高级检索

留言板

尊敬的读者、作者、审稿人, 关于本刊的投稿、审稿、编辑和出版的任何问题, 您可以本页添加留言。我们将尽快给您答复。谢谢您的支持!

姓名
邮箱
手机号码
标题
留言内容
验证码

“大气污染防治行动计划”执行以来我国夏季大气OH浓度变化的数值模拟

张丹瑜婷 廖宏 李柯 代慧斌 顾梓会

张丹瑜婷, 廖宏, 李柯, 等. 2023. “大气污染防治行动计划”执行以来我国夏季大气OH浓度变化的数值模拟[J]. 大气科学, 47(3): 713−724 doi: 10.3878/j.issn.1006-9895.2112.21218
引用本文: 张丹瑜婷, 廖宏, 李柯, 等. 2023. “大气污染防治行动计划”执行以来我国夏季大气OH浓度变化的数值模拟[J]. 大气科学, 47(3): 713−724 doi: 10.3878/j.issn.1006-9895.2112.21218
ZHANG Danyuting, LIAO Hong, LI Ke, et al. 2023. Numerical Simulation of Summertime OH Concentrations in China Since the Implementation of the Air Pollution Prevention and Control Action Plan [J]. Chinese Journal of Atmospheric Sciences (in Chinese), 47(3): 713−724 doi: 10.3878/j.issn.1006-9895.2112.21218
Citation: ZHANG Danyuting, LIAO Hong, LI Ke, et al. 2023. Numerical Simulation of Summertime OH Concentrations in China Since the Implementation of the Air Pollution Prevention and Control Action Plan [J]. Chinese Journal of Atmospheric Sciences (in Chinese), 47(3): 713−724 doi: 10.3878/j.issn.1006-9895.2112.21218

“大气污染防治行动计划”执行以来我国夏季大气OH浓度变化的数值模拟

doi: 10.3878/j.issn.1006-9895.2112.21218
基金项目: 国家自然科学基金项目 42021004 
详细信息
    作者简介:

    张丹瑜婷,女,1998年出生,硕士研究生,主要从事大气污染与气候变化等领域的研究。E-mail: danyutingzhang@nuist.edu.cn

    通讯作者:

    廖宏,E-mail: hongliao@nuist.edu.cn

  • 中图分类号: P402

Numerical Simulation of Summertime OH Concentrations in China Since the Implementation of the Air Pollution Prevention and Control Action Plan

Funds: National Natural Science Foundation of China (Grant 42021004)
  • 摘要: OH自由基是对流层中主要的氧化剂,是大气氧化性的重要表征。文章利用GEOS-Chem模式量化了2014~2017年“大气污染防治行动计划”执行以来,人为排放和气象因素变化对中国夏季大气OH浓度变化的贡献。模拟结果表明,2014~2017年间夏季整个中国OH浓度呈现上升趋势,最大上升出现在30°N附近的华南地区。在华北平原地区,OH浓度也呈明显的上升趋势(0.1×106 molecules cm−3 a−1),而OH浓度比较高的珠江三角洲地区的OH变化趋势较小。敏感性试验结果表明,气象和人为排放变化都对2014~2017年华北平原OH浓度上升有促进作用,但人为排放的贡献(OH增加10.0%)远大于气象的贡献(OH增加1.5%);OH浓度变化最大的南方地区主要是气象条件控制。进一步对气象因素分析发现,影响全国OH 变化最重要的气象要素是太阳短波辐射,决定了2014~2017年中国OH浓度增长趋势最大的区域。但在华北地区,2014~2017年短波辐射略微减少的影响被边界层高度明显降低带来的OH增加所抵消。
  • 图  1  2014~2017年中国夏季OH浓度均值模拟结果的空间分布。绿色方框分别代表华北平原(NCP)和珠江三角洲地区(PRD)

    Figure  1.  Spatial distributions of simulated mean summertime OH concentrations in China from 2014 to 2017. Green rectangles denote the North China Plain (NCP) and Pearl River Delta (PRD)

    图  2  2017年夏季重点城市群OH浓度(C)日变化。华北平原(NCP):35°~41°N,113.75°~118.75°E;长江三角洲(YRD):30°~33°N,118°~122°E;珠江三角洲(PRD):22°~23°N,112°~115°E;四川盆地(SCB):28.5°~31.5°N,103.5°~107°E

