Direct and indirect Z-scheme heterostructure-coupled photosystem enabling cooperation of CO2 reduction and H2O oxidation

被引:326
作者
Wang, Ying [1 ,2 ]
Shang, Xiaotong [1 ]
Shen, Jinni [1 ]
Zhang, Zizhong [1 ]
Wang, Debao [2 ]
Lin, Jinjin [1 ]
Wu, Jeffrey C. S. [3 ]
Fu, Xianzhi [1 ]
Wang, Xuxu [1 ]
Li, Can [4 ]
机构
[1] Fuzhou Univ, Coll Chem, Res Inst Photocatalysis, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
[2] Qingdao Univ Sci & Technol, Coll Chem & Mol Engn, Key Lab Inorgan Synthet & Appl Chem, State Key Lab Base Ecochem Engn, Qingdao 266042, Peoples R China
[3] Natl Taiwan Univ, Dept Chem Engn, Taipei 10617, Taiwan
[4] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
基金
中国国家自然科学基金;
关键词
BINUCLEAR RUTHENIUM(II) COMPLEX; PHOTOCATALYTIC WATER OXIDATION; VISIBLE-LIGHT; CARBON-DIOXIDE; FORMIC-ACID; TWIN REACTOR; SEMICONDUCTOR; TIO2; EVOLUTION; CATALYST;
D O I
10.1038/s41467-020-16742-3
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The stoichiometric photocatalytic reaction of CO2 with H2O is one of the great challenges in photocatalysis. Here, we construct a Cu2O-Pt/SiC/IrOx composite by a controlled photodeposition and then an artificial photosynthetic system with Nafion membrane as diaphragm separating reduction and oxidation half-reactions. The artificial system exhibits excellent photocatalytic performance for CO2 reduction to HCOOH and H2O oxidation to O-2 under visible light irradiation. The yields of HCOOH and O-2 meet almost stoichiometric ratio and are as high as 896.7 and 440.7 mu molg(-1)h(-1), respectively. The high efficiencies of CO2 reduction and H2O oxidation in the artificial system are attributed to both the direct Z-scheme electronic structure of Cu2O-Pt/SiC/IrOx and the indirect Z-scheme spatially separated reduction and oxidation units, which greatly prolong lifetime of photogenerated electrons and holes and prevent the backward reaction of products. This work provides an effective and feasible strategy to increase the efficiency of artificial photosynthesis.
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页数:11
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