摘要
可再生电能驱动CO_(2)电催化合成化学品或燃料,具有反应条件温和、产物选择性可调且可利用分布式可再生能源优势。合成气作为一类重要的化工原料气,可制备甲醇、乙醇、烯烃等大宗化学品,是CO_(2)电催化转化的重要途径,如何高电流密度、高选择性且精准调控碳氢比例(CO/H2)是需要解决的关键科学技术难题。本文从提升电流密度和效率、拓宽合成气比例角度出发,综述了CO_(2)电催化还原制合成气的最新研究进展,包括电极材料设计、电解液开发、电解槽结构创新等;论述了利用原位表征和理论模拟(DFT、MD)方法对CO_(2)电催化还原制合成气反应机理的研究进展。在此基础上,提出可通过催化剂多级形貌调控、多活性位点设计、CO_(2)捕集与转化系统集成、CO_(2)还原与阳极反应耦合等途径,提升CO_(2)电催化还原制合成气效率的策略。最后,探讨和展望了实现CO_(2)电催化还原制合成气工业化的挑战和问题。
Renewable electric energy drives CO_(2)electrocatalytic synthesis of chemicals or fuels,which has the advantages of mild reaction conditions,adjustable product selectivity and the use of distributed renewable energy.Syngas,as an important chemical raw gas,can be used to produce methanol,ethanol,olefins and other bulk chemicals,thus CO_(2)electrocatalytic reduction to syngas is one of important ways to CO_(2)utilization.However,accurately controlling the CO/H2 ratio with high current density and high selectivity is one of the key scientific problems.In this paper,from the perspective of improving current density and efficiency,and widening the proportion of syngas,we reviewed the latest research progress of CO_(2)electrocatalytic reduction to syngas,including electrode design,electrolyte development,and electrolyzer structure innovation,and so on.Then,the research progress on the electrocatalytic reduction mechanism of CO_(2)electrocatalytic reduction to syngas by in-situ characterization and theoretical simulation(DFT,MD)is discussed.Furthermore,it was concluded that the efficiency of CO_(2)electrocatalytic reduction to syngas can be improved through multi-stage morphology regulation of catalyst,multi-active site design,integration of CO_(2)capture and conversion system,and the coupling of CO_(2)reduction and anodic reaction.Finally,the challenges of the industrialization of CO_(2)electrocatalytic reduction to syngas are discussed and prospected.
作者
李鑫
曾少娟
彭奎霖
袁磊
张香平
LI Xin;ZENG Shaojuan;PENG Kuilin;YUAN Lei;ZHANG Xiangping(Henan Institute of Advanced Technology,Zhengzhou University,Zhengzhou 450003,Henan,China;Beijing Key Laboratory of Ionic Liquids Clean Process,State Key Laboratory of Multiphase Complex Systems,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China;Engineering Research Center of Advanced Functional Material Manufacturing of Ministry of Education,School of Chemical Engineering,Zhengzhou University,Zhengzhou 450001,Henan,China)
出处
《化工学报》
EI
CSCD
北大核心
2023年第1期313-329,共17页
CIESC Journal
基金
国家重点研发计划项目(2020YFA0710200)
国家自然科学基金项目(21890764,22122814,21838010)
山西省科技重大专项项目(20201102005)
中国科学院青年创新促进会项目(2018064)。
关键词
二氧化碳
合成气
电催化还原
催化剂
电解液
机理
CO_(2)
syngas
electrocatalytic reduction
catalyst
electrolytes
mechanism
