Impacts of Uncertainty in AVOC Emissions on the Summer ROx Budget and Ozone Production Rate in the Three Most Rapidly-Developing Economic Growth Regions of China

WANG Feng; AN Junling; LI Ying; TANG Yujia; LIN Jian; QU Yu; CHEN Yong; ZHANG Bing; ZHAI Jing

doi:10.1007/s00376-014-3251-z

Abstract:

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 \citeZhang2009 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.

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Impacts of Uncertainty in AVOC Emissions on the Summer ROx Budget and Ozone Production Rate in the Three Most Rapidly-Developing Economic Growth Regions of China

Corresponding author: AN Junling, anjl@mail.iap.ac.cn;

1. State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029;

2. University of Chinese Academy of Sciences, Beijing 100049;

3. Anhui Meteorological Bureau, Hefei 230061

Manuscript received: 2013-11-19

Manuscript revised: 2014-04-16

Fund Project: This research was partially 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), and the Carbon and Nitrogen Cycle Project of IAP, CAS. Special thanks are given to Prof. WANG Yuesi from IAP, CAS, for offering observed data of NOx and O3 in the Beijing-Tianjin-Hebei region. Many thanks are extended to the two anonymous reviewers for their key suggestions.

Abstract: 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 \citeZhang2009 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.

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Impacts of Uncertainty in AVOC Emissions on the Summer ROx Budget and Ozone Production Rate in the Three Most Rapidly-Developing Economic Growth Regions of China

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