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

Autor:	Desyatkin VG; Department of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, United States., Martin WB; Department of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, United States., Aliev AE; Alan G. MacDiarmid NanoTech Institute, University of Texas at Dallas, 800 West Campbell Road, Richardson, Texas 75080, United States., Chapman NE; Department of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, United States., Fonseca AF; Applied Physics Department, Institute of Physics 'Gleb Wataghin', University of Campinas, Campinas, São Paulo 13083-970, Brazil., Galvão DS; Applied Physics Department, Institute of Physics 'Gleb Wataghin', University of Campinas, Campinas, São Paulo 13083-970, Brazil., Miller ER; Department of Chemistry, Case Western Reserve University, 10900 Euclid Avenue, Cleveland, Ohio 44106, United States., Stone KH; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States., Wang Z; Alan G. MacDiarmid NanoTech Institute, University of Texas at Dallas, 800 West Campbell Road, Richardson, Texas 75080, United States., Zakhidov D; Department of Materials Science and Engineering, Stanford University; 496 Lomita Mall, Stanford, California 94305, United States., Limpoco FT; Oxford Instruments Asylum Research, 6310 Hollister Avenue, Santa Barbara, California 93117, United States., Almahdali SR; Department of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, United States., Parker SM; Department of Chemistry, Case Western Reserve University, 10900 Euclid Avenue, Cleveland, Ohio 44106, United States., Baughman RH; Alan G. MacDiarmid NanoTech Institute, University of Texas at Dallas, 800 West Campbell Road, Richardson, Texas 75080, United States., Rodionov VO; Department of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, United States.
Jazyk:	angličtina
Zdroj:	Journal of the American Chemical Society [J Am Chem Soc] 2022 Oct 05; Vol. 144 (39), pp. 17999-18008. Date of Electronic Publication: 2022 Sep 21.
DOI:	10.1021/jacs.2c06583
Abstrakt:	γ-Graphyne is the most symmetric sp 2 /sp 1 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.
Databáze:	MEDLINE
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