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Stretchable flexible electrodes based on in situ coating of graphite with PANI

Yan Peng1, §, Siyu Xie1, §, Xiaofan Zhu1, Yuke Deng3, Weiwei Guo1, Yuxiao Zhang2, and Yue Liu1,

+ Author Affiliations

 Corresponding author: Yuxiao Zhang, 1310114565@qq.com; Yue Liu, liuyue2023@kust.edu.cn

DOI: 10.1088/1674-4926/26060029CSTR: 32376.14.1674-4926.26060029

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Abstract: Stretchable bioelectrodes need both conductivity and deformation stability, but the conductive pathways of traditional rigid materials are prone to instability during stretching. In this study, polyaniline coated graphite powder (PANI@G) core shell fillers were constructed through the in situ oxidative polymerization of aniline and were sprayed onto a styrene-ethylene/butylene-styrene block copolymer (SEBS) substrate to prepare stretchable conductive films. The PANI coating layer improved the connection between graphite lamellae through interfacial interactions among nitrogen containing groups, oxygen containing functional groups, and conjugated structures. As a result, the film retained approximately 89% of its initial current at 75% strain, and the current drift was only 2.3% during 126 min of continuous stretching at 50% strain. The film was further patterned into lightweight flexible electrodes and realized electrical signal acquisition induced by electrical stimulation, providing an effective strategy for wearable flexible electrodes.

Keywords: PANI in situ coatinggraphitestretchable flexible electrode



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Sun J L, Tao Q Y, Hua Q L, et al. Self-powered flexible persistent displays for trajectory recognition. Nano Res, 2025, 18(11): 94907951 doi: 10.26599/NR.2025.94907951
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Zhao Q N, Gribkova E, Shen Y Y, et al. Highly stretchable and customizable microneedle electrode arrays for intramuscular electromyography. Sci Adv, 2024, 10(18): eadn7202 doi: 10.1126/sciadv.adn7202
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Wang D W, Li F, Zhao J P, et al. Fabrication of graphene/polyaniline composite paper via in situ anodic electropolymerization for high-performance flexible electrode. ACS Nano, 2009, 3(7): 1745 doi: 10.1021/nn900297m
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Kim H J, Sim K, Thukral A, et al. Rubbery electronics and sensors from intrinsically stretchable elastomeric composites of semiconductors and conductors. Sci Adv, 2017, 3(9): e1701114 doi: 10.1126/sciadv.1701114
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Marchianò V, Tricase A, Caputo M, et al. Tailoring water-based graphite conductive ink formulation for enzyme stencil-printing: Experimental design to enhance wearable biosensor performance. Chem Mater, 2024, 36(1): 358 doi: 10.1021/acs.chemmater.3c02229
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Yang D Z, Wang J C, Cao Y S, et al. Polyaniline-based biological and chemical sensors: Sensing mechanism, configuration design, and perspective. ACS Appl Electron Mater, 2023, 5(2): 593 doi: 10.1021/acsaelm.2c01405
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Feng Z, Wen J Y, Meng F Z, et al. In situ-polymerized PANI/WS2 nanocomposites for highly sensitive flexible ammonia gas sensors and respiration monitoring devices. ACS Appl Nano Mater, 2024, 7(3): 3385 doi: 10.1021/acsanm.3c05965
[23]
Tian X, Cui X X, Xiao Y W, et al. Pt/MoS2/polyaniline nanocomposite as a highly effective room temperature flexible gas sensor for ammonia detection. ACS Appl Mater Interfaces, 2023, 15(7): 9604 doi: 10.1021/acsami.2c20299
[24]
Yang C Q, Wang W W, Zhang D Z, et al. High-sensitivity wearable flexible pressure sensor based on MXene and polyaniline for human motion detection. ACS Appl Polym Mater, 2023, 5(12): 10386 doi: 10.1021/acsapm.3c02175
[25]
Das D, Das J, Debnath A, et al. Polyaniline-graphite on cellulose substrate: A flexible, low-cost, use-and-throw sensor for glucose concentration detection. Cellulose, 2023, 30(10): 6423 doi: 10.1007/s10570-023-05286-6
[26]
Chen C, Tu Q, Zhou X, et al. Flexible, stable and self-powered two-dimensional layered nanocomposites (PANI@MoS2) for trace ammonia gas detection. Adv Compos Hybrid Mater, 2024, 8(1): 98 doi: 10.21203/rs.3.rs-4390151/v1
[27]
Hossain M S, Padmanathan N, Badal M M R, et al. Highly sensitive potentiometric pH sensor based on polyaniline modified carbon fiber cloth for food and pharmaceutical applications. ACS Omega, 2024, 9(38): 40122 doi: 10.1021/acsomega.4c06090.s001
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Kumar N A, Choi H J, Shin Y R, et al. Polyaniline-grafted reduced graphene oxide for efficient electrochemical supercapacitors. ACS Nano, 2012, 6(2): 1715 doi: 10.1021/nn204688c
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Han X, Tao J, Liang Y G, et al. Ultraweak light-modulated heterostructure with bidirectional photoresponse for static and dynamic image perception. Nat Commun, 2024, 15: 10430 doi: 10.1038/s41467-024-54845-3
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[31]
Lv J, Thangavel G, Li Y, et al. Printable elastomeric electrodes with sweat-enhanced conductivity for wearables. Sci Adv, 2021, 7(29): eabg8433 doi: 10.1126/sciadv.abg8433
[32]
Liu Y, Tao J, Mo Y P, et al. Ultrasensitive touch sensor for simultaneous tactile and slip sensing. Adv Mater, 2024, 36(21): 2313857 doi: 10.1002/adma.202313857
[33]
Zhang Y X, Bao R R, Qiu J B, et al. Electrochromic-based visualised flexible biosensing platforms: from single device to multifunctional device integration. Chem Soc Rev, 2025, 54(24): 11827 doi: 10.1039/D5CS00386E
[34]
Zheng Y, Liu T, Wu J P, et al. Energy conversion analysis of multilayered triboelectric nanogenerators for synergistic rain and solar energy harvesting. Adv Mater, 2022, 34(28): 2202238 doi: 10.1002/adma.202202238
[35]
Xu B X, Akhtar A, Liu Y H, et al. An epidermal stimulation and sensing platform for sensorimotor prosthetic control, management of lower back exertion, and electrical muscle activation. Adv Mater, 2016, 28(22): 4462 doi: 10.1002/adma.201504155
Fig. 1.  (Color online) Schematic illustration of the structural design and conductive network construction of PANI@G core shell conductive fillers. (a) PANI is in situ coated on graphite powder to form core shell conductive fillers. (b) π−π interaction between the aromatic units of PANI and the sp2-carbon basal plane of graphite, hydrogen bonding between PANI amine/imine sites and oxygen-containing groups at graphite edge or defect sites and electrostatic interaction between protonated PANI and deprotonated carboxylate sites. (c) Comparative schematic illustration of the conductive network construction modes of graphite powder and PANI@G in an elastic matrix.

