Metal Organic Framework-Templated Synthesis of Bimetallic Selenides with Rich Phase Boundaries for Sodium-Ion Storage...

Two-phase or multiphase compounds have been evidenced to exhibit good electrochemical performance for energy applications; however, the mechanism insights into these materials, especially the performance improvement by engineering the high-active phase boundaries in bimetallic compounds, remain to be seen. Here, we report a bimetallic selenide heterostructure (CoSe₂/ZnSe) and the fundamental mechanism behind their superior electrochemical performance. The charge redistribution at the phase boundaries of CoSe₂/ZnSe was experimentally and theoretically proven. Benefiting from the abundant phase boundaries, CoSe₂/ZnSe exerts low Na⁺ adsorption energy and fast diffusion kinetics for sodium-ion batteries and high activity for oxygen evolution reaction. As expected, excellent sodium storage capability, specifically a superb cyclic stability of up to 800 cycles for the Na₃V₂(PO₄)₃∥CoZn-Se full cell, and efficient water oxidation with a small overpotential of 320 mV to reach 10 mA cm^-2 were obtained. This work demonstrates the importance of phase boundaries in bimetallic compounds to boost the performance in various fields.