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Regulating the Inner Helmholtz Plane with a High Donor Additive for Efficient Anode Reversibility in Aqueous Zn-Ion Batteries |
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| Authors: | Jinrong Luo Liang Xu Yijing Zhou Tianran Yan Yanyan Shao Dongzi Yang Liang Zhang Zhou Xia Tianheng Wang Prof Liang Zhang Prof Tao Cheng Prof Yuanlong Shao |
| Institution: | 1. College of Energy Soochow Institute for Energy and Materials Innovations (SIEMIS), Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, 215006 P. R. China
These authors contributed equally to this work.;2. Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou, 215123 P. R. China These authors contributed equally to this work.;3. College of Energy Soochow Institute for Energy and Materials Innovations (SIEMIS), Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, 215006 P. R. China;4. Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou, 215123 P. R. China;5. School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing, 210094 P. R. China;6. School of Materials Science and Engineering, Peking University, Beijing, 100871 P. R. China |
| Abstract: | The performance of aqueous Zn ion batteries (AZIBs) is highly dependent on inner Helmholtz plane (IHP) chemistry. Notorious parasitic reactions containing hydrogen evolution reactions (HER) and Zn dendrites both originate from abundant free H2O and random Zn deposition inside active IHP. Here, we report a universal high donor number (DN) additive pyridine (Py) with only 1 vol. % addition (Py-to-H2O volume ratio), for regulating molecule distribution inside IHP. Density functional theory (DFT) calculations and molecular dynamics (MD) simulation verify that incorporated Py additive could tailor Zn2+ solvation sheath and exclude H2O molecules from IHP effectively, which is in favor of preventing H2O decomposition. Consequently, even at extreme conditions such as high depth of discharge (DOD) of 80 %, the symmetric cell based on Py additive can sustain approximately 500 h long-term stability. This efficient strategy with high DN additives furnishes a promising direction for designing novel electrolytes and promoting the practical application of AZIBs, despite inevitably introducing trace organic additives. |
| Keywords: | Donor Number Inner Helmholtz Plane Solvation Sheath Zn Anode Zn Utilization Rate |