Heterogeneous reactivity of carbonyl sulfide on α-Al2O3 and γ-Al2O3

被引:39
作者
Liu, Yongchun [1 ]
He, Hong [1 ]
Mu, Yujing [1 ]
机构
[1] Chinese Acad Sci, Ecoenvironm Sci Res Ctr, State Key Lab Environm Chem & Ecotoxicol, Beijing 100085, Peoples R China
基金
中国国家自然科学基金;
关键词
heterogeneous reactivity; carbonyl sulfide; Al2O3; global flux; knudsen cell;
D O I
10.1016/j.atmosenv.2007.10.007
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The heterogeneous reactions of trace gases in the atmosphere on atmospheric particles could greatly affect the nitrogen, sulfur, ozone, and photochemical oxidant cycles. The uptake coefficient is an important kinetic parameter for atmospheric models to assess the role of heterogeneous reaction in the global cycles of trace gases. In this study, the heterogeneous uptake coefficients of carbonyl sulfide (OCS) on AL(2)O(3) have been measured using a Knudsen cell reactor at 300 K. Hydrogen sulfide (H,S) and carbon dioxide (CO,) were found to be the gaseous products. The reaction mechanism of OCS on Al2O3 was confirmed based on previous work and this study. The true initial uptake coefficient and steady-state uptake coefficient of OCS on alpha-Al2O3 were (3.8 +/- 0.8) x 10(-7) and (6.5 +/- 2.49) x 10(-8), and the corresponding uptake coefficients on gamma-Al2O3 were (7.0 +/- 0.7) x 10(-8) and (1.8 +/- 0.4) x 10(-8), respectively. The annual flux of OCS due to heterogeneous reaction on alpha-Al2O3 was calculated to be 0.11-0.63Tg yr(-1) based on the initial uptake coefficient and the steady-state uptake coefficient. When the fraction of Al2O3 in authentic atmospheric particles is taken into account, the annual flux of OCS due to heterogeneous reaction on atmospheric particles in the troposphere should be 0.02-0.10 Tg yr(-1). (c) 2007 Elsevier Ltd. All rights reserved.
引用
收藏
页码:960 / 969
页数:10
相关论文
共 36 条
[1]   Heterogeneous reaction of NO2 on hexane soot:: A Knudsen cell and FT-IR study [J].
Al-Abadleh, HA ;
Grassian, VH .
JOURNAL OF PHYSICAL CHEMISTRY A, 2000, 104 (51) :11926-11933
[2]   Climate forcing by aerosols - a hazy picture [J].
Anderson, TL ;
Charlson, RJ ;
Schwartz, SE ;
Knutti, R ;
Boucher, O ;
Rodhe, H ;
Heintzenberg, J .
SCIENCE, 2003, 300 (5622) :1103-1104
[3]   Atmospheric aerosols: Biogeochemical sources and role in atmospheric chemistry [J].
Andreae, MO ;
Crutzen, PJ .
SCIENCE, 1997, 276 (5315) :1052-1058
[4]   Knudsen cell studies of the uptake of gaseous HNO3 and other oxides of nitrogen on solid NaCl: The role of surface-adsorbed water [J].
Beichert, P ;
FinlaysonPitts, BJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (37) :15218-15228
[5]   Heterogeneous uptake kinetics of volatile organic compounds on oxide surfaces using a Knudsen cell reactor:: Adsorption of acetic acid, formaldehyde, and methanol on α-Fe2O3, α-Al2O3, and SiO2 [J].
Carlos-Cuellar, S ;
Li, P ;
Christensen, AP ;
Krueger, BJ ;
Burrichter, C ;
Grassian, VH .
JOURNAL OF PHYSICAL CHEMISTRY A, 2003, 107 (21) :4250-4261
[6]   A REANALYSIS OF CARBONYL SULFIDE AS A SOURCE OF STRATOSPHERIC BACKGROUND SULFUR AEROSOL [J].
CHIN, M ;
DAVIS, DD .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1995, 100 (D5) :8993-9005
[7]   POSSIBLE IMPORTANCE OF CSO FOR SULFATE LAYER OF STRATOSPHERE [J].
CRUTZEN, PJ .
GEOPHYSICAL RESEARCH LETTERS, 1976, 3 (02) :73-76
[8]   CLAUS CATALYSIS .2. AN FTIR STUDY OF THE ADSORPTION OF H2S ON THE ALUMINA CATALYST [J].
DATTA, A ;
CAVELL, RG .
JOURNAL OF PHYSICAL CHEMISTRY, 1985, 89 (03) :450-454
[9]   Airborne observations of dust aerosol over the North Atlantic Ocean during ACE 2:: Indications for heterogeneous ozone destruction [J].
de Reus, M ;
Dentener, F ;
Thomas, A ;
Borrmann, S ;
Ström, J ;
Lelieveld, J .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2000, 105 (D12) :15263-15275
[10]   Role of mineral aerosol as a reactive surface in the global troposphere [J].
Dentener, FJ ;
Carmichael, GR ;
Zhang, Y ;
Lelieveld, J ;
Crutzen, PJ .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1996, 101 (D17) :22869-22889