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Pt(1) enhanced C-H activation synergistic with Pt(n) catalysis for glycerol cascade oxidation to glyceric acid

The selective oxidation of glycerol to glyceric acid, an important value-added reaction from polyols, is a typical cascade catalytic process. It is still of great challenge to simultaneously achieve high glycerol activity and glyceric acid selectivity, suffering from either deep oxidation and C-C cl...

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Autores principales: An, Zhe, Zhang, Zilong, Huang, Zeyu, Han, Hongbo, Song, Binbin, Zhang, Jian, Ping, Qi, Zhu, Yanru, Song, Hongyan, Wang, Bin, Zheng, Lirong, He, Jing
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9482651/
https://www.ncbi.nlm.nih.gov/pubmed/36115832
http://dx.doi.org/10.1038/s41467-022-33038-w
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author An, Zhe
Zhang, Zilong
Huang, Zeyu
Han, Hongbo
Song, Binbin
Zhang, Jian
Ping, Qi
Zhu, Yanru
Song, Hongyan
Wang, Bin
Zheng, Lirong
He, Jing
author_facet An, Zhe
Zhang, Zilong
Huang, Zeyu
Han, Hongbo
Song, Binbin
Zhang, Jian
Ping, Qi
Zhu, Yanru
Song, Hongyan
Wang, Bin
Zheng, Lirong
He, Jing
author_sort An, Zhe
collection PubMed
description The selective oxidation of glycerol to glyceric acid, an important value-added reaction from polyols, is a typical cascade catalytic process. It is still of great challenge to simultaneously achieve high glycerol activity and glyceric acid selectivity, suffering from either deep oxidation and C-C cleavage or poor oxidation efficiency from glyceraldehyde to glyceric acid. Herein, this work, inspired by nature, proposes a cascade synergistic catalysis strategy by atomic and low-coordinated cluster Pt on well-defined Cu-CuZrO(x), which involves enhanced C-H activation on atomic Pt(1) and O-H activation on cluster Pt(n) in the oxidation of glycerol to glyceraldehyde, and cluster Pt(n) for C=O activation followed by O-H insertion and atomic Pt(1) for C-H activation in the tandem oxidation of glyceraldehyde to glyceric acid. The enhanced C-H activation in the cascade process by atomic Pt(1) is revealed to be essential for the high glycerol activity (90.0±0.1%) and the glyceric acid selectivity (80.2±0.2%).
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spelling pubmed-94826512022-09-19 Pt(1) enhanced C-H activation synergistic with Pt(n) catalysis for glycerol cascade oxidation to glyceric acid An, Zhe Zhang, Zilong Huang, Zeyu Han, Hongbo Song, Binbin Zhang, Jian Ping, Qi Zhu, Yanru Song, Hongyan Wang, Bin Zheng, Lirong He, Jing Nat Commun Article The selective oxidation of glycerol to glyceric acid, an important value-added reaction from polyols, is a typical cascade catalytic process. It is still of great challenge to simultaneously achieve high glycerol activity and glyceric acid selectivity, suffering from either deep oxidation and C-C cleavage or poor oxidation efficiency from glyceraldehyde to glyceric acid. Herein, this work, inspired by nature, proposes a cascade synergistic catalysis strategy by atomic and low-coordinated cluster Pt on well-defined Cu-CuZrO(x), which involves enhanced C-H activation on atomic Pt(1) and O-H activation on cluster Pt(n) in the oxidation of glycerol to glyceraldehyde, and cluster Pt(n) for C=O activation followed by O-H insertion and atomic Pt(1) for C-H activation in the tandem oxidation of glyceraldehyde to glyceric acid. The enhanced C-H activation in the cascade process by atomic Pt(1) is revealed to be essential for the high glycerol activity (90.0±0.1%) and the glyceric acid selectivity (80.2±0.2%). Nature Publishing Group UK 2022-09-17 /pmc/articles/PMC9482651/ /pubmed/36115832 http://dx.doi.org/10.1038/s41467-022-33038-w 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
An, Zhe
Zhang, Zilong
Huang, Zeyu
Han, Hongbo
Song, Binbin
Zhang, Jian
Ping, Qi
Zhu, Yanru
Song, Hongyan
Wang, Bin
Zheng, Lirong
He, Jing
Pt(1) enhanced C-H activation synergistic with Pt(n) catalysis for glycerol cascade oxidation to glyceric acid
title Pt(1) enhanced C-H activation synergistic with Pt(n) catalysis for glycerol cascade oxidation to glyceric acid
title_full Pt(1) enhanced C-H activation synergistic with Pt(n) catalysis for glycerol cascade oxidation to glyceric acid
title_fullStr Pt(1) enhanced C-H activation synergistic with Pt(n) catalysis for glycerol cascade oxidation to glyceric acid
title_full_unstemmed Pt(1) enhanced C-H activation synergistic with Pt(n) catalysis for glycerol cascade oxidation to glyceric acid
title_short Pt(1) enhanced C-H activation synergistic with Pt(n) catalysis for glycerol cascade oxidation to glyceric acid
title_sort pt(1) enhanced c-h activation synergistic with pt(n) catalysis for glycerol cascade oxidation to glyceric acid
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9482651/
https://www.ncbi.nlm.nih.gov/pubmed/36115832
http://dx.doi.org/10.1038/s41467-022-33038-w
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