Exsolution-Dissolution of Supported Metals on High-Entropy Co3MnNiCuZnOx: Toward Sintering-Resistant Catalysis

Jiahua Zhao; Jiafeng Bao; Shize Yang; Qiang Niu; Rongyong Xie; Qiuyue Zhang; Mingshu Chen; Pengfei Zhang; Sheng Dai

doi:10.1021/acscatal.1c03228

Exsolution-Dissolution of Supported Metals on High-Entropy Co₃MnNiCuZnOx: Toward Sintering-Resistant Catalysis

Jiahua Zhao, Jiafeng Bao, Shize Yang, Qiang Niu, Rongyong Xie, Qiuyue Zhang, Mingshu Chen, Pengfei Zhang, Sheng Dai

Chemical Sciences Division

Research output: Contribution to journal › Article › peer-review

72 Scopus citations

Abstract

Herein, in situ generation of CuCoNi nanoalloys over a high-entropy oxide Co₃MnNiCuZnOxmatrix has been employed to generate a sintering-resistant metal-oxide interface for the CO₂hydrogenation reaction. The high-entropy Co₃MnNiCuZnOxcatalyst with a single reverse spinel structure was synthesized by a mechanochemical redox-based process and thermal treatment just at 600 °C. Interestingly, the entropy-driven force allows the exsolution and dissolution of CuCoNi alloys under reductive and oxidative recyles, which results in the dynamics confinement of the supported metals. With high temperature (500 °C) CO₂hydrogenation as a model reaction, the restriction of CuCoNi nanoparticles over a high-entropy Co₃MnNiCuZnOxmatrix guaranteed long-term thermal stability (>100 h). In comparison, binary CoMnOxas a control catalyst deactivated in 10 h. This high-entropy stabilization may inspire a number of sintering-resistant catalysts in the near future.

Original language	English
Pages (from-to)	12247-12257
Number of pages	11
Journal	ACS Catalysis
Volume	11
Issue number	19
DOIs	https://doi.org/10.1021/acscatal.1c03228
State	Published - Oct 1 2021

Funding

This work was supported by the National Key R&D Program of China (2020YFB0606401). S.D. (discussion on interpretation of experimental results) was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program.

Keywords

RWGS reaction
high stability
high-entropy oxides
mechanochemical redox synthesis
transition metal

Access to Document

10.1021/acscatal.1c03228

Cite this

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title = "Exsolution-Dissolution of Supported Metals on High-Entropy Co3MnNiCuZnOx: Toward Sintering-Resistant Catalysis",

abstract = "Herein, in situ generation of CuCoNi nanoalloys over a high-entropy oxide Co3MnNiCuZnOxmatrix has been employed to generate a sintering-resistant metal-oxide interface for the CO2hydrogenation reaction. The high-entropy Co3MnNiCuZnOxcatalyst with a single reverse spinel structure was synthesized by a mechanochemical redox-based process and thermal treatment just at 600 °C. Interestingly, the entropy-driven force allows the exsolution and dissolution of CuCoNi alloys under reductive and oxidative recyles, which results in the dynamics confinement of the supported metals. With high temperature (500 °C) CO2hydrogenation as a model reaction, the restriction of CuCoNi nanoparticles over a high-entropy Co3MnNiCuZnOxmatrix guaranteed long-term thermal stability (>100 h). In comparison, binary CoMnOxas a control catalyst deactivated in 10 h. This high-entropy stabilization may inspire a number of sintering-resistant catalysts in the near future.",

keywords = "RWGS reaction, high stability, high-entropy oxides, mechanochemical redox synthesis, transition metal",

author = "Jiahua Zhao and Jiafeng Bao and Shize Yang and Qiang Niu and Rongyong Xie and Qiuyue Zhang and Mingshu Chen and Pengfei Zhang and Sheng Dai",

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doi = "10.1021/acscatal.1c03228",

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T1 - Exsolution-Dissolution of Supported Metals on High-Entropy Co3MnNiCuZnOx

T2 - Toward Sintering-Resistant Catalysis

AU - Zhao, Jiahua

AU - Bao, Jiafeng

AU - Yang, Shize

AU - Niu, Qiang

AU - Xie, Rongyong

AU - Zhang, Qiuyue

AU - Chen, Mingshu

AU - Zhang, Pengfei

AU - Dai, Sheng

PY - 2021/10/1

Y1 - 2021/10/1

N2 - Herein, in situ generation of CuCoNi nanoalloys over a high-entropy oxide Co3MnNiCuZnOxmatrix has been employed to generate a sintering-resistant metal-oxide interface for the CO2hydrogenation reaction. The high-entropy Co3MnNiCuZnOxcatalyst with a single reverse spinel structure was synthesized by a mechanochemical redox-based process and thermal treatment just at 600 °C. Interestingly, the entropy-driven force allows the exsolution and dissolution of CuCoNi alloys under reductive and oxidative recyles, which results in the dynamics confinement of the supported metals. With high temperature (500 °C) CO2hydrogenation as a model reaction, the restriction of CuCoNi nanoparticles over a high-entropy Co3MnNiCuZnOxmatrix guaranteed long-term thermal stability (>100 h). In comparison, binary CoMnOxas a control catalyst deactivated in 10 h. This high-entropy stabilization may inspire a number of sintering-resistant catalysts in the near future.

AB - Herein, in situ generation of CuCoNi nanoalloys over a high-entropy oxide Co3MnNiCuZnOxmatrix has been employed to generate a sintering-resistant metal-oxide interface for the CO2hydrogenation reaction. The high-entropy Co3MnNiCuZnOxcatalyst with a single reverse spinel structure was synthesized by a mechanochemical redox-based process and thermal treatment just at 600 °C. Interestingly, the entropy-driven force allows the exsolution and dissolution of CuCoNi alloys under reductive and oxidative recyles, which results in the dynamics confinement of the supported metals. With high temperature (500 °C) CO2hydrogenation as a model reaction, the restriction of CuCoNi nanoparticles over a high-entropy Co3MnNiCuZnOxmatrix guaranteed long-term thermal stability (>100 h). In comparison, binary CoMnOxas a control catalyst deactivated in 10 h. This high-entropy stabilization may inspire a number of sintering-resistant catalysts in the near future.

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