Efficient Preparation of Large-Area Graphene Oxide Sheets for Transparent Conductive Films

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1 Supporting Information Efficient Preparation of Large-Area Graphene Oxide Sheets for Transparent Conductive Films Jinping Zhao, Songfeng Pei, Wencai Ren*, Libo Gao and Hui-Ming Cheng* Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang , P.R. China address: Figure S1. XPS spectra of the rgo films assembled of GO sheets with average area of ~ (III), ~ (II) and ~7000 µm 2 (I), which were reduced by 55 wt% HI acid for 30s at 100 C.

2 Table S1 1 Opto-electrical property comparison of TCFs assembled with different kinds of graphene. Graphene type Electrical conductivity (S/cm) Sheet resistance (Ω/sq) Transmittance (%) σ DC /σ OP Reference Our work Reduced graphene oxide (Large GO sheets with a area of ~7000 µm 2 ) Zhu et al, 2 APL 95, Liu et al, 3 Nanotechnology 20, Becerril et al, 4 ACS Nano 2, Wu et al, 5 ACS Nano, 4, 43 5kΩ-1MΩ > Wu et al, 6 APL 92, Liang et al, , Wang et al, 8 Nano Letters, 8, 323 Zhao etal, Electrochimica Acta, 55, 491

3 Mattevi et al, 10 Adv.Funct. Mater.19, 2577 Kim et al, 11 Langmuir, 25, Eda et al, 12 Nature 3, 270 Eda et al, 13 APL 92, exfoliated with DMF Blake et al, 14 Nano Letters, 8, 1704 Solutionexfoliated graphene sheets by sonication exfoliated in sodium cholate solution exfoliated in sodium cholate solution Expandable graphite, exfoliated with DMF Green et al, 15 Nano Letters, 9,4031 De et al, 16 Small, 6,458 Li et al, 17 Nature 3, 538 CVD Cu substrate Cai et al, 18 APL 95, Cu substrate Li et al, 19 Nano Letters, 9,4359 Ni substrate Wang et al, 20 APL, 95,

