, Volume 26, Issue 16, pp 8867–8875 | Cite as

Mulberry-paper-based composites for flexible electronics and energy storage devices

  • Youngjae Seo
  • Byungil HwangEmail author
Original Research


Mulberry paper comprising holocellulose shows excellent mechanical and chemical stability suitable for paper-based electronics. However, most studies pertaining to paper-based electronics have used conventional paper. Therefore, in this study, we demonstrated Ag nanoparticle (AgNP)/Ag nanowire (AgNW) flexible composites on mulberry-paper substrates. The AgNP/AgNW composites were fabricated by the dry transfer method, where the AgNP/AgNW layers were transferred from a polymer substrate with a hydrophobic surface to the toner-printed mulberry paper via hot pressing. Microstructural analysis showed that the mulberry papers contained thicker fibres than those in conventional papers, which limited the uniform transfer of the AgNP/AgNW layers on the mulberry papers. Therefore, we optimised the hot pressing conditions to 30 MPa and 80 °C, which allowed for the successful formation of the AgNP/AgNW composites on mulberry papers. Cyclic bending test results over 10,000 cycles revealed that the mulberry-paper-based composites showed better mechanical reliability with 30–40% smaller increases in resistance compared to those in conventional A4-paper-based composites. Lastly, a flexible supercapacitor fabricated using the mulberry-paper-based composite as the current collector showed excellent reliability without significant capacitance degradation over 100 bending cycles.

Graphic abstract


Mulberry paper Holocellulose Composite Flexible Silver Nanowire 



This Research was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2018R1C1B5043900).

Supplementary material

10570_2019_2686_MOESM1_ESM.pdf (379 kb)
Supplementary material 1 (PDF 379 kb)


