Strain-Insensitive Stretchable Conductive Fiber Based on Helical Core with Double-Network Hydrogel

Abstract

The development of the highly stretchable and strain-insensitive conductive fibers exhibiting extremely small resistance change under large deformation is crucial for the electronic signal stability in the smart wearable fields. In this paper, an all-polymeric conductive microfiber (PU@PVA-PEDOT:PSS SI-CF) with desirable performances has been developed by using microfluidic spinning technology (MST), during which process the instinct strain-insensitive conductive polymer hydrogel core with semi-interpenetrating network is constructed into the helical structure. The configuration and performances of the PU@PVA-PEDOT:PSS SI-CF have been optimized by regulating the processing parameters of MST, and the fabricated microfiber exhibits excellent stretchability (up to 500%), high conductivity (147 S cm⁻¹), super conductance strain insensitivity (ultra-low resistance change of 5% at 100% strain), as well as excellent durability (2000 stretching-releasing cycles). The PU@PVA-PEDOT:PSS SI-CF shows great smart wearable application potential as the stretchable wire, the self-powered sensor, and the electro-thermal heater.

Keywords

Conductive fiber / Strain insensitivity / Microfluidic spinning technology / Semi-interpenetrating network / Engineering / Materials Engineering

References

[1] LiM, LiZQ, YeXR, HeWZ, QuLJ, TianMW. A smart self-powered rope for water/fire rescue. Adv Funct Mater, 2022, 33: 2210111

[2] WangLH, ShiBH, ZhaoHT, QiXJ, ChenJH, LiJJ, ShangYY, FuKK, ZhangXJ, TianMW, QuLJ. 3D-printed parahydrophobic functional textile with a hierarchical nanomicroscale structure. ACS Nano, 2022, 16: 16645

[3] LeeJ, LlerenaZB, WooJ, YoonK, LeeT. Recent advances in 1D stretchable electrodes and devices for textile and wearable electronics: materials, fabrications, and applications. Adv Mater, 2019, 32: 1902532

[4] LiWW, LiuJ, WeiJN, YangZY, RenCL, LiB. Recent progress of conductive hydrogel fibers for flexible electronics: fabrications, applications, and perspectives. Adv Funct Mater, 2023, 33: 2213485

[5] LiuZK, ZhuTX, WangJR, ZhengZJ, LiY, LiJS, LaiYK. Functionalized fiber-based strain sensors: pathway to next-generation wearable electronics. Nano-Micro Lett, 2022, 14: 61

[6] ChenSW, FanSC, QiJM, XiongZ, QiaoZ, WuZX, YeoJC, LimCT. Ultrahigh strain-insensitive integrated hybrid electronics using highly stretchable bilayer liquid metal based conductor. Adv Mater, 2022, 35: 2208569

[7] HeH, ChenR, YueSZ, YuSZ, WeiJ, OuyangJY. Salt-induced ductilization and strain-insensitive resistance of an intrinsically conducting polymer. Sci Adv, 2022, 8: eabq8160

[8] HeJ, ZhouRH, ZhangYF, GaoWC, ChenT, MaiWJ, PanCF. Strain-insensitive self-powered tactile sensor arrays based on intrinsically stretchable and patternable ultrathin conformal wrinkled graphene-elastomer composite. Adv Funct Mater, 2021, 32: 2107281

[9] VeeramuthuL, ChoCJ, LiangFC, VenkatesanM, KumarGR, HsuHY, ChungRJ, LeeCH, LeeWY, KuoCC. Human skin-inspired electrospun patterned robust strain-insensitive pressure sensors and wearable flexible light-emitting diodes. ACS Appl Mater Interfaces, 2022, 14: 30160

[10] ChenS, LiuHZ, LiuSQ, WangPP, ZengSS, SunLY, LiuL. Transparent and waterproof ionic liquid-based fibers for highly durable multifunctional sensors and strain-insensitive stretchable conductors. ACS Appl Mater Interfaces, 2018, 10: 4305

[11] LiSM, XuJW, MuY, WangP, ZhuH, LiuBH, ChenZ, HanZL, QuSX. Fatigue-resistant and hysteresis-free composite fibers with a heterogeneous hierarchical structure. Adv Funct Mater, 2023, 5: 1643

