Integrating CO₂ electroreduction with phenol hydrogenation on an oxygen-affinity tailored catalyst

Area of Science:

• Materials Science
• Catalysis
• Electrochemistry

Background:

• Electrocatalytic CO2 reduction (ECR) to formic acid is challenged by formate-electrolyte separation.
• In situ utilization of the formate-electrolyte mixture is an underexplored solution for CO2 valorization.

Purpose of the Study:

• To develop BiₓPd₁₋ₓTe nanocrystals (NCs) for simultaneous ECR and catalytic transfer hydrogenation (CTH).
• To enable precise tuning of surface oxygen affinities for optimized catalytic performance.

Main Methods:

• Microwave-assisted cation topological exchange for synthesizing BiₓPd₁₋ₓTe NCs.
• Electrocatalytic CO2 reduction and catalytic transfer hydrogenation experiments.
• Mechanistic studies using surface characterization and computational analysis.

Main Results:

• Optimized Bi₀.₁Pd₀.₉Te NCs achieved 92% Faradaic efficiency for formate production at -0.9 V vs RHE.
• High production rate of 860 mmol/h/gcat at 100 mA/cm² for formate.
• 98% selectivity toward cyclohexanone in phenol hydrogenation using the formate-electrolyte mixture.

Conclusions:

• Synergistic integration of ECR and CTH was pioneered.
• A novel CO2 valorization and biomass upgrading strategy was established.
• Uniformly dispersed Bi sites create an oxygen affinity gradient enhancing catalytic performance.