4.7 Article

Embedding Cs2AgBiBr6 QDs into Ce-UiO-66-H to in situ construct a novel bifunctional material for capturing and photocatalytic reduction of CO2

期刊

CHEMICAL ENGINEERING JOURNAL
卷 446, 期 -, 页码 -

出版社

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.137102

关键词

Lead-free halide perovskite; Metal-organic frameworks; CO2 adsorption; CO2 photocatalytic conversion; Cs2AgBiBr6/Ce-UiO-66-H composite

资金

  1. National Natural Science Foundation of China [22062016, 21861029]
  2. Project of Inner Mongolia Natural Science Foundation [2020BS02002, 2020ZD02]
  3. Project of Research and Development of the Applied Technology for Inner Mongolia of China [2020SGG0065]
  4. Grassland Talent Innovation Team of Inner Mongolia Region
  5. Initiative Research for High level Talents of Inner Mongolia University [12000-15031937]

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Solar-energy-driven CO2 conversion into valuable chemical fuels holds great renewable potential. However, most photocatalysts' weak CO2 adsorption limits further utilization of artificial photosynthesis. In this study, stable Cs2AgBiBr6/Ce-UiO-66-H composite was produced through in situ assembling, resulting in a tight contact interface between the two components. The optimized adsorption-photocatalyst exhibited outstanding performance for reductive CO2 deoxygenation, with a higher CO generation rate compared to pure Cs2AgBiBr6 and Ce-UiO-66-H. The excellent catalytic conversion is attributed to effective solar harvest and quick separation of photo-excited carriers in the assembled architecture. Importantly, the in-situ synthesis led to improved stability and abundant oxygen vacancies, enabling the material to maintain a constant CO2 conversion rate under wet air conditions.
Solar-energy-driven CO2 conversion into valuable chemical fuels holds great renewable potential. However, most photocatalysts' weak CO2 adsorption limits more artificial photosynthesis for further utilization. Herein, we present an in situ assembling approach to produce stable Cs2AgBiBr6/Ce-UiO-66-H composite, in which a tight contact interface between the two participated components was constructed. Benefiting from the photocatalytic properties and high adsorption capacity for CO2, the optimized 20Cs(2)AgBiBr(6)/Ce-UiO-66-H adsorptionphotocatalyst exhibits outstanding performance for reductive CO2 deoxygenation with considerable CO generation rate (309.01 mu mol g(-1)h(-1)) under simulated solar light irradiation with 300 W Xe lamp, which is about 2.1 and 2.7 times than that of pure Cs2AgBiBr6 and Ce-UiO-66-H, respectively. The excellent catalytic conversion of CO2 is ascribed to the effective solar harvest and quickly photo-excited carriers' separation in such assembled architecture. Importantly, due to the in-situ synthesis, Cs2AgBiBr6 QDs are intercalated in the Ce-UiO-66-H frameworks and it could lead to improved stability and induce abundant oxygen vacancies in Cs2AgBiBr6/Ce-UiO-66-H, which can maintain unchangeable CO2 conversion rate under wet air with consecutive ten hours of the recycling test. In this work, the combining metal-organic frameworks and lead-free halide perovskite provide great potential for artificial photocatalytic CO2-to-CO conversion under a mild gas-solid reaction condition via utilizing solar energy.

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