物理化学学报2026，Vol.42Issue(7)：170-184,15.DOI:10.1016/j.actphy.2026.100274
硫空位提升2D/2D In2.77S4/CuInS2 S型异质结光催化还原CO2为C2H4选择性
Sulfur vacancies boosting C2H4 selectivity of 2D/2D In2.77S4/CuInS2 S-scheme heterojunction for CO2 photoreduction
摘要
Abstract
Converting CO2 into multi-carbon hydrocarbons through artificial photosynthesis remains challenging due to sluggish C-C coupling dynamics and complex multi-electron processes.In this study,ultrathin In2.77S4/CuInS2 heterojunctions with abundant sulfur vacancies(SV)were synthesized via a one-step hydrothermal method.The S-scheme charge-transfer mechanism,driven by the built-in electric field,was confirmed through in situ X-ray photoelectron spectroscopy(XPS),femtosecond transient absorption spectroscopy(fs-TAS)and photoelectrochemical characterization.This S-scheme heterojunction not only enhanced the separation efficiency of photogenerated charge carriers but also maintained excellent reduction capability,enabling CO2 photoreduction to C2 hydrocarbons.Furthermore,experimental results and density functional theory(DFT)calculations demonstrated that SV shortened the Cu-In active site distance,optimized the local charge density and lowered the energy barrier for critical dimer formation(*CHOCO),thereby accelerating the C-C coupling kinetics.Finally,the In2.77S4/CuInS2-4 catalyst exhibited excellent yield(47.2 μmol g-1 h-1)and selectivity(99.1%)of C2H4,which attributed to the synergistic effect of efficient carrier rectification by the S scheme heterojunction and optimized C-C coupling dynamics facilitated by SV.Furthermore,isotope labeling confirmed CO2 as the sole carbon source for the reaction.Overall,this"sulfur vacancy-heterojunction"strategy for CO2 photoreduction to C2H4 with superior electron selectivity offers valuable insights into CO2 utilization.关键词
S型/光催化剂/C2H4/二氧化碳还原/In2.77S4/CuInS2Key words
S-scheme/Photocatalysts/C2H4/CO2 reduction/In2.77S4/CuInS2分类
化学化工引用本文复制引用
崔依琳,李中付,张维坤,高禹,董志超,刘从华..硫空位提升2D/2D In2.77S4/CuInS2 S型异质结光催化还原CO2为C2H4选择性[J].物理化学学报,2026,42(7):170-184,15.基金项目
本研究得到国家自然科学基金(22302114)、山东省自然科学基金(ZR2023QB210)、淄博市重点研发计划(校城融合)项目(2021SNPT0042)、湖南省环境光催化应用技术重点实验室开放课题(2114506)的资助. （22302114）
