Mechanism of Photocatalytic CO2 Reduction by Bismuth-Based Perovskite Nanocrystals at the Gas-Solid Interface

被引:226
作者
Bhosale, Sumit S. [1 ,2 ]
Kharade, Aparna K. [3 ]
Jokar, Efat [1 ,2 ,4 ]
Fathi, Amir [1 ,2 ]
Chang, Sue-min [3 ]
Diau, Eric Wei-Guang [1 ,2 ,4 ]
机构
[1] Natl Chiao Tung Univ, Dept Appl Chem, 1001 Ta Hsueh Rd, Hsinchu 30010, Taiwan
[2] Natl Chiao Tung Univ, Inst Mol Sci, 1001 Ta Hsueh Rd, Hsinchu 30010, Taiwan
[3] Natl Chiao Tung Univ, Inst Environm Engn, Hsinchu 30010, Taiwan
[4] Natl Chiao Tung Univ, Ctr Emergent Funct Matter Sci, 1001 Ta Hsueh Rd, Hsinchu 30010, Taiwan
关键词
LEAD-FREE; SURFACE; TIO2; PERFORMANCE; CRYSTAL; ANATASE; EMISSION; SITES; RB; CS;
D O I
10.1021/jacs.9b11089
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We report here a series of nontoxic and stable bismuth-based perovskite nanocrystals (PeNCs) with applications for photocatalytic reduction of carbon dioxide to methane and carbon monoxide. Three bismuth-based PeNCs of general chemical formulas A(3)Bi(2)I(9), in which cation A(+) = Rb+ or Cs+ or CH3NH3+ (MK), were synthesized with a novel ultrasonication top-down method. PeNC of Cs3Bi2I9 had the best photocatalytic activity for the reduction of CO2 at the gas solid interface with formation yields 14.9 mu mol g(-1) of methane and 77.6 mu mol g(-1) of CO, representing a much more effective catalyst than TiO2 (P25) under the same experimental conditions. The products of the photocatalytic reactions were analyzed using a gas chromatograph coupled with a mass spectrometer. According to electron paramagnetic resonance and diffuse-reflectance infrared spectra, we propose a reaction mechanism for photoreduction of CO2 via Bi-based PeNC photocatalysts to form CO, CH4, and other possible side products.
引用
收藏
页码:20434 / 20442
页数:9
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