Publication date: 15th December 2025
Proton-electron transfers (PET) are known to dictate most electrocatalytic reactions,[1] and significant focus is devoted on regulating them mostly by electrolyte engineering and ionomeric adlayers. In this work, we achieved interfacial PET tuning through the use of poly(ionic liquid) (PIL) binders.[2] These binders were used for electrochemical hydrogenations (ECH) of C=C, C≡C and C=O bonds in aqueous media, across a wide pH range of 12 units. When benchmarked against their commercial fluorinated counterparts (Nafion®, PVDF), PILs result in up to a 4-5 fold increase in hydrogenation yield and Faradaic efficiency, while also limiting catalyst leaching. PILs achieve such enhanced performance by regulating electrochemical hydrogen adsorption, thus suppressing the competing Hydrogen Evolution Reaction (HER), in favor of ECH. Kinetic and in-situ microenvironment studies show that the PIL binders’ positive charge introduces electrostatic effects, cation exclusion and local pH changes, that tailor the electrochemical double layer and consequently, charge transfer. Our method proves to be the solid-state analogue of electrolyte engineering, while being compatible with common electrolytes (H2SO4, NaOH, buffers) and circumvents additional electrode fabrication steps (e.g. adlayer addition). Hence, PIL binders come to the forefront of interfacial modulation for technologically relevant electrosynthetic reactions, while circumventing the use of fluorinated electrode constituents.
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