Amplified Trace Gas Removal in the Troposphere

被引:470
作者
Hofzumahaus, Andreas [1 ]
Rohrer, Franz [1 ]
Lu, Keding [1 ,2 ]
Bohn, Birger [1 ]
Brauers, Theo [1 ]
Chang, Chih-Chung [3 ]
Fuchs, Hendrik [1 ]
Holland, Frank [1 ]
Kita, Kazuyuki [4 ]
Kondo, Yutaka [5 ]
Li, Xin [1 ,2 ]
Lou, Shengrong [1 ,6 ]
Shao, Min [2 ]
Zeng, Limin [2 ]
Wahner, Andreas [1 ]
Zhang, Yuanhang [2 ]
机构
[1] Forschungszentrum Julich, Inst Chem & Dynam Geosphare Troposphare 2, D-52425 Julich, Germany
[2] Peking Univ, Coll Environm Sci & Engn, Beijing 100871, Peoples R China
[3] Acad Sinica, Res Ctr Environm Changes, Taipei 115, Taiwan
[4] Ibaraki Univ, Fac Sci, Ibaraki 3108512, Japan
[5] Univ Tokyo, Adv Sci & Technol Res Ctr, Tokyo 1538904, Japan
[6] Shanghai Jiao Tong Univ, Sch Environm Sci & Technol, Shanghai 200240, Peoples R China
关键词
OZONE PRODUCTION; ATMOSPHERIC OXIDATION; BOUNDARY-LAYER; ATLANTIC-OCEAN; OH REACTIVITY; HO2; RADICALS; FOREST; CH3C(O)O-2; PHASE;
D O I
10.1126/science.1164566
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The degradation of trace gases and pollutants in the troposphere is dominated by their reaction with hydroxyl radicals (OH). The importance of OH rests on its high reactivity, its ubiquitous photochemical production in the sunlit atmosphere, and most importantly on its regeneration in the oxidation chain of the trace gases. In the current understanding, the recycling of OH proceeds through HO2 reacting with NO, thereby forming ozone. A recent field campaign in the Pearl River Delta, China, quantified tropospheric OH and HO2 concentrations and turnover rates by direct measurements. We report that concentrations of OH were three to five times greater than expected, and we propose the existence of a pathway for the regeneration of OH independent of NO, which amplifies the degradation of pollutants without producing ozone.
引用
收藏
页码:1702 / 1704
页数:3
相关论文
共 24 条
[1]   Modelling the evolution of organic carbon during its gas-phase tropospheric oxidation: development of an explicit model based on a self generating approach [J].
Aumont, B ;
Szopa, S ;
Madronich, S .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2005, 5 :2497-2517
[2]  
Brasseur G.P., 2003, ATMOSPHERIC CHEM CHA
[3]   OH radicals in the boundary layer of the Atlantic Ocean 1. Measurements by long-path laser absorption spectroscopy [J].
Brauers, T ;
Hausmann, M ;
Bister, A ;
Kraus, A ;
Dorn, HP .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2001, 106 (D7) :7399-7414
[4]   Measurements of OH and HO2 concentrations in the Southern Ocean marine boundary layer -: art. no. 4475 [J].
Creasey, DJ ;
Evans, GE ;
Heard, DE ;
Lee, JD .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D15)
[5]   Missing OH reactivity in a forest: Evidence for unknown reactive biogenic VOCs [J].
Di Carlo, P ;
Brune, WH ;
Martinez, M ;
Harder, H ;
Lesher, R ;
Ren, XR ;
Thornberry, T ;
Carroll, MA ;
Young, V ;
Shepson, PB ;
Riemer, D ;
Apel, E ;
Campbell, C .
SCIENCE, 2004, 304 (5671) :722-725
[6]   Direct detection of OH formation in the reactions of HO2 with CH3C(O)O2 and other substituted peroxy radicals [J].
Dillon, T. J. ;
Crowley, J. N. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2008, 8 (16) :4877-4889
[7]   Photooxidation of trace gases in the troposphere [J].
Ehhalt, DH .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1999, 1 (24) :5401-5408
[8]   Known and unexplored organic constituents in the earth's atmosphere [J].
Goldstein, Allen H. ;
Galbally, Ian E. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2007, 41 (05) :1514-1521
[9]   A product yield study of the reaction of HO2 radicals with ethyl peroxy (C2H5O2), acetyl peroxy (CH3C(O)O2), and acetonyl peroxy (CH3C(O)CH2O2) radicals [J].
Hasson, AS ;
Tyndall, GS ;
Orlando, JJ .
JOURNAL OF PHYSICAL CHEMISTRY A, 2004, 108 (28) :5979-5989
[10]   Measurement of OH and HO2 in the troposphere [J].
Heard, DE ;
Pilling, MJ .
CHEMICAL REVIEWS, 2003, 103 (12) :5163-5198