Surface and Defect Engineering Coupling of Halide Double Perovskite Cs_2NaBiCl_6 for Efficient CO_2 Photoreduction

Jiacheng Pi; Xiaofang Jia; Zhangwen LongShuai YangHao WuDacheng ZhouQi WangHuibin ZhengYong YangJunying ZhangJianbei Qiu

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Surface and Defect Engineering Coupling of Halide Double Perovskite Cs_2NaBiCl_6 for Efficient CO_2 Photoreduction

机译：Surface and Defect Engineering Coupling of Halide Double Perovskite Cs_2NaBiCl_6 for Efficient CO_2 Photoreduction

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Non-toxic halide double perovskite materials have many advantages of leadhalide perovskite. Whereas, they usually exhibit poor stability and very lowintrinsic photocatalytic CO_2 reduction activity due to the insufficient separationof photogenerated charges and the lack of active sites. In this work, stablechlorine-deficient 3D hierarchical Cs_2NaBiCl_6 porous microspheres assembledby highly crystalline nanoflakes were prepared by a simple grinding method.An unprecedented CO yield of 30.22 μmol g~(?1) h~(?1) was achieved in the gas-solidphotocatalytic reduction of CO_2 without sacrificial agents, which is the highestvalue among lead-free halide perovskite photocatalysts. Experimental resultsand density-functional theory calculations show that the chlorine vacancyplays the triple role of suppressing photogenerated electron-holes recombination,enhancing CO_2 adsorption, and significantly reducing the free energybarrier for the key intermediate COOH* generation. In comparison with thepristine Cs_2NaBiCl_6, coupling of surface and defect engineering of the hierarchicalsample brings 12.34 times enhancement of CO_2 photoreduction activity.This work proposes a simple method to synthesize a chlorine-vacancy rich 3Dhierarchical lead-free halide perovskite and offers a new design idea to substantiallyenhance the photocatalytic activity, opening a door for the prospectivecontribution of these materials to carbon neutralization.

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来源
《Advanced energy materials》 |2022年第43期|2202074.1-2202074.13|共13页
作者
Jiacheng Pi; Xiaofang Jia; Zhangwen LongShuai YangHao WuDacheng ZhouQi WangHuibin ZhengYong YangJunying ZhangJianbei Qiu;
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Anyang Institute of TechnologyAnyang 455000, China;

Faculty of Material Science and EngineeringKunming University of Science and TechnologyKunming 650093, China, Key Lab. of Advanced Materials of Yunnan ProvinceKunming 650093, China;

Faculty of Material Science and EngineeringKunming University of Science and TechnologyKunming 650093, ChinaSchool of PhysicsBeihang UniversityBeijing 100191, China;

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正文语种英语
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chlorine vacancies; lead-free halide double perovskites; photocatalytic CO_2 reduction; three-dimensional hierarchical structures;

Surface and Defect Engineering Coupling of Halide Double Perovskite Cs_2NaBiCl_6 for Efficient CO_2 Photoreduction

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