Stabilization and manipulation of highly concentrated copper single atoms by high entropy oxides

Meijia Li; Kevin Michael Siniard; Darren M. Driscoll; Alexander S. Ivanov; Xinhui Lu; Hao Chen; Junyan Zhang; Felipe Polo-Garzon; Zhenzhen Yang; Sheng Dai

doi:10.1016/j.jcat.2024.115645

Stabilization and manipulation of highly concentrated copper single atoms by high entropy oxides

Meijia Li
, Kevin Michael Siniard
, Darren M. Driscoll
, Alexander S. Ivanov
, Xinhui Lu
, Hao Chen
, Junyan Zhang
, Felipe Polo-Garzon
, Zhenzhen Yang
, Sheng Dai

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

2 Scopus citations

Abstract

Facile and controllable methodologies capable of providing single atom catalysts (SACs) with high-density active metal sites and sintering-resistance under harsh conditions are highly desired and grand challenges in heterogeneous catalysis. Herein, the entropy effect was leveraged to stabilize and manipulate the electronic properties of copper SACs. The as-developed ultrasonication-driven approach could integrate highly concentrated Cu SAs within the lattice of fluorite-structured high entropy oxide (HEFO) under ambient conditions (CuO-HEFO). The dual benefits from the high entropy effect of the support and the in-situ lattice engineering led to the generation of abundant Cu¹⁺ species and oxygen defects, together with ultra-high stability and sintering-resistance under extremely harsh conditions. This was confirmed by deploying non-high entropy support (CuO-CeO₂) or Cu sites located on the surface of HEFO (CuO@HEFO). The catalytic activity of CuO-HEFO surpassed that of CuO-CeO₂ and CuO@HEFO in CO oxidation together with well-maintained long-term stability and resistance to gas impurities.

Original language	English
Article number	115645
Journal	Journal of Catalysis
Volume	437
DOIs	https://doi.org/10.1016/j.jcat.2024.115645
State	Published - Sep 2024

Funding

The research was supported financially by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program. NIST beamline 6-BM and the 28-ID-1 beamline of the National Synchrotron Light Source II was used, which is a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704.

Keywords

Cerium oxide
Copper oxide
High entropy oxides
Oxidation reaction
Ultrasonication

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10.1016/j.jcat.2024.115645

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title = "Stabilization and manipulation of highly concentrated copper single atoms by high entropy oxides",

abstract = "Facile and controllable methodologies capable of providing single atom catalysts (SACs) with high-density active metal sites and sintering-resistance under harsh conditions are highly desired and grand challenges in heterogeneous catalysis. Herein, the entropy effect was leveraged to stabilize and manipulate the electronic properties of copper SACs. The as-developed ultrasonication-driven approach could integrate highly concentrated Cu SAs within the lattice of fluorite-structured high entropy oxide (HEFO) under ambient conditions (CuO-HEFO). The dual benefits from the high entropy effect of the support and the in-situ lattice engineering led to the generation of abundant Cu1+ species and oxygen defects, together with ultra-high stability and sintering-resistance under extremely harsh conditions. This was confirmed by deploying non-high entropy support (CuO-CeO2) or Cu sites located on the surface of HEFO (CuO@HEFO). The catalytic activity of CuO-HEFO surpassed that of CuO-CeO2 and CuO@HEFO in CO oxidation together with well-maintained long-term stability and resistance to gas impurities.",

keywords = "Cerium oxide, Copper oxide, High entropy oxides, Oxidation reaction, Ultrasonication",

author = "Meijia Li and \{Michael Siniard\}, Kevin and Driscoll, \{Darren M.\} and Ivanov, \{Alexander S.\} and Xinhui Lu and Hao Chen and Junyan Zhang and Felipe Polo-Garzon and Zhenzhen Yang and Sheng Dai",

note = "Publisher Copyright: {\textcopyright} 2024",

year = "2024",

month = sep,

doi = "10.1016/j.jcat.2024.115645",

language = "English",

volume = "437",

journal = "Journal of Catalysis",

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T1 - Stabilization and manipulation of highly concentrated copper single atoms by high entropy oxides

AU - Li, Meijia

AU - Michael Siniard, Kevin

AU - Driscoll, Darren M.

AU - Ivanov, Alexander S.

AU - Lu, Xinhui

AU - Chen, Hao

AU - Zhang, Junyan

AU - Polo-Garzon, Felipe

AU - Yang, Zhenzhen

AU - Dai, Sheng

PY - 2024/9

Y1 - 2024/9

N2 - Facile and controllable methodologies capable of providing single atom catalysts (SACs) with high-density active metal sites and sintering-resistance under harsh conditions are highly desired and grand challenges in heterogeneous catalysis. Herein, the entropy effect was leveraged to stabilize and manipulate the electronic properties of copper SACs. The as-developed ultrasonication-driven approach could integrate highly concentrated Cu SAs within the lattice of fluorite-structured high entropy oxide (HEFO) under ambient conditions (CuO-HEFO). The dual benefits from the high entropy effect of the support and the in-situ lattice engineering led to the generation of abundant Cu1+ species and oxygen defects, together with ultra-high stability and sintering-resistance under extremely harsh conditions. This was confirmed by deploying non-high entropy support (CuO-CeO2) or Cu sites located on the surface of HEFO (CuO@HEFO). The catalytic activity of CuO-HEFO surpassed that of CuO-CeO2 and CuO@HEFO in CO oxidation together with well-maintained long-term stability and resistance to gas impurities.

AB - Facile and controllable methodologies capable of providing single atom catalysts (SACs) with high-density active metal sites and sintering-resistance under harsh conditions are highly desired and grand challenges in heterogeneous catalysis. Herein, the entropy effect was leveraged to stabilize and manipulate the electronic properties of copper SACs. The as-developed ultrasonication-driven approach could integrate highly concentrated Cu SAs within the lattice of fluorite-structured high entropy oxide (HEFO) under ambient conditions (CuO-HEFO). The dual benefits from the high entropy effect of the support and the in-situ lattice engineering led to the generation of abundant Cu1+ species and oxygen defects, together with ultra-high stability and sintering-resistance under extremely harsh conditions. This was confirmed by deploying non-high entropy support (CuO-CeO2) or Cu sites located on the surface of HEFO (CuO@HEFO). The catalytic activity of CuO-HEFO surpassed that of CuO-CeO2 and CuO@HEFO in CO oxidation together with well-maintained long-term stability and resistance to gas impurities.

KW - Cerium oxide

KW - Copper oxide

KW - High entropy oxides

KW - Oxidation reaction

KW - Ultrasonication

UR - https://www.scopus.com/pages/publications/85199278328

U2 - 10.1016/j.jcat.2024.115645

DO - 10.1016/j.jcat.2024.115645

M3 - Article

AN - SCOPUS:85199278328

SN - 0021-9517

VL - 437

JO - Journal of Catalysis

JF - Journal of Catalysis

M1 - 115645

ER -

Stabilization and manipulation of highly concentrated copper single atoms by high entropy oxides

Abstract

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Keywords

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