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Unveiling solvation structure and desolvation dynamics of hybrid electrolytes for ultralong cyclability and facile kinetics of Zn-Al alloy anodes

Journal Article


Abstract


  • Despite the high theoretical capacity and natural abundance of Al metal anodes, the reversible and fast multivalent storage of Al3+ ions remains challenging because their large charge density leads to strong electrostatic interactions with other components and sluggish kinetics. Herein, we report the record-high plating/stripping time (>8000 h) and high rate capability of Zn-Al alloy anodes in Al3+-containing hybrid electrolytes. The more reversible Al deposition on Zn in nitrile-based hybrid electrolyte than carbonate- and amide-based hybrid and aqueous electrolytes is attributed to weak Al3+-solvent interactions and fast Al3+ transfer kinetics. In particular, these electrochemical behaviors of nitrile-based electrolyte originate from a unique solvation structure, the interrelation among H2O, organic solvents, and Al3+, and the conformational change of bound/free solvents upon desolvation, as elaborated via theoretical simulations, two-dimensional infrared correlation spectroscopy, and other characterizations. The superiority of this hybrid electrolyte was confirmed by achieving a high specific capacity (183 mA h g���1 and 1.08 mA h cm���2) and long cycling of >5000 cycles of full cells integrating Zn-Al alloy anodes (25 ��m) with vanadium dioxide/carbon nanotubes (8 mg cm���2) and activated carbon (10 mg cm���2) cathodes, respectively, which considerably exceed those of Al-based full cells.

Publication Date


  • 2022

Citation


  • Dou, Q., Yao, N., Pang, W. K., Park, Y., Xiong, P., Han, X., . . . Park, H. S. (2022). Unveiling solvation structure and desolvation dynamics of hybrid electrolytes for ultralong cyclability and facile kinetics of Zn-Al alloy anodes. Energy and Environmental Science. doi:10.1039/d2ee02453e

Scopus Eid


  • 2-s2.0-85140099522

Volume


Issue


Place Of Publication


Abstract


  • Despite the high theoretical capacity and natural abundance of Al metal anodes, the reversible and fast multivalent storage of Al3+ ions remains challenging because their large charge density leads to strong electrostatic interactions with other components and sluggish kinetics. Herein, we report the record-high plating/stripping time (>8000 h) and high rate capability of Zn-Al alloy anodes in Al3+-containing hybrid electrolytes. The more reversible Al deposition on Zn in nitrile-based hybrid electrolyte than carbonate- and amide-based hybrid and aqueous electrolytes is attributed to weak Al3+-solvent interactions and fast Al3+ transfer kinetics. In particular, these electrochemical behaviors of nitrile-based electrolyte originate from a unique solvation structure, the interrelation among H2O, organic solvents, and Al3+, and the conformational change of bound/free solvents upon desolvation, as elaborated via theoretical simulations, two-dimensional infrared correlation spectroscopy, and other characterizations. The superiority of this hybrid electrolyte was confirmed by achieving a high specific capacity (183 mA h g���1 and 1.08 mA h cm���2) and long cycling of >5000 cycles of full cells integrating Zn-Al alloy anodes (25 ��m) with vanadium dioxide/carbon nanotubes (8 mg cm���2) and activated carbon (10 mg cm���2) cathodes, respectively, which considerably exceed those of Al-based full cells.

Publication Date


  • 2022

Citation


  • Dou, Q., Yao, N., Pang, W. K., Park, Y., Xiong, P., Han, X., . . . Park, H. S. (2022). Unveiling solvation structure and desolvation dynamics of hybrid electrolytes for ultralong cyclability and facile kinetics of Zn-Al alloy anodes. Energy and Environmental Science. doi:10.1039/d2ee02453e

Scopus Eid


  • 2-s2.0-85140099522

Volume


Issue


Place Of Publication