(661w) Structural Design of Transition Metal-Nitrogen Co-Decorated Nanocarbon Materials and CO2 Electroreduction Mechanism Research

Electrocatalysts play a key role in accelerating the sluggish electrochemical CO₂ reduction (ECR) involving multi-electron and proton transfer. Herein, we develop a proton capture strategy via accelerating the water dissociation reaction catalyzed by transition metal nanoparticles (NPs) adjacent to atomically dispersed and nitrogen coordinated single nickel (Ni-N_x) active sites to accelerate the proton transfer to the latter for boosting the intermediate protonation step, and hence the whole ECR process. This accelerated protonation process is amply demonstrated experimentally. Aberration-corrected scanning transmission electron microscopy and X-ray absorption spectroscopy, together with theoretical calculations, reveal that the Ni NPs accelerate the adsorbed H (H_ad) generation and transfer to the adjacent Ni-N_x sites for boosting the intermediate protonation and the overall ECR processes. This proton capture strategy is universal to design and prepare for various high-performance catalysts for diverse electrochemical reactions even beyond ECR