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Electrocatalytic water oxidation by a trinuclear copper complex

Geer, Ana and Jia, Xiaofan and McKeown, Bradley Aaron and Nielsen, Robert J. and Goddard, William Andrew and Gunnoe, T. Brent (2019) Electrocatalytic water oxidation by a trinuclear copper complex. In: 258th ACS National Meeting & Exposition, 25-29 August 2019, San Diego, CA.

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Considering the ongoing decrease in the cost of electricity, the development of electrocatalytic processes will gain increasingly more importance in the future. Moreover, with the dwindling of the primary energy source that drives our society, fossil fuels, and the consequences that their utilization has on the environment, it is pivotal to find alternative sustainable energy sources from renewable and carbon free resources. Artificial photosynthesis is a promising strategy for meeting the growing energy demands, where a crucial half-reaction in both natural and artificial photosynthesis is water oxidn. (2H₂O --> O₂ + 4H+ + 4e-), using water as a source of electrons and protons. Inspired by nature, where water oxidn. occurs at the Mn4CaO5 active site of the oxygen evolving complex (OEC) of photosystem II, there has been growing interest in synthetic multinuclear catalysts for promoting intramol. O-O bond formation, with an advantageous redox flexibility for multi-electron transfer arising from the multinuclear core. Here, we employ a mol. trinuclear copper(II) complex, [(DAM)Cu₃(µ³-O)]Cl₄ (DAM = dodecaaza macrotetracycle), as catalyst precursor for electrocatalytic water oxidn. Based on electrochem. studies, we show that this complex is likely an active homogeneous electrocatalyst for water oxidn. in aq. phosphate buffer soln. enabling oxygen evolution with a turnover frequency of approx. 6.0 s⁻¹ at pH =7.

Item Type:Conference or Workshop Item (Paper)
Related URLs:
URLURL TypeDescription Website
Nielsen, Robert J.0000-0002-7962-0186
Goddard, William Andrew0000-0003-0097-5716
Gunnoe, T. Brent0000-0001-5714-3887
Additional Information:© 2019 American Chemical Society.
Record Number:CaltechAUTHORS:20200430-094451257
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:102919
Deposited By: Tony Diaz
Deposited On:30 Apr 2020 17:18
Last Modified:30 Apr 2020 17:18

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