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高质量大面积石墨烯的化学气相沉积制备方法研究

王文荣 周玉修 李铁 王跃林 谢晓明

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高质量大面积石墨烯的化学气相沉积制备方法研究

王文荣, 周玉修, 李铁, 王跃林, 谢晓明

Research on synthesis of high-quality and large-scale graphene films by chemical vapor deposition

Wang Wen-Rong, Zhou Yu-Xiu, Li Tie, Wang Yue-Lin, Xie Xiao-Ming
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  • 石墨烯因其奇特的能带结构和优异的物理性能而成为近年来大家研究的热点, 但是目前单层石墨烯的质量与尺寸制约了其实际应用的发展. 本文采用常压化学气相沉积(CVD)方法, 基于铜箔衬底, 利用甲烷作为碳源制备了高质量大面积的单层与多层石墨烯. 研究发现: 高温度、稀薄的甲烷浓度、较短的生长时间以及合适的气体流速是制备高质量、大面积石墨烯的关键. Raman光谱, 扫描电子显微镜、透射电子显微镜等表征结果表明: 制备的石墨烯主要为单层, 仅铜箔晶界处有少量多层石墨烯. 电学测试表明CVD制备的石墨烯在低温时呈现出较明显的类半导体特性; 薄膜电阻随外界磁场的增大而减小.
    Graphene has received great interest because of its peculiar band structure and excellent physical properties. But today, the development of graphene is limited to its size and quality. In this paper, single- and multilayer graphene films were synthesized on copper foils by chemical vapor deposition(CVD) using methane at ambient pressure. Experiment results find the high temperature, low concentration of methane gas, shorter growth time and suitable gas flow are the key to get high-quality and large-scale graphene films. Raman spectra, scanning electron microscope(SEM) and transmission electron microscope(TEM) characterization indicate the graphene films are mostly single-layer, only with rare area having multilayer around copper boundaries. Further electrical tests show the graphene films grown by CVD method represent semiconductor behaviors under low temperature and the sheet resistance of graphene films is decreasing with the external magnetic field increasing.
    • 基金项目: 国家科技重大专项(批准号: 2011ZX02707)、中科院知识创新工程重要方向项目(批准号: KGCX2-YW-23)、国家自然科学基金创新团队(批准号: 61021064)、国家自然科学基金(批准号: 60936001, 60876037)资助的课题.
    • Funds: Project supported by the Important National Science and Technology Specific Projects (Grant No. 2011ZX02707), the Knowledge Innovation Program of the Chinese Academy of Sciences (Grant No. KGCX2-YW-23), the Foundation for Innovative Research Groups of the National Natural Science Foundation of China (Grant No. 61021064), and the National Natural Science Foundation of China (Grant Nos. 60936001, 60876037).
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    Geim A K, Novoselov K S 2007 Nature Mater. 6 183

    [2]

    Han T W, He P F 2010 Acta Phys. Sin. 59 3408 (in Chinese) [韩同伟, 贺鹏飞 2010 物理学报 59 3408]

    [3]

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    [4]

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    [5]

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    [6]

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    [7]

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    [8]

    Park N, Hong S, Kim G, Jhi S H 2007 J. Am. Chem. Soc. 1298999

    [9]

    Heo C, Yoo J, Lee S, Jo A, Jung S, Yoo H, Lee Y H, Suh M 2011Biomaterials 32 19

    [10]

    Bonaccorso F, Sun Z, Hasan T, Ferrari A C 2010 Nature Photonics4 611

    [11]

    Loh K P, Bao Q L, Eda G, Chhowalla M 2011 Nature Chemistry2 1015

    [12]

    Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y,Dubonos S V, Grigorieva I V, Firsov 2004 Science 306 666

    [13]

    Stankovich S , Dikin D A, Piner R D, Kohlhass K A, KleinhammesA, Jia Y, Wu Y, Nguyen S T, Ruoff R S 2007 Carbon 45 1558

    [14]

    Berger C, Song Z M, Li X B, Wu X S, Brown N, Naud C, MayouD, Li T, Hass J, Marchenkov A N, Conrad E H, First P N, Heer W A 2006 Science 312 1191

    [15]

    Rummeli M H, Bachmatiuk A, Scott A, Borrnert F, Warner J H,Hoffman V, Lin J H, Cuniberti G, Buchner B 2010 ACS Nano 44206

    [16]

    Wei D C, Liu Y Q, Zhang H L, Huang L P, Wu Bin, Chen J Y, Yu G 2009 J. Am. Chem. Soc. 131 11147

    [17]

    Ding X L, Ding G Q, Xie X M, Huang F Q, Jiang M H 2011Carbon 49 2522

    [18]

    Reina A, Jia X T, Ho J, Nezich D, Son H, Bulovic V, Dresselhaus M S, Kong J 2009 Nano Lett. 9 30

    [19]

    Pan Y, Shi D X, Gao H J 2007 Chin. Phys. 16 3151

    [20]

    Coraus J, N'Diaye A, Engler M, Busse C, Wall D, Buckanie N,Heringdorf F J M, Gastel R, Poelsema B, Michely T 2009 New J.Phys. 11 023006

    [21]

    Li X S, Cai W W, An J H, Kim S, Nah J, Yang D X, Piner R, Velamakanni A, Jung I, Tutuc E, Banerjee S K, Colombo L, Ruoff RS 2009 Science 324 1312

    [22]

    Su C Y, Fu D L, Lu A Y, Liu K K, Xu Y P, Juang Z Y, Li L J 2011 Nanotechnology 22 185309

    [23]

    Ferrari A C, Meyer J C, Scardaci V, Casiraghi C, Lazzeri M, MauriF, Piscanec S, Jiang D, Novoselov K S, Roth S, Geim A K 2006Phys. Rev. Lett. 97 187401

    [24]

    Ni Z H, Wang Y Y, Yu T, Shen Z X 2008 Nano Res. 1 273

    [25]

    Yutaka K 1982 J. Phys. C: Solid State Phys. 15 5425

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出版历程
  • 收稿日期:  2011-03-28
  • 修回日期:  2011-06-01
  • 刊出日期:  2012-03-15

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