高能二次电池用纳米管阵列限域金属Li阳极(Cu/TiO2@Li/MOF)的 构筑与性能调控

Lithium metal characterized with extremely high capacity and low negative electrochemical potential has been the key anode materials for high energy secondary batteries. However, its application is restricted due to the dendrite growth that results in low Coulombic efficiency, short cycle life and high safety risks of the batteries. In this project, a novel Cu/TiO2@Li/MOF anode is designed to solve this problem. By adjusting the orientation and structure of metallic Li in the Cu/TiO2 nanotubes coordinated with MOF based quasi-solid polymer electrolyte that has high Li+ transfer capability and excellent compatibility with Cu/TiO2@Li, the growth of metallic Li dendrite in charging and discharging process will be inhibited. With managing the TiO2 nanotube construction and the MOF coating structure, the electrode reversible regulation will be established and the process kinetics of the anode will be identified. In addition, the interaction mechanism of the electrolyte with the Cu/TiO2@Li/MOF anode as well as the compatibility between the anode and the cathode materials having high energy density, such as LiCo0.8Ni0.1Mn0.1O2, LiNi0.5Mn1.5O4, S, O2, will be investigated. Based on the anode technology prototype and intellectual property, this project will provide the theoretical and technical support for high energy secondary battery development.

金属Li阳极具有高比容与低电位的突出优势，是突破二次电池能量密度瓶颈的关键电极材料之一。本项目针对金属Li阳极一直存在Li枝晶生长并导致低库伦效率、短循环寿命与高安全风险这一核心问题，提出并构筑（Cu/TiO2@Li/MOF）新型阳极，通过Cu/TiO2纳米管整列中金属Li定向生长与结构调控，利用MOF类固体电解质高导Li+能力及其对Cu/TiO2@Li纳米管整列的高强复合，解决充放电过程中Li枝晶生长难题；阐明新型阳极电极过程动力学，从电解液组成、TiO2纳米管结构与MOF涂层结构等方面，建立新型阳极电极过程可逆调控方法；研究新型阳极适配电解液，揭示新型阳极与LiCo0.8Ni0.1Mn0.1O2、LiNi0.5Mn1.5O4、S和O2等高比能阴极的交互作用机制，形成基于新型阳极的高能锂二次电池技术原型与知识产权体系，为高能锂二次电池发展提供理论与技术支撑，并为其他金属二次电池提供借鉴。

金属Li阳极具有高比容与低电位的突出优势，是突破二次电池能量密度瓶颈的关键电极材料之一。本项目针对金属Li阳极一直存在Li枝晶生长并导致低库伦效率、短循环寿命与高安全风险这一核心问题，构筑了开放式改性碳纸电极和泡沫金属电极、半限域式层次孔炭和Al2O3纳米管电极以及全限域式中空炭纳米球电极，逐步实现了锂沉积/溶解行为的可控化，实现了高库伦效率和高循环稳定性的兼得。通过系列表征数据解释和分析了不同结构3D负极的锂沉积/溶解行为，并探究了其半电池和全电池的电化学性能。形成了基于新型限域式碳基阳极的高能锂二次电池技术原型与知识产权体系，为高能锂二次电池发展提供了理论与技术支撑。