Decades of extensive research have matured the development of carbon nanotubes (CNTs). Still, the properties of macroscale assemblages, such as sheets of carbon nanotubes, are not good enough to satisfy many applications. This paper gives an overview of different approaches to synthesize CNTs and then focuses on the floating catalyst method to form CNT sheets. A method is also described in this paper to modify the properties of macroscale carbon nanotube sheets produced by the floating catalyst method. The CNT sheet is modified to form a carbon nanotube hybrid (CNTH) sheet by incorporating metal, ceramic, or other types of nanoparticles into the high-temperature synthesis process to improve and customize the properties of the traditional nanotube sheet. This paper also discusses manufacturing obstacles and the possible commercial applications of the CNT sheet and CNTH sheet. Manufacturing problems include the difficulty of injecting dry nanoparticles uniformly, increasing the output of the process to reduce cost, and safely handling the hydrogen gas generated in the process. Applications for CNT sheet include air and water filtering, energy storage applications, and compositing CNTH sheets to produce apparel with anti-microbial properties to protect the population from infectious diseases. The paper also provides an outlook towards large scale commercialization of CNT material.

This work studies synthesis of carbon nanotube (CNT) sheet using the high temperature (1400 °C) floating catalyst chemical vapor deposition (FC-CVD) method. Three metallocenes—ferrocene, nickelocene, cobaltocene—and their combinations are used as precursors for metal catalysts in the synthesis process. For the carbon source, an alcohol fuel, a combination of methanol and n-hexane (9:1), is used. First, the metallocenes were dissolved in the alcohol fuel. Then, the fuel mixture was injected into a tube furnace using an ultrasonic atomizer with Ar/H₂ carrier gas in a ratio of about 12/1. The synthesis of CNTs from a combination of two or three metallocenes reduces the percentage of metal catalyst impurity in the CNT sheet. However, there is an increase in structural defects in the CNTs when using mixtures of two or three metallocenes as catalysts. Furthermore, the specific electrical conductivity of the CNT sheet was highest when using a mixture of ferrocene and cobaltocene as the catalyst. Overall, the multi-catalyst method described enables tailoring certain properties of the CNT sheet. However, the standard ferrocene catalyst seems most appropriate for large-scale manufacturing at the lowest cost.

Carbon nanotubes (CNTs) have extraordinary properties and are used for applications in various fields of engineering and research. Due to their unique combination of properties, such as good electrical and thermal conductivity and mechanical strength, there is an increasing demand to produce CNTs with enhanced and customized properties. CNTs are produced using different synthesis methods and have extraordinary properties individually at the nanotube scale. However, it is challenging to achieve these properties when CNTs are used to form macroscopic sheets, tapes, and yarns. To further improve the properties of macroscale forms of CNTs, various types of nanoparticles and microfibers can be integrated into the CNT materials. The nanoparticles and microfibers can be chosen to selectively enhance the properties of CNT materials at the macroscopic level. In this paper, we propose a technique to manufacture carbon hybrid materials (CHMs) by combining CNT non-woven fabric (in the form of sheets or tapes) with microfibers to form CNT-CF hybrid materials with new/improved properties. CHMs are formed by integrating or adding nanoparticles, microparticles, or fibers into the CNT sheet. The additive materials can be incorporated into the synthesis process from the inlet or the outlet of the reactor system. This paper focuses on CHMs produced using the gas phase pyrolysis method with microparticles/fibers integrated at the outlet of the reactor and continuous microfiber tapes integrated into the CNT sheet at the outlet using a tape feeding machine. After synthesis, characterizations such as microscopy and thermogravimetric analysis were used to study the morphology and composition of the CNTs, and examples for potential applications are discussed in this paper.

The overall hypothesis for this paper is that accurately tuning the gas phase pyrolysis synthesis process and using appropriate raw materials will enable manufacturing different types of carbon hybrid materials (CHM). Optimizing multiple variables including particle melting and vaporization temperatures, fuel flow rate, gas flow rates, gas velocity, and sock wind-up speed is needed to achieve reliability of the synthesis process. Results from our specific reactor are presented to show how the process variables interact and how they affect CNT sock yield and stability. Metal nanoparticle (NP) injection enables the formation of hybrid materials. Several types of CHM materials created by incorporating different types of NPs into the carbon nanotube (CNT) synthesis process and CNT sock are discussed. Many possible combinations of metal NPs can be used in the process to customize the properties of CHM. However, it is a complex problem to determine what metal compounds can chemically join with CNT. Some of the first results testing the new CHM process are presented in this paper.