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DOI10.1073/pnas.2113265119
Catalytic role of formaldehyde in particulate matter formation
Dovrou E.; Bates K.H.; Moch J.M.; Mickley L.J.; Jacob D.J.; Keutsch F.N.
发表日期2022
ISSN0027-8424
卷号119期号:6
英文摘要Formaldehyde (HCHO), the simplest and most abundant carbonyl in the atmosphere, contributes to particulate matter (PM) formation via two in-cloud processing pathways. First, in a catalytic pathway, HCHO reacts with hydrogen peroxide (H2O2) to form hydroxymethyl hydroperoxide (HMHP), which rapidly oxidizes dissolved sulfur dioxide (SO2,aq) to sulfate, regenerating HCHO. Second, HCHO reacts with dissolved SO2,aq to form hydroxymethanesulfonate (HMS), which upon oxidation with the hydroxyl radical (OH) forms sulfate and also reforms HCHO. Chemical transport model simulations using rate coefficients from laboratory studies of the reaction rate of HMHP with SO2,aq show that the HMHP pathways reduce the SO2 lifetime by up to a factor of 2 and contribute up to ∼18% of global sulfate. This contribution rises to >50% in isoprenedominated regions such as the Amazon. Combined with recent results on HMS, this work demonstrates that the one-carbon molecules HMHP and HCHO contribute significantly to global PM, with HCHO playing a crucial catalytic role. © 2022 National Academy of Sciences. All rights reserved.
英文关键词Catalysis; Dissolved sulfur dioxide; Formaldehyde; Hydroxymethanesulfonate; Hydroxymethyl hydroperoxide
语种英语
scopus关键词carbon; carbonyl derivative; formaldehyde; hydrogen peroxide; hydroxyl radical; hydroxymethanesulfonate; isoprene; sulfate; sulfonic acid derivative; sulfur dioxide; unclassified drug; aqueous solution; Article; catalysis; chemical reaction; mathematical analysis; oxidation; particulate matter; simulation; transport kinetics
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/250877
作者单位John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, United States; Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138, United States; Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, United States
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Dovrou E.,Bates K.H.,Moch J.M.,et al. Catalytic role of formaldehyde in particulate matter formation[J],2022,119(6).
APA Dovrou E.,Bates K.H.,Moch J.M.,Mickley L.J.,Jacob D.J.,&Keutsch F.N..(2022).Catalytic role of formaldehyde in particulate matter formation.Proceedings of the National Academy of Sciences of the United States of America,119(6).
MLA Dovrou E.,et al."Catalytic role of formaldehyde in particulate matter formation".Proceedings of the National Academy of Sciences of the United States of America 119.6(2022).
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