Fig. 2.  (Color online) Morphology, structural composition, and electrical properties of PANI@G composite fillers. (a) SEM images of PANI@G with different mass ratios of aniline monomer to graphite powder. (b) SEM images of PANI@G with different mass ratios of APS to aniline. (c) EDS elemental mapping of PANI@G under optimized conditions. (d) XRD patterns of PANI@G and Graphite powders. (e) TGA curves of Graphite powders, PANI, and PANI@G. (f) Comparison of resistivity and conductivity among PANI@G, Graphite powders, and PANI.

Fig. 3.  (Color online) Characterization of the interfacial chemical structure of PANI@G composite fillers. (a) High resolution C 1s, O 1s, and N 1s XPS spectra of PANI@G. (b) FTIR spectra of PANI and PANI@G. (c) Raman spectra of PANI and PANI@G.

Fig. 4.  (Color online) Optical, electrical, and deformation stability of PANI@G/SEBS stretchable conductive films. (a) Transmittance of PANI@G/SEBS films with different PANI@G loadings. (b) Sheet resistance of films with different conductive materials and loadings. (c) Stress strain curves of SEBS and PANI@G/SEBS films. (d) Current responses of films with different PANI@G loadings under 5 V. (e) Current changes of the 20.83 wt% PANI@G/SEBS film under different strains. (f) Comparison of stretching current responses among Graphite powders/SEBS, PANI/SEBS, and PANI@G/SEBS films. (g) Current drift of the 20.83 wt% PANI@G/SEBS film at 50% strain for 126 min. (h) Stress and current changes of the film during one stretching recovery process. (i) Current distribution of the film after 100 cyclic stretching cycles at 30% strain.

