基于卫星遥感和地面观测的人为源VOCs区域清单多维校验

本文针对京津冀区域，基于传统的排放因子法建立了区域人为源VOCs物种排放清单；并基于区域卫星遥感甲醛信息和典型城市地面VOCs观测信息，开展了VOCs物种清单多维校验研究.清单计算结果表明，该区域2013、2015和2017年VOCs排放量分别为202.67、207.34和193.42万t，以烷烃（29.83%~30.72%）、不饱和烃（16.54%~17.68%）、芳香烃（27.14%~27.51%）、醛（8.75%~9.52%）、酮（8.13%~9.04%）和醇醚酯（5.13%~6.60%）为主.2013~2017年VOCs清单排量，张家口、秦皇岛和衡水小幅上升（每年1.10%~1.66%），邢台和邯郸小幅下降（每年-1.46%~-1.12%），承德、唐山、保定和沧州呈稳定趋势，且与卫星遥感HCHO柱浓度年际变化呈现较好的一致性趋势；而北京、天津、廊坊和石家庄的VOCs排放年变幅（每年-6.51%、-3.30%、2.16%和0.11%）与HCHO柱浓度变幅（每年-1.17%、7.19%、-0.24%和6.68%）差异较大.在VOCs清单区域空间分布上，城市地区VOCs网格排放量与HCHO柱浓度取得了较好的线性相关性（R>0.5）；而在郊区地区，两者相关度仅为0.33，主要源于郊区天然源VOCs二次转化对HCHO的重要影响和贡献.最后，本文在北京市和邯郸市城区开展了VOCs地面浓度观测，回归了主要VOCs化合物与CO的排放比值（ER），对比发现：大部分烃类化合物的清单ER值与回归ER值具有较好的吻合度，但乙烷的清单ER值显著偏低（-156%~-73%），C8以上芳香烃有所偏高（54%~74%）.总体而言，本文建立的区域人为源VOCs物种清单具有较好的准确性和可靠性.

Multidimensional Verification of Anthropogenic VOCs Emissions Inventory Through Satellite Retrievals and Ground Observations

In this paper, a regional emissions inventory of anthropogenic VOCs was established based on the traditional emissions factor method for the Beijing-Tianjin-Hebei (BTH) region, followed by a multidimensional calibration study based on regional satellite remote sensing information for formaldehyde and typical urban ground VOCs. Inventory calculations showed that the VOCs emissions in BTH in 2013, 2015, and 2017 were 2026700, 2073400, and 1934200 tons, respectively, comprising alkanes (29.83% to 30.72%), unsaturated hydrocarbons (16.54% to 17.68%), aromatic hydrocarbons (27.14% to 27.51%), aldehydes (8.75% to 9.52%), ketones (8.13% to 9.04%), and aldehydes and ketones lipids (5.13% to 6.60%). During 2013-2017, the emission of VOCs in Zhangjiakou, Qinhuangdao, and Hengshui increased slightly (1.10% to 1.66% per year); emissions in Xingtai and Handan decreased slightly (-1.46% to -1.12% per year); and emissions in Chengde, Tangshan, Baoding, and Cangzhou were stable. There trends were consistent with the inter-annual trend of satellite-derived HCHO column concentrations. However, in Beijing, Tianjin, Langfang, and Shijiazhuang, annual variations in VOCs emissions (-6.51%, -3.30%, 2.16%, and 0.11% per year) and HCHO column concentrations (-1.17%, 7.19%, -0.24%, and 6.68% per year) were observed, respectively. In the regional VOCs inventory, a good linear correlation (R>0.5) was achieved between the grid emissions of VOCs and HCHO column concentrations in urban areas, while the correlation was only 0.33 in suburban areas. This is mainly due to the important influence of secondary conversion of VOCs originating from natural sources to HCHO in suburban areas. In addition, ground-level VOCs concentrations were observed in the urban areas of Beijing and Handan, where the emission ratios (ERs) of VOCs and CO were regressed. The ERs of most hydrocarbons were in good agreement with the regressed ERs, but the ERs of ethane were significantly lower (-156% to -73%) and the ERs of aromatic hydrocarbons above C8 were relatively high (54% to 74%). In general, the regional anthropogenic VOCs emissions inventory established in this paper offers high accuracy and reliability.