Tuning the Selectivity of Catalytic Carbon Dioxide Hydrogenation over Iridium/Cerium Oxide Catalysts with a Strong Metal–Support Interaction

  • Siwei Li
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
  • Yao Xu
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
  • Yifu Chen
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
  • Weizhen Li
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
  • Lili Lin
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
  • Mengzhu Li
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
  • Yuchen Deng
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
  • Xiaoping Wang
    Syncat@Beijing Synfuels China Technology Co., Ltd. Beijing 101407 China
  • Binghui Ge
    Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 P.R. China
  • Ce Yang
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
  • Siyu Yao
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
  • Jinglin Xie
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
  • Yongwang Li
    Syncat@Beijing Synfuels China Technology Co., Ltd. Beijing 101407 China
  • Xi Liu
    Syncat@Beijing Synfuels China Technology Co., Ltd. Beijing 101407 China
  • Ding Ma
    College of Chemistry and Molecular Engineering Peking University Beijing 100871 China

抄録

<jats:title>Abstract</jats:title><jats:p>A one‐step ligand‐free method based on an adsorption–precipitation process was developed to fabricate iridium/cerium oxide (Ir/CeO<jats:sub>2</jats:sub>) nanocatalysts. Ir species demonstrated a strong metal–support interaction (SMSI) with the CeO<jats:sub>2</jats:sub> substrate. The chemical state of Ir could be finely tuned by altering the loading of the metal. In the carbon dioxide (CO<jats:sub>2</jats:sub>) hydrogenation reaction it was shown that the chemical state of Ir species—induced by a SMSI—has a major impact on the reaction selectivity. Direct evidence is provided indicating that a single‐site catalyst is not a prerequisite for inhibition of methanation and sole production of carbon monoxide (CO) in CO<jats:sub>2</jats:sub> hydrogenation. Instead, modulation of the chemical state of metal species by a strong metal–support interaction is more important for regulation of the observed selectivity (metallic Ir particles select for methane while partially oxidized Ir species select for CO production). The study provides insight into heterogeneous catalysts at nano, sub‐nano, and atomic scales.</jats:p>

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