Research article Topical Sections

CVD-graphene growth on different polycrystalline transition metals

  • Received: 02 November 2016 Accepted: 19 January 2017 Published: 24 January 2017
  • The chemical vapor deposition (CVD) graphene growth on two polycrystalline transition metals (Ni and Cu) was investigated in detail using Raman spectroscopy and optical microscopy as a way to synthesize graphene of the highest quality (i.e. uniform growth of monolayer graphene), which is considered a key issue for electronic devices. Key CVD process parameters (reaction temperature, CH4/H2flow rate ratio, total flow of gases (CH4+H2), reaction time) were optimized for both metals in order to obtain the highest graphene uniformity and quality. The conclusions previously reported in literature about the performance of low and high carbon solubility metals in the synthesis of graphene and their associated reaction mechanisms, i.e. surface depositionand precipitation on cooling, respectively, was not corroborated by the results obtained in this work. Under the optimal reaction conditions, a large percentage of monolayer graphene was obtained over the Ni foil since the carbon saturation was not complete, allowing carbon atoms to be stored in the bulk metal, which could diffuse forming high quality monolayer graphene at the surface. However, under the optimal reaction conditions, the formation of a non-uniform mixture of few layers and multilayer graphene on the Cu foil was related to the presence of an excess of active carbon atoms on the Cu surface.

    Citation: M. P. Lavin-Lopez, L. Sanchez-Silva, J. L. Valverde, A. Romero. CVD-graphene growth on different polycrystalline transition metals[J]. AIMS Materials Science, 2017, 4(1): 194-208. doi: 10.3934/matersci.2017.1.194

    Related Papers:

  • The chemical vapor deposition (CVD) graphene growth on two polycrystalline transition metals (Ni and Cu) was investigated in detail using Raman spectroscopy and optical microscopy as a way to synthesize graphene of the highest quality (i.e. uniform growth of monolayer graphene), which is considered a key issue for electronic devices. Key CVD process parameters (reaction temperature, CH4/H2flow rate ratio, total flow of gases (CH4+H2), reaction time) were optimized for both metals in order to obtain the highest graphene uniformity and quality. The conclusions previously reported in literature about the performance of low and high carbon solubility metals in the synthesis of graphene and their associated reaction mechanisms, i.e. surface depositionand precipitation on cooling, respectively, was not corroborated by the results obtained in this work. Under the optimal reaction conditions, a large percentage of monolayer graphene was obtained over the Ni foil since the carbon saturation was not complete, allowing carbon atoms to be stored in the bulk metal, which could diffuse forming high quality monolayer graphene at the surface. However, under the optimal reaction conditions, the formation of a non-uniform mixture of few layers and multilayer graphene on the Cu foil was related to the presence of an excess of active carbon atoms on the Cu surface.


