Curvature-dominated microenvironment modulation enables efficient electrocatalytic oxygen reduction
Chuan Jing, Ziyang Guo, Yujia Yao, Runjing Xu, Dengfeng Li, Kailin Li, Yuxin Zhang
Abstract
The oxygen reduction reaction (ORR) critical for electrochemical energy conversion systems suffers from sluggish kinetics and high overpotentials that hinder the efficiency of these technologies. Herein, a curvature-dominated microenvironment modulation strategy is demonstrated to enhance ORR performance via engineering a helical hollow carbon nanotube with embedded sub-nano W<sub>2</sub>N clusters. This architecture yields optimized electrostatic field distributions and reduced d-band center of W<sub>2</sub>N, thereby promoting enrichment of OH-, adsorption of oxygen and desorption of oxygen intermediates (*OH). The catalyst shows remarkable ORR activity with high onset potential of 1.00 V and half-wave potential of 0.89 V, outperforming both Pt/C and other W<sub>2</sub>N-based catalysts. Theoretical calculations verify that the curved support enhances electron delocalization within the W<sub>2</sub>N clusters, regulating the interaction between the catalyst and reactants. Our findings establish a general design principle of curvature-induced microenvironment modulation and offer a new pathway toward designing efficient electrocatalysts for sustainable energy storage applications.