4 Ni substrate Kim et al, 21 Nature 457, 706 Ni substrate Reina et al, 22 Nano Letters, 9, 30 REFERENCES AND NOTES 1. De, S.; Coleman, J. N. Are There Fundamental Limitations on the Sheet Resistance and Transmittance of Thin Graphene Films? ACS Nano 2010, 4, Zhu, Y. W.; Cai, W. W.; Piner, R. D.; Velamakanni, A.; Ruoff, R. S. Transparent Self-Assembled Films of Reduced Graphene Oxide Platelets. Appl. Phys. Lett. 2009, 95, Liu, Y. Q.; Gao, L.; Sun, J.; Wang, Y.; Zhang, J. Stable Nafion-Functionalized Graphene Dispersions for Transparent Conducting Films. Nanotechnology 2009, 20, Becerril, H. A.; Mao, J.; Liu, Z.; Stoltenberg, R. M.; Bao, Z.; Chen, Y. Evaluation of Solution-Processed Reduced Graphene Oxide Films as Transparent Conductors. ACS Nano 2008, 2, Wu, J. B.; Agrawal, M.; Becerril, H. A.; Bao, Z. N.; Liu, Z. F.; Chen, Y. S.; Peumans, P. Organic Light-Emitting Diodes on Solution-Processed Graphene Transparent Electrodes. ACS Nano 2010, 4, Wu, J. B.; Becerril, H. A.; Bao, Z. N.; Liu, Z. F.; Chen, Y. S.; Peumans, P. Organic Solar Cells with Solution-Processed Graphene Transparent Electrodes. Appl. Phys. Lett. 2008, 92, Liang, Y. Y.; Frisch, J.; Zhi, L. J.; Norouzi-Arasi, H.; Feng, X. L.; Rabe, J. P.; Koch, N.; Mullen, K. Transparent, ly Conductive Graphene Electrodes from Acetylene-Assisted Thermolysis of Graphite Oxide Sheets and Nanographene Molecules. Nanotechnology 2009, 20, Wang, X.; Zhi, L. J.; Mullen, K. Transparent, Conductive Graphene Electrodes for Dye-Sensitized Solar Cells. Nano Lett. 2008, 8, Zhao, L.; Zhao, L.; Xu, Y. X.; Qiu, T. F.; Zhi, L. J.; Shi, G. Q. Polyaniline Electrochromic Devices with Transparent Graphene Electrodes. Electrochim. Acta 2009, 55, Mattevi, C.; Eda, G.; Agnoli, S.; Miller, S.; Mkhoyan, K. A.; Celik, O.; Mostrogiovanni, D.; Granozzi, G.; Garfunkel, E.; Chhowalla, M. Evolution of Electrical,, and Structural Properties of Transparent and Conducting ly Derived Graphene Thin Films. Adv. Funct. Mater. 2009, 19, Kim, Y. K.; Min, D. H. Durable Large-Area Thin Films of Graphene/Carbon Nanotube Double Layers as a Transparent Electrode. Langmuir 2009, 25, Eda, G.; Fanchini, G.; Chhowalla, M. Large-Area Ultrathin Films of Reduced Graphene Oxide as a Transparent and Flexible Electronic Material. Nat. Nanotechnol. 2008, 3, Eda, G.; Lin, Y. Y.; Miller, S.; Chen, C. W.; Su, W. F.; Chhowalla, M. Transparent and Conducting Electrodes for Organic Electronics from Reduced Graphene Oxide. Appl. Phys. Lett. 2008, 92, Blake, P.; Brimicombe, P. D.; Nair, R. R.; Booth, T. J.; Jiang, D.; Schedin, F.; Ponomarenko, L. A.; Morozov, S. V.; Gleeson, H. F.; Hill, E. W.; Geim, A. K.; Novoselov, K. S. Graphene-Based Liquid Crystal Device. Nano Lett. 2008, 8, Green, A. A.; Hersam, M. C. Solution Phase Production of Graphene with Controlled Thickness Via Density Differentiation. Nano Lett. 2009, 9, De, S.; King, P. J.; Lotya, M.; O'Neill, A.; Doherty, E. M.; Hernandez, Y.; Duesberg, G. S.; Coleman, J. N.

5 Flexible, Transparent, Conducting Films of Randomly Stacked Graphene from Surfactant-Stabilized, Oxide-Free Graphene Dispersions. Small 2010, 6, Li, X. L.; Zhang, G. Y.; Bai, X. D.; Sun, X. M.; Wang, X. R.; Wang, E.; Dai, H. J. ly Conducting Graphene Sheets and Langmuir-Blodgett Films. Nat. Nanotechnol. 2008, 3, Cai, W. W.; Zhu, Y. W.; Li, X. S.; Piner, R. D.; Ruoff, R. S. Large Area Few-Layer Graphene/Graphite Films as Transparent Thin Conducting Electrodes. Appl. Phys. Lett. 2009, 95, Li, X. S.; Zhu, Y. W.; Cai, W. W.; Borysiak, M.; Han, B. Y.; Chen, D.; Piner, R. D.; Colombo, L.; Ruoff, R. S. Transfer of Large-Area Graphene Films for -Performance Transparent Conductive Electrodes. Nano Lett. 2009, 9, Wang, Y.; Chen, X. H.; Zhong, Y. L.; Zhu, F. R.; Loh, K. P. Large Area, Continuous, Few-Layered Graphene as Anodes in Organic Photovoltaic Devices. Appl. Phys. Lett. 2009, 95, Kim, K. S.; Zhao, Y.; Jang, H.; Lee, S. Y.; Kim, J. M.; Kim, K. S.; Ahn, J. H.; Kim, P.; Choi, J. Y.; Hong, B. H. Large-Scale Pattern Growth of Graphene Films for Stretchable Transparent Electrodes. Nature 2009, 457, Reina, A.; Jia, X. T.; Ho, J.; Nezich, D.; Son, H. B.; Bulovic, V.; Dresselhaus, M. S.; Kong, J. Large Area, Few-Layer Graphene Films on Arbitrary Substrates by Vapor Deposition. Nano Lett. 2009, 9,

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