Fe‐Based Catalysts for the Direct Photohydrogenation of CO2 to Value‐Added Hydrocarbons

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Abstract
The solar‐driven conversion of CO2 into carbon‐based fuels and other valuable chemical feedstocks is actively being pursued as an approach for curbing greenhouse gas emissions. Herein, a series of novel Fe‐based catalysts with different chemical compositions are successfully fabricated through the hydrogen reduction of MgFeAl‐layered double hydroxide nanosheets at temperatures from 300 to 700 °C. The catalysts obtained are denoted herein as Fe‐x, where x is the reduction temperature in celsius. Fe‐500 offers outstanding activity for the photothermal conversion of CO2 to C2+ hydrocarbons under ultraviolet‐visible (UV‐Vis) irradiation (CO2 conversion 50.1%, C2+ selectivity 52.9%). Characterization studies using X‐ray diffraction, extended X‐ray absorption fine structure, Mössbauer spectroscopy, and high‐resolution transmission electron microscopy determine that the Fe‐500 catalyst is comprised of Fe and FeOx nanoparticles on a MgO–Al2O3 mixed metal oxide support. Density functional theory calculations establish that heterostructures consisting of partially oxidized metallic Fe nanoparticles improve the CC coupling ability of CO2 hydrogenation intermediates, thus enhancing the selectivity to C2+ products. This work introduces a novel photothermal hydrogenation strategy for converting CO2 into valuable chemicals and also opens new avenues toward the development of related solar energy utilization schemes.
Funding Information
  • National Natural Science Foundation of China (51825205, 51772305, 21871279, 21802154, 21902168)
  • Natural Science Foundation of Beijing Municipality (2191002, 2182078, 2194089)
  • Central China Normal University (2019YBZZ025, 6300‐30101202001)
  • K. C. Wong Education Foundation
  • Youth Innovation Promotion Association of the Chinese Academy of Sciences

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