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All-Temperature Zinc Batteries with High-Entropy Aqueous Electrolyte



Chongyin Yang, Jiale Xia, Chunyu Cui, Travis P. Pollard, Jenel Vatamanu, Antonio Faraone, Joseph Dura, Madhu Sudan N. Tyagi, Alex Kattan, Elijah Thimsen, Jijian Xu, Wentao Song, Enyuan Hu, Xiao Ji, Singyuk Hou, Xiyue Zhang, Michael S. Ding, Sooyeon Hwang, Dong Su, Yang Ren, Xiao-Qing Yang, Howard Wang, Oleg Borodin, Chunsheng Wang


Solvent-in-salt electrolytes have revolutionized both aqueous and non-aqueous batteries by extending the electrochemical stability window1,2,3 and enabling new battery chemisties4-6. However, the presence of both anions and solvent in the cation solvation shell not only limits the further extension of electrochemical stability window, but also the liquidus temperature range and ionic mobility. Herein, we report a high-entropy electrolyte, characterized by completely non-solvating of active cation and fully solvating of supporting cation enabling high ionic conductivity across an ultra-wide liquidus temperature range and a wide electrochemical stability window. Similar to the concept of high entropy alloys7, in the uncharted high-entropy electrolytes, solvent and salt structures are mutually frustrated by a supporting salt at a precise concentration, providing unprecedented thermal stability and negligible thermal hysteresis. As a representative for aqueous high-entropy electrolytes, Li2ZnCl4-9H2O forms fast-exchanging anion network, [ZnCl4m-]n and enables a two-volt zinc-VOPO4 battery to charge/discharge with about 100 percent Coulombic efficiency (CE) for up to 10,000 cycles at temperatures between −80 and +80 °C by providing energy density of 131 Wh per kg at room-temperature, while retaining 80 percent of its room-temperature capacity at −80°C. Aqueous Li2ZnCl4-9H2O high-entropy electrolyte also enables zinc-air batteries at −60 °C to provide >60% of the room-temperature capacity with excellent cycling stability. The universality of high-entropy electrolytes is demonstrated by a non-aqueous magnesium ion electrolyte, enabling magnesium batteries to achieve a high performance at a low temperature.


Electrolyte structure, Rechargeable Zn-ion battery, Mg-ion battery, Low-temperature electrolyte, High-temperature electrolyte, Small Angle Neutron Scattering, Inelastic Neutron Scattering


Yang, C. , Xia, J. , Cui, C. , Pollard, T. , Vatamanu, J. , Faraone, A. , Dura, J. , Tyagi, M. , Kattan, A. , Thimsen, E. , Xu, J. , Song, W. , Hu, E. , Ji, X. , Hou, S. , Zhang, X. , Ding, M. , Hwang, S. , Su, D. , Ren, Y. , Yang, X. , Wang, H. , Borodin, O. and Wang, C. (2023), All-Temperature Zinc Batteries with High-Entropy Aqueous Electrolyte, Nature (Accessed April 23, 2024)
Created January 8, 2023, Updated March 29, 2023