Charge Regulation on Hybrid Nanosheet Stereoassembly via Interfacial PO Coupling Enables Efficient Overall Water Splitting
Kaili Wu, Xin Wang, Wenqing Wang, Yan Luo, Wei Cao, Yiyao Cao, Haijiao Xie, Yan Yan, Huijuan Lin, Jixin Zhu, Kun Rui
Abstract
Abstract Precise regulation on interfacial electronic coupling is essential to achieve efficient catalysts with tailored electrocatalytic behaviors but remains challenging. Herein, a straightforward topochemical strategy is presented to realize Co‐based heterostructured nanofiber stereoassembled with PO coupled nanosheet (CoHF/PO). By constructing well‐defined metal oxide/phosphide interface, prominent electron redistribution can be established via interfacial PO coupling, which is strongly correlated with the catalytic activities. Density functional theory calculations indicate that the rational interface engineering renders accelerated charge transfer and more importantly, optimized surface adsorption/desorption behaviors, contributing to boosted kinetics for both hydrogen evolution reaction and oxygen evolution reaction. Particularly, CoHF/PO featuring promoted intrinsic activity and accessible active sites exhibits intriguing activity and stability at higher current densities in alkaline media, surpassing commercial Pt/C and Ir/C. This study is expected to demonstrate noteworthy promise of covalent coupling toward modulated electronic environment and interface chemistry for electrocatalytic applications and beyond.