sub> fate distribution. We show proof-of-concept experiments that demonstrate how SOA experiments can access a range of atmospheric chemical environments and propose several directions for future studies.</div>\",\"PeriodicalId\":21609,\"journal\":{\"name\":\"Science Advances\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":11.7000,\"publicationDate\":\"2024-09-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.science.org/doi/reader/10.1126/sciadv.ado1482\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science Advances\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://www.science.org/doi/10.1126/sciadv.ado1482\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science Advances","FirstCategoryId":"103","ListUrlMain":"https://www.science.org/doi/10.1126/sciadv.ado1482","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
引用次数: 0
摘要
二次有机气溶胶(SOA)是由挥发性有机化合物(VOC)氧化的低挥发性产物形成的大气颗粒物,对空气质量和气候都有影响。然而,目前的三维模型无法再现观测到的大气有机气溶胶的变化。由于许多 SOA 模型描述都来自环境试验室实验,因此我们在试验室中表现大气条件的能力直接影响到我们评估 SOA 对空气质量和气候影响的能力。在这里,我们开发了一种方法,利用全球建模和详细机制来设计模拟有机过氧自由基(RO2)大气化学性质的室内实验,RO2 是挥发性有机化合物氧化过程中的一个关键中间产物。借鉴数十年的实验室实验,我们建立了一个定量描述 RO2 化学性质的框架,并证明以前研究 SOA 形成的实验方法都无法获得相关的大气 RO2 归宿分布。我们展示了概念验证实验,证明了 SOA 实验如何能够进入一系列大气化学环境,并提出了未来研究的几个方向。
Can we achieve atmospheric chemical environments in the laboratory? An integrated model-measurement approach to chamber SOA studies
Secondary organic aerosol (SOA), atmospheric particulate matter formed from low-volatility products of volatile organic compound (VOC) oxidation, affects both air quality and climate. Current 3D models, however, cannot reproduce the observed variability in atmospheric organic aerosol. Because many SOA model descriptions are derived from environmental chamber experiments, our ability to represent atmospheric conditions in chambers directly affects our ability to assess the air quality and climate impacts of SOA. Here, we develop an approach that leverages global modeling and detailed mechanisms to design chamber experiments that mimic the atmospheric chemistry of organic peroxy radicals (RO2), a key intermediate in VOC oxidation. Drawing on decades of laboratory experiments, we develop a framework for quantitatively describing RO2 chemistry and show that no previous experimental approaches to studying SOA formation have accessed the relevant atmospheric RO2 fate distribution. We show proof-of-concept experiments that demonstrate how SOA experiments can access a range of atmospheric chemical environments and propose several directions for future studies.
期刊介绍:
Science Advances, an open-access journal by AAAS, publishes impactful research in diverse scientific areas. It aims for fair, fast, and expert peer review, providing freely accessible research to readers. Led by distinguished scientists, the journal supports AAAS's mission by extending Science magazine's capacity to identify and promote significant advances. Evolving digital publishing technologies play a crucial role in advancing AAAS's global mission for science communication and benefitting humankind.