Niobium Tungsten Oxide in a Green Water-in-Salt Electrolyte Enables Ultra-Stable Aqueous Lithium-Ion Capacitors

Abstract

Highlights

• A green water-in-salt electrolyte was developed using lithium acetate as solute with a wide electrochemical stability window of 2.8 V.

• Molecular dynamics simulation confirmed the nature of water-in-salt electrolyte, where hydrogen bonds of water–water were disrupted and ionic interactions became stronger than dilute solution.

• Nb₁₈W₁₆O₉₃-based lithium-ion capacitors delivered unexceptionable stability over 50,000 cycles.

Aqueous hybrid supercapacitors are attracting increasing attention due to their potential low cost, high safety and eco-friendliness. However, the narrow operating potential window of aqueous electrolyte and the lack of suitable negative electrode materials seriously hinder its future applications. Here, we explore high concentrated lithium acetate with high ionic conductivity of 65.5 mS cm⁻¹ as a green “water-in-salt” electrolyte, providing wide voltage window up to 2.8 V. It facilitates the reversible function of niobium tungsten oxide, Nb₁₈W₁₆O₉₃, that otherwise only operations in organic electrolytes previously. The Nb₁₈W₁₆O₉₃ with lithium-ion intercalation pseudocapacitive behavior exhibits excellent rate performance, high areal capacity, and ultra-long cycling stability. An aqueous lithium-ion hybrid capacitor is developed by using Nb₁₈W₁₆O₉₃ as negative electrode combined with graphene as positive electrode in lithium acetate-based “water-in-salt” electrolyte, delivering a high energy density of 41.9 W kg⁻¹, high power density of 20,000 W kg⁻¹ and unexceptionable stability of 50,000 cycles.