  1. An C-H, Kim S, Lee H-J, Hwang B (2017) Facile patterning using dry film photo-resists for flexible electronics: Ag nanowire networks and carbon nanotube networks. J Mater Chem C 5:4804–4809CrossRefGoogle Scholar
  2. Chan CH, Chia CH, Zakaria S, Sajab MS, Chin SX (2015) Cellulose nanofibrils: a rapid adsorbent for the removal of methylene blue. RSC Adv 5:18204–18212CrossRefGoogle Scholar
  3. Choi S-H, Kwon O-H, Kim H-C (2013) Study on process conditions for automatic debarking and xylem separator for paper mulberry. J Korea Tech Assoc Pulp Pap Ind 45:36–44CrossRefGoogle Scholar
  4. Damnalı OF, Eskizeybek V (2019) Synergistic impact of graphene and carbon nanotubes on waste paper for hybrid nanocomposite substrates. Cellulose 26:3935–3954CrossRefGoogle Scholar
  5. Durairaj A, Sakthivel T, Ramanathan S, Obadiah A, Vasanthkumar S (2019) Conversion of laboratory paper waste into useful activated carbon: a potential supercapacitor material and a good adsorbent for organic pollutant and heavy metals. Cellulose 26:3313–3324CrossRefGoogle Scholar
  6. Eder F, Klauk H, Halik M, Zschieschang U, Schmid G, Dehm C (2004) Organic electronics on paper. Appl Phys Lett 84:2673–2675CrossRefGoogle Scholar
  7. Gwon H et al (2011) Flexible energy storage devices based on graphene paper. Energy Environ Sci 4:1277–1283CrossRefGoogle Scholar
  8. Hunt WH (2004) Global perspectives on electronic materials: challenges and opportunities. JOM 56:17–21CrossRefGoogle Scholar
  9. Hwang B, Yun TG (2019) Stretchable and patchable composite electrode with trimethylolpropane formal acrylate-based polymer. Compos B Eng 163:185–192CrossRefGoogle Scholar
  10. Hwang B, Shin H-A-S, Kim T, Joo Y-C, Han SM (2014) Highly reliable Ag nanowire flexible transparent electrode with mechanically welded junctions. Small 10:3397–3404CrossRefGoogle Scholar
  11. Hwang B, An C-H, Becker S (2017a) Highly robust Ag nanowire flexible transparent electrode with UV-curable polyurethane-based overcoating layer. Mater Des 129:180–185CrossRefGoogle Scholar
  12. Hwang B, An Y, Lee H, Lee E, Becker S, Kim Y-H, Kim H (2017b) Highly flexible and transparent Ag nanowire electrode encapsulated with ultra-thin Al2O3: thermal, ambient, and mechanical stabilities. Sci Rep 7:41336CrossRefPubMedPubMedCentralGoogle Scholar
  13. Hwang B et al (2017c) Role of graphene in reducing fatigue damage in Cu/Gr nanolayered composite. Nano Lett 17:4740–4745CrossRefGoogle Scholar
  14. Jaehwan K, Yung BS (2002) Electro-active paper actuators. Smart Mater Struct 11:355CrossRefGoogle Scholar
  15. Jung YH et al (2015) High-performance green flexible electronics based on biodegradable cellulose nanofibril paper. Nat Commun 6:7170CrossRefPubMedPubMedCentralGoogle Scholar
  16. Kee S et al (2018) Highly deformable and see-through polymer light-emitting diodes with all-conducting-polymer electrodes. Adv Mater 30:1703437CrossRefGoogle Scholar
  17. Kim S, Hwang B (2018) Ag nanowire electrode with patterned dry film photoresist insulator for flexible organic light-emitting diode with various designs. Mater Des 160:572–577CrossRefGoogle Scholar
  18. Kim B-J et al (2012) Fatigue-free, electrically reliable copper electrode with nanohole array. Small 8:3300–3306CrossRefGoogle Scholar
  19. Kim B-J, Shin H-AS, Jung S-Y, Cho Y, Kraft O, Choi I-S, Joo Y-C (2013a) Crack nucleation during mechanical fatigue in thin metal films on flexible substrates. Acta Mater 61:3473–3481CrossRefGoogle Scholar
  20. Kim T, Canlier A, Kim GH, Choi J, Park M, Han SM (2013b) Electrostatic spray deposition of highly transparent silver nanowire electrode on flexible substrate. ACS Appl Mater Interfaces 5:788–794CrossRefPubMedPubMedCentralGoogle Scholar
  21. Kim D, Ko Y, Kwon G, Kim U-J, You J (2018a) Micropatterning silver nanowire networks on cellulose nanopaper for transparent paper electronics. ACS Appl Mater Interfaces 10:38517–38525CrossRefPubMedPubMedCentralGoogle Scholar
  22. Kim S et al (2018b) Facile fabrication of paper-based silver nanostructure electrodes for flexible printed energy storage system. Mater Des 151:1–7CrossRefGoogle Scholar
  23. Ko Y, Kim D, Kim U-J, You J (2017a) Vacuum-assisted bilayer PEDOT:pSS/cellulose nanofiber composite film for self-standing, flexible, conductive electrodes. Carbohydr Polym 173:383–391CrossRefGoogle Scholar