    加载中
    [1] Geim A K, Novoselov K S (2007) The rise of graphene. Nat Mater 6: 183–191. doi: 10.1038/nmat1849
    [2] Chen X, Zhang L, Chen S (2015) Large area CVD growth of graphene. Synth Met 210: 95–108. doi: 10.1016/j.synthmet.2015.07.005
    [3] Bhuyan MSA, Uddin MN, Islam MM, et al. (2016) Synthesis of graphene. Int Nano Lett 6: 65. doi: 10.1007/s40089-015-0176-1
    [4] Wang Y, Chen X, Zhong Y, et al. (2009) Large area, continuous, few-layered graphene as anodes in organic photovoltaic devices. Appl Phys Lett 95: 063302. doi: 10.1063/1.3204698
    [5] Dervishi E, Li Z, Watanabe F, et al. (2009) Large-scale graphene production by RF-cCVD method. Chem Commun, 4061–4063.
    [6] Zhang Y, Zhang L, Zhou C (2013) Review of chemical vapor deposition of graphene and related applications. Acc Chem Res 46: 2329–2339. doi: 10.1021/ar300203n
    [7] Cabrero-Vilatela A, Weatherup RS, Braeuninger-Weimer P, et al. (2016) Towards a general growth model for graphene CVD on transition metal catalysts. Nanoscale 8: 2149–2158. doi: 10.1039/C5NR06873H
    [8] Zhang X, Li H, Ding F (2014) Self-Assembly of Carbon Atoms on Transition Metal Surfaces-Chemical Vapor Deposition Growth Mechanism of Graphene. Adv Mater 26: 5488–5495. doi: 10.1002/adma.201305922
    [9] Losurdo M, Giangregorio MM, Capezzuto P, et al. (2011) Graphene CVD growth on copper and nickel: Role of hydrogen in kinetics and structure. Phys Chem Chem Phys 13: 20836–20843. doi: 10.1039/c1cp22347j
    [10] López GA, Mittemeijer EJ (2004) The solubility of C in solid Cu. Scripta Mater 51: 1–5. doi: 10.1016/j.scriptamat.2004.03.028
    [11] Xue Y, Wu B, Guo Y, et al. (2011) Synthesis of large-area, few-layer graphene on iron foil by chemical vapor deposition. Nano Res 4: 1208–1214. doi: 10.1007/s12274-011-0171-4
    [12] Chen X, Zhang L, Chen S (2015) Large area CVD growth of graphene. Synth Met 210: 95–108. doi: 10.1016/j.synthmet.2015.07.005
    [13] Zhao P, Kumamoto A, Kim S, et al. (2013) Self-Limiting Chemical Vapor Deposition Growth of Monolayer Graphene from Ethanol. J Phys Chem C 117: 10755–10763. doi: 10.1021/jp400996s
    [14] Yu Q, Lian J, Siriponglert S, et al. (2008) Graphene segregated on Ni surfaces and transferred to insulators. Appl Phys Lett 93: 113103. doi: 10.1063/1.2982585
    [15] Lavin-Lopez MP, Valverde JL, Cuevas MC, et al. (2014) Synthesis and characterization of graphene: Influence of synthesis variables. Phys Chem Chem Phys 16: 2962–2970. doi: 10.1039/c3cp54832e
    [16] Lavin-Lopez MP, Valverde JL, Ruiz-Enrique MI, et al. (2015) Thickness control of graphene deposited over polycrystalline nickel. New J Chem 39: 4414–4423. doi: 10.1039/C5NJ00073D
    [17] Lavin-Lopez MP, Valverde JL, Sanchez-Silva L, et al. (2016) Influence of the Total Gas Flow at Different Reaction Times for CVD-Graphene Synthesis on Polycrystalline Nickel. J Nanomater 2016: 9.
    [18] Wall M (2012) Raman spectroscopy optimizes graphene characterization. Adv Mater Processes 170: 35–38.
    [19] Suk JW, Kitt A, Magnuson CW, et al. (2011) Transfer of CVD-grown monolayer graphene onto arbitrary substrates. ACS Nano 5: 6916–6924. doi: 10.1021/nn201207c
    [20] Reina A, Jia X, Ho J, et al. (2009) Large area, few-layer graphene films on arbitrary substrates by chemical vapor deposition. Nano Lett 9: 30–35. doi: 10.1021/nl801827v
    [21] Lee S, Lee K, Zhong Z (2010) Wafer scale homogeneous bilayer graphene films by chemical vapor deposition. Nano Lett 10: 4702–4707. doi: 10.1021/nl1029978
