ACS Catal.大化所刘岳峰、中石化石油化工研究院彭博:自组装钼-铝复合材料高效RWGS催化剂-突破超小粒径与高负载量的权衡

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摘要:摘要Molybdenum carbides have received attention for the reverse water gas shift (RWGS) reaction. Normally, MoCxbased catalysts are s

摘要Molybdenum carbides have received attention for the reverse water gas shift (RWGS) reaction. Normally, MoCxbased catalysts are synthesized via a high - temperature carbonization of 1100 K, leading to the agglomeration of the active phase. In order to minimize the atomic motion leading to single growth, insertion of heteroatoms has been attempted with the usage of components in the catalyst substrate. The current work applied the self - assembling strategy to prepare a Mo - O - Al composite instead of traditional impregnation before carburization. The dynamic structure evolution and detailed coordination environment of the active phase are investigated by in situ X - ray diffraction, quasi in situ X - ray photoelectron spectroscopy, in situ transmission electron microscopy, and temperature - programmed surface reaction techniques. Our findings reveal that Al doping enables carburization at a lower temperature (200 °C) via the topotactic pathway, yieldingα(fcc); even at a loading as high as 40 wt %, the catalyst maintains an ultrasmall particle size (1 nm). The optimized catalyst exhibits a RWGS reaction rate of 52.1μ·g-1at 400 °C, representing a 2.5 - fold enhancement over bulkβC. This work provides a possible solution for maintaining high dispersion at high metal loading for catalyst preparation, specially requiring a high temperature during either synthesis or reaction.

KEYWORDS:molybdenum carbide nanoparticles, high loading, ultrasmall size, structure evolutions, reverse water gas shift reaction

文章核心要点

碳化钼因其高的逆水煤气变换反应(RWGS)性能而受到关注。通常,MoCx基催化剂是通过1100 K的高温碳化合成的,这会导致活性相的聚集。为了最小化导致单一生长的原子运动,尝试在催化剂基底中插入异原子。

要点1.本文工作应用自组装策略制备Mo - O - Al复合物,而不是在碳化之前进行传统的浸渍。通过原位X射线衍射、准原位X射线光电子能谱、原位透射电子显微镜和温度程序化表面反应技术研究了活性相的动态结构演变和详细的配位环境。

要点2.200°Cα - MoCxfcc);即使在高达40 wt%)。优化后的催化剂在400°C时表现出52.1 μmolCO2·g-1RWGS反应速率,比体相βC高2.5倍。

要点3.这项工作为在催化剂制备中保持高金属负载下的高分散性提供了一种可能的解决方案,尤其是在合成或反应过程中需要高温的情况下。

催化剂制备及结构表征催化性能机理研究

Shuo Cao, Ying Ma, Wei Chu, Bingsen Zhang, Bo Peng,* and Yuefeng Liu*. Self - Assembling of a Mo - Al Composite toward Efficient Catalysts for RWGS Reaction: Overcoming the Trade - off between Ultrasmall Size and High Loading.ACS Catal. 2025, 15, 15559 - 15569

DOI:10.1021/acscatal.5c02942

来源:云阳好先生做实事

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