摘要
Since the discovery of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)in the process of municipal solid waste incineration(MSWI),a large number of researches have been conducted to reveal their formation mechanisms and emission characteristics.As one of national priority control pollutants,chlorinated organics are inclined to transfer into PCDD/Fs in the heterogeneously catalyzed process,which has been considered to be one of great challenges in environmental catalysis.However,so far direct evidences to support such a conversion process are insufficient,and the reaction mechanisms are lack of exploration.This study investigated the catalytic elimination of chlorobenzene(CBz)over a range of industrially applied active species including Pt,Ru,V,Ce and Mn oxides,and explored their reaction byproducts,chlorine adsorption/desorption behaviors and PCDD/F formations.We found that all of these species could generate the PCDD/Fs,amongst which,Mn species were the most active for PCDD/F formation.Approximately 140 ng I-TEQg-1 PCDD/Fs were detected on the Mn-CNT surface after ageing at250℃for 30 h.Even using the dichloromethane(DCM)as a precursor,significant PCDD/Fs were still detected.The Ru and V species were shown to generate much less polychlorinated byproducts and PCDD/Fs,owning to their sufficiently high abilities in Cl desorption,which were through the semi-Deacon and Br(?)nsted H reactions,respectively.
基金
financially supported by the National Natural Science Foundation of China(Nos.21777140,21922607)
the Outstanding Youth Project of Zhejiang Natural Science Foundation(No.LR19E080004)。