[12] LiG, HuangKX, DengJ, GuoMX, CaiMK, ZhangY, GuoCF. Highly conducting and stretchable double-network hydrogel for soft bioelectronics. Adv Mater, 2022, 34: 2200261

[13] ZhangYF, GuoMM, ZhangY, TangCY, JiangC, DongYQ, LawWC, DuFP. Flexible, stretchable and conductive PVA/PEDOT:PSS composite hydrogels prepared by SIPN strategy. Polym Test, 2020, 81106213

[14] ZhuH, HuXC, LiuBH, ChenZ, QuSX. 3D printing of conductive hydrogel-elastomer hybrids for stretchable electronics. ACS Appl Mater Interface, 2021, 13: 59243

[15] WangMX, ChenZW, DongL, WuJJ, LiC, GaoQ, ShiJ, ZhuCH, MorikawaH. Conductance-stable and integrated helical fiber electrodes toward stretchy energy storage and self-powered sensing utilization. Chem Eng J, 2023, 457141164

[16] WuJP, SangM, ZhangJY, SunYX, WangXY, ZhangJS, PangHM, LuoTZ, PanSS, XuanSH, GongXL. Ultra-stretchable spiral hybrid conductive fiber with 500%-strain electric stability and deformation-independent linear temperature response. Small, 2023, 19: 2207454

[17] GaoYY, YuLY, LiYM, WeiLQ, YinJ, WangFJ, WangL, MaoJF. Maple leaf inspired conductive fiber with hierarchical wrinkles for highly stretchable and integratable electronics. ACS Appl Mater Interface, 2022, 14: 49059

[18] SunFQ, TianMW, SunXT, XuTL, LiuXQ, ZhuSF, ZhangXJ, QuLJ. Stretchable conductive fibers of ultrahigh tensile strain and stable conductance enabled by a worm-shaped graphene microlayer. Nano Lett, 2019, 19: 6592

[19] YoonK, LeeS, ShimD, LeeM, ChoS, KwonC, WonC, LeeJ, JungHH, LeeSM, JangKI, LeeJ, LeeT. Strain-insensitive stretchable fiber conductors based on highly conductive buckled shells for wearable electronics. ACS Appl Mater Interfaces, 2023, 15: 18281

[20] ZhouJ, TianGQ, JinG, XinYY, TaoR, LubineauG. Buckled conductive polymer ribbons in elastomer channels as stretchable fiber conductor. Adv Funct Mater, 2019, 30: 1907316

[21] LiYM, LiCF, ShanMQ, WeiLQ, LiuXL, GuoLM, WangFJ, ZhangZ, WangL, ShenL, MaoJF. Injectable, stretchable, and conductance-stable fiber for myocardial infarction repair. Compos Part B Eng, 2024, 273111242

[22] WuYT, YanT, ZhangKQ, PanZJ. A hollow core-sheath composite fiber based on polyaniline/polyurethane: preparation, properties, and multi-model strain sensing performance. Adv Mater Technol, 2022, 8: 2200777

[23] ZhengLJ, ZhuMM, WuBH, LiZL, SunST, WuPY. Conductance-stable liquid metal sheath-core microfibers for stretchy smart fabrics and self-powered sensing. Sci Adv, 2021, 7: 22

[24] LiuYY, TangYL, GuoXQ, QuLJ, LiuYC, ZhangXM, HuangT, XuLL, LiuH, TianMW. Template-free and stretchable conductive fiber with a built-in helical structure for strain-insensitive signal transmission. ACS Appl Mater Interface, 2023, 15: 46379

[25] WangSX, ChenYJ, PeiDF, ZhangXF, LiMJ, XuDM, LiCX. Rifled microtubes with helical and conductive ribs for endurable sensing device. Chem Eng J, 2023, 465142939

[26] ChenN, WeiW, NingNY, WuHG, TianM. All-Polymeric stretchable conductive fiber with versatile intelligent wearable applications via microfluidic spinning technology. Chem Eng J, 2024, 487150741

[27] ShaoL, GaoQ, ZhaoHM, XieCQ, FuJZ, LiuZJ, XiangMX, HeY. Fiber-based mini tissue with morphology-controllable gelMA microfibers. Small, 2018, 14: 1802187

[28] XuPD, XieRX, LiuYP, LuoGA, DingMY, LiangQL. Bioinspired microfibers with embedded perfusable helical channels. Adv Mater, 2017, 29: 1701664

