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A Simple, Low-cost, and Robust System to Measure the Volume of Hydrogen Evolved by Chemical Reactions with Aqueous Solutions

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Bioinspired Catalyst/Electrolyte Interfacial Hydrogen-Bond Network Engineering toward Proton Transfer Acceleration

Wenshu Luo^1,2, Qin Li^1,3, Han Tian¹

¹State Key Laboratory of High Performance Ceramics, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, P. R. China.

Journal of the American Chemical Society

|March 3, 2026

Summary

This study enhances biomass electrocatalysis by engineering interfaces with bioinspired ligands, accelerating proton transfer for efficient chemical production. This method boosts catalyst performance and stability for sustainable applications.

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Area of Science:

Electrochemistry
Materials Science
Sustainable Chemistry

Background:

Electrocatalytic oxidation of biomass-derived alcohols is key for sustainable chemical synthesis.
Sluggish proton-coupled electron transfer (PCET) kinetics hinder catalyst activity and stability.
Enzymatic proton relays offer inspiration for improving PCET mechanisms.

Purpose of the Study:

To develop a ligand-induced interfacial engineering strategy to enhance PCET kinetics in biomass electrocatalysis.
To improve the activity, selectivity, and stability of cobalt hydroxide (Co(OH)2) electrocatalysts.
To demonstrate the practical application of the engineered catalyst in biomass valorization.

Main Methods:

Interface modification of Co(OH)2 using terephthalic acid (TPA) as a bioinspired ligand.
Electrocatalytic glycerol electrooxidation experiments.
In situ spectroscopy, theoretical calculations, and molecular dynamics simulations for mechanistic studies.
Membrane-electrode-assembly (MEA) electrolyzer testing and kilogram-scale product synthesis.

Main Results:

TPA accelerates proton transfer and facilitates lattice-hydroxyl activation for efficient proton deintercalation.
The interface-modified catalyst achieved 95% selectivity for formate production from glycerol.
Exceptional current density (>800 mA cm-2 at 1.6 V) and stability (>2600 h) were recorded.
An MEA electrolyzer demonstrated efficient operation (1.29 V at 10 mA cm-2) and enabled kilogram-scale potassium diformate production.

Conclusions:

Ligand-induced interfacial engineering effectively enhances PCET kinetics and catalyst performance.
The developed strategy offers a rational and generalizable approach for designing advanced electrocatalysts.
This work shows significant potential for sustainable biomass valorization through efficient electrocatalysis.