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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...
Autores principales: | , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Royal Society of Chemistry
2017
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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. |
format | Online Article Text |
id | pubmed-5299936 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2017 |
publisher | Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
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
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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
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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
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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
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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
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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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