The gas-phase formation mechanism of iodic acid as an atmospheric aerosol source

被引:37
作者
Finkenzeller, Henning [1 ,2 ]
Iyer, Siddharth [3 ]
He, Xu-Cheng [4 ]
Simon, Mario [5 ]
Koenig, Theodore K. [1 ,2 ,6 ]
Lee, Christopher F. [1 ,2 ]
Valiev, Rashid [7 ]
Hofbauer, Victoria [8 ]
Amorim, Antonio [9 ,10 ]
Baalbaki, Rima [4 ]
Baccarini, Andrea [11 ,12 ]
Beck, Lisa [4 ]
Bell, David M. [11 ]
Caudillo, Lucia [5 ]
Chen, Dexian [8 ]
Chiu, Randall [1 ,2 ]
Chu, Biwu [4 ,13 ]
Dada, Lubna [4 ,11 ]
Duplissy, Jonathan [4 ,14 ]
Heinritzi, Martin [5 ]
Kemppainen, Deniz [4 ]
Kim, Changhyuk [15 ,16 ]
Krechmer, Jordan [17 ]
Kurten, Andreas [5 ]
Kvashnin, Alexandr [18 ]
Lamkaddam, Houssni [11 ]
Lee, Chuan Ping [11 ]
Lehtipalo, Katrianne [4 ,19 ]
Li, Zijun [20 ]
Makhmutov, Vladimir [18 ,21 ]
Manninen, Hanna E. [22 ]
Marie, Guillaume [5 ]
Marten, Ruby [11 ]
Mauldin, Roy L. [1 ,8 ]
Mentler, Bernhard [23 ]
Muller, Tatjana [5 ]
Petaja, Tuukka [4 ]
Philippov, Maxim [18 ]
Ranjithkumar, Ananth [24 ]
Rorup, Birte [4 ]
Shen, Jiali [4 ]
Stolzenburg, Dominik [4 ,25 ]
Tauber, Christian [25 ]
Tham, Yee Jun [4 ,26 ]
Tome, Antonio [27 ]
Vazquez-Pufleau, Miguel [25 ]
Wagner, Andrea C. [1 ,2 ,5 ]
Wang, Dongyu S. [11 ]
Wang, Mingyi [16 ]
Wang, Yonghong [4 ,13 ]
机构
[1] Univ Colorado Boulder, Dept Chem, Boulder, CO USA
[2] Univ Colorado Boulder, Cooperat Inst Res Environm Sci, Boulder, CO USA
[3] Tampere Univ, Fac Engn & Nat Sci, Phys Unit, Aerosol Phys Lab, Tampere, Finland
[4] Univ Helsinki, Inst Atmospher & Earth Syst Res, Helsinki, Finland
[5] Goethe Univ Frankfurt, Inst Atmospher & Environm Sci, Frankfurt, Germany
[6] Peking Univ, Coll Environm Sci & Engn, State Key Joint Lab Environm Simulat & Pollut Con, BIC ESAT & IJRC, Beijing, Beijing, Peoples R China
[7] Univ Helsinki, Dept Chem, Helsinki, Finland
[8] Carnegie Mellon Univ, Ctr Atmospher Particle Studies, Pittsburgh, PA USA
[9] Univ Lisbon, CENTRA, Lisbon, Portugal
[10] Univ Lisbon, Fac Ciencias, Lisbon, Portugal
[11] Paul Scherrer Inst, Lab Atmospher Chem, Villigen, Switzerland
[12] Ecole Polytech Fed Lausanne, Extreme Environm Res Lab, Lausanne, Switzerland
[13] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Beijing, Beijing, Peoples R China
[14] Univ Helsinki, Helsinki Inst Phys, Fac Sci, Phys, Helsinki, Finland
[15] Pusan Natl Univ, Sch Civil & Environm Engn, Busan, South Korea
[16] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
[17] Aerodyne Res, Billerica, MA USA
[18] Russian Acad Sci, Lebedev Phys Inst, Moscow, Russia
[19] Finnish Meteorol Inst, Helsinki, Finland
[20] Univ Eastern Finland, Dept Appl Phys, Kuopio, Finland
[21] Natl Res Univ, Moscow Inst Phys & Technol, Moscow, Russia
[22] CERN, European Org Nucl Res, Geneva, Switzerland
[23] Univ Innsbruck, Inst & Appl Phys, Innsbruck, Austria
[24] Univ Leeds, Sch Earth & Environm, Leeds, England
[25] Univ Vienna, Fac Phys, Vienna, Austria
[26] Sun Yat Sen Univ, Sch Marine Sci, Zhuhai, Peoples R China
[27] Univ Beira Interior, IDL, Covilha, Portugal
[28] Nanjing Univ, Sch Atmospher Sci, Joint Int Res Lab Atmospher & Earth Syst Res, Nanjing, Peoples R China
[29] Univ Reunion, LACy UMR8105, St Denis, France
[30] Beijing Univ Chem Technol BUCT, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Aerosol & Haze Lab, Beijing, Peoples R China
基金
欧盟地平线“2020”; 美国安德鲁·梅隆基金会; 瑞士国家科学基金会; 美国国家科学基金会; 欧洲研究理事会; 芬兰科学院; 中国国家自然科学基金;
关键词
PARTICLE FORMATION; SULFURIC-ACID; METHANESULFONIC-ACID; SEA-SURFACE; CHEMISTRY; NUCLEATION; EMISSIONS; IMPACTS; AMMONIA; COASTAL;
D O I
10.1038/s41557-022-01067-z
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Iodine is a reactive trace element in atmospheric chemistry that destroys ozone and nucleates particles. Iodine emissions have tripled since 1950 and are projected to keep increasing with rising O-3 surface concentrations. Although iodic acid (HIO3) is widespread and forms particles more efficiently than sulfuric acid, its gas-phase formation mechanism remains unresolved. Here, in CLOUD atmospheric simulation chamber experiments that generate iodine radicals at atmospherically relevant rates, we show that iodooxy hypoiodite, IOIO, is efficiently converted into HIO3 via reactions (R1) IOIO + O-3 -> IOIO4 and (R2) IOIO4 + H2O -> HIO3 + HOI + O-(1)(2). The laboratory-derived reaction rate coefficients are corroborated by theory and shown to explain field observations of daytime HIO3 in the remote lower free troposphere. The mechanism provides a missing link between iodine sources and particle formation. Because particulate iodate is readily reduced, recycling iodine back into the gas phase, our results suggest a catalytic role of iodine in aerosol formation.
引用
收藏
页码:129 / +
页数:14
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