Strain‐Mediated Sabatier Principle‐Guided the Design of Bimetallic Catalysts for High‐Performance Li‐CO₂ Batteries

Abstract Using PdCu alloy as a model system, winged oxidized carbon nanotube‐confined Pd x Cu y bimetallic catalysts with tunable compressive strain are engineered through atomic Cu incorporation into Pd lattices. This strain‐mediated approach effectively modulates the d‐band center of Pd to optimizes the antibonding state occupancy for a balanced adsorption landscape of CO 2 activation and Li 2 CO 3 decomposition that aligns with the Sabatier principle for optimal catalytic activity. Systematic investigations reveal that 0.73% compressive strain in Pd 5 Cu 3 optimally modulates the adsorption behavior of both CO 2 and Li 2 CO 3 while maintaining weakened Li─O bonding interactions to promote the decomposition of Li 2 CO 3 , achieving a superior stability at high current densities (> 1100 h at 1.0 A g −1 ). The findings highlight the pivotal role of strain‐driven electronic optimization strategy in designing high‐efficiency catalytic systems for advanced metal‐gas batteries.