Directed Electron Delivery from a Pb-Free Halide Perovskite to a Co(II) Molecular Catalyst Boosts CO2 Photoreduction Coupled with Water Oxidation

被引：47

作者：

Zhao, Jin-Shuang ^{[1
]}

Mu, Yan-Fei ^{[1
]}

Wu, Li-Yuan ^{[1
]}

Luo, Zhi-Mei ^{[2
]}

Velasco, Lucia ^{[3
]}

Sauvan, Maxime ^{[3
]}

Moonshiram, Dooshaye ^{[3
]}

Wang, Jia-Wei ^{[2
]}

Zhang, Min ^{[1
]}

Lu, Tong-Bu ^{[1
]}

机构：

[1] Tianjin Univ Technol, Sch Mat Sci & Engn, Inst New Energy Mat & Low Carbon Technol, MOE Int Joint Lab Mat Microstruct, Tianjin 300384, Peoples R China

[2] Sun Yat Sen Univ, Sch Chem Engn & Technol, Zhuhai 519082, Peoples R China

[3] Inst Ciencia Mat Madrid ICMM CSIC, Sor Juana Ines Cruz 3, Madrid 28049, Spain

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2024年 / 63卷 / 21期

基金：

国家重点研发计划;

关键词：

lead-free halide perovskite; directed electron transfer; CO2; reduction; molecular hybrid photocatalyst; cobalt phthalocyanine; K-EDGE; METAL; REDUCTION; NANOCRYSTALS; CSPBBR3;

D O I：

10.1002/anie.202401344

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The development of high-performance photocatalytic systems for CO2 reduction is appealing to address energy and environmental issues, while it is challenging to avoid using toxic metals and organic sacrificial reagents. We here immobilize a family of cobalt phthalocyanine catalysts on Pb-free halide perovskite Cs2AgBiBr6 nanosheets with delicate control on the anchors of the cobalt catalysts. Among them, the molecular hybrid photocatalyst assembled by carboxyl anchors achieves the optimal performance with an electron consumption rate of 300 +/- 13 mu molg(-1)h(-1) for visible-light-driven CO2-to-CO conversion coupled with water oxidation to O-2, over 8times of the unmodified Cs2AgBiBr6 (36 +/- 8 mu molg(-1)h(-1)), also far surpassing the documented systems (<150 mu molg(-1)h(-1)). Besides the improved intrinsic activity, electrochemical, computational, ex-/in situ X-ray photoelectron and X-ray absorption spectroscopic results indicate that the electrons photogenerated at the Bi atoms of Cs2AgBiBr6 can be directionally transferred to the cobalt catalyst via the carboxyl anchors which strongly bind to the Bi atoms, substantially facilitating the interfacial electron transfer kinetics and thereby the photocatalysis.

引用

页数：8

共 42 条

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