Fig. 5.  (Color online) Patterning processing, skin adhesion, and electrical stimulation induced electrical signal acquisition of PANI@G/SEBS flexible electrodes. (a) Schematic illustration of the PANI@G/SEBS flexible electrode structure and its use for skin electrical stimulation induced electrical signal acquisition. (b) Stretching and twisting demonstration of the laser patterned mesh electrode. (c) Conformal adhesion of the lightweight PANI@G/SEBS film on curved skin. (d) Photograph of a patterned electrode lighting bulbs. (e) Electrode geometric patterns and circuit patterns. (f) Electrical signals recorded during continuous, pulse, and intermittent grouped stimulation.

[1]
Kim D H, Lu N S, Ma R, et al. Epidermal electronics. Science, 2011, 333(6044): 838 doi: 10.1126/science.1206157
[2]
Xu H C, Liu Y, Mo Y P, et al. All-fiber anti-jamming capacitive pressure sensors based on liquid metals. Rare Met, 2025, 44(7): 4839 doi: 10.1007/s12598-024-03071-3
[3]
Deng Y K, Zhang Y X, Bai X M, et al. Photoluminescent-electrochromic synergy in passive devices for pressure visualization and multi-level encryption. Adv Funct Mater, 2026, 36(7): e12816 doi: 10.1002/adfm.202512816
[4]
Ma Z, Kong D S, Pan L J, et al. Skin-inspired electronics: emerging semiconductor devices and systems. J Semicond, 2020, 41(4): 041601 doi: 10.1088/1674-4926/41/4/041601
[5]
Meng J J, Sun J L, Zhang W, et al. Phase‐manipulated calcium borate‐based multicolor mechanoluminescence. Adv Mater, 2026, 38(11): e22179 doi: 10.1002/adma.202522179
[6]
O’Neill S J K, Huang Z H, Ahmed M H, et al. Tissue-mimetic supramolecular polymer networks for bioelectronics. Adv Mater, 2023, 35(1): 2207634 doi: 10.1002/adma.202207634
[7]
Zhang Y X, Wang C C, Tao J, et al. Strain-adaptive liquid metal interfaces overcome Poisson’s ratio constraints in piezoresistive sensors for infant sleep monitoring. Adv Sci, 2025, 12(44): e15117 doi: 10.1002/advs.202515117
[8]
Tan P, Wang H F, Xiao F R, et al. Solution-processable, soft, self-adhesive, and conductive polymer composites for soft electronics. Nat Commun, 2022, 13: 358 doi: 10.1038/s41467-022-28027-y
[9]
Liu Z Y, Wang X T, Qi D P, et al. High-adhesion stretchable electrodes based on nanopile interlocking. Adv Mater, 2017, 29(2): 1603382 doi: 10.1002/adma.201603382
[10]
Lee S, Ho D H, Jekal J, et al. Fabric-based lamina emergent MXene-based electrode for electrophysiological monitoring. Nat Commun, 2024, 15: 5974 doi: 10.1038/s41467-024-49939-x
[11]
Sun J L, Tao Q Y, Hua Q L, et al. Self-powered flexible persistent displays for trajectory recognition. Nano Res, 2025, 18(11): 94907951 doi: 10.26599/NR.2025.94907951
[12]
Zhao Q N, Gribkova E, Shen Y Y, et al. Highly stretchable and customizable microneedle electrode arrays for intramuscular electromyography. Sci Adv, 2024, 10(18): eadn7202 doi: 10.1126/sciadv.adn7202
[13]
Wang D W, Li F, Zhao J P, et al. Fabrication of graphene/polyaniline composite paper via in situ anodic electropolymerization for high-performance flexible electrode. ACS Nano, 2009, 3(7): 1745 doi: 10.1021/nn900297m
[14]
Kim H J, Sim K, Thukral A, et al. Rubbery electronics and sensors from intrinsically stretchable elastomeric composites of semiconductors and conductors. Sci Adv, 2017, 3(9): e1701114 doi: 10.1126/sciadv.1701114
[15]
Marchianò V, Tricase A, Caputo M, et al. Tailoring water-based graphite conductive ink formulation for enzyme stencil-printing: Experimental design to enhance wearable biosensor performance. Chem Mater, 2024, 36(1): 358 doi: 10.1021/acs.chemmater.3c02229
[16]
Tricase A, Imbriano A, Valentino M, et al. Water-based conductive ink formulations for enzyme-based wearable biosensors. Adv Sens Res, 2024, 3(3): 2300036 doi: 10.1002/adsr.202300036
[17]
Rahman F, Adhika D R, Mustofa A Z E, et al. Development of flexible medical electrodes using carrageenan-based bioplastics with the addition of conductive hybrid materials graphite and silver nanoparticles. ACS Omega, 2023, 8(49): 47086 doi: 10.1021/acsomega.3c06987
