Optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation

Abstract The precise fabrication and regulation of the stable catalysts with desired performance still challengeable for single atom catalysts. Here, the Ru single atoms with different coordination environment in Ni3FeN lattice are synthesized and studied as a typical case over alkaline methanol ele...

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Main Authors: Yunxiang Lin, Bo Geng, Ruyun Zheng, Wei Chen, Jiahui Zhao, Hengjie Liu, Zeming Qi, Zhipeng Yu, Kun Xu, Xue Liu, Li Yang, Lei Shan, Li Song
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-55615-x
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author Yunxiang Lin
Bo Geng
Ruyun Zheng
Wei Chen
Jiahui Zhao
Hengjie Liu
Zeming Qi
Zhipeng Yu
Kun Xu
Xue Liu
Li Yang
Lei Shan
Li Song
author_facet Yunxiang Lin
Bo Geng
Ruyun Zheng
Wei Chen
Jiahui Zhao
Hengjie Liu
Zeming Qi
Zhipeng Yu
Kun Xu
Xue Liu
Li Yang
Lei Shan
Li Song
author_sort Yunxiang Lin
collection DOAJ
description Abstract The precise fabrication and regulation of the stable catalysts with desired performance still challengeable for single atom catalysts. Here, the Ru single atoms with different coordination environment in Ni3FeN lattice are synthesized and studied as a typical case over alkaline methanol electrooxidation. The Ni3FeN with buried Ru atoms in subsurface lattice (Ni3FeN-Ruburied) exhibits high selectivity and Faradaic efficiency of methanol to formate conversion. Meanwhile, operando spectroscopies reveal that the Ni3FeN-Ruburied exhibits an optimized adsorption of reactants along with an inhibited surface structural reconstruction. Additional theoretical simulations demonstrate that the Ni3FeN-Ruburied displays a regulated local electronic states of surface metal atoms with an optimized adsorption of reactants and reduced energy barrier of potential determining step. This work not only reports a high-efficient catalyst for methanol to formate conversion in alkaline condition, but also offers the insight into the rational design of single atom catalysts with more accessible surficial active sites.
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institution Kabale University
issn 2041-1723
language English
publishDate 2025-01-01
publisher Nature Portfolio
record_format Article
series Nature Communications
spelling doaj-art-04d09c8325b84739ac2452f5bafd9c9d2025-01-05T12:40:03ZengNature PortfolioNature Communications2041-17232025-01-0116111310.1038/s41467-024-55615-xOptimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidationYunxiang Lin0Bo Geng1Ruyun Zheng2Wei Chen3Jiahui Zhao4Hengjie Liu5Zeming Qi6Zhipeng Yu7Kun Xu8Xue Liu9Li Yang10Lei Shan11Li Song12Institutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui UniversityInstitutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui UniversityInstitutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui UniversityCenter of Free Electron Laser & High Magnetic Field, School of Materials Science and Engineering, Anhui UniversityInstitutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui UniversityNational Synchrotron Radiation Laboratory, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, University of Science and Technology of ChinaInstitutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui UniversitySchool of Chemistry and Chemical Engineering, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui UniversityCenter of Free Electron Laser & High Magnetic Field, School of Materials Science and Engineering, Anhui UniversityInstitutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui UniversityInstitutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui UniversityNational Synchrotron Radiation Laboratory, University of Science and Technology of ChinaAbstract The precise fabrication and regulation of the stable catalysts with desired performance still challengeable for single atom catalysts. Here, the Ru single atoms with different coordination environment in Ni3FeN lattice are synthesized and studied as a typical case over alkaline methanol electrooxidation. The Ni3FeN with buried Ru atoms in subsurface lattice (Ni3FeN-Ruburied) exhibits high selectivity and Faradaic efficiency of methanol to formate conversion. Meanwhile, operando spectroscopies reveal that the Ni3FeN-Ruburied exhibits an optimized adsorption of reactants along with an inhibited surface structural reconstruction. Additional theoretical simulations demonstrate that the Ni3FeN-Ruburied displays a regulated local electronic states of surface metal atoms with an optimized adsorption of reactants and reduced energy barrier of potential determining step. This work not only reports a high-efficient catalyst for methanol to formate conversion in alkaline condition, but also offers the insight into the rational design of single atom catalysts with more accessible surficial active sites.https://doi.org/10.1038/s41467-024-55615-x
spellingShingle Yunxiang Lin
Bo Geng
Ruyun Zheng
Wei Chen
Jiahui Zhao
Hengjie Liu
Zeming Qi
Zhipeng Yu
Kun Xu
Xue Liu
Li Yang
Lei Shan
Li Song
Optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation
Nature Communications
title Optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation
title_full Optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation
title_fullStr Optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation
title_full_unstemmed Optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation
title_short Optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation
title_sort optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation
url https://doi.org/10.1038/s41467-024-55615-x
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