Статья

Scalable Synthesis and Characterization of Multilayer γ-Graphyne, New Carbon Crystals with a Small Direct Band Gap

Victor G. DesyatkinDepartment of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, United StatesWilliam Blake MartinDepartment of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, United StatesAli E. AlievAlan G. MacDiarmid NanoTech Institute, University of Texas at Dallas, 800 West Campbell Road, Richardson, Texas 75080, United StatesNathaniel E. ChapmanDepartment of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, United StatesAlexandre F. FonsecaApplied Physics Department, Institute of Physics “Gleb Wataghin”, University of Campinas, Campinas, São Paulo 13083-970, BrazilDouglas S. GalvãoApplied Physics Department, Institute of Physics “Gleb Wataghin”, University of Campinas, Campinas, São Paulo 13083-970, BrazilEricka Roy MillerDepartment of Chemistry, Case Western Reserve University, 10900 Euclid Avenue, Cleveland, Ohio 44106, United StatesKevin H. StoneStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United StatesZhong WangAlan G. MacDiarmid NanoTech Institute, University of Texas at Dallas, 800 West Campbell Road, Richardson, Texas 75080, United StatesDante ZakhidovDepartment of Materials Science and Engineering, Stanford University; 496 Lomita Mall, Stanford, California 94305, United StatesF. T. LimpocoOxford Instruments Asylum Research, 6310 Hollister Avenue, Santa Barbara, California 93117, United StatesSarah AlmahdaliDepartment of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, United StatesShane M. ParkerDepartment of Chemistry, Case Western Reserve University, 10900 Euclid Avenue, Cleveland, Ohio 44106, United StatesRay H. BaughmanAlan G. MacDiarmid NanoTech Institute, University of Texas at Dallas, 800 West Campbell Road, Richardson, Texas 75080, United StatesValentin O. RodionovDepartment of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, United States

2022en

ABI

Аннотация

γ-Graphyne is the most symmetric sp2/sp1 allotrope of carbon, which can be viewed as graphene uniformly expanded through the insertion of two-carbon acetylenic units between all the aromatic rings. To date, synthesis of bulk γ-graphyne has remained a challenge. We here report the synthesis of multilayer γ-graphyne through crystallization-assisted irreversible cross-coupling polymerization. A comprehensive characterization of this new carbon phase is described, including synchrotron powder X-ray diffraction, electron diffraction, lateral force microscopy, Raman spectroscopy, infrared spectroscopy, and cyclic voltammetry. Experiments indicate that γ-graphyne is a 0.48 eV band gap semiconductor, with a hexagonal a-axis spacing of 6.88 Å and an interlayer spacing of 3.48 Å, which is consistent with theoretical predictions. The observed crystal structure has an aperiodic sheet stacking. The material is thermally stable up to 240 °C but undergoes transformation at higher temperatures. While conventional 2D polymerization and reticular chemistry rely on error correction through reversibility, we demonstrate that a periodic covalent lattice can be synthesized under purely kinetic control. The reported methodology is scalable and inspires extension to other allotropes of the graphyne family.

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Идентификаторы

DOI: 10.1021/jacs.2c06583

Цитирования и источники

Цитирований: 2Использованных источников: 0

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