Dynamic Single-Atom Catalysts on Gallium To Overcome the Scaling Relationship Limit: AIMD Screening for CO₂ Reduction...

Area of Science:

• Materials Science
• Catalysis
• Electrochemistry

Background:

• Static single-atom catalysts (SACs) face scaling relationship limitations in electrochemical reactions.
• Developing advanced catalysts is crucial for efficient hydrogen evolution (HER) and CO2 reduction (CO2RR).

Purpose of the Study:

• To introduce and investigate dynamic single-atom catalysts (SACs) supported on Gallium (M-SAC@Ga) for HER and CO2RR.
• To screen s-, p-, d-, and f-block elements for stable and efficient dynamic SACs.

Main Methods:

• High-throughput screening using Density Functional Theory (DFT) and Ab Initio Molecular Dynamics (AIMD) calculations.
• Systematic evaluation of thermodynamic and electrochemical stabilities of M-SAC@Ga systems.

Main Results:

• Identified stable dynamic SACs including Re-, Pt-, Pd-, Rh-, Ir-, Au-, Ag-, Ru-, Tc-, Ni-, Cu-, Os-, Hg-, and Ge-SAC@Ga.
• Ni-SAC@Ga demonstrated low overpotentials for CO2RR, producing CHOOH, CO, CH3OH, and CH4.
• Dynamic coordination changes and atomic intelligence were key to mitigating scaling limits.

Conclusions:

• Dynamic SACs on Gallium offer a promising strategy to overcome limitations of static SACs.
• The study provides insights into designing next-generation electrocatalysts.
• D-electron count emerged as a universal descriptor for catalyst performance.