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<p>The reverse water-gas shift (RWGS) reaction holds great promise for CO<sub>2</sub> reduction and achieving carbon neutrality, particularly when driven by renewable and abundant solar energy. Among various investigated catalysts, Co-based materials have demonstrated high catalytic activity for CO<sub>2</sub> hydrogenation, and the easily accessible Co or CoO<sub><i>x</i></sub> catalysts tend to produce CH<sub>4</sub> (via the Sabatier reaction) rather than CO (via the RWGS reaction) at relatively low temperatures (⩽ 400 °C). Besides the composition tuning to construct specific active sites (such as forming Co<sub>2</sub>C), the manipulation of the chemical microenvironment is also considered a highly effective strategy for regulating product selectivity, as have been broadly demonstrated in electrochemistry and zeolite research fields. Herein, alkaline Sr sites aiming at enhancing the CO<sub>2</sub> coverage at catalyst surface are placed in close proximity to the catalytically active Co centers, thus offering balanced supply of reactants within the reactive zone. The as-designed SrCoO<sub><i>x</i></sub> catalyst through <i>in situ</i> decomposition of the SrCoO<sub>2.52</sub> precursor exhibits a significant enhancement in CO selectivity (from 42% to 91%) and exceptional stability throughout a 300-h continuous reaction. This work broadens the application scope of chemical microenvironment manipulation strategies and introduces a novel avenue for future photothermal catalyst development.</p>

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Chemical microenvironment manipulation promotes selective photothermal CO2 hydrogenation to CO over Co-based catalysts

  • 期刊论文

  • 发表日期：

    2025年5月8日

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  • Jun Wang,
  • Wangxi Liu,
  • Huiting Huang,
  • Yingfei Hu,
  • Minyue Zhao,
  • Zhexing Lin,
  • Zhengwei Yang,
  • Jianming Liu,
  • Jianyong Feng,
  • Tao Yu,
  • Zhigang Zou,
  • Zhaosheng Li

摘要

The reverse water-gas shift (RWGS) reaction holds great promise for CO2 reduction and achieving carbon neutrality, particularly when driven by renewable and abundant solar energy. Among various investigated catalysts, Co-based materials have demonstrated high catalytic activity for CO2 hydrogenation, and the easily accessible Co or CoOx catalysts tend to produce CH4 (via the Sabatier reaction) rather than CO (via the RWGS reaction) at relatively low temperatures (⩽ 400 °C). Besides the composition tuning to construct specific active sites (such as forming Co2C), the manipulation of the chemical microenvironment is also considered a highly effective strategy for regulating product selectivity, as have been broadly demonstrated in electrochemistry and zeolite research fields. Herein, alkaline Sr sites aiming at enhancing the CO2 coverage at catalyst surface are placed in close proximity to the catalytically active Co centers, thus offering balanced supply of reactants within the reactive zone. The as-designed SrCoOx catalyst through in situ decomposition of the SrCoO2.52 precursor exhibits a significant enhancement in CO selectivity (from 42% to 91%) and exceptional stability throughout a 300-h continuous reaction. This work broadens the application scope of chemical microenvironment manipulation strategies and introduces a novel avenue for future photothermal catalyst development.