物理化学学报2025，Vol.41Issue(3)：1-19,19.DOI:10.3866/PKU.WHXB202308052
缺陷态二维超薄材料用于光/电催化CO2还原的基础与展望
Defective Ultrathin Two-Dimensional Materials for Photo-/Electrocatalytic CO2 Reduction:Fundamentals and Perspectives
摘要
Abstract
Photo-/electrocatalytic reduction of carbon dioxide(CO2)to carbon-based fuel molecules driven by renewable energy is an attractive strategy for resource regeneration and energy storage,especially for achieving carbon peak and carbon-neutral goals.However,the high thermodynamic stability and chemical inertness of CO2 molecules make the conversion efficiency and selectivity of reduction products very low,which further hinders its application.In addition,different CO2 reduction products have similar reduction potential and usually face severe hydrogen evolution competition under aqueous system conditions,which makes the selectivity of specific reduction products unable to be effectively controlled.To overcome these bottlenecks,researchers have been working for many years to develop efficient photo/electrocatalysts to enhance the activity and product selectivity of CO2 reduction.Thanks to the ultrathin thickness and large specific surface area,ultrathin two-dimensional materials possess highly active sites with high density and high uniformity,which can effectively regulate the key thermodynamic and kinetic factors of CO2 photo-/electroreduction reactions.As a typical two-dimensional material,the defective ultrathin two-dimensional materials can provide a large number of electron-rich catalytic sites to efficiently adsorb and highly activate CO2 molecules,which can effectively reduce the reaction barrier,thus accelerating CO2 reduction and enhancing product selectivity.Moreover,the local atomic and electronic structure of the defects can effectively stabilize the intermediate of CO2 reduction reactions,thus further optimizing the kinetics of CO2 reduction reactions.Furthermore,the surface defects are beneficial to the mass and electron transfer in the catalytic process,thus further improving the catalytic activity of the catalysts.In this review,we overview the latest research progress in CO2 photo-/electrocatalytic reduction using defective ultrathin two-dimensional materials,including the controllable synthesis and fine structure characterization of defective ultrathin two-dimensional materials;the modulation effect of defect structure on the local atomic and electronic structure;the advantages of defective ultrathin two-dimensional materials for CO2 reduction.We also discuss the challenges and opportunities of defective ultrathin two-dimensional materials for future development of CO2 photo-/electrocatalytic reduction.It is expected that this review will provide a guide for designing highly efficient CO2 reduction systems.关键词
缺陷结构/二维超薄材料/二氧化碳还原/光/电催化反应Key words
Defect/Ultrathin two-dimensional materials/CO2 reduction/Photo-/Electrocatalysis分类
化学引用本文复制引用
陈润华,吴琼,罗婧宸,祖小龙,朱姗,孙永福..缺陷态二维超薄材料用于光/电催化CO2还原的基础与展望[J].物理化学学报,2025,41(3):1-19,19.基金项目
The project was supported by the National Key Research and Development Program of China(2019YFA0210004,2022YFA1502904,2021YFA1501502),the National Natural Science Foundation of China(22125503,21975242,U2032212),the Youth Innovation Promotion Association of CAS(CX2340007003),the Anhui Provincial Natural Science Foundation(2208085QB31). 国家重点研发计划(2019YFA0210004,2022YFA1502904,2021YFA1501502),国家自然科学基金(22125503,21975242,U2032212),中国科学院青年创新促进会优秀会员(CX2340007003),安徽省自然科学基金(2208085QB31)资助项目 （2019YFA0210004,2022YFA1502904,2021YFA1501502）
