Self-regeneration of supported transition metals by a high entropy-driven principle

Shengtai Hou, Xuefeng Ma, Yuan Shu, Jiafeng Bao, Qiuyue Zhang, Mingshu Chen, Pengfei Zhang () and Sheng Dai
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Shengtai Hou: Shanghai Jiao Tong University
Xuefeng Ma: Shanghai Jiao Tong University
Yuan Shu: Shanghai Jiao Tong University
Jiafeng Bao: Shanghai Jiao Tong University
Qiuyue Zhang: Xiamen University
Mingshu Chen: Xiamen University
Pengfei Zhang: Shanghai Jiao Tong University
Sheng Dai: Chemical Sciences Division, Oak Ridge National Laboratory

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract The sintering of Supported Transition Metal Catalysts (STMCs) is a core issue during high temperature catalysis. Perovskite oxides as host matrix for STMCs are proven to be sintering-resistance, leading to a family of self-regenerative materials. However, none other design principles for self-regenerative catalysts were put forward since 2002, which cannot satisfy diverse catalytic processes. Herein, inspired by the principle of high entropy-stabilized structure, a concept whether entropy driving force could promote the self-regeneration process is proposed. To verify it, a high entropy cubic Zr0.5(NiFeCuMnCo)0.5Ox is constructed as a host model, and interestingly in situ reversible exsolution-dissolution of supported metallic species are observed in multi redox cycles. Notably, in situ exsolved transition metals from high entropy Zr0.5(NiFeCuMnCo)0.5Ox support, whose entropic contribution (TΔSconfig = T⋆12.7 J mol−1 K−1) is predominant in ∆G, affording ultrahigh thermal stability in long-term CO2 hydrogenation (400 °C, >500 h). Current theory may inspire more STWCs with excellent sintering-resistance performance.

Date: 2021
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DOI: 10.1038/s41467-021-26160-8

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