Mimicking Noble Metals Using Hydrogen-Bonded Conducting Polymers for Electrocatalysis

Abstract

The most active and efficient catalysts for the electrochemical hydrogen evolution reaction rely on noble metals, a fact that increases the cost of producing hydrogen and thereby limits the widespread adoption of this fuel. Here we present metal-free polydopamine and polyguanine as selective organic hydrogen electrocatalysts1–3. The conducting functional polymers incorporate selective hydrogen-affine hydrogen bonds that possess a similar hydrogen binding energies and work function as e.g. platinum. We report the synthesis of hydrogen-selective electrocatalytic polyguanine and polydopamine and demonstrate the enhancement of the rate-determining step in the proton reduction. We further present mechanistic spectral IR-operando studies on the catalytic hydrogen bonded motifs as well as the continuous electrolysis to molecular hydrogen using polyguanine and polydopamine electrodes for several 100 hours without notable degradation.(1) Coskun, H.; Aljabour, A.; Schöfberger, W.; Hinterreiter, A.; Stifter, D.; Sariciftci, N. S.; Stadler, P. Cofunction of Protons as Dopant and Reactant Activate the Electrocatalytic Hydrogen Evolution in Emeraldine‐Polyguanine. Adv. Mater. Interfaces 2019, 1901364 DOI: 10.1002/admi.201901364.(2) Coskun, H.; Aljabour, A.; Uiberlacker, L.; Strobel, M.; Hild, S.; Cobet, C.; Farka, D.; Stadler, P.; Sariciftci, N. S. Chemical Vapor Deposition - Based Synthesis of Conductive Polydopamine Thin-Films. Thin Solid Films 2018, 645 (August 2017), 320–325 DOI: 10.1016/j.tsf.2017.10.063.(3) Coskun, H.; Aljabour, A.; Luna, P. De; Sun, H.; Nishiumi, N.; Yoshida, T.; Koller, G.; Ramsey, M. G.; Greunz, T.; Stifter, D.; Hassel, A. W.; Sariciftci, N. S.; Sargent, E. H.; Stadler, P. Hydrogen-Bonded Polymers Mimic Noble Metal Electrocatalysts. Adv. Mater., submitted.