摘要
纳米发电机有望能解决纳米技术中能源供应这一极其重要的问题,它使得纳米器件的能量供给系统与工作系统同时都能达到纳米量级,从而保持了自备电源的完整性和纳米器件系统的微型化等特点。它不仅为实现整个纳米器件工作系统的真正小型化奠定了理论基础,同时还能有效地收集自然界中甚至生物体内广泛存在却又一直被忽略的微量机械能来满足纳米器件正常运转所需的能量,这些能量的回收过程将有力地推动纳米技术的继续发展,其本身也有重大的应用前景。
目前所报道的纳米发电机以压电式为主,通过ZnO纳米材料特有的半导体性质和压电效应的耦合实现了电荷的产生、分离、累积和输运,从而将机械能转化为电能,这种发电机的可动部件多,容易导致器件的稳定性问题。因此,有必要开发出一种新型的、稳定性好的纳米发电机来有效地收集环境中被忽视的振动能,从而拓宽纳米发电机的应用范围。本文旨在通过对静电式纳米发电机的开发、优化而实现振动能的收集和电能的输出。本论文的主要内容包括以下几个方面：
(1)硅纳米线作为一种重要的一维半导体材料,由于其独特的电学和力学性能以及能与现代半导体技术和硅工业相兼容等特点而能够被广泛应用于化学催化、生物传感、电子器件和新能源等多个领域。我们通过改进的氧化物辅助生长法制备的硅纳米线中含有-石英,并通过实验进一步深入地探讨了这种良好的压电材料的形成机理。由于-石英的存在使所制备的硅纳米线表现出极好的驻极体效应,基于它而开发的纳米发电机的输出电流为2.8nA,转化率为2.2%。由此开辟了硅纳米线在微能源方面的新应用。
(2)氧化石墨烯由于其表面的含氧官能团的存在,使其性质与石墨烯相比,有很大的不同。在一个氧化石墨烯片上,存在有孤立的石墨烯“小区域”,这些“小区域”的尺寸只有几个纳米而且被无定形的含氧官能团包围着。所以,电荷很容易被储存在这些量子化水平的石墨烯中,或者很容易被电负性较高的含氧基团捕获在无定形的介质层上而使其带有静电。由这种带静电的氧化石墨烯膜组装成的柔性纳米发电机的输出电流高达3.23nA,能量转化效率为12.1%。更重要的是,所制备的纳米发电机的输出电流高度依赖于制备过程中的pH值,因而可用于纳米发电机制备过程的优化。
(3)氮化硼纳米片也是一种理想的具有蜂窝状的二维结构,石墨烯结构中的碳由sp2杂化结合形成的网状结构被硼原子和氮原子交替取代了,但与石墨烯良好的导电性相反的是,氮化硼并不导电,其禁带宽度为5.3-5.9eV。我们用化学法在高温条件下所制备的氮化硼纳米片因带有一定量的电荷而能将其运用于纳米发电机的开发。所制备的纳米发电机在外加1MΩ负载的情况下输出的平均电流为0.95nA,充分说明了器件的实用性。
(4)以碳纳米管为原料,用高温高压催化法制备的纳米金刚石表面比同条件下石墨为碳源的金刚石表面有较多的含氧官能团。这些含氧官能团能够使纳米金刚石在水中分散均匀,形成稳定的悬浮液,同时增加了对生物材料多巴胺的结合力。将这种纳米金刚石进行进一步的表面的修饰,有望突破其在纳米发电机领域的新应用。
The invention of nanogenerators provides a potential strategy to solve the critical problem of energy supplying in nanotechnology. Due to the presence of nanogenerators, the system of energy supplying and processing in nanodevices can work at nano levels, retaining the integrity of self-power and miniaturization of nanodevices. It not only lays the foundation for the miniaturization of nanodevices'working systems, but also can efficiently harvest the micro mechanical energy, which has been ignored and viewed as uselessness in the environment. Harvesting the ubiquitous mechanical energy has been proposed as an important and potential application, which will powerfully push the nanotechnology forward.
To date, a number of reports on nanogenerators have been published, such as ZnO nanowires, which could realize the charge generation, separation, accumulation and transfer due to the unique coupling of semiconducting and piezoelectric effect. These devices involved various movable parts, causing the problem of stability. As a result, it is important to design a novel device structure with stability to harvest the vibrational energy in the environment, which will broaden the applications of nanogenerators. This thesis aims to the exploitation and optimization of the novel structure, resulting in the harvesting of vibrational energy and output of electricity. The main research works are listed as follows:
(1) As an important1D semiconductor material, silicon nanowires (SiNWs) have been extensively used in chemistry, catalysis, biosensors, electronics and new energy resource, due to their unique electric and mechanics properties and compatibility to silicon industry. The SiNWs obtained from modified oxide-assisted growth contain alpha quartz, which is an excellent piezoelectric material. The existence of alpha quartz makes the as-prepared SiNWs exhibit an electret effect, and a series of experiments were carried out to explore the formation mechanism of the material. The SiNWs were utilized to fabricate a nanogenerator, which yielded an output current of2.8nA with a conversion efficiency of2.2%. These findings open up a novel application of SiNWs in micro energy.
(2) The presence of numerous oxygen-containing functional groups makes graphene oxide (GO) substantially different from graphene in that the former exhibits versatile and unique properties. Within a GO sheet, isolated pockets of graphene are surrounded by amorphous regions of oxygen-containing functional groups. Charges can be stored either in the discrete, quantized levels of the nanosized graphene, or trapped in the amorphous GO dielectric, where oxygen functionalities like epoxy and hydroxyl groups have high electron affinity. A flexible nanogenerator based on GO film was fabricated to harvest acoustic energy, whose output current is about3.23nA with a high conversion efficiency of12.1%. The generated current of the flexible nanogenerator sensitively depends on the pH value of the suspensions for GO films production, which is a good clue for the optimization of the device.
(3) Boron nitride nanosheet (BNNS) is an analogue of graphene in which alternating boron (B) and nitrogen (N) atoms substitute for C atoms in a honeycomb network with sp2bonding. BN is a promising material with a wide band gap (5.3-5.9eV). The as-prepared BNNSs were found to be charged, which were fabricated into a nanogenerator, yielding an output current of0.95nA with a load of1MQ, illustrating the practicality of the device.
(4) It was found that the O-containing functional groups on diamonds'surface from carbon nanotubes as carbon source are more than those from graphite, although the diamonds are fabricated by high pressure high temperature catalytic method under the same conditions. These O-containing functional groups enhanced their combination with bio-material—dopamine (DA), achieving ultra-dispersed and more stable suspension. With a further modification, the as-prepared nanodiamonds may find new applications.
引文
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