专栏名称: 科学温故
知幽渺之理而收显著之效:从实验到理论,探索催化反应隐藏的信息与机理,打开催化过程“黑匣子”
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【解读】Angew. Chem.:RWGS过程中Mo氧化物原位动态渗碳实现空前CO生成率

科学温故  · 公众号  ·  · 2024-08-19 10:09

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1 摘要 In-situ construction of active structure under reaction conditions is highly desired but still remains challenging in many important catalytic processes. Herein, we observe structural evolution of molybdenum oxide (MoO x ) into highly active molybdenum carbide (MoC x ) during reverse water-gas shift (RWGS) reaction. Surface oxygen atoms in various Mo-based catalysts are removed in H 2 -containing atmospheres and then carbon atoms can accumulate on surface to form MoC x phase with the RWGS reaction going on, both of which are enhanced by the presence of intercalated H species or Pt-dopants in MoO x . The structural evolution from MoO x to MoC x is accompanied by enhanced CO 2 conversion, which is positively correlated with the surface C/Mo ratio but negatively with the surface O/Mo ratio. As a result, an unprecedented CO formation rate of 7544.6 mmol·g catal -1 ·h -1 at 600 °C has been achieved over in-situ carbonized H-intercalated MoO 3 catalyst, which is even hig ………………………………

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