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One-pot ball-milling preparation of graphene/carbon black aqueous inks for highly conductive and flexible printed electronics

  • Xiao Yang (杨晓)
  • Xiao-Ming Li (李晓明)
  • Qing-Qiang Kong (孔庆强)
  • Zhuo Liu (刘卓)
  • Jing-Peng Chen (陈景鹏)
  • Hui Jia (贾辉)
  • Yan-Zhen Liu (刘燕珍)
  • Li-Jing Xie (谢莉婧)
  • Cheng-Meng Chen (陈成猛)Email author
Articles
  • 54 Downloads

Abstract

Stable aqueous carbon inks, with graphene sheets (GSs) and carbon black (CB) as conductive fillers, are prepared by a simple one-pot ball-milling method. The as-prepared composite ink with 10 wt% GSs shows optimized rheological properties (viscosity and thixotropy) for screen printing. The as-printed coatings based on the above ink are uniform and dense on a polyimide substrate, and exhibit a sandwich-type conductive three dimensional network at the microscale. The resistivity of the typical composite coating is as low as 0.23±0.01 Ω cm (92±4 Ω sq−1, 25 µm), which is 30% as that of a pure CB coating (0.77±0.01 Ω cm). It is noteworthy that the resistivity decreases to 0.18±0.01 Ω cm (72±4 Ω sq−1, 25 µm) after a further rolling compression. The coating exhibits good mechanical flexibility, and the resistance slightly increases by 12% after 3000 bending cycles. With the CB/GSs composite coatings as a flexible conductor, fascinating luminescent bookmarks and membrane switches were fabricated, demonstrating the tremendous potential of these coatings in the commercial production of flexible electronics and devices.

Keywords

graphene carbon black conductive inks printed electronics one-pot ball-milling 

一步球磨法制备石墨烯/炭黑水性导电油墨应用于柔性电子器件

摘要

本文以石墨烯和炭黑作为导电填料, 通过一步球磨法制备了高导电的水性碳系油墨. 当石墨烯质量分数为10%时, 复合油墨具有最优的流变学性能; 在丝网印刷中, 该油墨在聚酰亚胺基底上形成均匀致密的涂层. 在微观上, 涂层具有夹层三维网络结构, 电阻率为0.23±0.01 Ω cm (92±4 Ω sq−1, 25 μm), 是纯炭黑涂层电阻率(0.77±0.01 Ω cm)的30%. 辊压处理后, 电阻率降至0.18±0.01 Ω cm (72±4 Ω sq−1, 25 μm), 且涂层具有良好的机械柔性, 经过3000次循环弯折试验后电阻仅增加12%. 最后, 我们将石墨烯/炭黑复合涂层作为柔性导体, 成功组装了发光书签和薄膜开关, 表明该涂层在柔性电子器件大规模生产中具有巨大的潜力.

Notes

Acknowledgements

This research was supported by the Scientific and Technological Key Project of Shanxi Province (MC2016-04 and MC2016-08), Natural Science Foundation of Shanxi Province (201801D221156), DNL Cooperation Fund of CAS (DNL180308), Science and Technology Service Network Initiative of CAS (KFJ-STS-ZDTP-068), and Youth Innovation Promotion Association of CAS.

Conflict of interest The authors declare no conflict of interest.

Supplementary material

40843_2019_1210_MOESM1_ESM.pdf (3.7 mb)
One-Pot Ball-Milling Preparation of Graphene/Carbon Black Aqueous Inks for Highly Conductive and Flexible Printed Electronics

