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Covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design

Development of non-noble metal catalysts with similar activity and stability to noble metals is of significant importance in the conversion and utilization of clean energy. The catalytic hydrolysis of ammonia borane (AB) to produce 3 equiv. of H(2), as an example of where noble metal catalysts signi...

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Autores principales: Li, Zhao, He, Teng, Liu, Lin, Chen, Weidong, Zhang, Miao, Wu, Guotao, Chen, Ping
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5299936/
https://www.ncbi.nlm.nih.gov/pubmed/28451227
http://dx.doi.org/10.1039/c6sc02456d
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author Li, Zhao
He, Teng
Liu, Lin
Chen, Weidong
Zhang, Miao
Wu, Guotao
Chen, Ping
author_facet Li, Zhao
He, Teng
Liu, Lin
Chen, Weidong
Zhang, Miao
Wu, Guotao
Chen, Ping
author_sort Li, Zhao
collection PubMed
description Development of non-noble metal catalysts with similar activity and stability to noble metals is of significant importance in the conversion and utilization of clean energy. The catalytic hydrolysis of ammonia borane (AB) to produce 3 equiv. of H(2), as an example of where noble metal catalysts significantly outperform their non-noble peers, serves as an excellent test site for the design and optimization of non-noble metal catalysts. Our kinetic isotopic effect measurements reveal, for the first time, that the kinetic key step of the hydrolysis is the activation of H(2)O. Deducibly, a transition metal with an optimal electronic structure that bonds H(2)O and –OH in intermediate strengths would favor the hydrolysis of AB. By employing a covalent triazine framework (CTF), a newly developed porous material capable of donating electrons through the lone pairs on N, the electron densities of nano-sized Co and Ni supported on CTF are markedly increased, as well as their catalytic activities. Specifically, Co/CTF exhibits a total turnover frequency of 42.3 mol(H(2)) mol(Co) (–1) min(–1) at room temperature, which is superior to all peer non-noble metal catalysts ever reported and even comparable to some noble metal catalysts.
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spelling pubmed-52999362017-04-27 Covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design Li, Zhao He, Teng Liu, Lin Chen, Weidong Zhang, Miao Wu, Guotao Chen, Ping Chem Sci Chemistry Development of non-noble metal catalysts with similar activity and stability to noble metals is of significant importance in the conversion and utilization of clean energy. The catalytic hydrolysis of ammonia borane (AB) to produce 3 equiv. of H(2), as an example of where noble metal catalysts significantly outperform their non-noble peers, serves as an excellent test site for the design and optimization of non-noble metal catalysts. Our kinetic isotopic effect measurements reveal, for the first time, that the kinetic key step of the hydrolysis is the activation of H(2)O. Deducibly, a transition metal with an optimal electronic structure that bonds H(2)O and –OH in intermediate strengths would favor the hydrolysis of AB. By employing a covalent triazine framework (CTF), a newly developed porous material capable of donating electrons through the lone pairs on N, the electron densities of nano-sized Co and Ni supported on CTF are markedly increased, as well as their catalytic activities. Specifically, Co/CTF exhibits a total turnover frequency of 42.3 mol(H(2)) mol(Co) (–1) min(–1) at room temperature, which is superior to all peer non-noble metal catalysts ever reported and even comparable to some noble metal catalysts. Royal Society of Chemistry 2017-01-01 2016-08-30 /pmc/articles/PMC5299936/ /pubmed/28451227 http://dx.doi.org/10.1039/c6sc02456d Text en This journal is © The Royal Society of Chemistry 2016 http://creativecommons.org/licenses/by/3.0/ This is an Open Access article distributed under the terms of the Creative Commons Attribution 3.0 Unported License (http://creativecommons.org/licenses/by/3.0/) which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
spellingShingle Chemistry
Li, Zhao
He, Teng
Liu, Lin
Chen, Weidong
Zhang, Miao
Wu, Guotao
Chen, Ping
Covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design
title Covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design
title_full Covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design
title_fullStr Covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design
title_full_unstemmed Covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design
title_short Covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design
title_sort covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5299936/
https://www.ncbi.nlm.nih.gov/pubmed/28451227
http://dx.doi.org/10.1039/c6sc02456d
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