Enhancing coke resistance of Ni-based spinel-type oxides by tuning the configurational entropy

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-10-24 DOI:10.1016/j.jcat.2024.115819

Shuangshuang Zhang , Ying Gao , Qiang Niu , Pengfei Zhang

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Abstract

The reforming of CH₄ and CO₂ into syngas is a highly relevant technology for energy conservation and reducing greenhouse gas emissions, attracting widespread attention in the industry. Inspired by this, this work proposes a general criterion for coke-resistant nickel-based catalysts. By leveraging the high-entropy effect and the lattice distortion of the structure, a high-entropy (NiCaMgZnCo)Al₁₀O_x catalyst was synthesized. The high-entropy oxide exhibited good activity and stability during the DRM reaction over 100 h at 800°C and 650°C, producing only a minimal amount of easily removable carbon deposition. O₂-TPO, CO₂-TPD, CH₄-TPSR, CO₂-TPSR, DFT and in situ DRIFT were employed to investigate the mechanism of carbon deposition elimination on the surface of the high-entropy catalyst. Then, a high-entropy strategy for designing coke-resistant catalysts was proposed. This strategy may soon inspire the development of catalysts with enhanced stability and anti-coke deposition properties for various catalytic applications.

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通过调整构型熵增强镍基尖晶石型氧化物的抗焦性

将 CH4 和 CO2 转化为合成气是一项与节能和减少温室气体排放高度相关的技术，受到业界的广泛关注。受此启发，本研究提出了耐焦化镍基催化剂的一般标准。利用高熵效应和晶格畸变结构，合成了一种高熵 (NiCaMgZnCo)Al10Ox 催化剂。这种高熵氧化物在 800°C 和 650°C 温度下进行 DRM 反应 100 小时期间表现出良好的活性和稳定性，仅产生极少量的易去除碳沉积。采用 O2-TPO、CO2-TPD、CH4-TPSR、CO2-TPSR、DFT 和原位 DRIFT 等方法研究了高熵催化剂表面碳沉积消除的机理。然后，提出了一种设计抗焦催化剂的高熵策略。该策略可能很快会激励人们开发出具有更高的稳定性和抗焦炭沉积性能的催化剂，用于各种催化应用。

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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.