Journal
ACS NANO
Volume 14, Issue 10, Pages 13103-13114Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c04659
Keywords
CO2 reduction; perovskite quantum dot; photocatalysts reaction mechanism; active site; selectivity
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Funding
- National Natural Science Foundation of China [52002054, 21822601, 21777011]
- Fundamental Research Funds for the Central Universities [ZYGX2019Z021]
- 111 Project [B20030]
- Plan for National Youth Talents of the Central Committee
- China Postdoctoral Science Foundation [2020M673175]
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All-inorganic Pb-free bismuth (Bi) halogen per ovskite 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, arid the precise reaction path/mechanism promoted by the surface halogen; associatedactive sites is still poorly understood. Herein, we screen a series of nontoxic arid stable Cs3Bi2X9 = 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 mu mol 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 arid precisely unraveled based Orlin situ DRIFTS investigation. In combination with the DFT calculation, it was revealed that the surface Br sites allow for optimizing the coordination lmodes of surface bound intermediate species and reducing the reaction energy of the rate-limiting step of COON 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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