单层氢氧化物纳米片/石墨烯复合多层膜的制备及性能研究

Unilamellar hydroxide nanosheets, with a molecular-level thickness of about 1 nm versus two-dimensional (2D) lateral size ranging from submicrometer to several tens of micrometers, can be regarded as a new and very important class of inorganic functional materials. Unilamellar hydroxide nanosheets can also be viewed as inorganic macromolecules, and serve either as an ideal quantum system for fundamental study or as a basic building block for superlattice-like molecular-scale assembly to prepare functional nanofilms with high quality. This work aims to explore and develop the novel synthesis route of the new-type layered hydroxides, particularly the controlled synthesis of layered transition-metal hydroxides; to prepare unilamellar hydroxide nanosheet with specific composition and function through chemical exfoliation of the new-type layered hydroxide; to fabricate functional nanofilms with high quality based on layer-by-layer (LBL) self-assembly and/or Langmuir-Blodgett (LB) technique in molecule scale; particularly to integrate unilamellar hydroxide nanosheet with graphene (high specific surface area and high conductivity) for composite multilayer, which will be used for the development of a new-type electrochemical supercapacitor with high energy density and power density, achieving new breakthroughs in energy conversion technologies; to reveal the assembly rules and the basic principles of unilamellar hydroxide nanosheet for the design and preparation of the new-type unilamellar hydroxide nanosheet-based functional nanofilms. The work will be expected to promote our scientific research level on the chemical exfoliation, and molecular-scale assembly of unilamellar hydroxide nanosheets and form a cutting-edge research area both scientifically and internationally competitive.

单层氢氧化物纳米片是一类新型无机功能材料，厚度约1 nm，具有分子水平的二维尺度，可被看作"无机高分子"，既可作为研究量子物理属性的模型体系，也可作为组装基元进行超晶格结构的分子尺度组装，制备高品质功能薄膜。本工作旨在探索与发展新型层状氢氧化物控制合成的新方法，通过化学剥离制备具有特定组成及功能的单层氢氧化物纳米片；采用逐层自组装及Langmuir-Blodgett（LB）技术，实现高品质单层氢氧化物纳米片基功能薄膜的可控制备，尤其单层氢氧化物纳米片/石墨烯（Graphene）复合多层膜的制备，进而开发出具有高能量密度和功率密度的新型超级电容器，实现能量转换技术的新突破；揭示单层氢氧化物纳米片的组装规律和基本原理，为新型单层氢氧化物纳米片基功能薄膜的设计和制备提供实验与理论基础。该工作有助于提升我国在单层氢氧化物纳米片的化学剥离制备及分子尺度组装领域的科学研究水平，形成研究优势和国际影响。

本项目开展以来，我们探索与发展新型层状氢氧化物控制合成的新方法，特别利用油浴的合成方法有望实现了层状氢氧化物管锥状结构材料的大尺度制备。发展了新型化学剥离方法，实现了单层氢氧化物纳米片的可控制备。研究发现，带正电荷的单层氢氧化物纳米片与带负电荷的石墨烯（Graphene）通过静电自组装可形成超晶格结构复合材料。超晶格结构复合功能材料具有较高的电化学性能,该方面的研究为新型单层氢氧化物纳米片基功能薄膜的设计和制备提供实验与理论基础。在国家自科基金的资助下，课题负责人以第一作者或通讯作者发表研究论文20篇（SCI），其中在Advanced Functional Materials发表论文2篇（IF=12.124），ACS NANO发表论文1篇（IF=13.942），其中一篇论文入选ESI千分之一论文；申请国家发明专利4项，其中获授权发明专2项，出版英文专著1部，获湖南省自然科学奖二等奖1项。