气候变化领域集成服务门户(CCPortal): Large uncertainties in global hydroxyl projections tied to fate of reactive nitrogen and carbon

CCPortal

DOI	10.1073/pnas.2115204118
	Large uncertainties in global hydroxyl projections tied to fate of reactive nitrogen and carbon
	Murray L.T.; Fiore A.M.; Shindell D.T.; Naik V.; Horowitz L.W.
发表日期	2021
ISSN	0027-8424
卷号	118 期号:43
英文摘要	The hydroxyl radical (OH) sets the oxidative capacity of the atmosphere and, thus, profoundly affects the removal rate of pollutants and reactive greenhouse gases. While observationally derived constraints exist for global annual mean present-day OH abundances and interannual variability, OH estimates for past and future periods rely primarily on global atmospheric chemistry models. These models disagree ± 30% in mean OH and in its changes from the preindustrial to late 21st century, even when forced with identical anthropogenic emissions. A simple steady-state relationship that accounts for ozone photolysis frequencies, water vapor, and the ratio of reactive nitrogen to carbon emissions explains temporal variability within most models, but not intermodel differences. Here, we show that departure from the expected relationship reflects the treatment of reactive oxidized nitrogen species (NOy) and the fraction of emitted carbon that reacts within each chemical mechanism, which remain poorly known due to a lack of observational data. Our findings imply a need for additional observational constraints on NOy partitioning and lifetime, especially in the remote free troposphere, as well as the fate of carbon-containing reaction intermediates to test models, thereby reducing uncertainties in projections of OH and, hence, lifetimes of pollutants and greenhouse gases. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Atmospheric oxidative capacity; Forecasting change; Hydroxyl
语种	英语
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/238329
作者单位	Department of Earth and Environmental Sciences, University of Rochester, Rochester, NY 14627, United States; Department of Earth and Environmental Sciences, Columbia University, New York, NY 10027, United States; Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY 10964, United States; Nicholas School of the Environment, Duke University, Durham, NC 27708, United States; Geophysical Fluid Dynamics Laboratory, National Oceanic and Atmospheric Administration, Princeton, NJ 08540, United States
推荐引用方式 GB/T 7714	Murray L.T.,Fiore A.M.,Shindell D.T.,et al. Large uncertainties in global hydroxyl projections tied to fate of reactive nitrogen and carbon[J],2021,118(43).
APA	Murray L.T.,Fiore A.M.,Shindell D.T.,Naik V.,&Horowitz L.W..(2021).Large uncertainties in global hydroxyl projections tied to fate of reactive nitrogen and carbon.Proceedings of the National Academy of Sciences of the United States of America,118(43).
MLA	Murray L.T.,et al."Large uncertainties in global hydroxyl projections tied to fate of reactive nitrogen and carbon".Proceedings of the National Academy of Sciences of the United States of America 118.43(2021).