References

  1. 1.
    Singh R, Singh E, Nalwa HS. Inkjet printed nanomaterial based flexible radio frequency identification (RFID) tag sensors for the internet of nano things. RSC Adv, 2017, 7: 48597–48630CrossRefGoogle Scholar
  2. 2.
    Wood V, Panzer MJ, Chen J, et al. Inkjet-printed quantum dot-polymer composites for full-color AC-driven displays. Adv Mater, 2009, 21: 2151–2155CrossRefGoogle Scholar
  3. 3.
    Wu B, Zhang X, Huang B, et al. High-performance wireless ammonia gas sensors based on reduced graphene oxide and nano-silver ink hybrid material loaded on a patch antenna. Sensors, 2017, 17: 2070CrossRefGoogle Scholar
  4. 4.
    Cinti S, Arduini F. Graphene-based screen-printed electrochemical (bio)sensors and their applications: Efforts and criticisms. Biosens Bioelectron, 2017, 89: 107–122CrossRefGoogle Scholar
  5. 5.
    Secor EB, Dos Santos MH, Wallace SG, et al. Tailoring the porosity and microstructure of printed graphene electrodes via polymer phase inversion. J Phys Chem C, 2018, 122: 13745–13750CrossRefGoogle Scholar
  6. 6.
    Secor EB, Gao TZ, Dos Santos MH, et al. Combustion-assisted photonic annealing of printable graphene inks via exothermic binders. ACS Appl Mater Interfaces, 2017, 9: 29418–29423CrossRefGoogle Scholar
  7. 7.
    Naik AR, Kim JJ, Usluer Ö, et al. Direct printing of graphene electrodes for high-performance organic inverters. ACS Appl Mater Interfaces, 2018, 10: 15988–15995CrossRefGoogle Scholar
  8. 8.
    Sirringhaus H, Kawase T, Friend RH, et al. High-resolution inkjet printing of all-polymer transistor circuits. Science, 2000, 290: 2123–2126CrossRefGoogle Scholar
  9. 9.
    Huang X, Leng T, Zhang X, et al. Binder-free highly conductive graphene laminate for low cost printed radio frequency applications. Appl Phys Lett, 2015, 106: 203105CrossRefGoogle Scholar
  10. 10.
    Huang X, Leng T, Zhu M, et al. Highly flexible and conductive printed graphene for wireless wearable communications applications. Sci Rep, 2016, 5: 18298CrossRefGoogle Scholar
  11. 11.
    Tran TS, Dutta NK, Choudhury NR. Graphene inks for printed flexible electronics: Graphene dispersions, ink formulations, printing techniques and applications. Adv Colloid Interface Sci, 2018, 261: 41–61CrossRefGoogle Scholar
  12. 12.
    Kamyshny A, Magdassi S. Conductive nanomaterials for printed electronics. Small, 2014, 10: 3515–3535CrossRefGoogle Scholar
  13. 13.
    Secor EB, Gao TZ, Islam AE, et al. Enhanced conductivity, adhesion, and environmental stability of printed graphene inks with nitrocellulose. Chem Mater, 2017, 29: 2332–2340CrossRefGoogle Scholar
  14. 14.
    Hu G, Kang J, Ng LWT, et al. Functional inks and printing of two-dimensional materials. Chem Soc Rev, 2018, 47: 3265–3300CrossRefGoogle Scholar
  15. 15.
    Barragán-Iglesias P, Lou TF, Bhat VD, et al. Inhibition of poly(A)-binding protein with a synthetic RNA mimic reduces pain sensitization in mice. Nat Commun, 2018, 9: 10–38CrossRefGoogle Scholar
  16. 16.
    Zhao J, Song M, Wen C, et al. Microstructure-tunable highly conductive graphene-metal composites achieved by inkjet printing and low temperature annealing. J Micromech Microeng, 2018, 28: 035006CrossRefGoogle Scholar
  17. 17.
    Magdassi S, Grouchko M, Kamyshny A. Copper nanoparticles for printed electronics: Routes towards achieving oxidation stability. Materials, 2010, 3: 4626–4638CrossRefGoogle Scholar
  18. 18.
    Rösch R, Tanenbaum DM, Jørgensen M, et al. Investigation of the degradation mechanisms of a variety of organic photovoltaic devices by combination of imaging techniques—the ISOS-3 inter-laboratory collaboration. Energy Environ Sci, 2012, 5: 6521–6540CrossRefGoogle Scholar
  19. 19.
    Su C, Bu X, Xu L, et al. A novel LiFePO4/graphene/carbon composite as a performance-improved cathode material for lithium-ion batteries. Electrochim Acta, 2012, 64: 190–195CrossRefGoogle Scholar
