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Excluding the Trouble from Interfacial Water by Covalent Organic Polymer to Realize Extremely Reversible Zn Anode
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-05-24 , DOI: 10.1002/adfm.202302293 Xuyan Ni 1 , Jinqiu Zhou 2 , Haoqing Ji 3 , Yuejiao Chen 1 , Huaming Yu 1 , Yiwei Zheng 3 , Tao Qian 2, 4 , Mengfan Wang 3 , Libao Chen 1 , Chenglin Yan 3, 4
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-05-24 , DOI: 10.1002/adfm.202302293 Xuyan Ni 1 , Jinqiu Zhou 2 , Haoqing Ji 3 , Yuejiao Chen 1 , Huaming Yu 1 , Yiwei Zheng 3 , Tao Qian 2, 4 , Mengfan Wang 3 , Libao Chen 1 , Chenglin Yan 3, 4
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The side reactions related to water are the major issue hindering practical application of Zn metal batteries. To exclude the trouble from interfacial water, a covalent organic polymer (COP) layer with N, N′-Bis(salicylidene)ethylenediamine structure is designed, whose strong coordination ability with Zn2+ enhances the de-solvation kinetics of solvated Zn2+ which is conducive to interfacial water removal thus alleviating the side reactions related to water. This function has been certified by density functional theory along with molecular dynamics analysis. Moreover, measurements including in situ electrochemical gas chromatography, in situ optical microscopy, in situ X-ray diffraction and in situ Raman spectroscopy verify the weakened side reactions (including hydrogen evolution and corrosion) along with homogenous Zn deposition contributed from the covalent organic polymer layer. Benefiting from these merits, when assemble into cells based on common ZnSO4-based aqueous electrolyte, the COP layer-decorated anode exhibits excellent electrochemical performance of a high average Coulombic efficiency value 99.5% at a high capacity of 5.0 mA h cm−2. What's more, the symmetric cells can operate at −20 °C and the full cell with N/P ratio as low as 1.2 can cycle stably for 100 cycles, which would carry forward the promising practical application of Zn metal batteries.
中文翻译：
共价有机聚合物排除界面水困扰实现极可逆锌阳极
与水相关的副反应是阻碍锌金属电池实际应用的主要问题。为了排除界面水的问题，设计了具有N,N'-双(水杨基)乙二胺结构的共价有机聚合物(COP)层，其与Zn 2+ 的强配位能力增强了溶剂化Zn 2+ 的去溶剂化动力学有利于界面水的去除，从而减轻与水有关的副反应。该函数已得到密度泛函理论和分子动力学分析的验证。此外，包括原位电化学气相色谱、原位光学显微镜、原位 X 射线衍射和原位拉曼光谱在内的测量验证了副反应（包括析氢和腐蚀）的减弱以及共价有机聚合物层贡献的均匀锌沉积。受益于这些优点，当组装成基于普通ZnSO 4基水性电解质的电池时，COP层装饰的阳极表现出优异的电化学性能，在5.0 mA h cm -2 的高容量下平均库仑效率高达99.5% 。。此外，对称电池可以在-20℃下工作，N/P比低至1.2的全电池可以稳定循环100次，这将推动锌金属电池的实际应用。
更新日期：2023-05-24
中文翻译：
共价有机聚合物排除界面水困扰实现极可逆锌阳极
与水相关的副反应是阻碍锌金属电池实际应用的主要问题。为了排除界面水的问题，设计了具有N,N'-双(水杨基)乙二胺结构的共价有机聚合物(COP)层，其与Zn 2+ 的强配位能力增强了溶剂化Zn 2+ 的去溶剂化动力学有利于界面水的去除，从而减轻与水有关的副反应。该函数已得到密度泛函理论和分子动力学分析的验证。此外，包括原位电化学气相色谱、原位光学显微镜、原位 X 射线衍射和原位拉曼光谱在内的测量验证了副反应（包括析氢和腐蚀）的减弱以及共价有机聚合物层贡献的均匀锌沉积。受益于这些优点，当组装成基于普通ZnSO 4基水性电解质的电池时，COP层装饰的阳极表现出优异的电化学性能，在5.0 mA h cm -2 的高容量下平均库仑效率高达99.5% 。。此外，对称电池可以在-20℃下工作，N/P比低至1.2的全电池可以稳定循环100次，这将推动锌金属电池的实际应用。
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