  24. Ko Y, Kwon M, Bae WK, Lee B, Lee SW, Cho J (2017b) Flexible supercapacitor electrodes based on real metal-like cellulose papers. Nat Commun 8:536CrossRefPubMedPubMedCentralGoogle Scholar
  25. Lee BH, Ng MZ, Zinn AA, Gan CL (2015) Evaluation of copper nanoparticles for low temperature bonded interconnections. In: 2015 IEEE 22nd international symposium on the physical and failure analysis of integrated circuits, 29 June–2 July 2015, pp 102–106.
  26. Lee C, Kim H, Hwang B (2019) Fracture behavior of metal oxide/silver nanowire composite electrodes under cyclic bending. J Alloys Compd 773:361–366CrossRefGoogle Scholar
  27. Martins R, Ferreira I, Fortunato E (2011) Electronics with and on paper. Phys Status Solidi (RRL) Rapid Res Lett 5:332–335CrossRefGoogle Scholar
  28. Nilghaz A, Liu X, Ma L, Huang Q, Lu X (2019) Development of fabric-based microfluidic devices by wax printing. Cellulose 26:3589–3599CrossRefGoogle Scholar
  29. Park J et al (2012) Three-dimensional nanonetworks for giant stretchability in dielectrics and conductors. Nat Commun 3:916CrossRefGoogle Scholar
  30. Park J, Choi K, Cho B (2017) Evaluation of low-temperature cooking of paper mulberry bast fiber with potassium based cooking chemicals. J Korea Tech Assoc Pulp Pap Ind 49:35–40CrossRefGoogle Scholar
  31. Park M, Kim W, Hwang B, Han SM (2019) Effect of varying the density of Ag nanowire networks on their reliability during bending fatigue. Scr Mater 161:70–73CrossRefGoogle Scholar
  32. Qaiser N, Khan SM, Hussain MM (2018) In-plane and out-of-plane structural response of spiral interconnects for highly stretchable electronics. J Appl Phys 124:034905CrossRefGoogle Scholar
  33. Shimizu M, Kusumi R, Saito T, Isogai A (2019) Thermal and electrical properties of nanocellulose films with different interfibrillar structures of alkyl ammonium carboxylates. Cellulose 26:1657–1665CrossRefGoogle Scholar
  34. Siegel AC, Phillips ST, Dickey MD, Lu N, Suo Z, Whitesides GM (2010) Foldable printed circuit boards on paper substrates. Adv Funct Mater 20:28–35CrossRefGoogle Scholar
  35. Striemer CC, Krishnan R, Fauchet PM (2004) The development of nanocrystalline silicon for emerging microelectronic and nanoelectronic applications. JOM 56:20–25CrossRefGoogle Scholar
  36. Sumboja A, Foo CY, Wang X, Lee PS (2013) Large areal mass, flexible and free-standing reduced graphene oxide/manganese dioxide paper for asymmetric supercapacitor device. Adv Mater 25:2809–2815CrossRefGoogle Scholar
  37. Tao C, Yen C-S, Liu J-T, Chen C-J (2016) Analytical performance of paper electro-biosensor detection platform for point-of-care diagnosis. Cellulose 23:3799–3808CrossRefGoogle Scholar
  38. Tobjörk D, Österbacka R (2011) Paper electronics. Adv Mater 23:1935–1961CrossRefGoogle Scholar
  39. Wang K, Jiang J, Xu J, Feng J, Wang J (2016) Effective saccharification of holocellulose over multifunctional sulfonated char with fused ring structures under microwave irradiation. RSC Adv 6:14164–14170CrossRefGoogle Scholar
  40. Wei C, Fan L, Rao W, Bai Z, Xu W, Bao H, Xu J (2017) Electrothermochromic paper fabricated by depositing polypyrrole on one side. Cellulose 24:5187–5196CrossRefGoogle Scholar
  41. Wong WSY, Stachurski ZH, Nisbet DR, Tricoli A (2016) Ultra-durable and transparent self-cleaning surfaces by large-scale self-assembly of hierarchical interpenetrated polymer networks. ACS Appl Mater Interfaces 8:13615–13623CrossRefPubMedPubMedCentralGoogle Scholar
  42. Yao Y et al (2016) Light management in plastic–paper hybrid substrate towards high-performance optoelectronics. Energy Environ Sci 9:2278–2285CrossRefGoogle Scholar
  43. Yun TG, Kim D, Kim S-M, Kim I-D, Hyun S, Han SM (2018) Mulberry paper-based supercapacitor exhibiting high mechanical and chemical toughness for large-scale energy storage applications. Adv Energy Mater 8:1800064CrossRefGoogle Scholar
  44. Zheng Y, He Z, Gao Y, Liu J (2013) Direct desktop printed-circuits-on-paper flexible electronics. Sci Rep 3:1786CrossRefPubMedPubMedCentralGoogle Scholar

Copyright information

© Springer Nature B.V. 2019

Authors and Affiliations

  1. 1.School of Integrative EngineeringChung-Ang UniversitySeoulRepublic of Korea

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