机构地区:[1]State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry,Institute of Atmospheric Physics, Chinese Academy of Sciences [2]University of Chinese Academy of Sciences [3]Anhui Meteorological Bureau
出 处:《Advances in Atmospheric Sciences》2014年第6期1331-1342,共12页大气科学进展(英文版)
基 金:supported by the National Natural Science Foundation of China (Grant Nos. 41175105 and 41105098);the Beijing Natural Science Foundation (Grant No.8144054);a Key Project of CAS (Grant No.XDB05030301);the Carbon and Nitrogen Cycle Project of IAP, CAS
摘 要:High levels of uncertainty in non-methane volatile organic compound (NMVOC) emissions in China could lead to significant variation in the budget of the sum of hydroxyl (OH) and peroxy (HO2,RO2) radicals (ROx =OH + HO2 + RO2) and the ozone production rate [P(O3)],but few studies have investigated this possibility,particularly with three-dimensional air quality models.We added diagnostic variables into the WRF-Chem model to assess the impact of the uncertainty in anthropogenic NMVOC (AVOC) emissions on the ROx budget and P(O3) in the Beijing-Tianjin-Hebei region,Yangtze River Delta,and Pearl River Delta of China.The WRF-Chem simulations were compared with satellite and ground observations,and previous observation-based model studies.Results indicated that 68% increases (decreases) in AVOC emissions produced 4%-280% increases (2%-80% decreases) in the concentrations of OH,HO2,and RO2 in the three regions,and resulted in 35%-48% enhancements (26%-39% reductions) in the primary ROx production and ~ 65% decreases (68%-73% increases) of the P(O3) in Beijing,Shanghai,and Guangzhou.For the three cities,the two largest contributors to the ROx production rate were the reaction of O1D + H2O and photolysis of HCHO,ALD2,and others; the reaction of OH + NO2 (71%-85%) was the major ROx sink; and the major contributor to P(O3) was the reaction of HO2 + NO (~ 65%).Our results showed that AVOC emissions in 2006 from Zhang et al.(2009) have been underestimated by ~ 68% in suburban areas and by > 68% in urban areas,implying that daily and hourly concentrations of secondary organic aerosols and inorganic aerosols could be substantially underestimated,and cloud condensation nuclei could be underestimated,whereas local and regional radiation was overestimated.High levels of uncertainty in non-methane volatile organic compound (NMVOC) emissions in China could lead to significant variation in the budget of the sum of hydroxyl (OH) and peroxy (HO2,RO2) radicals (ROx =OH + HO2 + RO2) and the ozone production rate [P(O3)],but few studies have investigated this possibility,particularly with three-dimensional air quality models.We added diagnostic variables into the WRF-Chem model to assess the impact of the uncertainty in anthropogenic NMVOC (AVOC) emissions on the ROx budget and P(O3) in the Beijing-Tianjin-Hebei region,Yangtze River Delta,and Pearl River Delta of China.The WRF-Chem simulations were compared with satellite and ground observations,and previous observation-based model studies.Results indicated that 68% increases (decreases) in AVOC emissions produced 4%-280% increases (2%-80% decreases) in the concentrations of OH,HO2,and RO2 in the three regions,and resulted in 35%-48% enhancements (26%-39% reductions) in the primary ROx production and ~ 65% decreases (68%-73% increases) of the P(O3) in Beijing,Shanghai,and Guangzhou.For the three cities,the two largest contributors to the ROx production rate were the reaction of O1D + H2O and photolysis of HCHO,ALD2,and others; the reaction of OH + NO2 (71%-85%) was the major ROx sink; and the major contributor to P(O3) was the reaction of HO2 + NO (~ 65%).Our results showed that AVOC emissions in 2006 from Zhang et al.(2009) have been underestimated by ~ 68% in suburban areas and by > 68% in urban areas,implying that daily and hourly concentrations of secondary organic aerosols and inorganic aerosols could be substantially underestimated,and cloud condensation nuclei could be underestimated,whereas local and regional radiation was overestimated.
关 键 词:volatile organic compounds ROX OZONE WRF-Chem model
分 类 号:X51[环境科学与工程—环境工程] X16
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