American Chemical Society
am9b11337_si_001.pdf (3.51 MB)

Updating the Intrinsic Activity of a Single-Atom Site with a P–O Bond for a Rechargeable Zn–Air Battery

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journal contribution
posted on 2019-08-28, 16:36 authored by He Sun, Sisi Liu, Mengfan Wang, Tao Qian, Jie Xiong, Chenglin Yan
Rechargeable Zn–air batteries have drawn great attention over the past decade, but their further development will require efficient bifunctional electrocatalysts to drive the sluggish cathodic reactions. Although a single-atom catalyst with maximum utilization per metal atom shows great promise, its catalytic performance is still far from satisfactory. Here we tackle this challenge by introducing a P–O bond to update the intrinsic activity of a single-atom site and thus reduce the reaction overpotential of the Zn–air battery. The critical role of the P–O bond in producing a favorable surface electronic environment of the single-atom metal site and improving its catalytic activity is identified with density functional theory simulations. The P–O-doped, atomically dispersed catalyst is shown experimentally to deliver excellent bifunctional performance, with a remarkable half-wave potential of 0.89 V versus reversible hydrogen electrode (vs RHE) for oxygen reduction reaction and a reversible oxygen electrode index of 0.74 V, exceeding those of most reported nonprecious metal catalysts. When subjected to practical application, both aqueous and all-solid-state Zn–air batteries illustrate superior power density and robust cyclic performance, confirming their potential feasibility in next-generation electronic devices.