    [22] Lee D, Lee K, Jeong S, et al. (2012) Process optimization for synthesis of high-quality graphene films by low-pressure chemical vapor deposition. Jpn J Appl Phys 51.
    [23] Chen S, Cai W, Piner RD, et al. (2011) Synthesis and characterization of large-area graphene and graphite films on commercial Cu-Ni alloy foils. Nano Lett 11: 3519–3525. doi: 10.1021/nl201699j
    [24] Muñoz R, Gómez-Aleixandre C (2013) Review of CVD synthesis of graphene. Chem Vap Deposition 19: 297–322. doi: 10.1002/cvde.201300051
    [25] Seah CM, Chai SP, Mohamed AR (2014) Mechanisms of graphene growth by chemical vapour deposition on transition metals. Carbon 70: 1–21. doi: 10.1016/j.carbon.2013.12.073
    [26] Liu W, Li H, Xu C, et al. (2011) Synthesis of high-quality monolayer and bilayer graphene on copper using chemical vapor deposition. Carbon 49: 4122–4130. doi: 10.1016/j.carbon.2011.05.047
    [27] Li X, Magnuson CW, Venugopal A, et al. (2010) Graphene films with large domain size by a two-step chemical vapor deposition process. Nano Lett 10: 4328–4334. doi: 10.1021/nl101629g
    [28] Wang YM, Cheng S, Wei QM, et al. (2004) Effects of annealing and impurities on tensile properties of electrodeposited nanocrystalline Ni. Scripta Mater 51: 1023–1028. doi: 10.1016/j.scriptamat.2004.08.015
    [29] Shen Y, Lua AC (2013) A facile method for the large-scale continuous synthesis of graphene sheets using a novel catalyst. Sci Rep 3: 3037–3042.
    [30] Verguts K, Vermeulen B, Vrancken N, et al. (2016) Epitaxial Al2O3(0001)/Cu(111) Template Development for CVD Graphene Growth. J Phys Chem C 120: 297–304. doi: 10.1021/acs.jpcc.5b09461
    [31] Vlassiouk I, Smirnov S, Regmi M, et al. (2013) Graphene nucleation density on copper: Fundamental role of background pressure. J Phys Chem C 117: 18919–18926. doi: 10.1021/jp4047648
    [32] Liu W, Chung CH, Miao CQ, et al. (2010) Chemical vapor deposition of large area few layer graphene on Si catalyzed with nickel films. Thin Solid Films 518: S128–S132. doi: 10.1016/j.tsf.2009.10.070
    [33] Wan D, Lin T, Bi H, et al. (2012) Autonomously controlled homogenous growth of wafer-sized high-quality graphene via a smart Janus substrate. Adv Funct Mater 22: 1033–1039. doi: 10.1002/adfm.201102560
    [34] Mattevi C, Kim H, Chhowalla M (2011) A review of chemical vapour deposition of graphene on copper. J Mater Chem 21: 3324–3334. doi: 10.1039/C0JM02126A
    [35] Vlassiouk I, Regmi M, Fulvio P, et al. (2011) Role of hydrogen in chemical vapor deposition growth of large single-crystal graphene. ACS Nano 5: 6069–6076. doi: 10.1021/nn201978y
    [36] Zhang Y, Li Z, Kim P, et al. (2012) Anisotropic hydrogen etching of chemical vapor deposited graphene. ACS Nano 6: 126–132. doi: 10.1021/nn202996r
    [37] Li X, Cai W, Colombo L, et al. (2009) Evolution of graphene growth on Ni and Cu by carbon isotope labeling. Nano Lett 9: 4268–4272. doi: 10.1021/nl902515k
    [38] Takahashi K, Yamada K, Kato H, et al. (2012) In situ scanning electron microscopy of graphene growth on polycrystalline Ni substrate. Surf Sci 606: 728–732. doi: 10.1016/j.susc.2011.12.009
    [39] Genki O, Hiroki H, Nanao N, et al. (2012) Macroscopic Single-Domain Graphene Growth on Polycrystalline Nickel Surface. Appl Phys Express 5: 035501. doi: 10.1143/APEX.5.035501
    [40] Nakahara H, Fujita S, Minato T, et al. (2016) In-Situ RHEED Study on Graphene Growth During Chemical Vapor Deposition. e-J Surf Sci Nanotechnol 14: 39–42. doi: 10.1380/ejssnt.2016.39
    [41] Robertson AW, Warner JH (2011) Hexagonal Single Crystal Domains of Few-Layer Graphene on Copper Foils. Nano Lett 11: 1182–1189. doi: 10.1021/nl104142k
