科研成果 Publications

2019
Tan ZF, Lu KD, Hofzumahaus A, Fuchs H, Bohn B, Holland F, Liu YH, Rohrer F, Shao M, Sun K, et al. Experimental budgets of OH, HO2, and RO2 radicals and implications for ozone formation in the Pearl River Delta in China 2014. Atmospheric Chemistry and Physics [Internet]. 2019;(19):7129-7150. 访问链接
Shi ZB, T V, Kotthaus S, Harrison RM, Grimmond S, Yue SY, Zhu T, Lee J, Han YQ, Demuzere M. Introduction to the special issue “In-depth study of air pollution sources and processes within Beijing and its surrounding region (APHH-Beijing)”. Atmospheric Chemistry and Physics [Internet]. 2019;(19):7519-7546. 访问链接
Ma XF, Tan ZF, Lu KD, Yang XP, Liu YH, Li SL, Li X, Chen SY, Novelli A, Cho CM. Winter photochemistry in Beijing: Observation and model simulation of OH and HO2 radicals at an urban site. Science of the Total Environment [Internet]. 2019;(685):85-95. 访问链接
Tan ZF, Lu KD, Jiang MQ, Su R, Wang HL, Lou SR, Fu QY, Zhai CZ, Tan QW, Yue DL, et al. Daytime atmospheric oxidation capacity in four Chinese megacities during the photochemically polluted season: a case study based on box model simulation. Atmospheric Chemistry and Physics [Internet]. 2019;19(6):3493-3513. 访问链接
Song M, Liu X, Zhang Y, Shao M, Lu K, Tan Q, Feng M, Qu Y. Sources and abatement mechanisms of VOCs in southern China. Atmospheric Environment [Internet]. 2019;201:28-40. 访问链接
Chen X, Wang H, Liu Y, Su R, Wang H, Lou S, Lu K. Spatial characteristics of the nighttime oxidation capacity in the Yangtze River Delta, China. Atmospheric Environment [Internet]. 2019;208:150-157. 访问链接
Liu Y, Lu K, Li X, Dong HB, Tan Z, Wang H, Zou Q, Wu Y, Zeng L, Min K-E, et al. A Comprehensive Model Test of the HONO Sources Constrained to Field Measurements at Rural North China Plain. Environmental Science & Technology [Internet]. 2019. 访问链接
2018
Wu ZJ, Wang Y, Tan TY, Zhu YS, Li MR, Shang DJ, Wang HC, Lu KD, Guo S, Zeng LM, et al. Aerosol Liquid Water Driven by Anthropogenic Inorganic Salts: Implying Its Key Role in Haze Formation over the North China Plain. Environmental Science & Technology LettersEnvironmental Science & Technology LettersEnvironmental Science & Technology Letters. 2018;5:160-166.Abstract
This study reveals aerosol liquid water content (ALWC) in PM2.5 ranged from 2% up to 74%, and the associated secondary inorganic fraction rose from 24% to 55%, while ambient relative humidity (RH) increased from 15% to 83% in the atmosphere over Beijing. Unexpectedly, the secondary inorganic fraction in PM2.5 increased with an increase in the ambient RH, which is a meteorological parameter independent of anthropogenic activities, indicating the presence of a feedback mechanism driven by Henry's law and thermodynamic equilibrium. During haze episodes, simultaneously elevated RH levels and anthropogenic secondary inorganic mass concentrations resulted in an abundant ALWC. The condensed water could act as an efficient medium for multiphase reactions, thereby facilitating the transformation of reactive gaseous pollutants into particles and accelerating the formation of heavy haze. ALWC was well correlated with the mass concentrations of both nitrate and sulfate, indicating both nitrate and sulfate salts play key roles in determining ALWC. Coincident with a significant reduction in SO2 emissions throughout China, nitrates will become a dominant anthropogenic inorganic salt driving ALWC. Thus, the abundance of ALWC and its effects on the aerosol chemistry and climate should be reconsidered.
