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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...

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Autores principales: Liu, Wei, Feng, Haisong, Yang, Yusen, Niu, Yiming, Wang, Lei, Yin, Pan, Hong, Song, Zhang, Bingsen, Zhang, Xin, Wei, Min
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
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*).
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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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