Dopant-Tuned Restructuring\nKinetic for the Formation\nof Heterophase-Confined Metal-Nonmetal Diatomic Sites for Efficient\nOxygen Evolution Reaction

Engineering the electronic structure and microenvironments\nof active\nsites is an effective strategy to enhance the oxygen evolution reaction\n(OER) kinetics. Meanwhile, most OER materials act only as precatalysts;\ntherefore, understanding and modulation of restructuring kinetics\nis crucial for developing efficient OER active sites. Herein, a dopant-tuned\nrestructuring kinetic for the generation of heterophase-confined metal-nonmetal\ndiatomic sites has been achieved. Both operando spectra and theoretical\nevidence show that Zr dopants tune in situ restructuring kinetics\nand induce charge transfer between Ni and Se to generate Ni–Se\ndiatomic sites that coordinate dynamically with oxygenated intermediates\nand reduce energy barriers significantly. Consequently, the dense\nNi–Se diatomic sites display an overpotential of 224 mV vs\nreversible hydrogen electrode at 10 mAcm<sup>–2</sup> and stable\noperation over 500 h in alkaline conditions, one of the best performances\namong reported selenide-derived OER catalysts. Our results enable\nan in-depth understanding of dynamically restructured diatomic sites\nbeyond the conventional single-metal sites and expand the strategies\nfor engineering atomic/molecular-level active sites.