    Figure  2.  Daily variation of summertime OH concentrations in the four megacity clusters in 2017. North China Plain (NCP): 35–41°N, 113.75–118.75°E; Yangtze River Delta (YRD): 30–33°N, 118–122°E; Pearl River Delta (PRD): 22–23°N, 112–115°E; Sichuan Basin (SCB): 28.5–31.5°N, 103.5–107°E

    图  3  2014~2017年(a)中国年夏季Base模拟的OH浓度年际变化趋势;(b)气象和人为排放变化对中国夏季OH浓度的影响(2017年的Base模拟与2014年Base模拟的差值);(c)气象变化对中国夏季OH浓度的影响(MET17_EM14敏感性试验结果与2014年Base模拟的差值);(d)人为排放变化对中国夏季OH浓度的影响(EM17_MET14敏感性试验结果与2014年Base模拟的差值)

    Figure  3.  (a) Linear trends of summertime OH concentrations during 2014–2017 in China from the Expt Base simulation; (b) The impact of changes in both meteorology and anthropogenic emissions on the summertime OH concentrations during 2014–2017 in China (2017 Base simulation minus 2014 Base simulation); (c) The impact of changes in meteorology on the summertime OH concentrations during 2014–2017 in China (Expt MET17_EM14 minus 2014 Base simulation); (d) The impact of changes in anthropogenic emissions on the summertime OH concentrations during 2014–2017 in China (Expt EM17_MET14 minus 2014 Base simulation)

    图  4  2017年相比于2014年人为排放和气象参数对华北平原和珠江三角洲OH浓度贡献的季节变化(红色代表排放的贡献,蓝色代表气象的贡献):对(a)华北平原和(b)珠江三角洲的绝对贡献;对(c)华北平原和(d)珠江三角洲的相对贡献

    Figure  4.  Seasonal variation of the contributions (contr) of anthropogenic emissions and meteorology to the OH concentrations during 2014–2017 in the North China Plain and Pearl River Delta (red and blue represent the contributions of emissions and meteorology, respectively). Absolute contribution of (a) North China Plain and (b) Pearl River Delta; Relative contribution of (c) North China Plain and (d) Pearl River Delta

    图  5  LMG方法估算的气象要素对2014~2017年期间华北平原和珠江三角洲夏季OH浓度变化的相对重要性(不同的颜色代表着不同的气象要素,每个色块上方插入的值是每个气象要素贡献的百分比)

    Figure  5.  LMG method of estimating the relative contributions of the dominant meteorological variables to the summertime OH concentration changes during 2014–2017 in the North China Plain and Pearl River Delta (different colors represent the different meteorological variables, the value in each color block is the percentage contribution of each meteorological variable). SWGDN: surface incoming shortwave flux; PBLH.daytime: daytime planetary boundary layer height; T2: 2-meter-height air temperature; SLP: sea level pressure; RH1000: relative humidity at 1000 hPa. SWGDN: surface incoming shortwave flux; PBLH.daytime: daytime planetary boundary layer height; T2: 2-meter-height air temperature; SLP: sea level pressure; RH1000: relative humidity at 1000 hPa

    图  6  2017年与2014年中国夏季短波辐射(SWDGN)、白天边界层高度(PBLH.daytime)、地面2 m温度(T2)以及海平面气压(SLP)的差值分布

    Figure  6.  Differences in summertime (a) shortwave radiation (SWDGN), (b) daytime planetary boundary layer height (PBLH.daytime), (c) 2-m air temperature (T2), and (d) sea level pressure (SLP) between 2017 and 2014 (2017 minus 2014) in China

    表  1  GEOS-Chem敏感性试验设计

    Table  1.   Configurations of the GEOS-Chem experiments

    敏感性试验名称气象场年份人为排放年份
    Base2014~2017年2014~2017年
    MET17_EM142017年2014年
    EM17_MET142014年2017年
    下载: 导出CSV

