Over the years, extensive research has been carried out to optimize the oxygen evolution reaction (OER) by adopting different techniques as well as catalysts. Conducting organic polymers such as PEDOT have been employed to study the reaction but have failed to lower the over-potential for the reaction. Here we show electrochemically made, intimately blended, dual redox reversible materials incorporating PEDOT and metallacarboranes. The metallacarboranes act as doping agents but with tunable E1/2 potentials. The tunability of E1/2 allows the overlapping of the two redox potentials which subsequently leads to their synergy. The physico-chemical properties of the metallacarboranes fade and become integrated with PEDOT to form a dual redox reversible system. Therefore, the properties of the dopant are modified by the polymer. Thus, due to its high E1/2, the Co4+/3+ couple would not be an efficient electrocatalyst for water oxidation but when it is immersed in the PEDOT matrix the Co4+/3+ potential is more accessible so that very low overpotential values are obtained, which justifies the title of the work, How to switch from a poor PEDOT:X oxygen evolution reaction (OER) to a good one. The dual redox reversible system has been extensively characterized and has been shown to be a promising candidate for the water oxidation reaction.
Jewel A. M. Xavier and Isabel Fuentes have contributed equally to this work. We gratefully acknowledge the Spanish Ministerio de Economía y Competitividad (PID2019-106832RB-I00) and Generalitat de Catalunya (2017SGR1720). Jewel A. M. Xavier acknowledges the DOC-FAM programme under the Marie Sklodowska-Curie grant agreement no. 754397. This work was also funded by the Spanish Ministry of Science, through the “Severo Ochoa” Programme for Centers of Excellence in R&D (CEX2019-000917-S). Jewel A. M. Xavier and Miquel N. M are enrolled in the PhD program of UAB.
With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).