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Single-atom catalyst for high-performance methanol oxidation

Single-atom catalysts have been widely investigated for several electrocatalytic reactions except electrochemical alcohol oxidation. Herein, we synthesize atomically dispersed platinum on ruthenium oxide (Pt(1)/RuO(2)) using a simple impregnation-adsorption method. We find that Pt(1)/RuO(2) has good...

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Autores principales: Zhang, Zhiqi, Liu, Jiapeng, Wang, Jian, Wang, Qi, Wang, Yuhao, Wang, Kai, Wang, Zheng, Gu, Meng, Tang, Zhenghua, Lim, Jongwoo, Zhao, Tianshou, Ciucci, Francesco
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8413426/
https://www.ncbi.nlm.nih.gov/pubmed/34475400
http://dx.doi.org/10.1038/s41467-021-25562-y
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author Zhang, Zhiqi
Liu, Jiapeng
Wang, Jian
Wang, Qi
Wang, Yuhao
Wang, Kai
Wang, Zheng
Gu, Meng
Tang, Zhenghua
Lim, Jongwoo
Zhao, Tianshou
Ciucci, Francesco
author_facet Zhang, Zhiqi
Liu, Jiapeng
Wang, Jian
Wang, Qi
Wang, Yuhao
Wang, Kai
Wang, Zheng
Gu, Meng
Tang, Zhenghua
Lim, Jongwoo
Zhao, Tianshou
Ciucci, Francesco
author_sort Zhang, Zhiqi
collection PubMed
description Single-atom catalysts have been widely investigated for several electrocatalytic reactions except electrochemical alcohol oxidation. Herein, we synthesize atomically dispersed platinum on ruthenium oxide (Pt(1)/RuO(2)) using a simple impregnation-adsorption method. We find that Pt(1)/RuO(2) has good electrocatalytic activity towards methanol oxidation in an alkaline media with a mass activity that is 15.3-times higher than that of commercial Pt/C (6766 vs. 441 mA mg(‒1)(Pt)). In contrast, single atom Pt on carbon black is inert. Further, the mass activity of Pt(1)/RuO(2) is superior to that of most Pt-based catalysts previously developed. Moreover, Pt(1)/RuO(2) has a high tolerance towards CO poisoning, resulting in excellent catalytic stability. Ab initio simulations and experiments reveal that the presence of Pt‒O(3f) (3-fold coordinatively bonded O)‒Ru(cus) (coordinatively unsaturated Ru) bonds with the undercoordinated bridging O in Pt(1)/RuO(2) favors the electrochemical dehydrogenation of methanol with lower energy barriers and onset potential than those encountered for Pt‒C and Pt‒Ru.
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spelling pubmed-84134262021-09-22 Single-atom catalyst for high-performance methanol oxidation Zhang, Zhiqi Liu, Jiapeng Wang, Jian Wang, Qi Wang, Yuhao Wang, Kai Wang, Zheng Gu, Meng Tang, Zhenghua Lim, Jongwoo Zhao, Tianshou Ciucci, Francesco Nat Commun Article Single-atom catalysts have been widely investigated for several electrocatalytic reactions except electrochemical alcohol oxidation. Herein, we synthesize atomically dispersed platinum on ruthenium oxide (Pt(1)/RuO(2)) using a simple impregnation-adsorption method. We find that Pt(1)/RuO(2) has good electrocatalytic activity towards methanol oxidation in an alkaline media with a mass activity that is 15.3-times higher than that of commercial Pt/C (6766 vs. 441 mA mg(‒1)(Pt)). In contrast, single atom Pt on carbon black is inert. Further, the mass activity of Pt(1)/RuO(2) is superior to that of most Pt-based catalysts previously developed. Moreover, Pt(1)/RuO(2) has a high tolerance towards CO poisoning, resulting in excellent catalytic stability. Ab initio simulations and experiments reveal that the presence of Pt‒O(3f) (3-fold coordinatively bonded O)‒Ru(cus) (coordinatively unsaturated Ru) bonds with the undercoordinated bridging O in Pt(1)/RuO(2) favors the electrochemical dehydrogenation of methanol with lower energy barriers and onset potential than those encountered for Pt‒C and Pt‒Ru. Nature Publishing Group UK 2021-09-02 /pmc/articles/PMC8413426/ /pubmed/34475400 http://dx.doi.org/10.1038/s41467-021-25562-y Text en © The Author(s) 2021 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
Zhang, Zhiqi
Liu, Jiapeng
Wang, Jian
Wang, Qi
Wang, Yuhao
Wang, Kai
Wang, Zheng
Gu, Meng
Tang, Zhenghua
Lim, Jongwoo
Zhao, Tianshou
Ciucci, Francesco
Single-atom catalyst for high-performance methanol oxidation
title Single-atom catalyst for high-performance methanol oxidation
title_full Single-atom catalyst for high-performance methanol oxidation
title_fullStr Single-atom catalyst for high-performance methanol oxidation
title_full_unstemmed Single-atom catalyst for high-performance methanol oxidation
title_short Single-atom catalyst for high-performance methanol oxidation
title_sort single-atom catalyst for high-performance methanol oxidation
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8413426/
https://www.ncbi.nlm.nih.gov/pubmed/34475400
http://dx.doi.org/10.1038/s41467-021-25562-y
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