  20. 20.
    Murr LE. Nanoparticulate materials in antiquity: The good, the bad and the ugly. Mater Charact, 2009, 60: 261–270CrossRefGoogle Scholar
  21. 21.
    Khandavalli S, Park JH, Kariuki NN, et al. Rheological investigation on the microstructure of fuel cell catalyst inks. ACS Appl Mater Interfaces, 2018, 10: 43610–43622CrossRefGoogle Scholar
  22. 22.
    Youssry M, Madec L, Soudan P, et al. Non-aqueous carbon black suspensions for lithium-based redox flow batteries: rheology and simultaneous rheo-electrical behavior. Phys Chem Chem Phys, 2013, 15: 14476–14486CrossRefGoogle Scholar
  23. 23.
    Jo Y, Kim JY, Kim SY, et al. 3D-printable, highly conductive hybrid composites employing chemically-reinforced, complex dimensional fillers and thermoplastic triblock copolymers. Nanoscale, 2017, 9: 5072–5084CrossRefGoogle Scholar
  24. 24.
    Youssry M, Kamand FZ, Magzoub MI, et al. Aqueous dispersions of carbon black and its hybrid with carbon nanofibers. RSC Adv, 2018, 8: 32119–32131CrossRefGoogle Scholar
  25. 25.
    Latil S, Henrard L. Electric field effect in atomically thin carbon films. Science, 2004, 306: 666–669CrossRefGoogle Scholar
  26. 26.
    Raccichini R, Varzi A, Passerini S, et al. The role of graphene for electrochemical energy storage. Nat Mater, 2014, 14: 271–279CrossRefGoogle Scholar
  27. 27.
    Hernandez Y, Lotya M, Rickard D, et al. Measurement of multi-component solubility parameters for graphene facilitates solvent discovery. Langmuir, 2010, 26: 3208–3213CrossRefGoogle Scholar
  28. 28.
    Novoselov KS, Fal’ko VI, Colombo L, et al. A roadmap for graphene. Nature, 2012, 490: 192–200CrossRefGoogle Scholar
  29. 29.
    Arapov K, Jaakkola K, Ermolov V, et al. Graphene screen-printed radio-frequency identification devices on flexible substrates. Phys Status Solidi RRL, 2016, 10: 812–818CrossRefGoogle Scholar
  30. 30.
    Arapov K, Rubingh E, Abbel R, et al. Conductive screen printing inks by gelation of graphene dispersions. Adv Funct Mater, 2016, 26: 586–593CrossRefGoogle Scholar
  31. 31.
    Hyun WJ, Secor EB, Hersam MC, et al. High-resolution patterning of graphene by screen printing with a silicon stencil for highly flexible printed electronics. Adv Mater, 2015, 27: 109–115CrossRefGoogle Scholar
  32. 32.
    Zabek D, Seunarine K, Spacie C, et al. Graphene ink laminate structures on poly(vinylidene difluoride) (PVDF) for pyroelectric thermal energy harvesting and waste heat recovery. ACS Appl Mater Interfaces, 2017, 9: 9161–9167CrossRefGoogle Scholar
  33. 33.
    Xu Y, Hennig I, Freyberg D, et al. Inkjet-printed energy storage device using graphene/polyaniline inks. J Power Sources, 2014, 248: 483–488CrossRefGoogle Scholar
  34. 34.
    Wang R, Li W, Liu L, et al. Carbon black/graphene-modified aluminum foil cathode current collectors for lithium ion batteries with enhanced electrochemical performances. J Electroanal Chem, 2019, 833: 63–69CrossRefGoogle Scholar
  35. 35.
    Cai J, Hu N, Wu L, et al. Preparing carbon black/graphene/PVDF-HFP hybrid composite films of high piezoelectricity for energy harvesting technology. Compos Part A-Appl Sci Manufact, 2019, 121: 223–231CrossRefGoogle Scholar
  36. 36.
    Ji A, Chen Y, Wang X, et al. Inkjet printed flexible electronics on paper substrate with reduced graphene oxide/carbon black ink. J Mater Sci-Mater Electron, 2018, 29: 13032–13042CrossRefGoogle Scholar
  37. 37.
    Chen Y, Zhou L, Wei J, et al. Direct ink writing of flexible electronics on paper substrate with graphene/polypyrrole/carbon black ink. J Elec Materi, 2019, 48: 3157–3168CrossRefGoogle Scholar
  38. 38.
    Hua C, Li X, Shen L, et al. Influence of co-solvent hydroxyl group number on properties of water-based conductive carbon pastes. Particuology, 2017, 33: 35–41CrossRefGoogle Scholar
  39. 39.
