自支撑单壁碳纳米管薄膜的连续制备、结构和性能研究

Carbon nanotube (CNT) film has irreplaceable advantage in applications, but the current commercial CNT is provided mostly in powder form. Although several research groups have realized the batch preparation of free-standing multi-walled carbon nanotube (MWCNT) films by indirect methods, it is still difficult to prepare free-standing CNT films directly in batch. This has become one of the key bottlenecks to obstacle the research and application of CNTs. Since single-walled carbon nanotubes (SWCNTs) are better than MWCNTs in electrical and mechanical properties, it is a long-cherished wish of CNT researchers to succeed in fabricating free-standing SWCNT films continuously. Based on the experimental conditions of directly growing high conductivity and high strength SWCNT thin film and the practical experience of direct and continuous preparation of carbon nanotube fibers, we will explore an effective, low cost and easy scale-up approach to synthesize directly continuous free-standing SWCNT films. By this project, a new method is expected to be established, and the related technique procedure and experimental apparatus will be designed. The mechanism of free-standing and continuous growth of SWCNT films will be unveiled by investigating the effects of various experimental parameters on the continuous preparation of the free-standing film. Batch, direct and continuous preparation of free-standing SWCNT film will be realized via controlling and optimizing various influence factors. The structural characteristics and physical properties of as-prepared films will be studied, and the functional features and potential application value of the SWCNT films will be examined, in order to promote the research and development of carbon nanotubes.

目前商用碳纳米管主要基于粉末状原料，而薄膜状碳纳米管有其不可替代的优势。虽然有几个课题组用间接法实现了批量制备自支撑多壁碳纳米管薄膜，但是，仍难以批量直接制备自支撑的碳纳米管薄膜，已成为阻碍碳纳米管研究和应用的一个关键瓶颈。单壁碳纳米管的电学性质和力学性质均优于多壁碳纳米管，连续制备自支撑单壁碳纳米管薄膜是研究者梦寐以求的一个夙愿。本申请项目拟以本课题组已具有的高导电、高强度单壁碳管薄膜的制备工艺条件为基础，结合已实现连续直接制备碳纳米管纤维的经验，探索一个有效的、低成本、易扩量化的制备途径；建立连续直接制备自支撑单壁碳管薄膜的方法，设计工艺和实验装置；探索各种实验参数对实现自支撑单壁碳管薄膜的连续制备的影响，弄清其自支撑且连续生长的机制；调控和优化各种影响因素，实现批量直接连续制备；研究这种自支撑薄膜的结构特征和物理性质；进而揭示其功能特性和潜在应用价值，推动碳纳米管的研发。

连续且直接制备自支撑的单壁碳纳米管薄膜至今仍是一个艰巨的挑战。这种现状严重阻碍了碳纳米管薄膜的研发和产业化进程。本项目研究团队围绕项目研究目标开展研究工作，由于研究内容的挑战性和紧迫性，促使我们全力攻关，在立项当年就集中大量的时间探索实验方法和建立实验装置，取得了突破性进展，能够连续制备出自支撑碳纳米管薄膜，大大加快了本项目的研究进程。.重点理清了单壁碳纳米管从气相生长到形成均匀薄膜的过程和机制，详尽研究了单壁碳纳米管从气相生长到形成薄膜再到牵引薄膜的各个过程的诸多工艺参数和实验条件对产物形貌、结构和性能的影响，解决各个阶段的全程匹配等技术难点和关键科学问题。成功建立了高效、低成本、易规模化、连续制备自支撑单壁碳纳米管薄膜的方法。.设计和搭建了两套不同规格的实验装置，均实现了各个过程诸多工艺参数和实验条件的匹配和优化，得到稳定性和重复性佳的工艺条件，验证了所提出的技术方案的普适性。调控实验条件，实现了自支撑单壁、双壁或者多壁碳纳米管薄膜的连续制备。批量直接制备连续薄膜的生长速率可>100米/小时。提供了连续收集方法和装置。.自支撑单壁碳纳米管网络薄膜的连续制备，为深入和拓展碳纳米管薄膜的基础和应用基础研究提供了充足的保障。使我们摆脱了原位局域生长的碳纳米管网络薄膜在量产、尺寸拓展、性能提高和制备效率上的困扰，不仅在性能研究，而且在宏观尺度碳纳米结构复合材料、柔性可拉伸超级电容器、人工肌肉、太阳能电池、可拉伸应变传感器、热电模块等研究中均取得重要研究进展。.全面且超额完成了预期研究计划，取得若干自主创新性的重要研究结果。在Nat. Commun.、Adv. Mater.、Adv. Energy Mater.、Nano Energy、Small、Nanoscale等重要学术刊物上已发表SCI收录论文16篇，其中应邀撰写综述1篇。68.75%的论文发表在影响因子7.0以上的刊物。申请发明专利14项。国际国内学术会议邀请报告7人次。通过本项目的实施，培养博士毕业生8名，硕士毕业生1名。