Co 2 P-Assisted Atomic Co-N 4 Active Sites with a Tailored Electronic Structure Enabling Efficient ORR/OER for Rechargeable Zn-Air Batteries

• Published in: ACS applied materials & interfaces 2023-02, Vol.15 (7), p.9240-9249
• Main Authors: Liu, Xiaoyan, Wu, Jinfeng, Luo, Zhuyu, Liu, Ping, Tian, Yue, Wang, Xuewei, Li, Hexing
• Format: Article
• Language: English
• ISSN: 1944-8244; 1944-8252
• DOI: 10.1021/acsami.2c19713

Oxygen reduction and evolution reactions (ORR and OER, respectively) are vital steps for metal-air batteries, which are plagued by their sluggish kinetics. It is still a challenge to develop highly effective and low-cost non-noble-metal-based electrocatalysts. Herein, a simple and reliable method was reported to synthesize a Co P-assisted Co single-atom (Co-N centers) electrocatalyst (Co P/Co-NC) via evaporative drying and pyrolysis processes. The Co P nanoparticles and Co-N centers are uniformly distributed on the nitrogen-doped carbon matrix. Notably, Co P/Co-NC showed excellent activities in both ORR (initial potential, 1.01 V; half-wave potential, 0.88 V) and OER (overpotential, 369 mV at 10 mA cm ). The above results were comparable to those of commercial catalysts (such as Pt/C and RuO ). Based on the experimental and theoretical analyses, the impressive activity can be ascribed to the tailored electronic structure of Co-N centers by the adjacent Co P, enabling the electron transfer from the Co atom to the neighboring C atoms, leading to a downshift of the d-band center, and improved reaction kinetics were achieved. The assembled Zn-air batteries using Co P/Co-NC as the air cathode showed a peak power density of 187 mW cm and long-life cycling stability for 140 h at 5 mA cm . This work may pave a promising avenue to design hybrid bifunctional electrocatalysts for highly efficient ORR/OER.