Su R, Lu KD, Yu JY, Tan ZF, Jiang MQ, Li J, Xie SD, Wu YS, Zeng LM, Zhai CZ, et al. Exploration of the formation mechanism and source attribution of ambient ozone in Chongqing with an observation-based model. Science China-Earth SciencesScience China-Earth SciencesScience China-Earth Sciences. 2018;61:23-32.Abstract
An intensive field campaign was conducted in Chongqing during the summer of 2015 to explore the formation mechanisms of ozone pollution. The sources of ozone, the local production rates, and the controlling factors, as well as key species of volatile organic compounds (VOCs), were quantified by integrating a local ozone budget analysis, calculations of the relative incremental reactivity, and an empirical kinetic model approach. It was found that the potential for rapid local ozone formation exists in Chongqing. During ozone pollution episodes, the ozone production rates were found to be high at the upwind station Nan Quan, the urban station Chao Zhan, and the downwind station Jin-Yun Shan. The average local ozone production rate was 30x10(-9) V/V h(-1) and the daily integration of the produced ozone was greater than 180x10(-9) V/V. High ozone concentrations were associated with urban and downwind air masses. At most sites, the local ozone production was VOC-limited and the key species were aromatics and alkene, which originated mainly from vehicles and solvent usage. In addition, the air masses at the northwestern rural sites were NO (x) -limited and the local ozone production rates were significantly higher during the pollution episodes due to the increased NO (x) concentrations. In summary, the ozone abatement strategies of Chongqing should be focused on the mitigation of VOCs. Nevertheless, a reduction in NO (x) is also beneficial for reducing the regional ozone peak values in Chongqing and the surrounding areas.
Li ZY, Zhu R, Xie PH, Wang HC, Lu KD, Wang D. Intercomparison of in situ CRDS and CEAS for measurements of atmospheric N2O5 in Beijing, China. Science of the Total EnvironmentScience of the Total Environment. 2018;613:131-139.Abstract
Dinitrogen pentoxide (N2O5) is one of the basic trace gases which plays a key role in nighttime atmosphere. An intercomparison and validation of different N2O5 measurement methods is important for determining the true accuracy of these methods. Cavity ring down spectroscopy (CRDS) and cavity enhanced absorption spectrometer (CEAS) were used to measure N2O5 at the campus of the University of Chinese Academy of Sciences (UCAS) from February 21, 2016 to March 4, 2016. The detection limits were 1.6 ppt (1 sigma) at 30 s intervals for the CEAS instrument and 3.9 ppt (1 sigma) at 10 s time resolution for the CRDS instrument respectively. In this study, a comparison of the 1 min observations from the two instruments was presented. The two data sets showed a good agreement within their uncertainties, with an absolute shift of 15.6 ppt, slope of 0.94 and a correlation coefficient R-2 = 0.97. In general, the difference between the CRDS and CEAS instruments for N2O5 measurement can be explained by their combined measurement uncertainties. However, high relative humidity (> 60%) and high PM2.5 concentration (> 200 mu g/m(3)) may contribute to the discrepancies. The excellent agreement between the measurement by the CRDS and CEAS instruments demonstrates the capability of the two instruments for accurately measuring N2O5 with high sensitivity. (C) 2017 Elsevier B.V. All rights reserved.
Tan ZF, Lu KD, Zhang YH. Explicit diagnosis of the local ozone production rate and the ozone-NOx-VOC sensitivities. Science Bulletin [Internet]. 2018;(63):1067-1076. 访问链接
Chen X, Wang H, Lu K. Simulation of organic nitrates in Pearl River Delta in 2006 and the chemical impact on ozone production. Science China Earth Sciences. 2018;61(2):228-238.
Duan J, Qin M, Ouyang B, Fang W, Li X, Lu K, Tang K, Liang S, Meng F, Hu Z. Development of an incoherent broadband cavity-enhanced absorption spectrometer for in situ measurements of HONO and NO 2. Atmospheric Measurement Techniques. 2018;11(7).
Tham YJ, Wang Z, Li Q, Wang W, Wang X, Lu K, Ma N, Yan C, Kecorius S, Wiedensohler A. Heterogeneous N 2 O 5 uptake coefficient and production yield of ClNO 2 in polluted northern China: roles of aerosol water content and chemical composition. Atmospheric Chemistry and Physics. 2018;18(17):13155-13171.
Breton ML, Hallquist ÅM, Pathak RK, Simpson D, Wang Y, Johansson J, Zheng J, Yang Y, Shang D, Wang H. Chlorine oxidation of VOCs at a semi-rural site in Beijing: significant chlorine liberation from ClNO 2 and subsequent gas-and particle-phase Cl–VOC production. Atmospheric Chemistry and Physics. 2018;18(17):13013-13030.
