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CO2加氢制烯烃铁基催化剂失活机理研究

闫龙飞 范志辉 刘雯琦 田宁博 盛辉 党闪闪 张振洲 涂维峰

燃料化学学报2025,Vol.53Issue(11):1583-1589,7.
燃料化学学报2025,Vol.53Issue(11):1583-1589,7.DOI:10.1016/S1872-5813(25)60552-4

CO2加氢制烯烃铁基催化剂失活机理研究

Study on deactivation mechanism of iron-based catalyst for hydrogenation of CO2 to olefins

闫龙飞 1范志辉 1刘雯琦 1田宁博 1盛辉 1党闪闪 1张振洲 1涂维峰1

作者信息

  • 1. 郑州大学炼焦煤资源绿色开发全国重点实验室,河南郑州 450000
  • 折叠

摘要

Abstract

Hydrogenation of CO2 to olefins catalyzed by iron-based catalysts is an important platform reaction for high-value utilization of CO2 resources.Revealing its deactivation behavior and mechanism is the premise of designing stable and efficient industrial iron-based catalysts.FeZn catalyst was prepared by coprecipitation method,and the catalytic activity and structural evolution of Fe-based catalyst for hydrogenation of CO2 to olefins under industrial reaction conditions were studied by XRD,Raman,O2-TPO and ICP-OES.The results show that under the conditions of 320 ℃,2 MPa,CO2∶H2∶Ar=1∶3∶3,GHSV=30000 mL/(gh),the CO2 conversion and olefin selectivity can reach 33.3%and 52.8%,but the activity stability time is only 28 h.In an industrial fixed-bed reactor,the oxidation degree of the active phase of catalyst Fe5C2 is gradually intensified along the reactant flow direction,and the phase separation of FeZn catalyst occurs,and the surface carbon and ZnO species migrate along the reactant flow direction,resulting in the coverage of the active phase,and the contents of Fe3O4 and ZnO are gradually increased along the axial direction of the catalyst bed,which reduces the reaction activity of hydrogenation of CO2 to olefins and slowly increases the selectivity of CO.

关键词

CO2加氢/烯烃/铁基催化剂/失活

Key words

hydrogenation of CO2/olefin/iron-based catalyst/deactivation

分类

化学

引用本文复制引用

闫龙飞,范志辉,刘雯琦,田宁博,盛辉,党闪闪,张振洲,涂维峰..CO2加氢制烯烃铁基催化剂失活机理研究[J].燃料化学学报,2025,53(11):1583-1589,7.

基金项目

The project was supported by General Projects of National Natural Science Foundation(22478365,22208314,22238003)and Natural Science Foundation of Henan Province(232300421090).国家自然科学基金面上项目(22478365,22208314,22238003)和河南省自然科学基金(232300421090)资助 (22478365,22208314,22238003)

燃料化学学报

OA北大核心

2097-213X

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