Optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Precise fabrication of stable single-atom catalysts with desired performance remains a challenge.
• Methanol electrooxidation is crucial for energy conversion, particularly in alkaline media.

Purpose of the Study:

• To synthesize and investigate ruthenium single atoms within a Ni3FeN lattice for alkaline methanol electrooxidation.
• To understand the structure-performance relationship of single-atom catalysts with varying coordination environments.

Main Methods:

• Synthesis of Ni3FeN lattice with buried Ru single atoms (Ni3FeN-Ru_buried).
• Electrochemical testing for methanol electrooxidation.
• Operando spectroscopies to study catalyst behavior under reaction conditions.
• Theoretical simulations to analyze electronic structure and reaction mechanisms.

Main Results:

• Ni3FeN-Ru_buried demonstrated high selectivity and Faradaic efficiency for methanol to formate conversion.
• Operando spectroscopies indicated optimized reactant adsorption and inhibited surface reconstruction for Ni3FeN-Ru_buried.
• Theoretical simulations revealed regulated local electronic states and reduced energy barriers for the potential-determining step.

Conclusions:

• The Ni3FeN-Ru_buried catalyst is highly efficient for methanol to formate conversion in alkaline conditions.
• This study provides insights into the rational design of single-atom catalysts with accessible active sites.