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Surface-Catalyzed C-C Covalent Coupling Strategies toward the Synthesis of Low-Dimensional Carbon-Based Nanostructures

  • [设施]:合肥光源
  • [期刊/会议名称]:Accounts of Chemical Research
  • [摘要]:CONSPECTUS: Carbon-based nanostructures have attracted tremendous interest because of their versatile and tunable properties, which depend on the bonding type of the constituting carbon atoms. Graphene, as the most prominent representative of the pi-conjugated carbon-based materials, consists entirely of sp(2)-hybridized carbon atoms and exhibits a zero band gap. Recently, countless efforts were made to open and tune the band gap of graphene for its applications in semiconductor devices. One promising method is periodic perforation, resulting in a graphene nanomesh (GNM), which opens the band gap while maintaining the exceptional transport properties. However, the typically employed lithographic approach for graphene perforation is difficult to control at the atomic level. The complementary bottom-up method using surface-assisted carbon carbon (C-C) covalent coupling between organic molecules has opened up new possibilities for atomically precise fabrication of conjugated nanostructures like GNM and graphene nanoribbons (GNR), although with limited maturity. A general drawback of the bottom-up approach is that the desired structure usually does not represent the global thermodynamic minimum. It is therefore impossible to improve the long-range order by postannealing, because once the C-C bond formation becomes reversible, graphene as the thermodynamically most stable structure will be formed. This means that only carefully chosen precursors and reaction conditions can lead to the desired (non-graphene) material. One of the most popular and frequently used organic reactions for on-surface C-C coupling is the Ullmann reaction of aromatic halides. While experimentally simple to perform, the irreversibility of the C-C bond formation makes it a challenge to obtain long-range ordered nanostructures. With no postreaction structural improvement possible, the assembly process must be optimized to result in defect-free nanostructures during the initial reaction, requiring complete reaction of the precursors in the right positions. Incomplete connections typically result when mobile precursor monomers are blocked from reaching unsaturated reaction sites of the preformed nanostructures. ...
  • [发表日期]:2015
  • [第一作者]:范其瑭
  • [第一作者单位]:中国科学技术大学 国家同步辐射实验室
  • [通讯作者]:朱俊发
  • [通讯作者单位]:中国科学技术大学 国家同步辐射实验室
  • [论文类型]:期刊
  • [期刊分类]:
  • [学科分类]:化学
  • [影响因子]:24.368
  • [关键词]:
  • [卷号]:8
  • [期号]:48
  • [起止页码]:2484-2494
  • [简介]: