Boosting the Proton‐coupled Electron Transfer via Fe−P Atomic Pair for Enhanced Electrochemical CO<sub>2</sub> Reduction
Qiao Zhang, Hsin‐Jung Tsai, Fuhua Li, Zhiming Wei, Qinye He, Jie Ding, Yuhang Liu, Zih‐Yi Lin, Xiaoju Yang, Zhaoyang Chen, Fangxin Hu, Xuan Yang, Qing Tang, Hong Bin Yang, Sung‐Fu Hung, Yueming Zhai
Abstract
Abstract Single‐atom catalysts exhibit superior CO 2 ‐to‐CO catalytic activity, but poor kinetics of proton‐coupled electron transfer (PCET) steps still limit the overall performance toward the industrial scale. Here, we constructed a Fe−P atom paired catalyst onto nitrogen doped graphitic layer (Fe 1 /PNG) to accelerate PCET step. Fe 1 /PNG delivers an industrial CO current of 1 A with FE CO over 90 % at 2.5 V in a membrane‐electrode assembly, overperforming the CO current of Fe 1 /NG by more than 300 %. We also decrypted the synergistic effects of the P atom in the Fe−P atom pair using operando techniques and density functional theory, revealing that the P atom provides additional adsorption sites for accelerating water dissociation, boosting the hydrogenation of CO 2 , and enhancing the activity of CO 2 reduction. This atom‐pair catalytic strategy can modulate multiple reactants and intermediates to break through the inherent limitations of single‐atom catalysts.