Promoting Oxygen Reduction Reaction on Carbon-based Materials by Selective Hydrogen Bonding
Li Yang1,2,3, Yue Zhang1, Yan Huang4
1Institutes of Physical Science and Information Technology, Anhui University, Hefei, Anhui, 230601, P. R. China.
Abstract:
Electrochemical 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.
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