Efficient Interfacial Charge Transfer Enables Nearly 100% Selectivity for Solar-Light-Driven CO2 Conversion

被引:5
作者
Tang, Wangzhong [1 ,2 ]
Meng, Jie [1 ,2 ]
Ding, Tao [3 ]
Huang, Haisen [1 ,2 ]
Tan, Chuntian [1 ,2 ]
Zhong, Qingao [1 ,2 ]
Cao, Heng [3 ]
Li, Qunxiang [1 ,2 ]
Xu, Xiaoliang [1 ,2 ]
Yang, Jinlong [1 ,2 ]
机构
[1] Univ Sci & Technol China, Sch Chem & Mat Sci, Hefei 230026, Anhui, Peoples R China
[2] Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
[3] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230026, Anhui, Peoples R China
来源
ACS CATALYSIS | 2024年 / 14卷 / 10期
基金
中国国家自然科学基金;
关键词
2D/2D composites; transition-metal dichalcogenides; photocatalysis; CO2; reduction; reactionmechanism; RESE2;
D O I
10.1021/acscatal.4c01020
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The performance of transition-metal dichalcogenides (TMDs) as cocatalysts in CO2 photoreduction is considerably limited by their inherent poor conductivity and stacked structures. Herein, we report a rational assembly of TMDs on graphitic carbon nitride, which can be used as a cocatalyst ensemble for efficient and highly selective CO2 photoreduction. As an example, ReSe2 ultrathin nanosheet-graphitic carbon nitride (ReSe2/C3N4) composites are synthesized, in which efficient electron transfer is demonstrated by quasi in situ X-ray photoelectron spectroscopy and femtosecond transient absorption spectroscopy. In situ diffuse reflectance infrared Fourier-transform spectroscopy and theoretical calculations reveal that ReSe2/C3N4 composites could decrease the energy barrier of COOH* formation, thereby promoting the generation of COOH*. Consequently, optimized ReSe2/C3N4 composites exhibit a CO selectivity of 98% with a CO evolution rate of 19.6 mu mol<middle dot>g(-1)<middle dot>h(-1). This study demonstrates the rational design of TMD-based cocatalysts on 2D platforms for efficient and highly selective CO2 photoreduction.
引用
收藏
页码:7506 / 7513
页数:8
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