Atmospheric heterogeneous reaction of chlorobenzene on mineralα-Fe_(2)O_(3)particulates:a chamber experiment study  

作　　者：Meiling Chen Mengjie Yin Yuetan Su Ruizhe Li Kezhou Liu Zhongbiao Wu Xiaole Weng 

机构地区：[1]Key Laboratory of Environment Remediation and Ecological Health(Ministry of Education),College of Environmental and Resource Sciences,Zhejiang University,Hangzhou 310058,China [2]ZJU-Hangzhou Global Scientific and Technological Innovation Center,Zhejiang University,Hangzhou 311215,China [3]School of Automation(School of Artificial Intelligence),Hangzhou Dianzi University,Hangzhou 310018,China [4]Zhejiang Provincial Engineering Research Centre of Industrial Boiler&Furnace Flue Gas Pollution Control,Hangzhou 311200,China

出　　处：《Frontiers of Environmental Science & Engineering》2023年第11期169-180,共12页环境科学与工程前沿（英文）

基　　金：supported by the National Natural Science Foundation of China(No.22176169,52070168);the Key R&D Plan of Zhejiang Province(No.2023C03127);the Fundamental Research Funds for the Central Universities(No.226-2022-00150).

摘　　要：Despite the large emission of chlorinated volatile organic compounds(CVOCs)into the atmosphere,the ultimate fate of these compounds remains largely unknown.Herein,we explore the photochemical conversion of an important class of CVOCs,namely chlorobenzene(CB),on mineralα-Fe_(2)O_(3)particulates under atmospheric relevant conditions.A series of chamber reactions composed of the CB with/without SO_(2)or NO_(2)are performed,followed by in situ diffuse reflectance infrared Fourier transform spectroscopy measurements and density functional theory calculations.We show that CB can be considerably degraded byα-Fe_(2)O_(3)under light irradiation,whereas the reaction is markedly suppressed by adding SO_(2)or NO_(2)owing to their competitive adsorption and surface acidification.In particular,we discover that CB can be ultimately converted into polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)under dark state or light irradiation,suggesting a possible origin of atmospheric PCDD/Fs from this overlooked photochemical source.

关 键 词：Photochemical conversion CHLOROBENZENE α-Fe_(2)O_(3) PCDD Fs Mineral particulate 

分 类 号：X51[环境科学与工程—环境工程]