Pathways of sulfate enhancement by natural and anthropogenic mineral aerosols in China

被引:128
作者
Huang, Xin [1 ,2 ,3 ]
Song, Yu [1 ]
Zhao, Chun [4 ]
Li, Mengmeng [1 ]
Zhu, Tong [1 ]
Zhang, Qiang [5 ]
Zhang, Xiaoye [6 ]
机构
[1] Peking Univ, State Key Joint Lab Environm Simulat & Pollut Con, Dept Environm Sci, Beijing 100871, Peoples R China
[2] Nanjing Univ, Inst Climate & Global Change Res, Nanjing 210008, Jiangsu, Peoples R China
[3] Nanjing Univ, Sch Atmospher Sci, Nanjing 210008, Jiangsu, Peoples R China
[4] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA
[5] Tsinghua Univ, Minist Educ, Key Lab Earth Syst Modeling, Ctr Earth Syst Sci,Inst Global Change Studies, Beijing 100084, Peoples R China
[6] Chinese Acad Meteorol Sci, Key Lab Atmospher Chem, CMA, Beijing, Peoples R China
基金
中国国家自然科学基金;
关键词
GENERAL-CIRCULATION MODEL; SULFUR-DIOXIDE; CATALYZED OXIDATION; SPATIAL/TEMPORAL VARIABILITY; CHEMICAL CHARACTERISTICS; HETEROGENEOUS OXIDATION; TROPOSPHERIC AEROSOLS; ATMOSPHERIC AEROSOLS; SEASONAL-VARIATIONS; ACID DEPOSITION;
D O I
10.1002/2014JD022301
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
China, the world's largest consumer of coal, emits approximately 30 million tons of sulfur dioxide (SO2) per year. SO2 is subsequently oxidized to sulfate in the atmosphere. However, large gaps exist between model-predicted and measured sulfate levels in China. Long-term field observations and numerical simulations were integrated to investigate the effect of mineral aerosols on sulfate formation. We found that mineral aerosols contributed a nationwide average of approximately 22% to sulfate production in 2006. The increased sulfate concentration was approximately 2 mu gm(-3) in the entire China. In East China and the Sichuan Basin, the increments reached 6.3 mu gm(-3) and 7.3 mu gm(-3), respectively. Mineral aerosols led to faster SO2 oxidation through three pathways. First, more SO2 was dissolved as cloud water alkalinity increased due to water-soluble mineral cations. Sulfate production was then enhanced through the aqueous-phase oxidation of S(IV) (dissolved sulfur in oxidation state + 4). The contribution to the national sulfate production was 5%. Second, sulfate was enhanced through S(IV) catalyzed oxidation by transition metals. The contribution to the annual sulfate production was 8%, with 19% during the winter that decreased to 2% during the summer. Third, SO2 reacts on the surface of mineral aerosols to produce sulfate. The contribution to the national average sulfate concentration was 9% with 16% during the winter and a negligible effect during the summer. The inclusion of mineral aerosols does resolve model discrepancies with sulfate observations in China, especially during the winter. These three pathways, which are not fully considered in most current chemistry-climate models, will significantly impact assessments regarding the effects of aerosol on climate change in China.
引用
收藏
页码:14165 / 14179
页数:15
相关论文
共 93 条
[1]   Transition metal-catalyzed oxidation of atmospheric sulfur: Global implications for the sulfur budget [J].
Alexander, Becky ;
Park, Rokjin J. ;
Jacob, Daniel J. ;
Gong, Sunling .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2009, 114
[2]  
[Anonymous], 2013, CHIN CIT STAT YB 201
[3]   Chemical composition of atmospheric aerosols from Zhenbeitai, China, and Gosan, South Korea, during ACE-Asia [J].
Arimoto, R ;
Zhang, XY ;
Huebert, BJ ;
Kang, CH ;
Savoie, DL ;
Prospero, JM ;
Sage, SK ;
Schloesslin, CA ;
Khaing, HM ;
Oh, SN .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2004, 109 (D19) :D19S041-15
[4]   Adsorption of sulfur dioxide on hematite and goethite particle surfaces [J].
Baltrusaitis, Jonas ;
Cwiertny, David M. ;
Grassian, Vicki H. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2007, 9 (41) :5542-5554
[5]   Massive volcanic SO2 oxidation and sulphate aerosol deposition in Cenozoic North America [J].
Bao, Huiming ;
Yu, Shaocai ;
Tong, Daniel Q. .
NATURE, 2010, 465 (7300) :909-912
[6]   Marine boundary layer dust and pollutant transport associated with the passage of a frontal system over eastern Asia [J].
Bates, TS ;
Quinn, PK ;
Coffman, DJ ;
Covert, DS ;
Miller, TL ;
Johnson, JE ;
Carmichael, GR ;
Uno, I ;
Guazzotti, SA ;
Sodeman, DA ;
Prather, KA ;
Rivera, M ;
Russell, LM ;
Merrill, JT .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2004, 109 (D19) :D19S191-18
[7]   Do sulfate and nitrate coatings on mineral dust have important effects on radiative properties and climate modeling? [J].
Bauer, S. E. ;
Mishchenko, M. I. ;
Lacis, A. A. ;
Zhang, S. ;
Perlwitz, J. ;
Metzger, S. M. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2007, 112 (D6)
[8]   Impact of heterogeneous sulfate formation at mineral dust surfaces on aerosol loads and radiative forcing in the Goddard Institute for Space Studies general circulation model [J].
Bauer, SE ;
Koch, D .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2005, 110 (D17) :91-105
[9]   TRANSITION-METAL-CATALYZED OXIDATION OF SULFUR(IV) OXIDES - ATMOSPHERIC-RELEVANT PROCESSES AND MECHANISMS [J].
BRANDT, C ;
VANELDIK, R .
CHEMICAL REVIEWS, 1995, 95 (01) :119-190
[10]   On the potential high acid deposition in northeastern China [J].
Cao, Junji ;
Tie, Xuexi ;
Dabberdt, Walter F. ;
Jie, Tang ;
Zhao, Zhuzi ;
An, Zhisheng ;
Shen, Zhenxing ;
Feng, Yinchang .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2013, 118 (10) :4834-4846