[29] DuFP, CaoNN, ZhangYF, FuP, WuYG, LinZD, ShiR, AminiA, ChengC. PEDOT:PSS/graphene quantum dots films with enhanced thermoelectric properties via strong interfacial interaction and phase separation. Sci Rep, 2018, 8: 6441

[30] OuyangJ. “Secondary doping” methods to significantly enhance the conductivity of PEDOT:PSS for its application as transparent electrode of optoelectronic devices. Displays, 2013, 34: 423

[31] WuHG, ChenHG, YaoPJ, WangR. Stretchable and highly sensitive strain sensor based on conductive polymer aerogel for human physiological information detection. Nano Select, 2021, 2: 802

[32] ZhangJ, YanS, YuanD, AliciG, NguyenNT, WarkianiME, LiWH. Fundamentals and applications of inertial microfluidics: a review. Lab Chip, 2016, 16: 10

[33] SharifiF, BaiZH, MontazamiR, HashemiN. Mechanical and physical properties of poly(vinyl alcohol) microfibers fabricated by a microfluidic approach. RSC Adv, 2016, 6: 55343

[34] WuHG, LiuQ, DuWC, LiC, ShiGQ. Transparent polymeric strain sensors for monitoring vital signs and beyond. ACS Appl Mater Interfaces, 2018, 10: 3895

[35] SongXK, JiJJ, ZhouNJ, ChenMJ, QuRX, LiHY, ZhangLA, MaSY, MaZJ, WeiY. Stretchable conductive fibers: design, properties and applications. Prog Mater Sci, 2024, 144101288

[36] TianGQ, ZhouJ, XinYY, TaoR, JinG, LubineauG. Copolymer-enabled stretchable conductive polymer fibers. Polymer, 2019, 177: 189

[37] KimD, AhnSK, YoonJ. Highly stretchable strain sensors comprising double network hydrogels fabricated by microfluidic devices. Adv Mater Technol, 2019, 4: 1800739

[38] ShuaiLYZ, GuoZH, ZhangPP, WanJM, PuX, WangZL. Stretchable, self-healing, conductive hydrogel fibers for strain sensing and triboelectric energy-harvesting smart textiles. Nano Energy, 2020, 78105389

[39] SongJC, ChenS, SunLJ, GuoYF, ZhangLZ, WangSL, XuanHX, GuanQB, YouZW. Mechanically and electronically robust transparent organohydrogel fibers. Adv Mater, 2020, 32: 1906994

[40] ZhaoX, ChenF, LiYH, LuH, ZhangN, MaMM. Bioinspired ultra-stretchable and anti-freezing conductive hydrogel fibers with ordered and reversible polymer chain alignment. Nat Commun, 2018, 9: 3579

[41] SchultheissA, RevauxA, CarellaA, BrinkmannM, ZengHY, DemadrilleR, SimonatoJP. Electrical and mechanical properties of intrinsically flexible and stretchable PEDOT polymers for thermotherapy. ACS Appl Polym Mater, 2021, 3: 5942

[42] ZhuTY, FengQC, WanN, ZhangC, LiB, LiuTX. Articular cartilage-inspired 3D superelastic and fatigue-resistant spongy conductors against harsh environments. Sci China Mater, 2022, 66: 1527

[43] NingC, DongK, ChengRW, YiJ, YeCY, PengX, ShengFF, JiangY, WangZL. Flexible and stretchable fiber-shaped triboelectric nanogenerators for biomechanical monitoring and human-interactive sensing. Adv Funct Mater, 2020, 31: 2006679

[44] FuK, ZhouJ, WuHU, SuZQ. Fibrous self-powered sensor with high stretchability for physiological information monitoring. Nano Energy, 2021, 88106258

[45] ZhouJ, ZhangY, MulleM, LubineauG. Temperature sensing of micron scale polymer fibers using fiber Bragg gratings. Meas Sci Technol, 2015, 26085003

Funding

the National Natural Science Foundation of China(51903006)

the Beijing Natural Science Foundation(2232049)

Young Elite Scientist Sponsorship Program by BAST(BYESS2022211)

The Beijing Outstanding Youth Foundation(BPHR202203066)

The Beijing Scholar Program(RCQJ20303)

RIGHTS & PERMISSIONS

Donghua University, Shanghai, China