Stability of tropospheric hydroxyl chemistry

被引:111
作者
Lelieveld, J
Peters, W
Dentener, FJ
Krol, MC
机构
[1] Max Planck Inst Chem, D-55020 Mainz, Germany
[2] Inst Marine & Atmospher Res, NL-3508 TA Utrecht, Netherlands
[3] Commiss European Communities, Joint Res Ctr, Inst Environm, I-21020 Ispra, Va, Italy
关键词
D O I
10.1029/2002JD002272
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
[1] Tropospheric hydroxyl (OH) is the cleaning agent of the atmosphere, because most oxidation processes are initiated by OH. If the OH chemical system were unstable, runaway growth of oxidants (autocatalytic conditions) or of reduced gases (catastrophic conditions) might occur, especially because the atmospheric composition is changing rapidly. We present simulations with a global chemistry-transport model, indicating that during the past century, global mean OH has nevertheless remained nearly constant. This constancy is remarkable, because CH4 and CO, the main OH sinks, have increased strongly. We studied the system's sensitivity to perturbations using the OH recycling probability, calculated from primary OH formation and OH recycling. We conclude that the constancy of global mean OH does not imply that regional OH has not changed or that the system is insensitive to perturbations. Over the tropical oceans, where OH concentrations are highest, the system stability is relatively low. During the past century, the OH concentration decreased substantially in the marine troposphere, however, on a global scale, it has been compensated by an increase over the continents associated with strong pollution emissions of nitrogen oxides. Our results suggest that the changing atmospheric composition due to industrialization has been accompanied with a 60% increase in the tropospheric oxidation power (i.e., gross OH production).
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页数:11
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共 47 条
[1]   ORGANIC NITRATES IN REMOTE MARINE ENVIRONMENTS - EVIDENCE FOR LONG-RANGE TRANSPORT [J].
ATHERTON, CS .
GEOPHYSICAL RESEARCH LETTERS, 1989, 16 (11) :1289-1292
[2]   EVIDENCE FOR GREATER-THAN-OR-EQUAL-TO-C-3 ALKYL NITRATES IN RURAL AND REMOTE ATMOSPHERES [J].
ATLAS, E .
NATURE, 1988, 331 (6155) :426-428
[3]   PHOTOCHEMICAL THEORY OF TROPOSPHERIC OZONE [J].
CHAMEIDES, W ;
WALKER, JCG .
JOURNAL OF GEOPHYSICAL RESEARCH, 1973, 78 (36) :8751-8760
[4]   DISCUSSION OF CHEMISTRY OF SOME MINOR CONSTITUENTS IN STRATOSPHERE AND TROPOSPHERE [J].
CRUTZEN, P .
PURE AND APPLIED GEOPHYSICS, 1973, 106 (5-7) :1385-1399
[6]   A MODEL STUDY OF ATMOSPHERIC TEMPERATURES AND THE CONCENTRATIONS OF OZONE, HYDROXYL, AND SOME OTHER PHOTOCHEMICALLY ACTIVE GASES DURING THE GLACIAL, THE PREINDUSTRIAL HOLOCENE AND THE PRESENT [J].
CRUTZEN, PJ ;
BRUHL, C .
GEOPHYSICAL RESEARCH LETTERS, 1993, 20 (11) :1047-1050
[7]   Diurnal ozone cycle in the tropical and subtropical marine boundary layer [J].
de Laat, ATJ ;
Lelieveld, J .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2000, 105 (D9) :11547-11559
[8]   Simulation of the transport of Rn222 using on-line and off-line global models at different horizontal resolutions:: a detailed comparison with measurements [J].
Dentener, F ;
Feichter, J ;
Jeuken, A .
TELLUS SERIES B-CHEMICAL AND PHYSICAL METEOROLOGY, 1999, 51 (03) :573-602
[9]   REACTION OF N2O5 ON TROPOSPHERIC AEROSOLS - IMPACT ON THE GLOBAL DISTRIBUTIONS OF NOX, O3, AND OH [J].
DENTENER, FJ ;
CRUTZEN, PJ .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1993, 98 (D4) :7149-7163
[10]   THE CHEMISTRY OF THE HYDROXYL RADICAL IN THE TROPOSPHERE [J].
EHHALT, DH ;
DORN, HP ;
POPPE, D .
PROCEEDINGS OF THE ROYAL SOCIETY OF EDINBURGH SECTION B-BIOLOGICAL SCIENCES, 1990, 97 :17-34