Metal-Doped PdH(111) Catalysts for CO₂ Reduction

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• Palladium Hydride (PdH)-based catalysts are promising for CO2 reduction and hydrogen evolution.
• Understanding dopant effects on PdH catalytic properties is crucial for optimizing performance.

Purpose of the Study:

• To systematically screen transition metal dopants in PdH(111) for improved CO2 reduction and hydrogen evolution.
• To investigate the impact of doping configurations on catalyst stability, activity, and selectivity.

Main Methods:

• Density Functional Theory (DFT) calculations were employed for systematic screening.
• Six doping configurations (single, dimer, triangle, parallelogram, island, overlayer) were analyzed for 22 transition metals.
• Catalyst stability, activity, and selectivity were evaluated based on DFT predictions.

Main Results:

• Several dopants, notably Titanium (Ti) and Niobium (Nb), exhibited excellent predicted catalytic activity and CO2 selectivity.
• These dopants demonstrated good stability, evidenced by negative doping formation energies.
• Improved performance is attributed to reaction intermediates forming dual C-Metal and O-Metal bonds, enhancing HOCO* binding and CO2 activation.

Conclusions:

• Transition metal doping significantly enhances PdH catalyst performance for CO2 reduction and hydrogen evolution.
• Ti and Nb are identified as highly promising dopants for next-generation catalysts.
• The study provides fundamental insights into the mechanism of improved catalytic activity through optimized intermediate binding.