新型磷烯异质结构及其储锂/钠增强机理研究

Owing to unique structure, anisotropy and abnormal interface synergetic effect, the doped phosphorene heterostructures have great potential in high-performance anodes for lithium/sodium ion batteries (LIBs and SIBs). However, the investigations are still in their infancy and there still exist many problems associated with physical mechanisms of enhanced energy storage in the designed heterostructures. In this project, we will design and construct phosphorene heterostructures by coupling it with 0D, 1D or 2D quantum structures. The adsorption, migration/diffusion and insertion/extraction of lithium/sodium ions in the vdW phosphorene heterostructures are calculated to reveal the underlying physical mechanisms. The structural and doping effect on the storage performances are further investigated for impurity doped vdW phosphorene heterostructure as anodes materials. Based on the theoretical results of doped phosphorene vdW heterostructure, we will prepare high-quality doped phosphorene via ion implantation technique, and then fabricate doped phosphorene vdW heterostructure composites through self-assembly technique. The Li/Na storage performances for phosphorene vdW heterostructure as anodes materials are measured. Our results provide theoretical guidance and technical support for novel heterostructure composite for high-performance LIBs and SIBs.

由于具有结构增强、各向异性和界面协同效应，掺杂磷烯异质结构在高性能锂/钠离子电池负极方面具有巨大的应用前景，引起了人们的极大关注。针对磷烯异质结构设计及掺杂增强储能中存在的诸多问题，本项目以不同维度(0D,1D,2D)量子结构为复合对象，系统分析弱范德瓦尔斯力耦合异质结构的结构特性和电子输运性质，探索其作为锂/钠电池负极的离子吸附、迁移和扩散规律以及嵌入/脱出机制，揭示2D+nD(n=0,1或2) vdW异质结构和掺杂对磷烯协同增强储锂/钠性能的调控规律。在vdW异质结构与掺杂调控理论设计基础上，利用离子注入技术制备高质量掺杂磷烯，并通过自组装工艺制备掺杂磷烯vdW异质结构材料，系统探索高效磷烯vdW异质结构电池负极的实现路径与构效关系。本项目将为新型高性能锂/钠离子电池负极材料的研发提供理论指导和技术支撑。

由于独特的结构增强和界面协同效应，以范德瓦尔斯异质结构为代表的异相杂化材料在高性能锂/钠离子电池负极方面具有巨大的应用前景。本项目针对异相杂化材料负极的结构稳定性、输运动力学协同等关键问题，以磷烯等二维体系和过渡金属化合物为主要研究对象，通过微纳结构设计、掺杂、缺陷和异质结调控等方式，在异相杂化材料设计与输运性质、储锂/钠增强机制及电化学性能调控三个方面开展了较为系统的研究工作。提出利用异质界面增强磷烯储锂/钠性能的思路，探索了缺陷、掺杂及异质结构设计对界面载流子传输和离子嵌入/脱出的调控规律。设计并构建磷烯/石墨烯、磷烯/C3N等二维范德瓦尔斯异质结构，揭示了新型异质结构通过载流子输运与结构稳定性协同提升增强电极储锂/钠性能的微观机制。构筑了石墨烯/磷烯纳米点、FeP2/P/C等磷基异相杂化材料以及一系列中空微纳结构异相杂化材料和自支撑纳米复合材料电极，结合第一性原理计算和非原位实验表征揭示了异相杂化策略增强储锂/钠性能的重要机制和规律，设计与制备的系列高性能电极材料为实际应用打下了良好的基础。研究成果已在ACS. Appl. Mater. Interface, Chem. Eng. J., J. Power Sources, Electrochim. Acta等国际期刊发表标注论文近30篇, 授权国家发明专利1项, 培养博士生4名及硕士毕业生8名。