Metal-Tannin Coordination Assembly Route to Nanostructured High-Entropy Oxide Perovskites with Abundant Defects

Dong Chen; Siyang Nie; Liang Wu; Xiao Zheng; Shengyu Du; Xiaolan Duan; Qiang Niu; Pengfei Zhang; Sheng Dai

doi:10.1021/acs.chemmater.1c03930

Metal-Tannin Coordination Assembly Route to Nanostructured High-Entropy Oxide Perovskites with Abundant Defects

Dong Chen, Siyang Nie, Liang Wu, Xiao Zheng, Shengyu Du, Xiaolan Duan, Qiang Niu, Pengfei Zhang, Sheng Dai

Chemical Sciences Division

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

23 Scopus citations

Abstract

High-entropy oxide perovskites (HEOPs), the incorporation of five or more elements into ABO₃, possess great flexibility in the composition and electron structure and thus merit untold scientific and technological potential. However, the conventional synthetic methods at high temperatures tend to obtain the bulk with a low surface area, limited exposed active sites, and result in poor catalytic activity. Herein, we report a metal-tannin coordination assembly strategy to synthesize HEOP nanoparticles (NPs) with a size of 10-30 nm and abundant oxygen vacancies. Interestingly, up to 10 immiscible metal elements could be confined into the single HEOP NPs. Meanwhile, the as-synthesized La(FeCoNiCrMn)₃ NPs exhibit better CO oxidation activity than single-metal-oxide perovskites and the conventionally solid-state prepared HEOP catalysts. Moreover, the entropy-stabilized NPs function well in moisture- or SO₂-containing reaction conditions. This work opens up new opportunities to design nanostructured high-entropy materials for heterogeneous catalysis.

Original language	English
Pages (from-to)	1746-1755
Number of pages	10
Journal	Chemistry of Materials
Volume	34
Issue number	4
DOIs	https://doi.org/10.1021/acs.chemmater.1c03930
State	Published - Feb 22 2022

Funding

This work was supported by the National Key R & D Program Plan (2020YFB0606400), the National Natural Science Foundation of China (Grant Nos. 21776174; 22178219), the Inner Mongolia Key R & D Program Plan (2021ZD0042), the Shanghai Rising-Star Program (20QA1405200), and the Shanghai Jiao Tong University Scientific and Technological Innovation Funds (No. 2019QYB06). S.D. (discussion of the results) was supported by U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division.

Funders	Funder number
Inner Mongolia Key R & D Program Plan	2021ZD0042
National Key R & D Program Plan	2020YFB0606400
Shanghai Jiao Tong University Scientific and Technological Innovation Funds	2019QYB06
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering
National Natural Science Foundation of China	21776174, 22178219
Shanghai Rising-Star Program	20QA1405200

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10.1021/acs.chemmater.1c03930

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title = "Metal-Tannin Coordination Assembly Route to Nanostructured High-Entropy Oxide Perovskites with Abundant Defects",

abstract = "High-entropy oxide perovskites (HEOPs), the incorporation of five or more elements into ABO3, possess great flexibility in the composition and electron structure and thus merit untold scientific and technological potential. However, the conventional synthetic methods at high temperatures tend to obtain the bulk with a low surface area, limited exposed active sites, and result in poor catalytic activity. Herein, we report a metal-tannin coordination assembly strategy to synthesize HEOP nanoparticles (NPs) with a size of 10-30 nm and abundant oxygen vacancies. Interestingly, up to 10 immiscible metal elements could be confined into the single HEOP NPs. Meanwhile, the as-synthesized La(FeCoNiCrMn)3 NPs exhibit better CO oxidation activity than single-metal-oxide perovskites and the conventionally solid-state prepared HEOP catalysts. Moreover, the entropy-stabilized NPs function well in moisture- or SO2-containing reaction conditions. This work opens up new opportunities to design nanostructured high-entropy materials for heterogeneous catalysis.",

author = "Dong Chen and Siyang Nie and Liang Wu and Xiao Zheng and Shengyu Du and Xiaolan Duan and Qiang Niu and Pengfei Zhang and Sheng Dai",

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T1 - Metal-Tannin Coordination Assembly Route to Nanostructured High-Entropy Oxide Perovskites with Abundant Defects

AU - Chen, Dong

AU - Nie, Siyang

AU - Wu, Liang

AU - Zheng, Xiao

AU - Du, Shengyu

AU - Duan, Xiaolan

AU - Niu, Qiang

AU - Zhang, Pengfei

AU - Dai, Sheng

PY - 2022/2/22

Y1 - 2022/2/22

N2 - High-entropy oxide perovskites (HEOPs), the incorporation of five or more elements into ABO3, possess great flexibility in the composition and electron structure and thus merit untold scientific and technological potential. However, the conventional synthetic methods at high temperatures tend to obtain the bulk with a low surface area, limited exposed active sites, and result in poor catalytic activity. Herein, we report a metal-tannin coordination assembly strategy to synthesize HEOP nanoparticles (NPs) with a size of 10-30 nm and abundant oxygen vacancies. Interestingly, up to 10 immiscible metal elements could be confined into the single HEOP NPs. Meanwhile, the as-synthesized La(FeCoNiCrMn)3 NPs exhibit better CO oxidation activity than single-metal-oxide perovskites and the conventionally solid-state prepared HEOP catalysts. Moreover, the entropy-stabilized NPs function well in moisture- or SO2-containing reaction conditions. This work opens up new opportunities to design nanostructured high-entropy materials for heterogeneous catalysis.

AB - High-entropy oxide perovskites (HEOPs), the incorporation of five or more elements into ABO3, possess great flexibility in the composition and electron structure and thus merit untold scientific and technological potential. However, the conventional synthetic methods at high temperatures tend to obtain the bulk with a low surface area, limited exposed active sites, and result in poor catalytic activity. Herein, we report a metal-tannin coordination assembly strategy to synthesize HEOP nanoparticles (NPs) with a size of 10-30 nm and abundant oxygen vacancies. Interestingly, up to 10 immiscible metal elements could be confined into the single HEOP NPs. Meanwhile, the as-synthesized La(FeCoNiCrMn)3 NPs exhibit better CO oxidation activity than single-metal-oxide perovskites and the conventionally solid-state prepared HEOP catalysts. Moreover, the entropy-stabilized NPs function well in moisture- or SO2-containing reaction conditions. This work opens up new opportunities to design nanostructured high-entropy materials for heterogeneous catalysis.

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Metal-Tannin Coordination Assembly Route to Nanostructured High-Entropy Oxide Perovskites with Abundant Defects

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