Unraveling the Solvation Structure and Electrolyte Interface through Carbonyl Chemistry for Durable and Dendrite-Free Zn Anode |
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Authors: | Heng Cao Xiaoqin Zhang Bin Xie Xiaomin Huang Fengyu Xie Yu Huo Qiaoji Zheng Ruyi Zhao Qiang Hu Ling Kang Shude Liu Dunmin Lin |
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Affiliation: | 1. College of Chemistry and Materials Science, Sichuan Normal University, Chengdu, 610066 P. R. China;2. School of Energy Science and Engineering, Harbin Institute of Technology, Harbin, 150001 P. R. China;3. School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 610054 P. R. China;4. Shanghai Key Laboratory of Multidimensional Information Processing, East China Normal University, 500 Dongchuan Road, Shanghai, 200241 P. R. China;5. College of Textiles, Donghua University, Shanghai, 201620 P. R. China |
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Abstract: | Aqueous Zn ion batteries are appealing systems owing to their safety, low cost, and environmental friendliness; however, their practical applicability is impeded by the growth of Zn dendrites and side reactions. Herein, a dual-functional electrolyte additive, namely acetylacetone (AT) is utilized for the simultaneous regulation of the solventized structure and anode–electrolyte interface (AEI) to achieve a durable, dendrite-free Zn anode. Theoretical calculations and experimental characterizations reveal that the AT molecule can be adsorbed onto Zn metal surface to reconstruct the AEI and allow for the primordial desolvation of [Zn(H2O)6]2+ at locations away from the surface of the Zn anode during deposition, which is attributed to the strong polarity of the carbonyl functional group. In addition, the two carbonyls of AT can replace two H2O molecules in the primary solventized structure of Zn2+ to reduce the number of active H2O molecules, efficiently suppressing Zn dendrite growth and detrimental reactions. As a proof of concept, a Zn//Cu cell is constructed in ZnSO4 containing 3 vol.% AT electrolyte, delivering stable cycling over 1800 cycles while maintaining a high Coulombic efficiency of 99.74%. This study provides a practical approach for inhibiting dendrite growth and side reactions by harnessing carbonyl chemistry. |
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Keywords: | acetylacetone anode–electrolyte interface aqueous Zn ion batteries electrolyte additives Zn dendrites |
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