DOI: 10.1002/smll.74322 ISSN: 1613-6810

Tip‐Induced Electric Field Enhancement Synergizes With Heterogeneous Interfaces in Ni@Pt Metallic Aerogels for Superior Oxygen Reduction and Ultra‐Stable Zinc–Air Batteries

Liu Liu, Jiahan Guan, Shuhan Sun, Ke Yuan, Jiaxin Lu, Ran Xie, Zhonghao Xia, Yifan Wang, Xiaodong Wu, Sheng Cui

ABSTRACT

Constructing heterogeneous interfaces is an effective strategy to enhance the oxygen reduction reaction (ORR) kinetics of electrocatalysts, yet the controllable fabrication of such interfaces remains challenging. Herein, an interface regulation strategy is proposed, which achieves the fabrication of heterogeneous interface Ni/Pt metallic aerogels (Ni@Pt) with tip‐like structures via sodium citrate ligand‐mediated Ni core stabilization, ammonium fluoride etchant‐induced interface activation, and NaBH 4 gradient reduction technology. MATLAB simulation results confirm that a significant enhancement of the local electric field occurs in the tip region of the Ni@Pt 3 structure, accompanied by an increase in OH concentration. Furthermore, Extended X‐ray Absorption Fine Structure (EXAFS) analysis indicates that a compressive strain of 0.79% exists in this region. Thus, Ni@Pt 3 exhibits excellent bifunctional catalytic activity, achieving a half‐wave potential of 0.88 V, a kinetic current density of 11.92 mA cm −2 , and an OER overpotential of 350 mV. Notably, ZABs based on it show 1.48 V open‐circuit voltage, 203 mW/cm 2 peak power, and 1300 h cycling stability. Density Functional Theory (DFT) calculations confirm that, due to the compressive strain in the Pt lattice, the ORR activity is enhanced by reducing the binding strength between the catalyst surface and the adsorbed * OH intermediate.

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