Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.185
Publication date: 6th July 2018
The need for better energy storage and conversion devices has never been so urgent in order to enable the rapid deployment of renewable energies and reduce our use of fossil fuels. While batteries spurred the spread of portable electronics, their limited energy density hampers their use for large scale applications. Hydrogen has long been envisioned as a viable energy carrier owing to its very large energy density, nevertheless its electrochemical production by electrolysis, the most efficient carbon-free production route at large scale, greatly suffers from the slow kinetics associated with the oxygen evolution reaction (OER). The key challenges that need to be addressed to improve the OER kinetics are well-spotted and researchers eagerly pushed to better understand the reaction leading to numerous progresses since our early vision of this reaction. Hence, while some works were devoted to finding physical descriptors capable of describing the OER activity following a Sabatier principle, recent developments in the field point towards the complexity of such reaction. Indeed, a substantial body of evidence now points towards the involvement of the bulk chemistry of the most active transition metal oxides in the OER mechanism. Hence, we recently found that bulk oxygen atoms are evolved under OER conditions for cobalt-based perovskites materials,1 eventually triggering a new mechanism into which chemical steps and proton exchange are rate limiting. We could then demonstrate that the origin for the often observed activity-stability relationship for OER electrocatalysts is nested into the existence of a common intermediate which is reactive surface oxygen in the form of oxyl-group.2 Overall, the line becomes blurrier between heterogeneous and homogeneous catalysis when using transition metal oxides as OER catalysts for which complex surface dynamics are at play.3 Hence, efforts must be paid to understanding and stabilizing these intermediates in order to break this relationship and further enhance the stability of OER electrocatalysts. We will therefore discuss in this talk our recent efforts at designing chemical approach to counterbalance the chemical reactivity of the most active transition metal oxides through a combined crystallographic and electrolyte engineering approach.
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