插层结构水滑石阵列的合成及超电容性能研究

The depletion of traditional energy resources as well as global warming evoke considerable attention in developing advanced energy-storage and delivery systems. Electrochemical capacitors (also known as supercapacitors or ultracapacitors), as emerging energy storage devices, have attracted intensive interest due to their high power density, long cycle life, short charging time and good safety record.The rational design of novel electrode based on structural and compositional considerations is highly essential for achieving high-performance supercapacitors. Transition metal-containing layered double hydroxides (LDHs), are promising pseudocapacitive materials owing to their high redox activity, low cost and environmentally friendly nature. This project focuses on the fabrication of high-performance supercapacitor materials based on intercalated LDHs arry and intends to demonstrate the relationship between the structure and performance of the obtained materials. The resulting new type of electrode would possess the following advantages: (i) the well-arrayed electroactive material provides large specific surface area for the redox reaction as well as effective pathway for fast electron transport between electroactive center and current collector; (ii) the enhanced conductivity of the electrode reduces the interfacial resistance, which consequently accelerates electron transfer at high charge-discharge current density; (iii) the feasible design strategy guarantees facile manipulation and long-term stability of energy storage devices. The design strategy for highly oriented array electrode presented in this project can be generalized to the fabrication of other heterogeneous nanocomposite structure based on hydroxides/oxides for the purpose of obtaining high-performance supercapacitors.

超级电容器作为一种新型的储能器件，因其功率密度高、循环寿命长、绿色环保等优点，已广泛应用于工业大型UPS电源系统、电动汽车及航空航天等领域。发展具有大容量、高能量密度、高稳定性的电极材料是超级电容器研究领域的关键问题。含过渡金属（如Mn、Fe、Co、Ni等）的水滑石类层状材料（LDHs），具有较高的比表面积和电化学活性，是极具发展前景的一类超电容材料。本项目以构筑高性能水滑石基超电容材料为研究目标，围绕此类电极材料的结构设计、制备规律、结构与电化学性能的强化开展基础和应用基础研究。通过调变材料的化学组成、结构和主客体协同作用，研究电解质在电极材料中的传质动力学、电子的传导机制，及其对电极材料电化学性能的影响。通过解决此类超电容材料的可控组装和储能性能中的关键科学问题，构筑具有特色的研究体系，为高性能超级电容器电极材料的结构设计和性能调控提供实验基础和有益探索。

含过渡金属（如Mn、Fe、Co、Ni等）的水滑石（LDHs）类层状材料，具有较高的比表面积和电化学活性，且对环境友好、容易合成，是极具发展前景的一类超电容材料。基于含过渡金属LDHs类层状化合物的电化学活性及其结构和组成的可调控性，本项目围绕LDHs插层结构纳米片阵列的结构设计、可控制备和功能强化开展了如下研究工作：.（1）插层结构设计：以几何匹配、电荷密度匹配为指导原则，设计了多种阴离子插层及不同导电物种表面修饰的LDH基杂化阵列结构电极材料。.（2）发展了多种插层结构组装方法：采用原位聚合、拓扑转变、重构组装等多种制备方法，获得了片层垂直于基底取向的LDH阵列结构，并对其组成、形貌等进行了调控。.（3）以电化学储能性能为导向，实现了功能强化：通过调控材料的化学组成、插层结构和主客体相互作用，对电子的传导及电解质的传递动力学进行了优化，显著提升了电极材料的储能性能，获得了几类性能优异的超电容材料。. 项目执行期间，在Angew. Chem. Int. Ed.、Adv. Funct. Mater.、Small等刊物发表SCI论文7篇（IF均大于6.0），申请国家发明专利6项（获授权1项）；参与撰写专著两部（含一部英文专著）。项目负责人获得2013年全国优秀博士论文提名；获得2016年“北京市科技新星”计划资助；获得2016年中国科协“青年人才托举工程”项目资助；获得2015年中国石油和化学工业联合会颁发的科技进步一等奖（排名第11）。