[18]
Ma B, Huang K, Chen G S, et al. A dual-mode wearable sensor with coupled ion and pressure sensing. Soft Sci, 2024, 4(1): 8 doi: 10.20517/ss.2023.41
[19]
Yang D Z, Wang J C, Cao Y S, et al. Polyaniline-based biological and chemical sensors: Sensing mechanism, configuration design, and perspective. ACS Appl Electron Mater, 2023, 5(2): 593 doi: 10.1021/acsaelm.2c01405
[20]
Das J, Debnath A, Deb K, et al. Pressure sensors painted on flexible cellulose substrates from polyaniline-based conductive ink. ACS Appl Electron Mater, 2023, 5(6): 2988 doi: 10.1021/acsaelm.2c01745
[21]
Tang C Y, Xu M Z, Yi W T, et al. Ultrasensitive textile strain sensors redefine wearable silent speech interfaces with high machine learning efficiency. npj Flex Electron, 2024, 8: 27 doi: 10.1038/s41528-024-00315-1
[22]
Feng Z, Wen J Y, Meng F Z, et al. In situ-polymerized PANI/WS2 nanocomposites for highly sensitive flexible ammonia gas sensors and respiration monitoring devices. ACS Appl Nano Mater, 2024, 7(3): 3385 doi: 10.1021/acsanm.3c05965
[23]
Tian X, Cui X X, Xiao Y W, et al. Pt/MoS2/polyaniline nanocomposite as a highly effective room temperature flexible gas sensor for ammonia detection. ACS Appl Mater Interfaces, 2023, 15(7): 9604 doi: 10.1021/acsami.2c20299
[24]
Yang C Q, Wang W W, Zhang D Z, et al. High-sensitivity wearable flexible pressure sensor based on MXene and polyaniline for human motion detection. ACS Appl Polym Mater, 2023, 5(12): 10386 doi: 10.1021/acsapm.3c02175
[25]
Das D, Das J, Debnath A, et al. Polyaniline-graphite on cellulose substrate: A flexible, low-cost, use-and-throw sensor for glucose concentration detection. Cellulose, 2023, 30(10): 6423 doi: 10.1007/s10570-023-05286-6
[26]
Chen C, Tu Q, Zhou X, et al. Flexible, stable and self-powered two-dimensional layered nanocomposites (PANI@MoS2) for trace ammonia gas detection. Adv Compos Hybrid Mater, 2024, 8(1): 98 doi: 10.21203/rs.3.rs-4390151/v1
[27]
Hossain M S, Padmanathan N, Badal M M R, et al. Highly sensitive potentiometric pH sensor based on polyaniline modified carbon fiber cloth for food and pharmaceutical applications. ACS Omega, 2024, 9(38): 40122 doi: 10.1021/acsomega.4c06090.s001
[28]
Kumar N A, Choi H J, Shin Y R, et al. Polyaniline-grafted reduced graphene oxide for efficient electrochemical supercapacitors. ACS Nano, 2012, 6(2): 1715 doi: 10.1021/nn204688c
[29]
Han X, Tao J, Liang Y G, et al. Ultraweak light-modulated heterostructure with bidirectional photoresponse for static and dynamic image perception. Nat Commun, 2024, 15: 10430 doi: 10.1038/s41467-024-54845-3
[30]
Du X J, Wang H, Wang Y F, et al. An ultra-conductive and patternable 40 nm-thick polymer film for reliable emotion recognition. Adv Mater, 2024, 36(31): 2403411 doi: 10.1002/adma.202403411
[31]
Lv J, Thangavel G, Li Y, et al. Printable elastomeric electrodes with sweat-enhanced conductivity for wearables. Sci Adv, 2021, 7(29): eabg8433 doi: 10.1126/sciadv.abg8433
[32]
Liu Y, Tao J, Mo Y P, et al. Ultrasensitive touch sensor for simultaneous tactile and slip sensing. Adv Mater, 2024, 36(21): 2313857 doi: 10.1002/adma.202313857
[33]
Zhang Y X, Bao R R, Qiu J B, et al. Electrochromic-based visualised flexible biosensing platforms: from single device to multifunctional device integration. Chem Soc Rev, 2025, 54(24): 11827 doi: 10.1039/D5CS00386E
[34]
Zheng Y, Liu T, Wu J P, et al. Energy conversion analysis of multilayered triboelectric nanogenerators for synergistic rain and solar energy harvesting. Adv Mater, 2022, 34(28): 2202238 doi: 10.1002/adma.202202238
[35]
Xu B X, Akhtar A, Liu Y H, et al. An epidermal stimulation and sensing platform for sensorimotor prosthetic control, management of lower back exertion, and electrical muscle activation. Adv Mater, 2016, 28(22): 4462 doi: 10.1002/adma.201504155
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    Received: Revised: Online: Accepted Manuscript: 28 July 2026

