General synthesis of neighboring dual-atomic sites with a specific pre-designed distance via an interfacial-fixing strategy

Abstract A potential non-precious metal catalyst for oxygen reduction reaction should contain metal-N4 moieties. However, most of the current strategies to regulate the distances between neighboring metal sites are not pre-designed but depend on the probability by tuning the metal loading or the sup...

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Main Authors: Yan Yan, Rui Yu, Mingkai Liu, Zehua Qu, Jifeng Yang, Siyuan He, Hongliang Li, Jie Zeng
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-55630-y
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author Yan Yan
Rui Yu
Mingkai Liu
Zehua Qu
Jifeng Yang
Siyuan He
Hongliang Li
Jie Zeng
author_facet Yan Yan
Rui Yu
Mingkai Liu
Zehua Qu
Jifeng Yang
Siyuan He
Hongliang Li
Jie Zeng
author_sort Yan Yan
collection DOAJ
description Abstract A potential non-precious metal catalyst for oxygen reduction reaction should contain metal-N4 moieties. However, most of the current strategies to regulate the distances between neighboring metal sites are not pre-designed but depend on the probability by tuning the metal loading or the support. Herein, we report a general method for the synthesis of neighboring metal-Nx moieties (metal = Fe, Cu, Co, Ni, Zn, and Mn) via an interfacial-fixing strategy. Specifically, polydopamine is used to coat nanotemplates made of metal oxides, followed by pyrolysis to form a metal-oxide skeleton coated by rich nitrogen-doped carbon shells. After chemically etching the skeleton, only interfacial metal atoms strongly bonded with the support via nitrogen atoms are retained. The high purity (>95%) of dual Fe sites was confirmed by both the direct visualization of local regions and the indirect evidence of the averaged information. When these neighboring metal-Nx moieties are applied for oxygen reduction reaction, Fe-Nx moieties exhibit the superior activity, even outperforming commercial Pt/C in the aspects of the half-wave potential, methanol tolerance, carbon monoxide tolerance, and robustness.
format Article
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institution Kabale University
issn 2041-1723
language English
publishDate 2025-01-01
publisher Nature Portfolio
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series Nature Communications
spelling doaj-art-3c6bba58889144f3bb67f30922b66ca52025-01-05T12:38:42ZengNature PortfolioNature Communications2041-17232025-01-0116111310.1038/s41467-024-55630-yGeneral synthesis of neighboring dual-atomic sites with a specific pre-designed distance via an interfacial-fixing strategyYan Yan0Rui Yu1Mingkai Liu2Zehua Qu3Jifeng Yang4Siyuan He5Hongliang Li6Jie Zeng7Anhui University of TechnologyAnhui University of TechnologyAnhui University of TechnologyState Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan UniversityAnhui University of TechnologyAnhui University of TechnologyHefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of ChinaAnhui University of TechnologyAbstract A potential non-precious metal catalyst for oxygen reduction reaction should contain metal-N4 moieties. However, most of the current strategies to regulate the distances between neighboring metal sites are not pre-designed but depend on the probability by tuning the metal loading or the support. Herein, we report a general method for the synthesis of neighboring metal-Nx moieties (metal = Fe, Cu, Co, Ni, Zn, and Mn) via an interfacial-fixing strategy. Specifically, polydopamine is used to coat nanotemplates made of metal oxides, followed by pyrolysis to form a metal-oxide skeleton coated by rich nitrogen-doped carbon shells. After chemically etching the skeleton, only interfacial metal atoms strongly bonded with the support via nitrogen atoms are retained. The high purity (>95%) of dual Fe sites was confirmed by both the direct visualization of local regions and the indirect evidence of the averaged information. When these neighboring metal-Nx moieties are applied for oxygen reduction reaction, Fe-Nx moieties exhibit the superior activity, even outperforming commercial Pt/C in the aspects of the half-wave potential, methanol tolerance, carbon monoxide tolerance, and robustness.https://doi.org/10.1038/s41467-024-55630-y
spellingShingle Yan Yan
Rui Yu
Mingkai Liu
Zehua Qu
Jifeng Yang
Siyuan He
Hongliang Li
Jie Zeng
General synthesis of neighboring dual-atomic sites with a specific pre-designed distance via an interfacial-fixing strategy
Nature Communications
title General synthesis of neighboring dual-atomic sites with a specific pre-designed distance via an interfacial-fixing strategy
title_full General synthesis of neighboring dual-atomic sites with a specific pre-designed distance via an interfacial-fixing strategy
title_fullStr General synthesis of neighboring dual-atomic sites with a specific pre-designed distance via an interfacial-fixing strategy
title_full_unstemmed General synthesis of neighboring dual-atomic sites with a specific pre-designed distance via an interfacial-fixing strategy
title_short General synthesis of neighboring dual-atomic sites with a specific pre-designed distance via an interfacial-fixing strategy
title_sort general synthesis of neighboring dual atomic sites with a specific pre designed distance via an interfacial fixing strategy
url https://doi.org/10.1038/s41467-024-55630-y
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