    Lin X, Zhang K, Li K, et al. Dependence of rheological behaviors of polymeric composites on the morphological structure of carbonaceous nanoparticles. J Appl Polym Sci, 2018, 135: 46416CrossRefGoogle Scholar
  40. 40.
    Chakraborty G, Gupta A, Pugazhenthi G, et al. Facile dispersion of exfoliated graphene/PLA nanocomposites via in situ poly-condensation with a melt extrusion process and its rheological studies. J Appl Polym Sci, 2018, 135: 46476CrossRefGoogle Scholar
  41. 41.
    Mao T, Tang Y, Zhang Y, et al. Carbon nanotubes/polyaniline nanocomposite coatings: Preparation, rheological behavior, and their application in paper surface treatment. J Appl Polym Sci, 2018, 135: 46329CrossRefGoogle Scholar
  42. 42.
    Eom Y, Kim F, Yang SE, et al. Rheological design of 3D printable all-inorganic inks using BiSbTe-based thermoelectric materials. J Rheology, 2019, 63: 291–304CrossRefGoogle Scholar
  43. 43.
    Wang S, Zhong Y, Fang H. Deformation characteristics of a single droplet driven by a piezoelectric nozzle of the drop-on-demand inkjet system. J Fluid Mech, 2019, 869: 634–645CrossRefGoogle Scholar
  44. 44.
    Kitsomboonloha R, Morris SJS, Rong X, et al. Femtoliter-scale patterning by high-speed, highly scaled inverse gravure printing. Langmuir, 2012, 28: 16711–16723CrossRefGoogle Scholar
  45. 45.
    Taroni M, Breward CJW, Howell PD, et al. Boundary conditions for free surface inlet and outlet problems. J Fluid Mech, 2012, 708: 100–110CrossRefGoogle Scholar
  46. 46.
    Su FY, You C, He YB, et al. Flexible and planar graphene conductive additives for lithium-ion batteries. J Mater Chem, 2010, 20: 9644–9650CrossRefGoogle Scholar
  47. 47.
    Ruschau GR, Yoshikawa S, Newnham RE. Resistivities of conductive composites. J Appl Phys, 1992, 72: 953–959CrossRefGoogle Scholar
  48. 48.
    Hof F, Kampioti K, Huang K, et al. Conductive inks of graphitic nanoparticles from a sustainable carbon feedstock. Carbon, 2017, 111: 142–149CrossRefGoogle Scholar
  49. 49.
    Jason Jan C, Walton MD, McConnell EP, et al. Carbon black thin films with tunable resistance and optical transparency. Carbon, 2006, 44: 1974–1981CrossRefGoogle Scholar
  50. 50.
    Lu H, Liu Y, Gou J, et al. Electroactive shape-memory polymer nanocomposites incorporating carbon nanofiber paper. Int J Smart Nano Mater, 2010, 1: 2–12CrossRefGoogle Scholar
  51. 51.
    Pahalagedara LR, Siriwardane IW, Tissera ND, et al. Carbon black functionalized stretchable conductive fabrics for wearable heating applications. RSC Adv, 2017, 7: 19174–19180CrossRefGoogle Scholar
  52. 52.
    Jimenez MJM, de Oliveira RF, Bufon CCB, et al. Enhanced mobility and controlled transparency in multilayered reduced graphene oxide quantum dots: a charge transport study. Nanotechnology, 2019, 30: 275701CrossRefGoogle Scholar
  53. 53.
    Yu S, Wang X, Xiang H, et al. 1-D polymer ternary composites: Understanding materials interaction, percolation behaviors and mechanism toward ultra-high stretchable and super-sensitive strain sensors. Sci China Mater, 2019, 62: 995–1004CrossRefGoogle Scholar
  54. 54.
    Zhang Q, Xu Y, Yang Y, et al. Conductive mechanism of carbon black/polyimide composite films. J Polymer Eng, 2018, 38: 147–156CrossRefGoogle Scholar

Copyright information

© Science China Press and Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  • Xiao Yang (杨晓)
    • 1
    • 2
  • Xiao-Ming Li (李晓明)
    • 1
  • Qing-Qiang Kong (孔庆强)
    • 1
    • 2
  • Zhuo Liu (刘卓)
    • 1
  • Jing-Peng Chen (陈景鹏)
    • 1
    • 2
  • Hui Jia (贾辉)
    • 1
    • 2
  • Yan-Zhen Liu (刘燕珍)
    • 1
  • Li-Jing Xie (谢莉婧)
    • 1
  • Cheng-Meng Chen (陈成猛)
    • 1
    Email author
  1. 1.CAS Key Laboratory of Carbon Materials, Institute of Coal ChemistryChinese Academy of SciencesTaiyuanChina
  2. 2.University of Chinese Academy of SciencesBeijingChina

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