    表  2  OH自由基浓度的观测结果与GEOS-Chem模式模拟结果

    Table  2.   The observed and GEOS-Chem modeled OH radical concentrations

    观测点位置观测时间观测OH浓度/106 molecules cm−3模拟OH浓度/106 molecules cm−3观测值参考文献
    河北望都(38.7°N,115.2°E)2014年夏季峰值5~15日均值2.4Tan et al.(2017)
    北京IAP(39.6°N,116.2°E)2017年夏季均值5.82日均值2.4Woodward-Massey et al.(2020)
    北京PKU(40°N, 116.3°E)2017年冬季峰值1.5~2.0日均值0.3Ma et al.(2019)
    广东广州(23.5°N,113.0°E)2006年夏季峰值15~26日均值3.9*Lu et al.(2013)
    广东鹤山(22.7°N,112.9°E)2014年秋季日最大中值4.5日均值2.9Tan et al.(2019)
    四川成都(30. 4°N, 103.8°E)2019年夏季峰值10~20日均值3.5*Yang et al.(2021)
    *2006年与2019年不在本文模式模拟的时间范围之内,分别选择了与观测时间较近的2014和2017年的模拟与观测进行对比
    下载: 导出CSV
  • [1] Chen L, Zhu J, Liao H, et al. 2020. Meteorological influences on PM2.5 and O3 trends and associated health burden since China’s clean air actions [J]. Sci Total Environ., 744: 140837. doi: 10.1016/j.scitotenv.2020.140837
    [2] Dang R J, Liao H, Fu Y. 2021. Quantifying the anthropogenic and meteorological influences on summertime surface ozone in China over 2012–2017 [J]. Sci. Total Environ., 754: 142394. doi: 10.1016/j.scitotenv.2020.142394
    [3] Ehhalt D H, Rohrer F. 2000. Dependence of the OH concentration on solar UV [J]. J. Geophys. Res. Atmos., 105(D3): 3565−3571. doi: 10.1029/1999JD901070
    [4] Fu Y, Liao H, Yang Y. 2019. Interannual and decadal changes in tropospheric ozone in China and the associated chemistry-climate interactions: A review [J]. Adv. Atmos. Sci., 36(9): 975−993. doi: 10.1007/s00376-019-8216-9
    [5] Groemping U. 2006. Relative importance for linear regression in R: The package relaimpo [J]. Journal of Statistical Software, 17(1): 1−27. doi: 10.18637/jss.v017.i01
    [6] Guenther A B, Jiang X, Heald C L, et al. 2012. The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): An extended and updated framework for modeling biogenic emissions [J]. Geoscientific Model Development, 5(6): 1471−1492. doi: 10.5194/gmd-5-1471-2012
    [7] Krishnamurthy V, Shukla J. 2000. Intraseasonal and interannual variability of rainfall over India [J]. J. Climate, 13(24): 4366−4377. doi: 10.1175/1520-0442(2000)013<0001:IAIVOR>2.0.CO;2
    [8] Lelieveld J, Dentener F J, Peters W, et al. 2004. On the role of hydroxyl radicals in the self-cleansing capacity of the troposphere [J]. Atmos. Chem. Phys. , 4(9−10): 2337−2344. doi:10.5194/acp-4-2337-2004
    [9] Li M, Zhang Q, Kurokawa J I, et al. 2017. MIX: A mosaic Asian anthropogenic emission inventory under the international collaboration framework of the MICS–Asia and HTAP [J]. Atmos. Chem. Phys., 17(2): 935−963. doi: 10.5194/acp-17-935-2017
    [10] Li K, Jacob D J, Liao H, et al. 2019. Anthropogenic drivers of 2013–2017 trends in summer surface ozone in China [J]. Proc. Natl. Acad. Sci. USA, 116(2): 422−427. doi: 10.1073/pnas.1812168116
    [11] Li K, Jacob D J, Liao H, et al. 2021. Ozone pollution in the North China Plain spreading into the late-winter haze season [J]. Proc. Natl. Acad. Sci. USA, 118(10): e2015797118. doi: 10.1073/pnas.2015797118
    [12] Liu S, Xing J, Zhang H L, et al. 2019. Climate-driven trends of biogenic volatile organic compound emissions and their impacts on summertime ozone and secondary organic aerosol in China in the 2050s [J]. Atmos. Environ., 218: 117020. doi: 10.1016/j.atmosenv.2019.117020
    [13] 娄梦筠. 2019. 我国不同地区大气边界层与PM2.5相互作用的观测研究 [D]. 中国气象科学研究院博士学位论文.

