Regulating Lateral Adsorbate Interaction for Efficient Electroreforming of Bio-polyols

Area of Science:

• Electrochemistry
• Catalysis
• Materials Science

Background:

• Heterogeneous electrocatalysis selectivity is a major challenge.
• Developing new strategies beyond catalyst design is crucial.

Purpose of the Study:

• To control electrocatalytic pathways via lateral adsorbate interactions for bio-polyol oxidation.
• To enhance selectivity in electrocatalytic processes.

Main Methods:

• Utilizing redox-innocent 1,1,1,3,3,3-hexafluoro-2-propanol (HFIP) as an adsorbate.
• Forming a mixed adsorbate layer with bio-polyols on a nickel oxyhydroxide catalyst.
• Employing in situ spectroscopic analysis and DFT calculations.

Main Results:

• Achieved over a 2-fold enhancement in oxalate selectivity to 55% for glycerol oxidation.
• Demonstrated the strategy's applicability to various bio-polyol substrates.
• Revealed that hydrogen-bonded adsorbate interactions tune adsorption energies and oxidation capabilities.

Conclusions:

• Introducing redox-innocent adsorbates can create lateral interactions to tune electrocatalytic reactions.
• This approach offers a new perspective for enhancing selectivity in electrocatalysis.
• The method effectively tailors oxidation capabilities toward desired products.