摘要
Photocatalytic CO_(2)reduction to CH_(4)is regarded as one of the most promising strategies for mitigating environmental and energy challenges,offering a sustainable pathway toward achieving carbon neutrality.However,its practical application is hindered by low catalytic performance and product selectivity,primarily owing to inefficient electron transfer and insufficient stabilization of key reaction intermediates.Herein,an S-scheme heterojunction of In_(2)O_(3)/TiO_(2)is synthesized via a two-step method to enhance photogenerated charge carrier separation and transfer.The optimized photocatalyst demonstrates exceptional performance,achieving a CH_(4)yield of 64.1μmol g−1 h−1 accompanied by an ultrahigh electron selectivity of 96.0%.The integration of density functional theory(DFT)calculations with in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)analyses demonstrates that the heterojunction significantly enhances CO_(2)activation,as evidenced by the upshifted d-band center and increased crystal orbital Hamilton population(COHP)values.Furthermore,the In_(2)O_(3)/TiO_(2)heterojunction exhibits enhanced adsorption of CO_(2)and key intermediates,thereby improving reaction kinetics and thermodynamics.These properties facilitate the hydrogenation of ^(*)COOH,ultimately promoting CH_(4)generation.This work not only provides a mechanistic understanding of S-scheme heterojunctions in CO_(2)photoreduction but also provides a new design strategy for developing highly efficient photocatalysts.
出处
《SusMat》
2025年第4期98-107,共10页
可持续发展材料(英文)
基金
supported by the National Natural Science Foundation of China(Grant Nos.52373223,52400120,52463031)
the Sichuan Science and Technology Program(Grant No.2025NSFTD0003)
the Natural Science Foundation of Chongqing(Grant No.CSTB2023NSCQ-MSX0397)
the Science and Technology Research Program of Chongqing Municipal Education Commission(Grant No.KJQN202300560).
作者简介
Correspondence:Chunhui Wang(wangch87@ynu.edu.cn);Correspondence:Peng Chen(pengchen@cqnu.edu.cn);Correspondence:Ming Huang(huangming@uestc.edu.cn)。
