Journal of Thin Films, Coating Science Technology & Application Review Article

Advancing Conductive Ink Formulations for DIW with Graphene and Hybrid Nanostructures

  1. Jhunjhun Kumar Mishra School of Mech Engineering, Lovely Professional University
  2. Vishal Francis School of Mech Engineering, Lovely Professional University

Abstract

The development of solvent-based conductive inks for direct ink writing (DIW) has gained significant attention as a pathway toward flexible, wearable, and scalable electronic devices. This review critically examines conductive fillers, binders, solvent systems, and hybrid ink strategies reported in recent literature. Graphene and carbon nanotubes (CNTs) remain the most studied fillers due to their high intrinsic conductivity and unique dimensionality, but challenges such as restacking, bundling, and high viscosity necessitate dispersion control and optimized formulations. Binder materials play a decisive role in balancing dispersion stability with electrical performance: polyvinylpyrrolidone (PVP) consistently demonstrates superior stabilization at low concentrations compared to insulating binders such as polyvinyl alcohol (PVA) or brittle systems such as sodium silicate. Similarly, solvent selection is critical for DIW compatibility; ethanol-based systems require modification with ethylene glycol (EG) or terpineol to mitigate aggregation, suppress coffee-ring effects, and ensure rheological suitability. A key advancement highlighted in this review is the adoption of hybrid fillers, particularly graphene-CNT and graphene-Ag systems, which leverage synergistic conduction pathways to achieve conductivities in the range of 10³–10⁴ S/cm while maintaining flexibility. Literature consistently confirms that hybrid conductive inks, when stabilized with ≤3 wt% PVP in ethanol-EG or ethanol-terpineol blends, outperform single-filler systems in both conductivity and mechanical durability. Overall, hybrid architecture emerge as the most promising route for DIW-enabled printed electronics, providing a balance of printability, stability, and high electrical performance suitable for next-generation applications.

Keywords

References (40)

