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A biosynthetic model of cytochrome c oxidase as an electrocatalyst for oxygen reduction
Creating an artificial functional mimic of the mitochondrial enzyme cytochrome c oxidase (CcO) has been a long-term goal of the scientific community as such a mimic will not only add to our fundamental understanding of how CcO works but may also pave the way for efficient electrocatalysts for oxygen...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Pub. Group
2015
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4633646/ https://www.ncbi.nlm.nih.gov/pubmed/26455726 http://dx.doi.org/10.1038/ncomms9467 |
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author | Mukherjee, Sohini Mukherjee, Arnab Bhagi-Damodaran, Ambika Mukherjee, Manjistha Lu, Yi Dey, Abhishek |
author_facet | Mukherjee, Sohini Mukherjee, Arnab Bhagi-Damodaran, Ambika Mukherjee, Manjistha Lu, Yi Dey, Abhishek |
author_sort | Mukherjee, Sohini |
collection | PubMed |
description | Creating an artificial functional mimic of the mitochondrial enzyme cytochrome c oxidase (CcO) has been a long-term goal of the scientific community as such a mimic will not only add to our fundamental understanding of how CcO works but may also pave the way for efficient electrocatalysts for oxygen reduction in hydrogen/oxygen fuel cells. Here we develop an electrocatalyst for reducing oxygen to water under ambient conditions. We use site-directed mutants of myoglobin, where both the distal Cu and the redox-active tyrosine residue present in CcO are modelled. In situ Raman spectroscopy shows that this catalyst features very fast electron transfer rates, facile oxygen binding and O–O bond lysis. An electron transfer shunt from the electrode circumvents the slow dissociation of a ferric hydroxide species, which slows down native CcO (bovine 500 s(−1)), allowing electrocatalytic oxygen reduction rates of 5,000 s(−1) for these biosynthetic models. |
format | Online Article Text |
id | pubmed-4633646 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2015 |
publisher | Nature Pub. Group |
record_format | MEDLINE/PubMed |
spelling | pubmed-46336462015-11-25 A biosynthetic model of cytochrome c oxidase as an electrocatalyst for oxygen reduction Mukherjee, Sohini Mukherjee, Arnab Bhagi-Damodaran, Ambika Mukherjee, Manjistha Lu, Yi Dey, Abhishek Nat Commun Article Creating an artificial functional mimic of the mitochondrial enzyme cytochrome c oxidase (CcO) has been a long-term goal of the scientific community as such a mimic will not only add to our fundamental understanding of how CcO works but may also pave the way for efficient electrocatalysts for oxygen reduction in hydrogen/oxygen fuel cells. Here we develop an electrocatalyst for reducing oxygen to water under ambient conditions. We use site-directed mutants of myoglobin, where both the distal Cu and the redox-active tyrosine residue present in CcO are modelled. In situ Raman spectroscopy shows that this catalyst features very fast electron transfer rates, facile oxygen binding and O–O bond lysis. An electron transfer shunt from the electrode circumvents the slow dissociation of a ferric hydroxide species, which slows down native CcO (bovine 500 s(−1)), allowing electrocatalytic oxygen reduction rates of 5,000 s(−1) for these biosynthetic models. Nature Pub. Group 2015-10-12 /pmc/articles/PMC4633646/ /pubmed/26455726 http://dx.doi.org/10.1038/ncomms9467 Text en Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ |
spellingShingle | Article Mukherjee, Sohini Mukherjee, Arnab Bhagi-Damodaran, Ambika Mukherjee, Manjistha Lu, Yi Dey, Abhishek A biosynthetic model of cytochrome c oxidase as an electrocatalyst for oxygen reduction |
title | A biosynthetic model of cytochrome c oxidase as an electrocatalyst for oxygen reduction |
title_full | A biosynthetic model of cytochrome c oxidase as an electrocatalyst for oxygen reduction |
title_fullStr | A biosynthetic model of cytochrome c oxidase as an electrocatalyst for oxygen reduction |
title_full_unstemmed | A biosynthetic model of cytochrome c oxidase as an electrocatalyst for oxygen reduction |
title_short | A biosynthetic model of cytochrome c oxidase as an electrocatalyst for oxygen reduction |
title_sort | biosynthetic model of cytochrome c oxidase as an electrocatalyst for oxygen reduction |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4633646/ https://www.ncbi.nlm.nih.gov/pubmed/26455726 http://dx.doi.org/10.1038/ncomms9467 |
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