4.7 Article

Efficient Visible-Light Photoreduction of CO2 to CH4 over an Fe-Based Metal-Organic Framework (PCN-250-Fe3) in a Solid-Gas Mode

Journal

ACS APPLIED ENERGY MATERIALS
Volume 5, Issue 2, Pages 2384-2390

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsaem.1c03868

Keywords

CO2 reduction; photocatalyst; PCN-250-Fe-3; visible-light irradiation; solid-gas mode

Funding

  1. National Natural Science Foundation of China [21671119, 21971143]
  2. Distinguished Youth Foundation of Hubei Province [2020CFA092]
  3. 111 Project [DT20015]
  4. Program for Innovative Teams of Outstanding Young and Middle-aged Researchers in the Higher Education Institutions of Hubei Province [T201904]
  5. opening fund of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry [2020-13]

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Researchers have developed a low-cost and photosensitive metal-organic framework (MOF) called PCN-250-Fe-3 using a facile hydrothermal method. This MOF exhibits highly efficient CO2 photoreduction under visible-light irradiation, outperforming most other MOF photocatalysts under solid-gas reaction conditions.
Solar-driven highly efficient CO2 photoreduction by water oxidation to produce high-value-added chemical feedstocks of fuels remains extremely challenging. Over the past few decades, two types of reaction modes (solid-liquid or solid-gas) have been developed by researchers to achieve substrate-based photocatlytic CO2 reduction. In the absence of organic solvents, photosensitizers, and organic sacrificial agents, the solid-gas mode may be more suitable for photocatalytic CO2 reduction. A facile hydrothermal method was used to fabricate a low-cost and photosensitive azobenzene tetracarboxylic acid-based metal-organic framework (MOF), PCN-250-Fe-3, which offers the advantages of visible-light and CO2 adsorption and facilitates an electron-coupled proton transition. Notably, PCN-250-Fe-3 exhibited a maximum photocatalytic activity of 16.32 mu mol g(-1) with ca. 77.57% selectivity in 4 h without the use of photosensitizers or organic sacrificial agents under visible-light irradiation. This photocatalytic performance is superior to that of most nonporphyrin-based MOF photocatalysts under solid-gas reaction conditions. This study provides unique insight into enhancing the efficiency of the photoreduction of CO2 to CH4 by pure water.

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