Abstract
Measurements of column-averaged dry-air mole fractions of carbon dioxide and carbon monoxide, CO2 (XCO2) and CO (XCO), were performed throughout 2019 at an urban site in Beijing using a compact Fourier Transform Spectrometer (FTS) EM27/SUN. This data set is used to assess the characteristics of combustion-related CO2 emissions of urban Beijing by analyzing the correlated daily anomalies of XCO and XCO2 (e.g., ΔXCO and ΔXCO2). The EM27/SUN measurements were calibrated to a 125HR-FTS at the Xianghe station by an extra EM27/SUN instrument transferred between two sites. The ratio of ΔXCO over ΔXCO2 (ΔXCO:ΔXCO2) is used to estimate the combustion efficiency in the Beijing region. A high correlation coefficient (0.86) between ΔXCO and ΔXCO2 is observed. The CO:CO2 emission ratio estimated from inventories is higher than the observed ΔXCO:ΔXCO2 (10.46 ± 0.11 ppb ppm−1) by 42.54%–101.15%, indicating an underestimation in combustion efficiency in the inventories. Daily ΔXCO:ΔXCO2 are influenced by transportation governed by weather conditions, except for days in summer when the correlation is low due to the terrestrial biotic activity. By convolving the column footprint [ppm (µmol m−2 s−1)−1] generated by the Weather Research and Forecasting-X-Stochastic Time-Inverted Lagrangian Transport models (WRF-X-STILT) with two fossil-fuel emission inventories (the Multi-resolution Emission Inventory for China (MEIC) and the Peking University (PKU) inventory), the observed enhancements of CO2 and CO were used to evaluate the regional emissions. The CO2 emissions appear to be underestimated by 11% and 49% for the MEIC and PKU inventories, respectively, while CO emissions were overestimated by MEIC (30%) and PKU (35%) in the Beijing area.
摘要
城市作为主要碳源,在全球碳循环中起重要作用。本文利用小型傅里叶光谱仪 EM27/SUN FTS在北京城区开展连续高精度大气温室气体CO2及人为排放示踪污染气体CO的大气柱平均干空气混合比 (XCO2, XCO)观测。为获取EM27/SUN绝对精度,实验前后已与TCCON香河站的高分辨率光谱仪125HR-FTS交叉对比。 XCO和XCO2的日变化异常(ΔXCO, ΔXCO2) 高度相关 (R2=0.86),通过研究ΔXCO与ΔXCO2的比例关系 (ΔXCO:ΔXCO2) 有助于解析北京城区人为碳排放相关的燃烧效率。除去夏季受生态吸收影响的数据后,2019年北京城区ΔXCO:ΔXCO2 (10.46 ± 0.11 ppb ppm−1) , 明显高于同期北半球城区TCCON FTS站点观测比例值。逐日ΔXCO:ΔXCO2 易受周围气象场传输影响,通过WRF-XSTILT 大气传输模型对不同来源聚类分析可知,来自南部污染区的ΔXCO:ΔXCO2明显低于西北干净源。利用WRF-XSTILT和两种“自下而上”碳排放清单 (MEIC, PKU) 估计的CO:CO2比观测结果高42.54%-101.15%,表明清单对北京城区燃烧效率的低估。进一步将粗网格分辨率模型CAMS作为大背景,北京地区MEIC和PKU的分别约低估了11 % 和49 %的人为CO2排放量,而CO排放量被高估30 %和35%。
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Acknowledgements
We want to thank the TCCON community for providing the FTIR observations of Pasadena, Karlsruhe, Tsukuba, and Paris. This study is supported by grants from the National Key Research and Development Program of China (Grant No. 2017YFB0504000), National Natural Science Foundation of China (Grant No. 41875043), the Strategic Priority Research 275 Program of the Chinese Academy of Sciences (Grant No. XDA17010102), External Cooperation Program of the Chinese Academy of Science (Grant No. GJHZ1802), Youth Innovation Promotion Association, CAS.
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• Daytime column-averaged dry-air mole fractions of atmospheric CO2 and CO are provided in urban Beijing based on a portable FTS since 2019.
• The CO:CO2 emission ratio estimated by MEIC and PKU is 42.54% and 101.15% higher than the observed ΔXCO:ΔXCO2 (10.46 ppb ppm−1), indicating an underestimation of the combustion efficiency in inventories.
• The MEIC underestimates CO2 emissions by about 11% and overestimates 30% CO emissions by 30%; PKU underestimates CO2 emissions by 49% and overestimates CO emissions by 35%.
This paper is a contribution to the special issue on Carbon Neutrality: Important Roles of Renewable Energies, Carbon Sinks, NETs and non-CO2 GHGs.
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Che, K., Liu, Y., Cai, Z. et al. Characterization of Regional Combustion Efficiency using ΔXCO: ΔXCO2 Observed by a Portable Fourier-Transform Spectrometer at an Urban Site in Beijing. Adv. Atmos. Sci. 39, 1299–1315 (2022). https://doi.org/10.1007/s00376-022-1247-7
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DOI: https://doi.org/10.1007/s00376-022-1247-7