Xiao Tang1, Dong Zhou2, Bao Zhang3,4, Shijian Wang1, Peng Li5, Hao Liu1, Xin Guo1, Pauline Jaumaux1, Xiaochun Gao1, Yongzhu Fu6, Chengyin Wang7, Chunsheng Wang8, Guoxiu Wang9. 1. Centre for Clean Energy Technology, Faculty of Science, University of Technology Sydney, Sydney, NSW, Australia. 2. Centre for Clean Energy Technology, Faculty of Science, University of Technology Sydney, Sydney, NSW, Australia. zhoudong087@gmail.com. 3. Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA. 4. School of Optical and Electronic Information, Huazhong University of Science and Technology, Wuhan, PR China. 5. College of Material Science and Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing, PR China. 6. College of Chemistry and Molecular Engineering, Zhengzhou University, Zhengzhou, China. 7. College of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, China. 8. Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA. Cswang@umd.edu. 9. Centre for Clean Energy Technology, Faculty of Science, University of Technology Sydney, Sydney, NSW, Australia. Guoxiu.Wang@uts.edu.au.
Abstract
Rechargeable multivalent metal (e.g., Ca, Mg or, Al) batteries are ideal candidates for large-scale electrochemical energy storage due to their intrinsic low cost. However, their practical application is hampered by the low electrochemical reversibility, dendrite growth at the metal anodes, sluggish multivalent-ion kinetics in metal oxide cathodes and, poor electrode compatibility with non-aqueous organic-based electrolytes. To circumvent these issues, here we report various aqueous multivalent-ion batteries comprising of concentrated aqueous gel electrolytes, sulfur-containing anodes and, high-voltage metal oxide cathodes as alternative systems to the non-aqueous multivalent metal batteries. This rationally designed aqueous battery chemistry enables satisfactory specific energy, favorable reversibility and improved safety. As a demonstration model, we report a room-temperature calcium-ion/sulfur| |metal oxide full cell with a specific energy of 110 Wh kg-1 and remarkable cycling stability. Molecular dynamics modeling and experimental investigations reveal that the side reactions could be significantly restrained through the suppressed water activity and formation of a protective inorganic solid electrolyte interphase. The unique redox chemistry of the multivalent-ion system is also demonstrated for aqueous magnesium-ion/sulfur||metal oxide and aluminum-ion/sulfur||metal oxide full cells.
Rechargeable multivalent n class="Chemical">metal (e.g., Ca, Mg or, Al) batteries are ideal candidates for large-scale electrochemical energy storage due to their intrinsic low cost. However, their practical application is hampered by the low electrochemical reversibility, dendrite growth at the metal anodes, sluggish multivalent-ion kinetics in metal oxide cathodes and, poor electrode compatibility with non-aqueous organic-based electrolytes. To circumvent these issues, here we report various aqueous multivalent-ion batteries comprising of concentrated aqueous gel electrolytes, sulfur-containing anodes and, high-voltage metal oxide cathodes as alternative systems to the non-aqueous multivalent metalbatteries. This rationally designed aqueous battery chemistry enables satisfactory specific energy, favorable reversibility and improved safety. As a demonstration model, we report a room-temperature calcium-ion/sulfur| |metal oxide full cell with a specific energy of 110 Wh kg-1 and remarkable cycling stability. Molecular dynamics modeling and experimental investigations reveal that the side reactions could be significantly restrained through the suppressed water activity and formation of a protective inorganic solid electrolyte interphase. The unique redox chemistry of the multivalent-ion system is also demonstrated for aqueous magnesium-ion/sulfur||metal oxide and aluminum-ion/sulfur||metal oxide full cells.
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