Interactions between Organic Oxidation and Acid-base Chemistry during Particle Formation and Growth

颗粒形成和生长过程中有机氧化和酸碱化学之间的相互作用

• 批准号: 2132089
• 负责人: Neil Donahue
• 金额: $ 84.92万
• 依托单位: Carnegie-Mellon University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-01-01 至 2024-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2132089&HistoricalAwards=false
• 关键词: Interactions; between; Organic; Oxidation; Acid

This project involves the investigation of the formation and growth of new particles in the atmosphere. The effort includes the design and participation of experiments as part of the Cosmics Leaving Outdoor Droplets (CLOUD) consortium at CERN and participation in complementary experiments at Carnegie Mellon University (CMU). By improving the understanding of mechanisms for new particle formation, this project addresses vital national and international interests associated with climate change and air quality.This effort will study new particle formation involving nitric acid, sulfuric acid, ammonia, and amines, and particle formation by highly oxygenated organic compounds from both terpene and aromatic precursors. Experiments seek to answer the following questions: (1) How do the temperature dependencies of autoxidation as well as peroxy-radical ‘dimerization’ reactions across different systems (i.e., α pinene−RO2 + isoprene−RO2 → ROOR+O2) combine to control particle formation and growth in “pure organic” systems? (2) Do oxidized-organic and acid-base systems interact synergistically or independently during particle formation and growth, or can they even ‘spoil’ each other and inhibit nucleation? The two interconnected projects will focus on the interactions between acids, bases, and highly oxidized (and polar) organics ranging from particle formation itself to growth up to 5-10 nm. Key issues are to determine when nitric acid participates directly in particle formation versus activating growth of formed particles, and whether the acid-base and organic particle formation pathways proceed independently in the atmosphere or interact, either synergistically or antagonistically. Observables including measured formation and growth rates, gas-phase vapor measurements, and particle composition will combine to tightly constrain these coupled systems. At CLOUD the CMU team will use an iodide chemical ionization mass spectrometer to measure the composition of gases and growing particles, the later by thermal desorption from teflon filters (FIGAERO CIMS).This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

该项目涉及对大气中新粒子的形成和生长的研究。这项工作包括设计和参与实验，作为欧洲核子研究中心的宇宙学离开户外水滴（CLOUD）联盟的一部分，并参与卡内基梅隆大学（CMU）的补充实验。通过提高对新粒子形成机制的认识，该项目将致力于解决与气候变化和空气质量相关的重大国家和国际利益。该项目将研究涉及硝酸、硫酸、氨和胺的新粒子形成，以及萜烯和芳香族前体的高度氧化有机化合物的粒子形成。实验试图回答以下问题：（1）在不同的系统中，自氧化以及过氧自由基“二聚”反应的温度依赖性如何（即，α-蒎烯− RO 2+异戊二烯− RO 2 → ROOR+ O 2）联合收割机控制“纯有机”系统中颗粒的形成和生长？(2)氧化有机物和酸碱系统在颗粒形成和生长过程中是协同作用还是独立作用，或者它们甚至可以相互“破坏”并抑制成核？ 这两个相互关联的项目将专注于酸，碱和高度氧化（和极性）有机物之间的相互作用，从颗粒形成本身到生长到5-10 nm。关键问题是确定硝酸何时直接参与颗粒形成与活化形成颗粒的生长，以及酸碱和有机颗粒形成途径是否在大气中独立进行或相互作用，协同或拮抗。包括测量的形成和生长速率、气相蒸汽测量和颗粒组成在内的可观测量将联合收割机紧密地约束这些耦合系统。在CLOUD，CMU团队将使用碘化物化学电离质谱仪测量气体和增长颗粒的组成，后者通过从TECHNOLOGY过滤器（FIGAERO CIMS）的热解吸来测量。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Iodine oxoacids enhance nucleation of sulfuric acid particles in the atmosphere