    Lou Mengyun. 2019. On the atmospheric boundary layer and PM2.5 interaction in China: A perspective from radiosonde observations [D]. Ph. D. dissertation (in Chinese), Chinese Academy of Meteorological Sciences.
    [14] Lu K D, Hofzumahaus A, Holland F, et al. 2013. Missing OH source in a suburban environment near Beijing: Observed and modelled OH and HO2 concentrations in summer 2006 [J]. Atmos. Chem. Phys., 13(2): 1057−1080. doi: 10.5194/acp-13-1057-2013
    [15] Lu K D, Guo S, Tan Z F, et al. 2019. Exploring atmospheric free-radical chemistry in China: The self-cleansing capacity and the formation of secondary air pollution [J]. Natl. Sci. Rev., 6(3): 579−594. doi: 10.1093/nsr/nwy073
    [16] Ma X F, Tan Z F, Lu K D, et al. 2019. Winter photochemistry in Beijing: Observation and model simulation of OH and HO2 radicals at an urban site [J]. Sci. Total Environ., 685: 85−95. doi: 10.1016/j.scitotenv.2019.05.329
    [17] Ren X J, Yang D J, Yang X Q. 2015. Characteristics and mechanisms of the subseasonal eastward extension of the South Asian high [J]. J. Climate, 28(17): 6799−6822. doi: 10.1175/JCLI-D-14-00682.1
    [18] Rohrer F, Berresheim H. 2006. Strong correlation between levels of tropospheric hydroxyl radicals and solar ultraviolet radiation [J]. Nature, 442(7099): 184−187. doi: 10.1038/nature04924
    [19] Shah V, Jacob D J, Li K, et al. 2020. Effect of changing NOx lifetime on the seasonality and long-term trends of satellite-observed tropospheric NO2 columns over China [J]. Atmos. Chem. Phys., 20(3): 1483−1495. doi: 10.5194/acp-20-1483-2020
    [20] Shao M, Tang X Y, Zhang Y H, et al. 2006. City clusters in China: Air and surface water pollution [J]. Front. Ecol. Environ., 4(7): 353−361. doi: 10.1890/1540-9295(2006)004[0353:CCICAA]2.0.CO;2
    [21] Shu L, Xie M, Wang T J, et al. 2016. Integrated studies of a regional ozone pollution synthetically affected by subtropical high and typhoon system in the Yangtze River Delta region, China [J]. Atmos. Chem. Phys., 16(24): 15801−15819. doi: 10.5194/acp-16-15801-2016
    [22] Su M F, Lin Y P, Fan X Q, et al. 2012. Impacts of global emissions of CO, NOx, and CH4 on China tropospheric hydroxyl free radicals [J]. Adv. Atmos. Sci., 29(4): 838−854. doi: 10.1007/s00376-012-1229-2
    [23] Tan Z F, Fuchs H, Lu K D, et al. 2017. Radical chemistry at a rural site (Wangdu) in the North China Plain: Observation and model calculations of OH, HO2 and RO2 radicals [J]. Atmos. Chem. Phys., 17(1): 663−690. doi: 10.5194/acp-17-663-2017
    [24] Tan Z F, Lu K D, Hofzumahaus A, et al. 2019. Experimental budgets of OH, HO2, and RO2 radicals and implications for ozone formation in the Pearl River Delta in China 2014 [J]. Atmos. Chem. Phys., 2019,19(10): 7129−7150. doi: 10.5194/acp-19-7129-2019
    [25] 王耀庭, 李威, 张小玲, 等. 2012. 北京城区夏季静稳天气下大气边界层与大气污染的关系 [J]. 环境科学研究, 25(10): 1092–1098.