蒋美青, 陆克定, 苏榕, 谭照峰, 王红丽, 李莉, 伏晴艳, 翟崇治, 谭钦文, 岳玎利. 我国典型城市群 O3 污染成因和关键 VOCs 活性解析. 科学通报. 2018;63:1130.PKU 
Wang L, Wang X, Gu R, Wang H, Yao L, Wen L, Zhu F, Wang W, Xue L, Yang L, et al. Observations of fine particulate nitrated phenols in four sites in northern China: concentrations, source apportionment, and secondary formation. Atmospheric Chemistry and Physics [Internet]. 2018;18:4349–4359. 访问链接
Wang HC, Lu KD, Guo S, Wu ZJ, Shang DJ, Tan ZF, Wang YJ, Le Breton M, Lou SR, Tang MJ, et al. Efficient N2O5uptake and NO3oxidation in the outflow of urban Beijing. Atmos. Chem. Phys. [Internet]. 2018;(18):9705-9721. 访问链接Abstract
Nocturnal reactive nitrogen compounds play an important role in regional air pollution. Here we present the measurements of dinitrogen pentoxide (N2O5) associated with nitryl chloride (ClNO2) and particulate nitrate (pNO3-) in a suburban site of Beijing in the summer of 2016. High levels of N2O5 and ClNO2 were observed in the outflow of the urban Beijing air masses, with 1-min average maxima of 937 pptv and 2900 pptv, respectively. The N2O5 uptake coefficients, γ, and ClNO2 yield, f, were experimentally determined from the observed parameters. The N2O5 uptake coefficient ranged from 0.012 to 0.055, with an average of 0.034 ± 0.018, which is in the upper range of previous field studies reported in North America and Europe but is a moderate value in the North China Plain (NCP), which reflects efficient N2O5 heterogeneous processes in Beijing. The ClNO2 yield exhibited high variability, with a range of 0.50 to unity and an average of 0.73 ± 0.25. The concentration of the nitrate radical (NO3) was calculated assuming that the thermal equilibrium between NO3 and N2O5 was maintained. In NOx-rich air masses, the oxidation of nocturnal biogenic volatile organic compounds (BVOCs) was dominated by NO3 rather than O3. The production rate of organic nitrate (ON) via NO3+BVOCs was significant, with an average of 0.10 ± 0.07 ppbv h-1. We highlight the importance of NO3 oxidation of VOCs in the formation of ON and subsequent secondary organic aerosols in summer in Beijing. 
Tan ZF, Lu KD, Jiang MQ, Su R, Dong HB, Zeng LM, Xie SD, Tan QW, Zhang YH. Exploring ozone pollution in Chengdu, southwestern China: A case study from radical chemistry to O3-VOC-NOx sensitivity. Science of the Total Environment [Internet]. 2018;(636):775-786. 访问链接Abstract
We present the in-situ measurements in Chengdu, a major city in south west of China, in September 2016. The concentrations of ozone and its precursor were measured at four sites. Although the campaign was conducted in early autumn, up to 100 ppbv (parts per billion by volume) daily maximum ozone was often observed at all sites. The observed ozone concentrations showed good agreement at all sites, which implied that ozone pollution is a regional issue in Chengdu. To better understand the ozone formation in Chengdu, an observation based model is used in this study to calculate the ROx radical concentrations (ROx = OH + HO2 + RO2) and ozone production rate (P(O3)). The model predicts OH daily maximum is in the range of 4–8 × 106 molecules cm−3 , and HO2 and RO2 are in the range of 3–6 × 108 molecules cm−3 . The modelled radical concentrations show a distinct difference between ozone pollution and attainment period. The relative incremental reactivity (RIR) results demonstrate that anthropogenic VOCs reduction is the most efficient way to mitigate ozone pollution at all sites, of which alkenes dominate >50% of the ozone production. Empirical kinetic modelling approach shows that three out of four sites are under the VOC-limited regime, while Pengzhou is in a transition regime due to the local petrochemical industry. The ozone budget analysis showed that the local ozone production driven by the photochemical process is important to the accumulation of ozone concentrations.
Lu KD, Guo S, Tan ZF, Wang HC, Shang DJ, Liu YH, Li X, Wu ZJ, Hu M, Zhang YH. Exploring the Atmospheric Free Radical chemistry in China: the self-cleansing capacity and the formation of secondary air pollution. National Scinence Review [Internet]. 2018:1-16. 访问链接Abstract
Since 1971, it is known that the atmospheric free radicals play a pivotal role in maintaining the oxidizing power of the troposphere. The existence of the oxidizing power is an important feature of the troposphere to remove primary air pollutants emitted from human-beings as well as those from biosphere. Nevertheless, serious secondary air pollution incidents can take place due to fast oxidation of the primary pollutants. Elucidating the atmospheric free radical chemistry is a demanding task in the field of atmospheric chemistry worldwide which includes two kinds of work: firstly, the setup of reliable radical detection systems; secondly, integrated field studies which enable closure studies on the sources and sinks of targeted radicals like OH and NO3. In this review, we try to review the Chinese efforts to explore the atmospheric free radical chemistry in the such chemical complex environments and the possible link of this fast gas phase oxidation with the fast formation of secondary air pollutions in the city-cluster areas in China.

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