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Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes
The design and exploitation of high-performance catalysts have gained considerable attention in selective hydrogenation reactions, but remain a huge challenge. Herein, we report a RuNi single atom alloy (SAA) in which Ru single atoms are anchored onto Ni nanoparticle surface via Ru–Ni coordination a...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9178046/ https://www.ncbi.nlm.nih.gov/pubmed/35676245 http://dx.doi.org/10.1038/s41467-022-30536-9 |
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author | Liu, Wei Feng, Haisong Yang, Yusen Niu, Yiming Wang, Lei Yin, Pan Hong, Song Zhang, Bingsen Zhang, Xin Wei, Min |
author_facet | Liu, Wei Feng, Haisong Yang, Yusen Niu, Yiming Wang, Lei Yin, Pan Hong, Song Zhang, Bingsen Zhang, Xin Wei, Min |
author_sort | Liu, Wei |
collection | PubMed |
description | The design and exploitation of high-performance catalysts have gained considerable attention in selective hydrogenation reactions, but remain a huge challenge. Herein, we report a RuNi single atom alloy (SAA) in which Ru single atoms are anchored onto Ni nanoparticle surface via Ru–Ni coordination accompanied with electron transfer from sub-surface Ni to Ru. The optimal catalyst 0.4% RuNi SAA exhibits simultaneously improved activity (TOF value: 4293 h(–1)) and chemoselectivity toward selective hydrogenation of 4-nitrostyrene to 4-aminostyrene (yield: >99%), which is, to the best of our knowledge, the highest level compared with reported heterogeneous catalysts. In situ experiments and theoretical calculations reveal that the Ru–Ni interfacial sites as intrinsic active centers facilitate the preferential cleavage of N–O bond with a decreased energy barrier by 0.28 eV. In addition, the Ru–Ni synergistic catalysis promotes the formation of intermediates (C(8)H(7)NO* and C(8)H(7)NOH*) and accelerates the rate-determining step (hydrogenation of C(8)H(7)NOH*). |
format | Online Article Text |
id | pubmed-9178046 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-91780462022-06-10 Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes Liu, Wei Feng, Haisong Yang, Yusen Niu, Yiming Wang, Lei Yin, Pan Hong, Song Zhang, Bingsen Zhang, Xin Wei, Min Nat Commun Article The design and exploitation of high-performance catalysts have gained considerable attention in selective hydrogenation reactions, but remain a huge challenge. Herein, we report a RuNi single atom alloy (SAA) in which Ru single atoms are anchored onto Ni nanoparticle surface via Ru–Ni coordination accompanied with electron transfer from sub-surface Ni to Ru. The optimal catalyst 0.4% RuNi SAA exhibits simultaneously improved activity (TOF value: 4293 h(–1)) and chemoselectivity toward selective hydrogenation of 4-nitrostyrene to 4-aminostyrene (yield: >99%), which is, to the best of our knowledge, the highest level compared with reported heterogeneous catalysts. In situ experiments and theoretical calculations reveal that the Ru–Ni interfacial sites as intrinsic active centers facilitate the preferential cleavage of N–O bond with a decreased energy barrier by 0.28 eV. In addition, the Ru–Ni synergistic catalysis promotes the formation of intermediates (C(8)H(7)NO* and C(8)H(7)NOH*) and accelerates the rate-determining step (hydrogenation of C(8)H(7)NOH*). Nature Publishing Group UK 2022-06-08 /pmc/articles/PMC9178046/ /pubmed/35676245 http://dx.doi.org/10.1038/s41467-022-30536-9 Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Liu, Wei Feng, Haisong Yang, Yusen Niu, Yiming Wang, Lei Yin, Pan Hong, Song Zhang, Bingsen Zhang, Xin Wei, Min Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes |
title | Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes |
title_full | Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes |
title_fullStr | Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes |
title_full_unstemmed | Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes |
title_short | Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes |
title_sort | highly-efficient runi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9178046/ https://www.ncbi.nlm.nih.gov/pubmed/35676245 http://dx.doi.org/10.1038/s41467-022-30536-9 |
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