Stabilizing the Electrochemistry of Lithium-Selenium Battery via In situ Gelated Polymer Electrolyte: A Look from Anode

Li metal possesses a high theoretical specific capacity, high electronic conductivity, and a low electrochemical potential, making it a promising anode material for building next-generation rechargeable metal batteries. In case conventional liquid electrolytes were used, and the anode using Li metal has been hindered by unstable(electro)chemistry at Li/electrolyte interface and the accompanied dendrite issue. Specifically, for the Li-Se batteries, the dissolution and shuttle of polyselenide intermediates lead to the deposition of poorly-conductive species on the anode, which further aggravates the chemical environment at the anode. In this work, we proposed to stabilize the Li-Se electrochemistry by constructing a gel polymer electrolyte via in situ gelations of conventional ether-based electrolytes at room temperature. The results demonstrate that the in situ gelated electrolyte helps to build electrochemically stable electrode/electrolyte interfaces and promote the efficient transfer of charge carriers across the interface. Compared with the liquid electrolytes, the gelated electrolyte shows improved chemical compatibility with the Li metal anode, which effectively alleviates the unfavorable side reactions and dendrite formation at the anode/electrolyte interface, and the polyselenide shuttle from the cathode to the anode. As a result, the Li-Se battery shows a higher Coulombic efficiency and improved cycling performance.