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      Yan Peng, Siyu Xie, Xiaofan Zhu, Yuke Deng, Weiwei Guo, Yuxiao Zhang, Yue Liu. Stretchable flexible electrodes based on in situ coating of graphite with PANI[J]. Journal of Semiconductors, 2026, In Press. doi: 10.1088/1674-4926/26060029 ****Y Peng, S Y Xie, X F Zhu, Y K Deng, W W Guo, Y X Zhang, and Y Liu, Stretchable flexible electrodes based on in situ coating of graphite with PANI[J]. J. Semicond., 2026, accepted doi: 10.1088/1674-4926/26060029
      Citation:
      Yan Peng, Siyu Xie, Xiaofan Zhu, Yuke Deng, Weiwei Guo, Yuxiao Zhang, Yue Liu. Stretchable flexible electrodes based on in situ coating of graphite with PANI[J]. Journal of Semiconductors, 2026, In Press. doi: 10.1088/1674-4926/26060029 ****
      Y Peng, S Y Xie, X F Zhu, Y K Deng, W W Guo, Y X Zhang, and Y Liu, Stretchable flexible electrodes based on in situ coating of graphite with PANI[J]. J. Semicond., 2026, accepted doi: 10.1088/1674-4926/26060029

      Stretchable flexible electrodes based on in situ coating of graphite with PANI

      DOI: 10.1088/1674-4926/26060029
      CSTR: 32376.14.1674-4926.26060029
      More Information
      • Yan Peng is currently an undergraduate student majoring in Materials Science and Engineering at Kunming University of Science and Technology. Her research interest lies in flexible visual electronic devices
      • Siyu Xie is currently an MS candidate in the College of Materials Science and Engineering, Kunming University of Science and Technology. He received his Bachelor’s degree in materials science and engineering from Kunming University of Science and Technology, China, in 2020. His current research interests focus on flexible electronic devices
      • Yuxiao Zhang obtained a bachelor’s degree from Dalian University of Technology in 2021. In 2026, he received a master's degree from Kunming University of Science and Technology, under the guidance of Professor Yang Zhengwen. Currently, he is pursuing a doctoral degree at Beihang University, under the supervision of Professor Pan Caofeng. His main research field is electrochromic and sensor visualization integrated devices
      • Yue Liu received her BS (2017) in materials science and engineering from the China University of Geosciences (Beijing), China. She received her PhD (2022) in the group of Prof. Caofeng Pan from the Beijing Institute of Nanoenergy and Nanosystems, Chinese Academy of Sciences, China. She has been working in the group of Prof. Jianbei Qiu at the Kunming University of Science and Technology as a specially-appointed professor since 2023. Her main research interests include flexible visual electronic skin (E-skin) and its applications in human–machine interfaces
      • Corresponding author: 1310114565@qq.comliuyue2023@kust.edu.cn
      • Available Online: 2026-07-28

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