苯甲醛
苯甲醇
异质结
光催化
双功能
材料科学
空位缺陷
氧化还原
光化学
催化作用
密度泛函理论
化学工程
化学
光电子学
有机化学
计算化学
结晶学
工程类
冶金
作者
Chaohui Ruan,Chengyu Wang,Yu‐Cheng Chen,Zhongliao Wang,Keting Wang,Ying Zhou,Sujuan Zhang,Gaoli Chen,Xiuzhen Zheng,Sugang Meng,Shifu Chen
标识
DOI:10.1016/j.seppur.2024.127929
摘要
CO2 photoreduction into chemical fuels is hopeful and sustainable for a carbon–neutral future. Herein, a bifunctional dual-vacancy-modified hollow heterojunction photocatalyst is ingeniously designed for CO2 photoreduction to CO coupling with selective oxidation of benzyl alcohol to benzaldehyde. Synergistic catalysis effect resulted from hollow heterostructures, TiO2 with O vacancies (TiO2-x) and Zn0.3-xCd0.7S with Zn vacancies (ZCS) leads to excellent photoreduction and photoxidation performances. The optimized sample (TiO2-x/ZCS hollow sphere) exhibits highest photocatalytic activity of all the obtained samples. The yields of CO and benzaldehyde are 105 and 323.5 μmol g–1h−1, respectively. The construction of Z-scheme heterojunction realizes the spatial separation of redox reaction sites, and the dual-vacancy distributed on the heterojunction enhance the interfacial reactivity. Additionally, density functional theory calculation and in-situ technology reveal that Zn vacancy in ZCS and O vacancy in TiO2-x function as active sites for the binding and activation of *COOH and *PhCH2O-, respectively, thereby stabilizing the crucial step in the formation of intermediates such as CO and benzaldehyde. This work enhances the utilization of photogenerated carrier, and affords a new opportunity to design hollow heterojunction with dual-vacancy engineering to boost photocatalytic performance for coupling reaction system.
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