Cuboidal molybdenum sulfur cluster as a platform to construct novel catalyst for propane dehydrogenation

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Catalysis Pub Date : 2024-11-10 DOI:10.1016/j.jcat.2024.115831

Tianci Zheng , Shaoxia Weng , Alan J. McCue , Nan Yang , Haowen Ma , Yuan Xie , Yanjun Lin , Yanan Liu , Dianqing Li

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Abstract

Growing demand of short chain olefins such as propylene for plastic production drives the development of high performing catalysts for propane dehydrogenation (PDH). Here, a confinement strategy originating from metal-sulfur clusters was employed to fabricate defective MoPtS_x phase via anchoring by coordinatively unsaturated Al sites present on alumina, followed by reduction under H₂ flow at high temperature. This catalyst with a low Pt content exhibits great ability for C–H activation with high intrinsic activity and facile propylene desorption in PDH reaction. More importantly, this catalyst shows excellent stability during long-term tests with both stable conversion and selectivity. Through combined X-ray absorption spectroscopy, electron microscopy and electron paramagnetic resonance measurements it could be affirmed that the isolated and electron-enriched Pt sites as well as their proximity to adjacent sulfur vacancies is vital for the first and second C–H bond activation, and suppressing of C–C cleavage which otherwise lead to coking.

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以立方体钼硫簇为平台构建新型丙烷脱氢催化剂

塑料生产对丙烯等短链烯烃日益增长的需求推动了丙烷脱氢 (PDH) 高效催化剂的开发。在这里，我们采用了一种源自金属硫簇的限制策略，通过氧化铝上存在的配位不饱和铝位点的锚定来制造有缺陷的 MoPtSx 相，然后在高温 H2 流动条件下进行还原。这种铂含量较低的催化剂具有很强的 C-H 活化能力，在 PDH 反应中具有很高的内在活性和丙烯脱附能力。更重要的是，该催化剂在长期试验中表现出了极佳的稳定性，转化率和选择性都很稳定。通过结合 X 射线吸收光谱、电子显微镜和电子顺磁共振测量，可以确定孤立铂位点和电子富集铂位点之间的相互作用以及它们与相邻硫空位的接近程度对于第一和第二 C-H 键的活化至关重要，同时抑制了 C-C 裂解，否则会导致结焦。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.