    Wang Yaoting, Li Wei, Zhang Xiaoling, et al. 2012. Relationship between atmospheric boundary layer and air pollution in summer stable weather in the Beijing Urban Area [J]. Research of Environmental Sciences, 25(10): 1092−1098. doi:10.13198/j.res.2012.10.19.wangyt.011
    [26] Woodward-Massey R, Slater E J, Alen J, et al. 2020. Implementation of a chemical background method for atmospheric OH measurements by laser-induced fluorescence: Characterisation and observations from the UK and China [J]. Atmos. Meas. Tech., 13(6): 3119−3146. doi: 10.5194/amt-13-3119-2020
    [27] Xue T, Zheng Y X, Geng G N, et al. 2020. Estimating spatiotemporal variation in ambient ozone exposure during 2013–2017 using a Data–Fusion Model [J]. Environ. Sci. Technol., 54(23): 14877−14888. doi: 10.1021/acs.est.0c03098
    [28] 杨闻达, 程鹏, 田智林, 等. 2017. 广州市夏秋季HONO污染特征及白天未知源分析 [J]. 中国环境科学, 37(6): 2029−2039. doi: 10.3969/j.issn.1000-6923.2017.06.005

    Yang Wenda, Cheng Peng, Tian Zhilin, et al. 2017. Study on HONO pollution characteristics and daytime unknown sources during summer and autumn in Guangzhou, China [J]. China Environmental Science, 37(6): 2029−2039. doi: 10.3969/j.issn.1000-6923.2017.06.005
    [29] Yang X P, Lu K D, Ma X F, et al. 2021. Observations and modeling of OH and HO2 radicals in Chengdu, China in summer 2019 [J]. Sci. Total Environ., 772: 144829. doi: 10.1016/j.scitotenv.2020.144829
    [30] 岳玎利, 钟流举, 沈劲, 等. 2015. 珠三角地区日间HNO2和O3对OH自由基生成的影响 [J]. 中国科技论文, 10(12): 1387−1391. doi: 10.3969/j.issn.2095-2783.2015.12.008

    Yue Dingli, Zhong Liuju, Shen Jin, et al. 2015. Effect of atmospheric HNO2 and O3 on OH radical formation during daytime in the Pearl River Delta Region [J]. China Sciencepaper, 10(12): 1387−1391. doi: 10.3969/j.issn.2095-2783.2015.12.008
    [31] 岳玎利, 钟流举, 沈劲, 等. 2016. 珠三角地区秋季HNO2污染特性及其对OH自由基的影响 [J]. 环境科学与技术, 39(2): 162−166. doi: 10.3969/j.issn.1003-6504.2016.02.030

    Yue Dingli, Zhong Liuju, Shen Jin, et al. 2016. Pollution properties of atmospheric HNO2 and its effect on OH radical formation in the PRD region in autumn [J]. Environ. Sci. Technol., 39(2): 162−166. doi: 10.3969/j.issn.1003-6504.2016.02.030
    [32] Zhang Y H, Hu M, Zhong L J, et al. 2008. Regional integrated experiments on air quality over Pearl River Delta 2004 (PRIDE-PRD2004): Overview [J]. Atmos. Environ., 42(25): 6157−6173. doi: 10.1016/j.atmosenv.2008.03.025
    [33] Zhang H N, Wang Y H, Park T W, et al. 2017. Quantifying the relationship between extreme air pollution events and extreme weather events [J]. Atmospheric Research, 188: 64−79. doi: 10.1016/j.atmosres.2016.11.010
    [34] Zheng B, Tong D, Li M, et al. 2018. Trends in China’s anthropogenic emissions since 2010 as the consequence of clean air actions [J]. Atmos. Chem. Phys., 18(19): 14095−14111. doi: 10.5194/acp-18-14095-2018
    [35] Zhu T, Shang J, Zhao D F. 2011. The roles of heterogeneous chemical processes in the formation of an air pollution complex and gray haze [J]. Sci. China Chem., 54(1): 145−153. doi: 10.1007/s11426-010-4181-y
  • 加载中
图(6) / 表(2)
计量
  • 文章访问数:  565
  • HTML全文浏览量:  85
  • PDF下载量:  113
  • 被引次数: 0
出版历程
  • 收稿日期:  2021-11-19
  • 录用日期:  2022-01-18
  • 网络出版日期:  2022-01-21
  • 刊出日期:  2023-05-15

目录

    /

    返回文章
    返回