• DOI: 10.1126/science.adh2526
• 发表时间: 2023-12
• 期刊: Science
• 影响因子: 56.9
• 作者: Xucheng He;M. Simon;Siddharth Iyer;Hong-Bin Xie;B. Rörup;Jiali Shen;Henning Finkenzeller;D. Stolzenburg;Rongjie Zhang;A. Baccarini;Y. J. Tham;Mingyi Wang;Stavros Amanatidis;A. A. Piedehierro-A.;A. Amorim;Rima Baalbaki;Zoé Brasseur;L. Caudillo;Biwu Chu;L. Dada;J. Duplissy;I. El Haddad;R. Flagan;Manuel Granzin;A. Hansel;M. Heinritzi;V. Hofbauer;T. Jokinen;D. Kemppainen;W. Kong;J. Krechmer;A. Kürten;Houssni Lamkaddam;Brandon Lopez;Fangfang Ma;Naser G. A. Mahfouz;Vladimir Makhmutov;Hanna E. Manninen;Guillaume Marie;R. Marten;Dario Massabò;R. Mauldin;B. Mentler;A. Onnela;T. Petäjä;Joschka Pfeifer;M. Philippov;A. Ranjithkumar;M. Rissanen;S. Schobesberger;W. Scholz;Benjamin Schulze;Mihnea Surdu;R. Thakur;A. Tomé;A. Wagner;Dongyu S. Wang;Yonghong Wang;Stefan K. Weber;A. Welti;P. Winkler;Marcel Zauner-Wieczorek;U. Baltensperger;J. Curtius;T. Kurtén;D. Worsnop;R. Volkamer;K. Lehtipalo;J. Kirkby;Neil M. Donahue;M. Sipilä;M. Kulmala

Sulfur Dioxide Transported From the Residual Layer Drives Atmospheric Nucleation During Haze Periods in Beijing

• DOI: 10.1029/2022gl100514
• 发表时间: 2023-03
• 期刊: Geophysical Research Letters
• 影响因子: 5.2
• 作者: Yonghong Wang;Yongjing Ma;Chao Yan;L. Yao;Runlong Cai;Shuying Li;Zhuohui Lin;Xiujuan Zhao;Rujing Yin;C. Deng;J. Kangasluoma;Xucheng He;S. Hakala;Xiaolong Fan;Siyu Chen;Qingxin Ma;V. Kerminen;T. Petäjä;J. Xin;Lin Wang;Baoxian Liu;Weigang Wang;Maofa Ge;Jingkun Jiang;Yongchun Liu;Federico Bianchi;Biwu Chu;N. Donahue;S. Martin;Hong S. He;M. Kulmala

Precursor apportionment of atmospheric oxygenated organic molecules using a machine learning method

使用机器学习方法对大气含氧有机分子进行前体分配

• DOI: 10.1039/d2ea00128d
• 发表时间: 2023
• 期刊: Environmental Science: Atmospheres
• 作者: Qiao, Xiaohui;Li, Xiaoxiao;Yan, Chao;Sarnela, Nina;Yin, Rujing;Guo, Yishuo;Yao, Lei;Nie, Wei;Huang, Dandan;Wang, Zhe
• 通讯作者: Wang, Zhe

An intercomparison study of four different techniques for measuring the chemical composition of nanoparticles

四种不同纳米颗粒化学成分测量技术的比较研究

• DOI: 10.5194/acp-23-6613-2023
• 发表时间: 2023
• 期刊: Atmospheric Chemistry and Physics
• 影响因子: 6.3
• 作者: Caudillo, Lucía;Surdu, Mihnea;Lopez, Brandon;Wang, Mingyi;Thoma, Markus;Bräkling, Steffen;Buchholz, Angela;Simon, Mario;Wagner, Andrea C.;Müller, Tatjana
• 通讯作者: Müller, Tatjana

Formation Process of Particles and Cloud Condensation Nuclei Over the Amazon Rainforest: The Role of Local and Remote New‐Particle Formation

• DOI: 10.1029/2022gl100940
• 发表时间: 2022-11
• 期刊: Geophysical Research Letters
• 影响因子: 5.2
• 作者: Bin Zhao;J. Fast;M. Shrivastava;N. Donahue;Yang Gao;J. Shilling;Ying Liu;R. Zaveri;B. Gaudet;Shuxiao Wang;Jian Wang;Zeqi Li;Jiwen Fan