    [42] Yao Y, Li Z, Lin Z, et al. (2011) Controlled Growth of Multilayer, Few-Layer, and Single-Layer Graphene on Metal Substrates. J Phys Chem C 115: 5232–5238. doi: 10.1021/jp109002p
    [43] Kasap S, Khaksaran H, Celik S, et al. (2015) Controlled growth of large area multilayer graphene on copper by chemical vapour deposition. Phys Chem Chem Phys 17: 23081–23087. doi: 10.1039/C5CP01436K
    [44] Van Tu N, Huu Doan L, Van Chuc N, et al. (2013) Synthesis of multi-layer graphene films on copper tape by atmospheric pressure chemical vapor deposition method. Adv Nat Sci Nanosci Nanotechnol 4: 035012. doi: 10.1088/2043-6262/4/3/035012
    [45] Shi Y, Wang D, Zhang J, et al. (2015) Synthesis of multilayer graphene films on copper by modified chemical vapor deposition. Mater Manuf Process 30: 711–716. doi: 10.1080/10426914.2014.984201
    [46] Wu W, Yu Q, Peng P, et al. (2012) Control of thickness uniformity and grain size in graphene films for transparent conductive electrodes. Nanotechnology 23.
    [47] Ferrari AC, Meyer JC, Scardaci V, et al. (2006) Raman spectrum of graphene and graphene layers. Phys Rev Lett 97: 187401. doi: 10.1103/PhysRevLett.97.187401
    [48] Li X, Cai W, An J, et al. (2009) Large-area synthesis of high-quality and uniform graphene films on copper foils. Science 324: 1312–1314. doi: 10.1126/science.1171245
    [49] Jeong-Yuan H, Chun-Chiang K, Li-Chyong C, et al. (2010) Correlating defect density with carrier mobility in large-scaled graphene films: Raman spectral signatures for the estimation of defect density. Nanotechnology 21: 465705. doi: 10.1088/0957-4484/21/46/465705
    [50] Bointon TH, Barnes MD, Russo S, et al. (2015) High Quality Monolayer Graphene Synthesized by Resistive Heating Cold Wall Chemical Vapor Deposition. Adv Mater 27: 4200–4206. doi: 10.1002/adma.201501600
    [51] Ferrari AC (2007) Raman spectroscopy of graphene and graphite: Disorder, electron-phonon coupling, doping and nonadiabatic effects. Solid State Commun 143: 47–57. doi: 10.1016/j.ssc.2007.03.052
    [52] Nemanich RJ, Solin SA (1979) First- and second-order Raman scattering from finite-size crystals of graphite. Phys Rev B 20: 392–401. doi: 10.1103/PhysRevB.20.392
    [53] Calizo I, Teweldebrhan D, Bao W, et al. (2008) Spectroscopic Raman nanometrology of graphene and graphene multilayers on arbitrary substrates. J Phys 109: 5.
    [54] Zhang Y, Gao T, Gao Y, et al. (2011) Defect-like structures of graphene on copper foils for strain relief investigated by high-resolution scanning tunneling microscopy. ACS Nano 5: 4014–4022. doi: 10.1021/nn200573v
    [55] Nie S, Wofford JM, Bartelt NC, et al. (2011) Origin of the mosaicity in graphene grown on Cu(111). Phys Rev B Condens Matter 84: 155425. doi: 10.1103/PhysRevB.84.155425
    [56] Rybin MG, Pozharov AS, Obraztsova ED (2010) Control of number of graphene layers grown by chemical vapor deposition. Phys Status Solidi C 7: 2785–2788. doi: 10.1002/pssc.201000241
    [57] Liang C, Wang W, Li T, et al. (2012) Optimization on the synthesis of large-area single-crystal graphene domains by chemical vapor deposition on copper foils. Xi'an.
  • Reader Comments
  • © 2017 the Author(s), licensee AIMS Press. This is an open access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0)
通讯作者: 陈斌, bchen63@163.com
  • 1. 

    沈阳化工大学材料科学与工程学院 沈阳 110142

  1. 本站搜索
  2. 百度学术搜索
  3. 万方数据库搜索
  4. CNKI搜索

Metrics

Article views(8656) PDF downloads(1790) Cited by(12)

Article outline

Figures and Tables

Figures(8)

/

DownLoad:  Full-Size Img  PowerPoint
Return
Return

Catalog