Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
Publication date: 22nd December 2022
While considerable efforts have been devoted to developing functionalized covalent organic frameworks (COFs) for oxygen evolution electrocatalysts in recent years,1-3 studies related to the identification of the true catalytically active species for oxygen evolution reaction (OER) remain lacking in the field. In this work, we investigated the true active species of a cobalt-functionalized COF (TpBpy-Co) as electrochemical OER catalyst through a series of electrochemical measurements and post-mortem characterizations. Our results demonstrate that Co(II) ions, coordinated on the COF backbone, are transformed into cobalt-based nanoparticles when exposing TpBpy-Co in alkaline media; they are mostly transformed into cobalt hydroxide (Co(OH)2) before OER. Furthermore, we have observed the oxidation of cobalt species to form cobalt oxide (Co3O4) even after 1 min of applying an anodic potential. Feasibly, these new cobalt species act as the true active species for oxygen evolution. No final conclusion regarding TpBpy-Co works as a secondary active species can be made, as TpBpy-Co is structurally unstable in alkaline electrolyte and mixed with more active OER catalysts, cobalt-based nanoparticles. Above all, our results highlight that more attention should be paid to identifying the true active species for COF electrocatalysts, and a strong coordination between COFs and metal center under electrochemical operational conditions is crucial for developing true COF OER catalysts.
This work was funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) – Project-ID 358283783 – SFB 1333/2 2022. Financial support by the Max Planck Society and by the Cluster of Excellence e-conversion (EXC 2089) and chemistry department of University of Stuttgart.
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