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

作者：Zhenhua Li, Jinjia Liu, Run Shi, Geoffrey I N Waterhouse, X. Wen, Tierui Zhang · 发表于：Advanced Energy Materials · 年份：2021 · DOI：10.1002/aenm.202002783 · 被引用次数：115 · 研究领域：Materials Science

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.