Promoting Oxygen Reduction Reaction on Carbon‐based Materials by Selective Hydrogen Bonding

Abstract

AbstractElectrochemical oxygen reduction reaction (ORR) is fundamental for many energy conversion and storage devices. Selective tuning of *OOH/*OH adsorption energy to break the intrinsic scaling limitation (ΔG*OOH=ΔG*OH+3.2 eV) is effective in optimizing the ORR limiting potential (UL), which is practically challenging to achieve by constructing a particular catalyst. Herein, using first‐principles calculations, we elucidated how to rationally plant an additional *OH that can selectively interact with the ORR intermediate of *OOH via hydrogen bonding, while not affecting the *OH intermediate. Guided by the design principle, we successfully tailored a series of novel carbon‐based catalysts, with merits of low‐cost, long‐lasting, synthesis feasibility, exhibiting a high UL (1.06 V). Our proposed strategy comes up with a new linear scaling relationship of ΔG*OOH=ΔG*OH+2.84 eV. This approach offers a great possibility for the rational design of efficient catalysts for ORR and other chemical reactions.