临沂市夏季羰基化合物来源及其对大气氧化性的影响  

Study on the sources of carbonyl compound pollution and its effect on atmospheric oxidation capacity in summer in Linyi City

作　　者：杨雪 赵世阳 张根[2] 胡书豪 王金鹤[1] 朱超 YANG Xue;ZHAO Shiyang;ZHANG Gen;HU Shuhao;WANG Jinhe;ZHU Chao(School of Municipal and Environmental Engineering,Shandong Jianzhu University,Ji'nan,250101,China;State Key Laboratory of Severe Weather&Key Laboratory of Atmospheric Chemistry of CMA,Chinese Academy of Meteorological Sciences,Beijing,100081,China)

机构地区：[1]山东建筑大学市政与环境工程学院,济南250101 [2]中国气象科学研究院大气成分与环境气象研究所(碳中和监测与评估中心),中国气象局大气化学重点开放实验室,北京100081

出　　处：《环境化学》2025年第1期221-233,共13页Environmental Chemistry

基　　金：国家自然科学基金(42005092,42275127,42075112);山东省自然科学基金(ZR2020QD058);山东建筑大学博士科研基金(XNBS1936)资助.

摘　　要：羰基化合物在大气光化学中扮演着重要角色,影响大气自由基丰度、大气氧化性强度以及臭氧(O_(3))光化学反应产率.通过对2022年8月临沂市大气羰基化合物及相关物种外场观测,结果发现甲醛(HCHO)体积分数φ(HCHO)和乙醛(CH3CHO)体积分数φ(CH_(3)CHO)分别为(4.95±2.01)×10^(−9)和(3.34±1.40)×10^(−9).根据多元线性回归结果发现二次生成是HCHO和CH3CHO主要来源,分别贡献其总体积分数的34.28%和35.95%.用基于观测约束的模式(Observation-Based Model,OBM)分析发现影响甲醛二次净生成速率的主要前体物为生物源烯烃和人为源烯烃(主要是正丁烯、乙烯和丙烯).影响乙醛二次净生成速率的主要前体物是人为源烯烃(正丁烯和丙烯)、烷烃(正己烷和正丁烷)和苯.烯烃类物质是影响临沂市羰基化合物体积分数水平的关键前体物物种.羰基化合物对大气氧化性的贡献最强,占比高达为74.64%.本研究强调了烯烃对羰基化合物污染的重要影响,并指出光化学污染日,羰基化合物对大气氧化性的重要作用,对未来国内外中小城市羰基化合物污染控制具有指导意义.Carbonyl compounds play an important role in atmospheric photo-chemistry,affecting the abundant of atmospheric radical,atmospheric oxidative capacity and ozone(O_(3))photo-chemistry production.Through the field observation of atmospheric carbonyl compounds and related species in Linyi City in August 2022,it was found that the volume fractionφ(HCHO)of formaldehyde(HCHO)and the volume fractionφ(CH_(3)CHO)of acetaldehyde(CH_(3)CHO)were(4.95±2.01)×10^(−9) and(3.34±1.40)×10^(−9) respectively.The sources of formaldehyde and acetaldehyde were analyzed using multiple linear regression analysis and their secondary production was found to contribute mostly,i.e.,34.28%and 35.95%of their total volume fractions,respectively.The Observation-Based Model(OBM)analysis revealed that the main precursors controlling the secondary production of formaldehyde were biogenic alkenes and anthropogenic alkenes(mainly n-butene,ethylene and propylene).The main precursors for the secondary production of acetaldehyde were anthropogenic sources of alkenes(n-butene and propylene),alkanes(n-hexane and n-butane),and benzene.Alkenes were the key species affecting the volume fraction levels of carbonyl compounds in Linyi.The atmospheric oxidative capacity was mostly influenced by the carbonyl compounds,which made up a significant percentage of 74.64%.This study emphasizes the important influence of alkenes on carbonyl compound pollution,and points out the important role of carbonyl compound on atmospheric oxidation during photochemical pollution days,which has a guiding effect on carbonyl compound pollution control in small and medium-sized cities in China and abroad in the future.

关 键 词：羰基化合物 OBM模型 相对增量反应活性(RIR) 关键前体物 大气氧化性 

分 类 号：X-1[环境科学与工程] O6[理学—化学]