Evolution of Fe Sites in Conversion of CO_(2)to Methanol to Aromatics in Tandem H-[Fe]-ZSM-5/ZnO-ZrO_(2)Catalysts  

作　　者：Dhrumil R.Shah Atticus Tucker Zhenhua Xie Jingguang G.Chen Christopher W.Jones 

机构地区：[1]School of Chemical and Biomolecular Engineering,Georgia Institute of Technology,Atlanta,GA 30332 [2]Department of Chemical Engineering,Columbia University,New York,NY 10027-7041

出　　处：《CCS Chemistry》2024年第12期2895-2907,共13页中国化学会会刊(英文)

基　　金：supported by the U.S.Department of Energy,Office of Fossil Energy under Award Number DE-FE0031719;Christopher W.Jones acknowledges the John F.BrockⅢChair in Chemical and Biomolecular Engineering at Georgia Tech.This work was performed in part at the Georgia Tech Institute for Matter and Systems,a member of the National Nanotechnology Coordinated Infrastructure,which is supported by the National Science Foundation(ECCS-2025462);This research used beamline 7-BM(QAS)of the National Synchrotron Light SourceⅡ(NSLS-Ⅱ)at Brookhaven National Laboratory(Contract No.DESC0012704);supported in part by the Synchrotron Catalysis Consortium(Grant No.DE-SC0012653).

摘　　要：In this study,H-[Fe]-ZSM-5/ZnO-ZrO_(2)composites are investigated as tandem catalysts for conversion of CO_(2)to mixed aromatic compounds in the presence of H2.Fe-MFI of varying Si/Fe ratios is synthesized to study the effect of Fe content in the MFI on the aromatic selectivity.The CO_(2)to aromatics selectivity over H-[Fe]-ZSM-5/ZnO-ZrO_(2)is maximized at Si/Fe ratio=160.At lower Fe contents,the CO_(2)to aromatics selectivity is affected by limiting the Lewis acid site density.At high Fe loadings,the reduction of Fe sites leads to more production of CO and oxygenates.The reduction during pretreatment and reaction provides reduced Fe2+extraframework ions,with the appearance of these species concomitant with enhanced CO and oxygenate formation during the reaction.

关 键 词：CO_(2)utilization tandem catalysis FE-MFI heterogeneous catalysis CO_(2)to aromatics methanol to aromatics zeolite acid catalysis 

分 类 号：O64[理学—物理化学]