Changing aerosol chemistry is redefining HONO sources

IF 15.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2025-06-05 DOI:10.1038/s41467-025-60614-7

Yusheng Zhang, Yongchun Liu, Wei Ma, Chenjie Hua, Feixue Zheng, Chaofan Lian, Weigang Wang, Men Xia, Zhixin Zhao, Jinwen Li, Jiali Xie, Zongcheng Wang, Yuzheng Wang, Xin Chen, Ying Zhang, Zemin Feng, Chao Yan, Biwu Chu, Wei Du, Veli-Matti Kerminen, Federico Bianchi, Tuukka Petäjä, Douglas Worsnop, Markku Kulmala

{"title":"Changing aerosol chemistry is redefining HONO sources","authors":"Yusheng Zhang, Yongchun Liu, Wei Ma, Chenjie Hua, Feixue Zheng, Chaofan Lian, Weigang Wang, Men Xia, Zhixin Zhao, Jinwen Li, Jiali Xie, Zongcheng Wang, Yuzheng Wang, Xin Chen, Ying Zhang, Zemin Feng, Chao Yan, Biwu Chu, Wei Du, Veli-Matti Kerminen, Federico Bianchi, Tuukka Petäjä, Douglas Worsnop, Markku Kulmala","doi":"10.1038/s41467-025-60614-7","DOIUrl":null,"url":null,"abstract":"Heterogeneous reactions of NO2 on particulate matter have been considered an important source of HONO (Nitrous acid) in the troposphere, whereas its contribution is controversial due to the lack of uptake coefficient of NO2 (γNO2) on the surfaces of ambient particulate matter (PM). Here we investigate the the γNO2 to form HONO and its evolution based on long-term comprehensive field observations (2019–2023) in Beijing and a random forest model with Shapley additive explanations. The γNO2 on ambient PM is on the order of 10−6, decreasing markedly from 3.07 ± 5.99 × 10−6 in 2019 to 1.43 ± 3.22 × 10−6 in 2023. This decrease is driven by the increase in aerosol pH, linked to increased ratio of NH4NO3 to (NH4)2SO4, resulting from an unbalanced desulfurization and denitrification. This study implies that the role of the heterogeneous reaction of NO2 on aerosol surfaces in HONO production is declining in Beijing, providing valuable insights into the atmospheric chemistry in urban environments.","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"5 1","pages":""},"PeriodicalIF":15.7000,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-025-60614-7","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

Abstract

Heterogeneous reactions of NO₂ on particulate matter have been considered an important source of HONO (Nitrous acid) in the troposphere, whereas its contribution is controversial due to the lack of uptake coefficient of NO₂ (γ_NO2) on the surfaces of ambient particulate matter (PM). Here we investigate the the γ_NO2 to form HONO and its evolution based on long-term comprehensive field observations (2019–2023) in Beijing and a random forest model with Shapley additive explanations. The γ_NO2 on ambient PM is on the order of 10⁻⁶, decreasing markedly from 3.07 ± 5.99 × 10⁻⁶ in 2019 to 1.43 ± 3.22 × 10⁻⁶ in 2023. This decrease is driven by the increase in aerosol pH, linked to increased ratio of NH₄NO₃ to (NH₄)₂SO₄, resulting from an unbalanced desulfurization and denitrification. This study implies that the role of the heterogeneous reaction of NO₂ on aerosol surfaces in HONO production is declining in Beijing, providing valuable insights into the atmospheric chemistry in urban environments.

Abstract Image

查看原文本刊更多论文

不断变化的气溶胶化学正在重新定义HONO来源

NO2在颗粒物上的非均相反应被认为是对流层中HONO（亚硝酸）的重要来源，但由于环境颗粒物（PM）表面缺乏NO2的吸收系数（γNO2），其贡献存在争议。本文基于北京地区2019-2023年的长期综合野外观测资料和Shapley加性解释的随机森林模型，研究了γNO2形成HONO的过程及其演变。大气PM上的γNO2为10−6量级，从2019年的3.07±5.99 × 10−6显著下降到2023年的1.43±3.22 × 10−6。这种减少是由气溶胶pH值的增加所驱动的，这与由不平衡的脱硫和反硝化引起的NH4NO3与（NH4）2SO4的比例增加有关。该研究表明，NO2在气溶胶表面的非均相反应在北京地区HONO产生中的作用正在减弱，为了解城市环境的大气化学提供了有价值的见解。

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

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.