Hu Hong, Yu Wang, Yaqin Zhang, Bing Han, Qing Li, Xun Guo, Ying Guo, Ao Chen, Zhiquan Wei, Zhaodong Huang, Yuwei Zhao, Jun Fan, Chunyi Zhi
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The as-obtained HIC solid electrolyte possesses an unprecedentedly high ionic conductivity at room and low temperatures (≈11.2 mS cm<sup>−1</sup> at 25 °C and ≈2.78 mS cm<sup>−1</sup> at −40 °C) with ultra-low activation energy (≈0.12 eV), while restraining dendrite growth and exhibiting low overpotential even at a high current density (<200 mV at 5.0 mA cm<sup>−2</sup>) during Zn symmetric cell cycling. This HIC also allows solid-state Zn||covalent organic framework full cells to work at low temperatures, providing superior stability. More importantly, the HIC can even support zinc-ion hybrid supercapacitors to work, achieving extraordinary rate capability and a power density comparable to aqueous solution-based supercapacitors. 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引用次数: 0
摘要
开发符合当前固态设备要求的新型离子导体迫在眉睫,但仍然充满挑战。氢键离子共晶体(HIC)是一种基于氢键和库仑相互作用的多组分晶体。由于氢键网络和离子晶体的独特性,氢键离子共晶体具有柔性骨架。更重要的是,其表面的阴离子空位可能有助于解离和吸附多余的阴离子,从而在晶界形成阳离子传输通道。本文证明,通过调整锌盐和咪唑的比例而优化的 HIC 可以构建基于晶界的快速 Zn2+ 传输通道。所获得的 HIC 固体电解质在室温和低温条件下具有前所未有的高离子电导率(25 °C时≈11.2 mS cm-1,-40 °C时≈2.78 mS cm-1)和超低活化能(≈0.12 eV),同时抑制了枝晶的生长,在锌对称电池循环过程中,即使在高电流密度(5.0 mA cm-2 时为 200 mV)下也能表现出低过电位。这种 HIC 还允许固态 Zn||共价有机框架全电池在低温下工作,提供了卓越的稳定性。更重要的是,HIC 甚至可以支持锌离子混合超级电容器工作,实现超常的速率能力和与基于水溶液的超级电容器相当的功率密度。这项工作为设计具有极高离子电导率和出色界面兼容性的易制备、低成本和环保型离子导体提供了一条途径。
Hydrogen-Bonded Ionic Co-Crystals for Fast Solid-State Zinc Ion Storage
The development of new ionic conductors meeting the requirements of current solid-state devices is imminent but still challenging. Hydrogen-bonded ionic co-crystals (HICs) are multi-component crystals based on hydrogen bonding and Coulombic interactions. Due to the hydrogen bond network and unique features of ionic crystals, HICs have flexible skeletons. More importantly, anion vacancies on their surface can potentially help dissociate and adsorb excess anions, forming cation transport channels at grain boundaries. Here, it is demonstrated that a HIC optimized by adjusting the ratio of zinc salt and imidazole can construct grain boundary-based fast Zn2+ transport channels. The as-obtained HIC solid electrolyte possesses an unprecedentedly high ionic conductivity at room and low temperatures (≈11.2 mS cm−1 at 25 °C and ≈2.78 mS cm−1 at −40 °C) with ultra-low activation energy (≈0.12 eV), while restraining dendrite growth and exhibiting low overpotential even at a high current density (<200 mV at 5.0 mA cm−2) during Zn symmetric cell cycling. This HIC also allows solid-state Zn||covalent organic framework full cells to work at low temperatures, providing superior stability. More importantly, the HIC can even support zinc-ion hybrid supercapacitors to work, achieving extraordinary rate capability and a power density comparable to aqueous solution-based supercapacitors. This work provides a path for designing facilely prepared, low-cost, and environmentally friendly ionic conductors with extremely high ionic conductivity and excellent interface compatibility.
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.