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Title: Intramolecular hydrogen-bonding in a cobalt aqua complex and electrochemical water oxidation activity

Abstract

Water oxidation is catalysed in Nature by a redox cofactor embedded in a hydrogen-bonded network designed to orchestrate proton transfer throughout the challenging 4 electron reaction. In order to mimic aspects of this microenvironment, [CoLDMA(CH3CN)2][BF4]2 (2) was synthesized, where LDMA is a dipyridyldiamine ligand with two dimethylamine bases in the secondary coordination sphere. Structural characterization of the corresponding aqua complexes establish hydrogen bonding between the bound water and pendant base(s). Cyclic voltammetry of [CoLDMA(CH3CN)2][BF4]2 (2) reveals enhanced oxidative current upon titration with water and controlled potential electrolysis confirms evolution of O2. The related complex [CoLH(CH3CN)2][BF4]2 (1), which has the same primary coordination environment as 2 but lacks pendant bases, is inactive. The structural and electrochemical studies illustrate the role positioned proton relays can play in promoting redox reactivity.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Department of Chemistry, University of California, Irvine, USA
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1420343
Alternate Identifier(s):
OSTI ID: 1505134
Grant/Contract Number:  
SC0012150; CHE-1338173
Resource Type:
Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Name: Chemical Science Journal Volume: 9 Journal Issue: 10; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Khosrowabadi Kotyk, Juliet F., Hanna, Caitlin M., Combs, Rebecca L., Ziller, Joseph W., and Yang, Jenny Y. Intramolecular hydrogen-bonding in a cobalt aqua complex and electrochemical water oxidation activity. United Kingdom: N. p., 2018. Web. doi:10.1039/C7SC04960A.
Khosrowabadi Kotyk, Juliet F., Hanna, Caitlin M., Combs, Rebecca L., Ziller, Joseph W., & Yang, Jenny Y. Intramolecular hydrogen-bonding in a cobalt aqua complex and electrochemical water oxidation activity. United Kingdom. doi:10.1039/C7SC04960A.
Khosrowabadi Kotyk, Juliet F., Hanna, Caitlin M., Combs, Rebecca L., Ziller, Joseph W., and Yang, Jenny Y. Mon . "Intramolecular hydrogen-bonding in a cobalt aqua complex and electrochemical water oxidation activity". United Kingdom. doi:10.1039/C7SC04960A.
@article{osti_1420343,
title = {Intramolecular hydrogen-bonding in a cobalt aqua complex and electrochemical water oxidation activity},
author = {Khosrowabadi Kotyk, Juliet F. and Hanna, Caitlin M. and Combs, Rebecca L. and Ziller, Joseph W. and Yang, Jenny Y.},
abstractNote = {Water oxidation is catalysed in Nature by a redox cofactor embedded in a hydrogen-bonded network designed to orchestrate proton transfer throughout the challenging 4 electron reaction. In order to mimic aspects of this microenvironment, [CoLDMA(CH3CN)2][BF4]2 (2) was synthesized, where LDMA is a dipyridyldiamine ligand with two dimethylamine bases in the secondary coordination sphere. Structural characterization of the corresponding aqua complexes establish hydrogen bonding between the bound water and pendant base(s). Cyclic voltammetry of [CoLDMA(CH3CN)2][BF4]2 (2) reveals enhanced oxidative current upon titration with water and controlled potential electrolysis confirms evolution of O2. The related complex [CoLH(CH3CN)2][BF4]2 (1), which has the same primary coordination environment as 2 but lacks pendant bases, is inactive. The structural and electrochemical studies illustrate the role positioned proton relays can play in promoting redox reactivity.},
doi = {10.1039/C7SC04960A},
journal = {Chemical Science},
number = 10,
volume = 9,
place = {United Kingdom},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/C7SC04960A

Citation Metrics:
Cited by: 3 works
Citation information provided by
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    • DOI: 10.1021/ja304525n

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    journal, December 2013

    • Zhang, Teng; Wang, Cheng; Liu, Shubin
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    Amine Oxidative N-Dealkylation via Cupric Hydroperoxide Cu-OOH Homolytic Cleavage Followed by Site-Specific Fenton Chemistry
    journal, February 2015

    • Kim, Sunghee; Ginsbach, Jake W.; Lee, Jung Yoon
    • Journal of the American Chemical Society, Vol. 137, Issue 8
    • DOI: 10.1021/ja508371q

    Energetics of Proton-Coupled Electron Transfer in High-Valent Mn 2 (μ-O) 2 Systems:  Models for Water Oxidation by the Oxygen-Evolving Complex of Photosystem II
    journal, January 1996

    • Baldwin, Michael J.; Pecoraro, Vincent L.
    • Journal of the American Chemical Society, Vol. 118, Issue 45
    • DOI: 10.1021/ja9626906

    Intramolecular Proton Transfer Boosts Water Oxidation Catalyzed by a Ru Complex
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    • Matheu, Roc; Ertem, Mehmed Z.; Benet-Buchholz, Jordi
    • Journal of the American Chemical Society, Vol. 137, Issue 33
    • DOI: 10.1021/jacs.5b06541

    Electrocatalytic Hydrogen Evolution under Acidic Aqueous Conditions and Mechanistic Studies of a Highly Stable Molecular Catalyst
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    • Tsay, Charlene; Yang, Jenny Y.
    • Journal of the American Chemical Society, Vol. 138, Issue 43
    • DOI: 10.1021/jacs.6b05851

    Lability and Basicity of Bipyridine-Carboxylate-Phosphonate Ligand Accelerate Single-Site Water Oxidation by Ruthenium-Based Molecular Catalysts
    journal, October 2017

    • Shaffer, David W.; Xie, Yan; Szalda, David J.
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    • DOI: 10.1021/jacs.7b06096

    Electrostatic Effects on Proton Coupled Electron Transfer in Oxomanganese Complexes Inspired by the Oxygen-Evolving Complex of Photosystem II
    journal, May 2013

    • Amin, Muhamed; Vogt, Leslie; Vassiliev, Serguei
    • The Journal of Physical Chemistry B, Vol. 117, Issue 20
    • DOI: 10.1021/jp403321b

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