Enhancing CO₂ electroreduction performance through transition metal atom doping and strain engineering in γ-GeSe: a...

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• Electrocatalytic CO2 reduction (CO2RR) is vital for sustainable energy, but developing stable, active, and selective catalysts remains challenging.
• Single-atom catalysts (SACs) offer high atomic utilization efficiency, making them promising for CO2RR.
• Monolayer γ-GeSe doped with transition metals (TM@γ-GeSe) are explored as potential SACs for CO2RR.

Purpose of the Study:

• To investigate the potential of TM@γ-GeSe for electrocatalytic CO2RR.
• To identify stable TM@γ-GeSe SACs with high activity and selectivity.
• To understand the effect of strain engineering on catalytic performance and selectivity.

Main Methods:

• Systematic design and screening of 26 TM@γ-GeSe SACs using theoretical calculations.
• Mechanistic investigations of CO2RR pathways.
• Application of strain engineering and work function as a descriptor.

Main Results:

• Four stable TM@γ-GeSe SACs (TM = Rh, Pd, Pt, Au) were identified.
• Rh@γ-GeSe and Pd@γ-GeSe exhibited exceptional CO2RR activity with limiting potentials of -0.26 V and -0.35 V, respectively.
• Pd@γ-GeSe showed high selectivity for formic acid production. Tensile strain enhanced formic acid selectivity for Rh@γ-GeSe, while compressive strain favored hydrogen evolution.

Conclusions:

• TM@γ-GeSe SACs, particularly Rh and Pd, demonstrate significant potential for electrocatalytic CO2RR.
• Strain engineering offers a viable strategy to tune catalytic activity and product selectivity.
• This theoretical study provides insights for designing advanced γ-GeSe-based catalysts for CO2RR.