Статья

Identification of Halogen-Associated Active Sites on Bismuth-Based Perovskite Quantum Dots for Efficient and Selective CO<sub>2</sub>-to-CO Photoreduction

Jianping ShengResearch Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, ChinaYe HeResearch Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, ChinaJieyuan LiResearch Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, ChinaChaowei YuanChongqing Key Laboratory of Catalysis and New Environmental Materials, College of Environment and Resources, Chongqing Technology and Business University, Chongqing 400067, ChinaHongwei HuangNational Laboratory of Mineral Materials, School of Materials Science and Technology, China University of Geosciences, Beijing 100083, ChinaShengyao WangCollege of Science, Key Laboratory of Environment Correlative Dietology of Ministry of Education, Huazhong Agricultural University, Wuhan 430070, ChinaYanjuan SunResearch Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, ChinaZhiming WangResearch Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, ChinaFan DongResearch Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China

2020en

ABI

Аннотация

All-inorganic Pb-free bismuth (Bi) halogen perovskite quantum dots (PQDs) with distinct structural and photoelectric properties provide plenty of room for selective photoreduction of CO2. However, the efficient conversion of CO2-to-CO with high selectivity on Bi-based PQDs driven by solar light remains unachieved, and the precise reaction path/mechanism promoted by the surface halogen-associated active sites is still poorly understood. Herein, we screen a series of nontoxic and stable Cs3Bi2X9 (X = Cl, Br, I) PQDs for selective photocatalytic reduction of CO2-to-CO at the gas–solid interface. Among all the reported pure-phase PQDs, the as-synthesized Cs3Bi2Br9 PQDs exhibited the highest CO2-to-CO conversion efficiency generating 134.76 μmol g–1 of CO yield with 98.7% selectivity under AM 1.5G simulated solar illumination. The surface halogen-associated active sites and reaction intermediates were dynamically monitored and precisely unraveled based on in situ DRIFTS investigation. In combination with the DFT calculation, it was revealed that the surface Br sites allow for optimizing the coordination modes of surface-bound intermediate species and reducing the reaction energy of the rate-limiting step of COOH– intermediate formation from •CO2–. This work presents a mechanistic insight into the halogen-involved catalytic reaction mechanism in solar fuel production.

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Идентификаторы

DOI: 10.1021/acsnano.0c04659

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Цитирований: 2Использованных источников: 0

Показатели — AkademScholar