Over the past decade, carbon nanotubes (CNTs) and related fullerene carbons have gained great attention in materials research due to the novel properties of this class of materials in electrical, magnetic, nonlinear optical, mechanical, and catalytic applications [1-22]. The potential usages of these new forms of carbon have been since proposed for various technological fields spanning from more classical type applications, such as the catalysts in heterogeneous catalysis and carbon adsorbents in separation technology, to display devices, chemical mapping, bio/mechanical sensors/devices, energy storage, and molecular electronic devices/connectors [1-6]. Although tremendous technological progress and research accomplishments have been made since the discoveries of fullerene carbons and CNTs [3, 5, 6], the new developments in nanoscience and nanotechnology research in turn impose us with higher demands and standards for the future nanocarbons preparation. Even today, controlled synthesis of high-quality CNTs is still a problem largely hindering the actual applications of these fascinating materials. In certain application areas such as energy storage and heterogeneous catalysis, furthermore, large quantities of the CNTs are required. Clearly, the further progress of the entire field depends heavily on our ability to develop newer synthetic methodologies for nanocarbon materials with desired quality and quantity.

In this chapter, we will look at a less common aspect of the CNTs fabrication—solid-state synthesis of CNTs. Our attention will be directed to several important case studies, each representing a typical synthetic method. The chapter is thus focused on a comprehensive review on representative synthetic methodologies. It is our aim that the chapter will allow interested readers to have a general picture on various solid-state methods for the CNTs preparation with certain in-depth details.

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