Energy Platform for Directed Charge Transfer in the Cascade Z-Scheme Heterojunction: CO2 Photoreduction without a Cocatalyst

被引:200
作者
Bian, Ji [1 ,2 ]
Zhang, Ziqing [1 ]
Feng, Jiannan [1 ]
Thangamuthu, Madasamy [3 ]
Yang, Fan [1 ]
Sun, Ling [1 ]
Li, Zhijun [1 ]
Qu, Yang [1 ]
Tang, Dongyan [2 ]
Lin, Zewei [2 ]
Bai, Fuquan [4 ,5 ]
Tang, Junwang [3 ]
Jing, Liqiang [1 ]
机构
[1] Heilongjiang Univ, Dept Key Lab Funct Inorgan Mat Chem, Int Joint Res Ctr & Lab Catalyt Technol, Sch Chem & Mat Sci,Minist Educ, Harbin 150080, Peoples R China
[2] Harbin Inst Technol, Sch Chem & Chem Engn, Harbin 150001, Peoples R China
[3] UCL, Dept Chem Engn, Torrington Pl, London WC1E 7JE, England
[4] Jilin Univ, Int Joint Res Lab Nanomicro Architecture Chem, Inst Theoret Chem, Changchun 130021, Peoples R China
[5] Jilin Univ, Coll Chem, Changchun 130021, Peoples R China
基金
英国工程与自然科学研究理事会; 中国国家自然科学基金;
关键词
charge lifetime; charge modulation; heterojunctions; photocatalysis; Z-Scheme heterojunctions; 001; FACETS; REDUCTION; EFFICIENT; NANOSHEETS; METHANOL; G-C3N4;
D O I
10.1002/anie.202106929
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A universal strategy is developed to construct a cascade Z-Scheme system, in which an effective energy platform is the core to direct charge transfer and separation, blocking the unexpected type-II charge transfer pathway. The dimension-matched (001)TiO2-g-C3N4/BiVO4 nanosheet heterojunction (T-CN/BVNS) is the first such model. The optimized cascade Z-Scheme exhibits approximate to 19-fold photoactivity improvement for CO2 reduction to CO in the absence of cocatalysts and costly sacrificial agents under visible-light irradiation, compared with BVNS, which is also superior to other reported Z-Scheme systems even with noble metals as mediators. The experimental results and DFT calculations based on van der Waals structural models on the ultrafast timescale reveal that the introduced T as the platform prolongs the lifetimes of spatially separated electrons and holes and does not compromise their reduction and oxidation potentials.
引用
收藏
页码:20906 / 20914
页数:9
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