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Programmable Solid-Electrolyte Interfaces for Efficient and Selective Electrochemical Hydrogenations.

Anastasios Orestis Grammenos¹, Jessica Brandt¹, Yu Zhang²

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Summary

This summary is machine-generated.

Fluorine-free poly(ionic liquid)s act as active electrolyte layers, not just binders, enhancing electrochemical hydrogenation (ECH) yields and selectivity. These novel binders improve catalyst performance and stability by actively modulating the electrode-interface.

Keywords:

cation effect electrochemical hydrogenation electrochemical interface electrode binder poly(ionic liquid)

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Area of Science:

Electrochemistry
Materials Science
Catalysis

Background:

Electrode binders are typically passive components in electrochemical systems.
The solid-liquid interface at electrodes significantly influences reaction kinetics and selectivity.
Understanding and controlling this interface is crucial for optimizing electrosynthetic processes.

Purpose of the Study:

To investigate the active role of fluorine-free poly(ionic liquid)s (PILs) as electrode binders.
To explore how PILs modulate the electrode-electrolyte interface and influence electrochemical reactions.
To enhance electrochemical hydrogenation (ECH) selectivity and efficiency using PIL binders.

Main Methods:

Utilized fluorine-free poly(ionic liquid)s (PILs) as binders for Palladium on Carbon (Pd-C) catalysts.
Investigated the modulation of the electric double layer, interfacial pH, and proton-electron transfer kinetics.
Compared the performance of PIL-modified electrodes against those using Nafion and PVDF binders across various pH values (0.6, 5.2, 13).

Main Results:

PIL binders function as solid-state electrolyte layers, creating intrinsic electric fields.
PILs reshape the electric double layer by repelling cations and modulating pH, suppressing hydrogen evolution reaction (HER) and promoting ECH.
Achieved up to fivefold higher ECH yields and fourfold greater Faradaic efficiencies compared to Nafion/PVDF, with reduced palladium leaching.

Conclusions:

Polymer binders can act as active, field-modulating media, not just passive additives.
PILs offer a strategy for binder-controlled interfacial design in electrosynthesis.
This work extends classical electrolyte-effect concepts to polymer-confined interfaces.