期刊
ADVANCED ENERGY MATERIALS
卷 12, 期 43, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202202074
关键词
chlorine vacancies; lead-free halide double perovskites; photocatalytic CO; (2) reduction; three-dimensional hierarchical structures
类别
资金
- National Natural Science Foundation of China-Yunnan Joint Fund [U1902222, U2102215]
- National Natural Science Foundation of China [12064021, 51862020, 51972010]
- Yunnan Major Scientific and Technological Projects [202202AG050016]
- Natural Science Foundation of Yunnan Province [202001AT070037, 202101AT070104, 202101AT070097]
- High-Performance Computing platform of Beihang University (BHHPC)
In this study, stable chlorine-deficient Cs2NaBiCl6 porous microspheres were synthesized and exhibited high photocatalytic activity for CO2 reduction. The enhanced activity was achieved by suppressing electron-hole recombination, enhancing CO2 adsorption, and reducing the energy barrier for COOH* generation.
Non-toxic halide double perovskite materials have many advantages of lead halide perovskite. Whereas, they usually exhibit poor stability and very low intrinsic photocatalytic CO2 reduction activity due to the insufficient separation of photogenerated charges and the lack of active sites. In this work, stable chlorine-deficient 3D hierarchical Cs2NaBiCl6 porous microspheres assembled by highly crystalline nanoflakes were prepared by a simple grinding method. An unprecedented CO yield of 30.22 mu mol g(-1) h(-1) was achieved in the gas-solid photocatalytic reduction of CO2 without sacrificial agents, which is the highest value among lead-free halide perovskite photocatalysts. Experimental results and density-functional theory calculations show that the chlorine vacancy plays the triple role of suppressing photogenerated electron-holes recombination, enhancing CO2 adsorption, and significantly reducing the free energy barrier for the key intermediate COOH* generation. In comparison with the pristine Cs2NaBiCl6, coupling of surface and defect engineering of the hierarchical sample brings 12.34 times enhancement of CO2 photoreduction activity. This work proposes a simple method to synthesize a chlorine-vacancy rich 3D hierarchical lead-free halide perovskite and offers a new design idea to substantially enhance the photocatalytic activity, opening a door for the prospective contribution of these materials to carbon neutralization.
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