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加州大学水浒分校Haddon在Acc Chem Res最新综述，关于石墨烯和碳纳米管
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UCR的Robert Haddon教授曾首次预测并发现碱金属掺杂C60的超导性质，他也是纳米碳材料领域的大牛之一。在最新一期的Acc Chem Res上，他的小组发表了一篇名为Effect of Covalent Chemistry on the Electronic Structure and Properties of Carbon Nanotubes and Graphene的综述（Vol. 46, No. 1, 2013, 65-76），长达12页，内容非常有特色，基本上是围绕他本人研究组的三方面工作，参考文献仅53篇。不像一般的综述，涵盖面广而不精。虽然他的研究组也做应用研究，但是从本文可以看出其理论功底之深厚。 摘要如下： In this Account, we discuss the chemistry of graphitic materials with particular reference to three reactions studied by our research group: (1) aryl radical addition, from diazonium precursors, (2) Diels–Alder pericyclic reactions, and (3) organometallic complexation with transition metals. We provide a unified treatment of these reactions in terms of the degenerate valence and conduction bands of graphene at the Dirac point and the relationship of their orbital coefficients to the HOMO and LUMO of benzene and to the Clar structures of graphene. In the case of the aryl radical addition and the Diels–Alder reactions, there is full rehybridization of the derivatized carbon atoms in graphene from sp2 to sp3, which removes these carbon atoms from conjugation and from the electronic band structure of graphene (referred to as destructive rehybridization). The radical addition process requires an electron transfer step followed by the formation of a σ-bond and the creation of a π-radical in the graphene lattice, and thus, there is the potential for unequal degrees of functionalization in the A and B sublattices and the possibility of ferromagnetism and superparamagnetism in the reaction products. With regard to metal functionalization, we distinguish four limiting cases: (a) weak physisorption, (b) ionic chemisorption, in which there is charge transfer to the graphitic structure and preservation of the conjugation and band structure, (c) covalent chemisorption, in which there is strong rehybridization of the graphitic band structure, and (d) covalent chemisorption with formation of an organometallic hexahapto-metal bond that largely preserves the graphitic band structure (constructive rehybridization). The constructive rehybridization that accompanies the formation of bis-hexahapto-metal bonds, such as those in (η6-SWNT)Cr(η6-SWNT), interconnects adjacent graphitic surfaces and significantly reduces the internanotube junction resistance in single-walled carbon nanotube (SWNT) networks. The conversion of sp2 hybridized carbon atoms to sp3 can introduce a band gap into graphene, influence the electronic scattering, and create dielectric regions in a graphene wafer. However, the organometallic hexahapto (η6) functionalization of the two-dimensional (2D) graphene π-surface with transition metals provides a new way to modify graphitic structures that does not saturate the functionalized carbon atoms and, by preserving their structural integrity, maintains the delocalization in these extended periodic π-electron systems and offers the possibility of three-dimensional (3D) interconnections between adjacent graphene sheets. These structures may find applications in interconnects, 3D-electronics, organometallic catalysis, atomic spintronics and in the fabrication of new electronic materials.      [ Last edited by zxs1989 on 2013-2-11 at 15:39 ] |
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