  1. Bastola AK, Paudel M, Dasari TRT, Shrestha M. Direct ink writing of multifunctional inks for printed electronics: Materials, rheology, and device integration. Mater Today Electron. 2023; 6: 100058.
  2. Hong H, Jiang L, Tu H, Zhang J, Xu S. Formulation of UV curable nano-silver conductive ink for direct screen-printing on common fabric substrates for wearable electronic applications. Smart Mater Struct. 2021; 30(4): 045001.
  3. Huang Q, Zhu Y. Printing conductive nanomaterials for flexible and stretchable electronics: A review of materials, processes, and applications. Adv Mater Technol. 2019; 4(3): 1800546.
  4. Ibrahim N, Akindoyo JO, Mariatti M. Recent advances in conductive polymer nanocomposites for flexible electronics: Processing, properties, and applications. J Sci: Adv Mater Devices. 2021; 7: 100395.
  5. Karagiannidis PG, Hill EW, Lin C-T, et al. Microfluidization of graphite and formulation of stable graphene inks for printed electronics. ACS Nano. 2017; 11(3): 2742–2755.
  6. Karim N, Afroj S, Tan S, Novoselov KS, Yeates SG. All inkjet-printed graphene-based conductive patterns for wearable e-textile applications. Sci Rep. 2019; 9: 8035.
  7. Liu L, Zhang Y, Wu H, et al. Understanding the dispersion and electrical properties of carbon black/graphene hybrid nanomaterials in conductive inks. J Colloid Interface Sci. 2021; 582: 12–21.
  8. Phillips C, Al-Ahmadi A, Potts SJ, Claypole T, Deganello D. The role of polymer binders in the formulation of carbon-based conductive inks for screen printing. J Mater Sci. 2017; 52: 9520–9530.
  9. Saidina DS, Eawwiboonthanakit N, Mariatti M, et al. Effect of polymeric binders on the performance of graphene-based conductive inks for flexible electronics. J Electron Mater. 2019; 48(6): 3428–3450.
  10. Tran TS, Dutta NK, Choudhury NR. Graphene inks for printed flexible electronics: A review of formulation, rheology, stability, and applications. Adv Colloid Interface Sci. 2018; 261: 41–61.
  11. Zhang J, Ahmadi M, Fargas G, et al. Recent advances in metallic inks for additive manufacturing of flexible electronics. Metals. 2022; 12(2): 234.
  12. Huang L, Huang Y, Liang J, Wan X, Chen Y. Graphene-based conducting inks for direct inkjet printing of flexible conductive patterns and their applications in electric circuits and chemical sensors. Nano Research. 2011;4(7):675-684. doi:10.1007/s12274-011-0123-z
  13. Karim N, Afroj S, Tan S, Novoselov KS, Yeates SG. All Inkjet-Printed Graphene-Silver Composite Ink on Textiles for Highly Conductive Wearable Electronics Applications. Scientific Reports. 2019;9(1). doi:10.1038/s41598-019-44420-y
  14. Eghan B, Ofori EA, Seidu RK, Tawiah B, Acquaye R. Systematic Review of Conductive Inks for E-textiles: Formulation, Printing Methods, Challenges, and Opportunities. AATCC Journal of Research. 2025;12(1). doi:10.1177/24723444241303970
  15. Boumegnane A, Nadi A, Cochrane C, et al. Formulation of conductive inks printable on textiles for electronic applications: A review. Text Prog. 2022; 54(2): 103–200.
  16. Camargo JR, Orzari LO, Araújo DAG, et al. Development of conductive inks for electrochemical sensors and biosensors. Microchem J. 2021; 164: 105998.
  17. Saidina DS, Eawwiboonthanakit N, Mariatti M, et al. Recent development of graphene-based ink and other conductive material-based inks for flexible electronics. J Electron Mater. 2019; 48(6): 3428–3450.
  18. Hong H, Jiang L, Tu H, et al. Formulation of UV curable nano-silver conductive ink for direct screen-printing on common fabric substrates for wearable electronic applications. Smart Mater Struct. 2021; 30(4): 045001.
  19. Karagiannidis PG, Hill EW, Lin C-T, et al. Microfluidization of graphite and formulation of graphene-based conductive inks. ACS Nano. 2017; 11(3): 2742–2755.
  20. Shankar R, Groven L, Amert A, Whites KW, Kellar JJ. Non-aqueous synthesis of silver nanoparticles using tin acetate as a reducing agent for the conductive ink formulation in printed electronics. Journal of Materials Chemistry. 2011;21(29):10871. doi:10.1039/c0jm04521g
  21. Yaqoob AA, Umar K, Ibrahim MNM. Silver nanoparticles: Various methods of synthesis, size affecting factors and their potential applications—A review. Appl Nanosci. 2020; 10(5): 1369–1378.
  22. Kamyshny A, Magdassi S. Conductive nanomaterials for 2D and 3D printed flexible electronics. Chemical Society Reviews. 2019;48(6):1712-1740. doi:10.1039/c8cs00738a
  23. Ibrahim N, Akindoyo JO, Mariatti M. Recent development in silver-based ink for flexible electronics. J Sci: Adv Mater Devices. 2021; 7(1): 100395.
  24. Kholuiskaya SN, Siracusa V, Mukhametova GM, Wasserman LA, Kovalenko VV, Iordanskii AL. An Approach to a Silver Conductive Ink for Inkjet Printer Technology. Polymers. 2024;16(12):1731. doi:10.3390/polym16121731
  25. Bastola AK, et al. Formulation of functional materials for inkjet printing: A pathway towards fully 3D printed electronics. Mater Today Electron. 2023; 6: 100058.
  26. Htwe YZN, Mariatti M. Performance of water-based printed hybrid graphene/silver nanoparticle conductive inks for flexible strain sensor applications. Synth Met. 2023; 300: 117495.
  27. Phillips C, Al-Ahmadi A, Potts SJ, Claypole T, Deganello D. The effect of graphite and carbon black ratios on conductive ink performance. Journal of Materials Science. 2017;52(16):9520-9530. doi:10.1007/s10853-017-1114-6
  28. Saidina DS, Mariatti M, Zubir SA, Fontana S, Hérold C. Performance of graphene hybrid-based ink for flexible electronics. Journal of Materials Science: Materials in Electronics. 2019;30(22):19906-19916. doi:10.1007/s10854-019-02357-y
  29. Zhao C, Wang J, Qian B, Zhang Z. Preparation of paper-based conductive pattern for 3D printing. J Phys: Commun. 2023; 7(3): 035003.
  30. Guan LS. Application and research status of graphene conductive ink. Mod Chem Res. 2018; 12: 137–139.
  31. Liu L, Zhang Y, Wu H, et al. Highly conductive graphene/carbon black screen-printing inks for flexible electronics. J Colloid Interface Sci. 2021; 582: 12–21.
  32. Htwe YZN, et al. Performance of inkjet-printed strain sensor based on graphene/silver nanoparticles hybrid conductive inks on polyvinyl alcohol substrate. J Mater Sci: Mater Electron. 2020; 31: 15361–15371.
  33. Zhou F, et al. 3D printing of free-standing and flexible nitrogen-doped graphene/polyaniline electrode for electrochemical energy storage. Chem Phys Lett. 2019; 728: 6–13.
  34. Kant T, et al. Flexible printed paper electrode with silver nano-ink for electrochemical applications. Microchem J. 2020; 155: 104687.
  35. Kwon YJ, Kim Y, Jeon H, Cho S, Lee W, Lee JU. Graphene/carbon nanotube hybrid as a multi-functional interfacial reinforcement for carbon fiber-reinforced composites. Composites Part B: Engineering. 2017;122:23-30. doi:10.1016/j.compositesb.2017.04.005
  36. Xu LY, Yang GY, Jing HY, Wei J, Han YD. Ag–graphene hybrid conductive ink for writing electronics. Nanotechnology. 2014; 25(5): 055201(9p). doi:10.1088/0957–4484/25/5/055201.
  37. Hong Z, Zheng Z, Kong L, Zhao L, Liu S, Li W, et al. Welded Carbon Nanotube–Graphene Hybrids with Tunable Strain Sensing Behavior for Wide-Range Bio-Signal Monitoring. Polymers. 2024;16(2):238. doi:10.3390/polym16020238
  38. Wang J, Li L, Liu H, Hou Q. Graphene/Carbon Nanotube Conductive Ink-Based Biomimetic Structure for Self-Powered Flexible Medical Monitoring Devices. ACS Applied Nano Materials. 2024;7(2):1863-1875. doi:10.1021/acsanm.3c05095
  39. Htwe YZN, Mariatti M. Printed graphene and hybrid conductive inks for flexible, stretchable, and wearable electronics: Progress, opportunities, and challenges. J Sci: Adv Mater Devices. 2022; 7(2): 100435.
  40. Kien-Cuong Pham, McPhailDavid S, Cecilia Mattevi, Wee Andrew TS, Chua Daniel HC. Graphene-Carbon Nanotube Hybrids as Robust Catalyst Supports in Proton Exchange Membrane Fuel Cells. J Electrochem Soc. 2016; 163(3): F255–F263.
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