Work

Multiscale Engineering of N‐CoP@NC/3D‐NC Bifunctional Electrocatalyst: Synergistic Interface and Doping Design for High‐Performance Zinc–Air Batteries

Year: 2025

Type: article

Abstract: ABSTRACT The development of cost‐effective, high‐performance bifunctional oxygen electrocatalysts is pivotal for zinc‐air batteries (ZABs). Here, we report an innovative multiscale optimization strategy that synergistically integrates hierarchical structural design with atomic‐level electronic engineering to fabricate an encapsulated N‐doped cobalt phosphide catalyst (N‐CoP@NC) embedded within a 3D porous nitrogen‐doped carbon scaffold (3D‐NC). The macro/mesoscopic design employs NaCl‐templated 3D‐NC frameworks to create optimized mass transport pathways and high surface area, while the atomic/nanoscale engineering achieves precise nitrogen doping into CoP lattices and strategic construction of metal‐carbon interfaces, enabling electronic structure modulation. Mechanistic insights from theoretical calculation reveal that nitrogen incorporation fundamentally induces an electron‐depletion effect in the carbon shell, precisely tuning the adsorption energy of oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) intermediates and significantly improving intrinsic activity. The resulting N‐CoP@NC/3D‐NC catalyst exhibits exceptional bifunctional performance with a half‐wave potential of 0.80V versus RHE towards ORR and an overpotential of 380 mV at 10 mA cm −2 for OER. When deployed in ZABs, it achieves a large peak power density of 127 mW cm −2 and robust cycling stability (683 h with <4% efficiency decay), surpassing Pt/C+Ir/C benchmarks. This work pioneers a novel electrocatalyst design paradigm via synergistic interface engineering and heteroatom doping.

Source: Small

DOI: 10.1002/smll.202513939