Towards nano-organic chemistry: perspectives for a bottom-up approach to the synthesis of low-dimensional carbon nanostructures Francesco Mercuri, * a Matteo Baldoni ab and Antonio Sgamellotti a Received 15th August 2011, Accepted 27th October 2011 DOI: 10.1039/c1nr11112d Low-dimensional carbon nanostructures, such as nanotubes and graphenes, represent one of the most promising classes of materials, in view of their potential use in nanotechnology. However, their exploitation in applications is often hindered by difficulties in their synthesis and purification. Despite the huge efforts by the research community, the production of nanostructured carbon materials with controlled properties is still beyond reach. Nonetheless, this step is nowadays mandatory for significant progresses in the realization of advanced applications and devices based on low-dimensional carbon nanostructures. Although promising alternative routes for the fabrication of nanostructured carbon materials have recently been proposed, a comprehensive understanding of the key factors governing the bottom-up assembly of simple precursors to form complex systems with tailored properties is still at its early stages. In this paper, following a survey of recent experimental efforts in the bottom-up synthesis of carbon nanostructures, we attempt to clarify generalized criteria for the design of suitable precursors that can be used as building blocks in the production of complex systems based on sp 2 carbon atoms and discuss potential synthetic strategies. In particular, the approaches presented in this feature article are based on the application of concepts borrowed from traditional organic chemistry, such as valence-bond theory and Clar sextet theory, and on their extension to the case of complex carbon nanomaterials. We also present and discuss a validation of these approaches through first-principle calculations on prototypical systems. Detailed studies on the processes involved in the bottom-up fabrication of low-dimensional carbon nanostructures are expected to pave the way for the design and optimization of precursors and efficient synthetic routes, thus allowing the development of novel materials with controlled morphology and properties that can be used in technological applications. a ISTM-CNR, UdR INSTM and Department of Chemistry, University of Perugia, Perugia, 06123, Italy. E-mail: francesco.mercuri@cnr.it; Fax: +39 075 585526 b Physikalische Chemie, Technische Universit € at Dresden, D-01062 Dresden, Germany Francesco Mercuri Francesco Mercuri graduated in chemistry in 1995 at the University of Perugia, Italy, where he also obtained a PhD in chemistry and an international master in computational engi- neering. Since 2001 he has been a CNR researcher, currently at the ISMN Bologna, Italy. He collaborated as staff scientist at the Max-Planck-Institut Stutt- gart and Dresden (Germany), at the CSCS/ETH (Switzer- land) and as visiting scientist at the ENSCP (Paris, France), at the University of Oxford (UK) and at the CSIC-ICMAB (Barcelona, Spain). He was awarded the Alessandro Vaciago prize of the Accademia dei Lincei in 2008. His main research interests are in the field of computational modeling in materials science and nanotechnology. Matteo Baldoni Matteo Baldoni received his MSc in chemistry from the University of Perugia, Italy, in 2004. After a research stage at the Technische Universit € at Dresden, Germany, in 2006, he obtained his PhD in theoretical chemistry from the University of Perugia in 2008. This was fol- lowed by post-doctoral appoint- ments at the University of Perugia and at the Technische Universit € at Dresden, where he is currently working. His research interests focus on the modeling of low-dimensional carbon and inorganic nanostructures and on the computational study of lithium-ion batteries. This journal is ª The Royal Society of Chemistry 2012 Nanoscale, 2012, 4, 369–379 | 369 Dynamic Article Links C < Nanoscale Cite this: Nanoscale, 2012, 4, 369 www.rsc.org/nanoscale FEATURE ARTICLE Downloaded by University of Nottingham on 26/04/2013 13:23:09. Published on 14 December 2011 on http://pubs.rsc.org | doi:10.1039/C1NR11112D View Article Online / Journal Homepage / Table of Contents for this issue