A biosynthetic model of cytochrome c oxidase as an electrocatalyst for oxygen reduction

Sohini Mukherjee, Arnab Mukherjee, Ambika Bhagi-Damodaran, Manjistha Mukherjee, Yi Lu, Abhishek Dey

Research output: Contribution to journalArticlepeer-review

54 Scopus citations

Abstract

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.

Original languageEnglish (US)
Article number8467
JournalNature communications
Volume6
DOIs
StatePublished - Oct 12 2015
Externally publishedYes

Bibliographical note

Funding Information:
This research is sponsored by Department of Science and Technology, India and US National Institute of Health (GM062211).

Publisher Copyright:
© 2015 Macmillan Publishers Limited. All rights reserved.

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