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Biomimetic caged platinum catalyst for hydrosilylation reaction with high site selectivity

Natural enzymes exhibit unparalleled selectivity due to the microenvironment around the active sites, but how to design artificial catalysts to achieve similar performance is a formidable challenge for the catalysis community. Herein, we report that a less selective platinum catalyst becomes highly...

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Autores principales: Pan, Ganghuo, Hu, Chunhua, Hong, Song, Li, Huaping, Yu, Dongdong, Cui, Chengqian, Li, Qiaosheng, Liang, Nianjie, Jiang, Ying, Zheng, Lirong, Jiang, Lei, Liu, Yuzhou
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7782696/
https://www.ncbi.nlm.nih.gov/pubmed/33397921
http://dx.doi.org/10.1038/s41467-020-20233-w
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author Pan, Ganghuo
Hu, Chunhua
Hong, Song
Li, Huaping
Yu, Dongdong
Cui, Chengqian
Li, Qiaosheng
Liang, Nianjie
Jiang, Ying
Zheng, Lirong
Jiang, Lei
Liu, Yuzhou
author_facet Pan, Ganghuo
Hu, Chunhua
Hong, Song
Li, Huaping
Yu, Dongdong
Cui, Chengqian
Li, Qiaosheng
Liang, Nianjie
Jiang, Ying
Zheng, Lirong
Jiang, Lei
Liu, Yuzhou
author_sort Pan, Ganghuo
collection PubMed
description Natural enzymes exhibit unparalleled selectivity due to the microenvironment around the active sites, but how to design artificial catalysts to achieve similar performance is a formidable challenge for the catalysis community. Herein, we report that a less selective platinum catalyst becomes highly active and selective for industrially relevant hydrosilylation of a broad range of substrates when a porous cage ligand is used for confinement around the catalytic active site. The catalyst is more than ten times more active than Karstedt’s catalyst while being recyclable. Properties such as size-selective catalysis and Michaelis-Menten kinetics support the proposed enzyme-like model. This biomimetic catalyst exhibits remarkable site-selectivity through the cage’s confining effect, which amplifies small steric differences into dramatic reactivity changes for similar functional groups within a molecule.
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spelling pubmed-77826962021-01-11 Biomimetic caged platinum catalyst for hydrosilylation reaction with high site selectivity Pan, Ganghuo Hu, Chunhua Hong, Song Li, Huaping Yu, Dongdong Cui, Chengqian Li, Qiaosheng Liang, Nianjie Jiang, Ying Zheng, Lirong Jiang, Lei Liu, Yuzhou Nat Commun Article Natural enzymes exhibit unparalleled selectivity due to the microenvironment around the active sites, but how to design artificial catalysts to achieve similar performance is a formidable challenge for the catalysis community. Herein, we report that a less selective platinum catalyst becomes highly active and selective for industrially relevant hydrosilylation of a broad range of substrates when a porous cage ligand is used for confinement around the catalytic active site. The catalyst is more than ten times more active than Karstedt’s catalyst while being recyclable. Properties such as size-selective catalysis and Michaelis-Menten kinetics support the proposed enzyme-like model. This biomimetic catalyst exhibits remarkable site-selectivity through the cage’s confining effect, which amplifies small steric differences into dramatic reactivity changes for similar functional groups within a molecule. Nature Publishing Group UK 2021-01-04 /pmc/articles/PMC7782696/ /pubmed/33397921 http://dx.doi.org/10.1038/s41467-020-20233-w Text en © The Author(s) 2021 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/.
spellingShingle Article
Pan, Ganghuo
Hu, Chunhua
Hong, Song
Li, Huaping
Yu, Dongdong
Cui, Chengqian
Li, Qiaosheng
Liang, Nianjie
Jiang, Ying
Zheng, Lirong
Jiang, Lei
Liu, Yuzhou
Biomimetic caged platinum catalyst for hydrosilylation reaction with high site selectivity
title Biomimetic caged platinum catalyst for hydrosilylation reaction with high site selectivity
title_full Biomimetic caged platinum catalyst for hydrosilylation reaction with high site selectivity
title_fullStr Biomimetic caged platinum catalyst for hydrosilylation reaction with high site selectivity
title_full_unstemmed Biomimetic caged platinum catalyst for hydrosilylation reaction with high site selectivity
title_short Biomimetic caged platinum catalyst for hydrosilylation reaction with high site selectivity
title_sort biomimetic caged platinum catalyst for hydrosilylation reaction with high site selectivity
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7782696/
https://www.ncbi.nlm.nih.gov/pubmed/33397921
http://dx.doi.org/10.1038/s41467-020-20233-w
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