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Dongyue Sun

Diimine-dioxime cobalt complexes for electrocatalytic hydrogen production: Mechanistic study and optimization through the integration of an electron reservoir

Published on 12 October 2017


Thesis presented on October 12, 2017

Abstract:
The production of H2 through sunlight-driven water splitting appears to be a promising solution for our future energy supply. Earth-abundant catalysts should be developed to replace platinum as water splitting catalysts. Bio-inspired cobalt diimine-dioxime complexes have emerged as one of the most versatile series of non-noble metal catalysts. In this work, the mechanism for H2 evolution mediated by this series of catalysts has been reinvestigated, and kinetic information have been determined thanks to recent advancements in electrochemical methodology. Their superior hydrogen evolution performance has been shown through comparative catalytic Tafel plots. Secondly, a synthetic route towards the incorporation of fullerene moieties, as electron reservoirs, in the vicinity of the catalytic center, has been developed. The resulting catalyst has shown improved catalytic activity and has been implemented in an operational H2-evolving photocathode based on organic semi-conductors.

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