Abstract
The pursuit of high-mileage models results in the recurrence of lithium metal batteries (LMBs) to researchers’ horizon. However, the lithium (Li) metal anode for LMBs undergoes the uncontrollable formation of Li dendrites and infinite volume change during cycling, impeding its practical application. To overcome these challenges, we developed a metal-organic framework (MOF)-derived pathway to construct lithiophilic three-dimensional (3D) skeleton using different substrates (e.g., carbon cloth (CC) and Cu mesh) for dendrite-free lithium metal anodes. As a typical example, the MOF-derived ZnO/nitrogen-doped carbon (NC) nanosheet-modified 3D CC was well-constructed as a lithiophilic hierarchical host (CC@ZnO/NC@Li) for molten Li infiltration. Benefiting from the lithiophilic N-functional groups and LiZn alloy, the synthesized CC@ZnO/NC@Li composite anode promoted the uniform distribution of Li, resulting in a dendrite-free morphology. Meanwhile, the 3D conductive carbon skeleton enhanced the reaction kinetics and buffered the volume change of the electrode. The CC@ZnO/NC@Li composite anode presented a prolonged lifespan of over 1000 cycles at 5 mA cm−2 with a low overpotential of 19 mV. Coupled with a LiFePO4 cathode, the CC@ZnO/NC@Li composite anode also exhibited superior electrochemical properties in the full-cell system. This versatile strategy may open up the channel of designing multi-functional lithiophilic 3D hosts for the Li metal anode.
摘要
对高续航里程车型的追求使锂金属电池(LMBs)再次引起研究人 员的关注. 然而, 锂金属负极在循环过程中会出现不可控的锂枝晶形成 和无限大的体积变化, 阻碍了其实际应用. 为了解决这些棘手问题, 本 文采用一种金属有机框架(MOF)衍生路线, 在不同的基底(如碳布和铜 网)上通用地构建出亲锂三维骨架, 以实现无枝晶锂金属负极. 作为一 个典型的例子. MOF衍生的ZnO/NC(氮掺杂碳)纳米片修饰的三维碳布 (CC)被较好地构建为亲锂宿主, 用于灌注熔融锂(标记为CC@ZnO/NC@Li). 得益于亲锂的N官能团和LiZn合金, 制备的CC@ZnO/NC@Li 复合负极极大地促进了锂的均匀分布, 使电极呈现为无枝晶形貌. 同时, 三维导电碳骨架可增强反应动力学并缓冲电极的体积变化. 因此, CC@ZnO/NC@Li复合负极具有延长的循环寿命, 可在5 mA cm−2下以 19 mV的低过电位稳定循环超过1000次. 与LiFePO4正极相匹配时, CC@ZnO/NC@Li复合负极在全电池系统中也表现出了优异的电化学 性能. 这种通用策略可为设计金属锂的多功能亲锂性三维宿主拓宽途 径.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (51771076 and 51621001), Guangdong “Pearl River Talents Plan” (2017GC010218), the R&D Program in Key Areas of Guangdong Province (2020B0101030005), and Guangdong Basic and Applied Basic Research Foundation (2020B1515120049).
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Author contributions Zeng L and Zhou T designed the samples and performed the experiments; Zeng L and Xu X wrote the manuscript; Li F and Zhang D were involved in the discussion and writing of the manuscript; Shen J assisted with the drawing of the flow chart. Liu J and Zhu M directed the project.
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Liyan Zeng received her bachelor’s degree from the Northeastern University in 2018. She is currently a postgraduate student under the supervision of Prof. Jun Liu at the South China University of Technology (SCUT). Her research interests are electrode materials for sodium-ion batteries and lithium metal anode batteries.
Jun Liu is a professor of material science and engineering at SCUT. He received his PhD degree in chemical engineering and technology at Dalian University of Technology in 2011. His current research interests mainly include high-energy density Li/Na-ion batteries, all-solid-state batteries, lithium sulfur batteries, and novel energy devices.
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General construction of lithiophilic 3D skeleton for dendrite-free lithium metal anode via a versatile MOF-derived route
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Zeng, L., Zhou, T., Xu, X. et al. General construction of lithiophilic 3D skeleton for dendrite-free lithium metal anode via a versatile MOF-derived route. Sci. China Mater. 65, 337–348 (2022). https://doi.org/10.1007/s40843-021-1764-x
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DOI: https://doi.org/10.1007/s40843-021-1764-x