Wrinkled and Fibrous Conductive Bandages with Tunable Mechanoelectrical Response Toward Wearable Strain Sensors

Abstract

Wearable strain sensors (WSSs) have found widespread applications, where the key is to optimize their sensing and wearing performances. However, the intricate material designs for developing WSSs often rely on costly reagents and/or complex processes, which bring barriers to their large-scale production and use. Herein, a facile and affordable (material cost of < $0.002/cm²) method is presented for fabricating conductive bandage (CB)-based WSSs by electrospraying a carbon nanotube (CNT) layer on commercial self-adhesive bandages with excellent biosafety, stretchability, mechanical compliance, breathability and cost effectiveness. The wrinkled and fibrous structures of self-adhesive bandages were rationally leverage to control the geometry of CNT layer, thereby ensuring tunable mechanoelectrical sensitivities (gauge factors of 2 ~ 850) of CBs. Moreover, a strain-sensing mechanism directly mediated by the highly wrinkled microstructure is unveiled, which can work in synergy with a training-loosened-fibrous microstructure. The excellent performance of CBs for monitoring full-range strain signals in human bodies was further demonstrated. CBs would possess great potential for being developed into WSSs because of their outstanding cost-performance ratio.

Keywords

Flexible electronics / Carbon nanotubes / Nonwoven fabrics / Wrinkles / Strain sensors

References

[1] Nguyen PQ, Soenksen LR, Donghia NM, Angenent-Mari NM, de Puig H, Huang A, Lee R, Slomovic S, Galbersanini T, Lansberry G, Sallum HM, Zhao EM, Niemi JB, Collins JJ. Wearable materials with embedded synthetic biology sensors for biomolecule detection. Nat Biotechnol, 2021, 39: 1366,

[2] Meng KY, Xiao X, Wei WX, Chen GR, Nashalian A, Shen S, Xiao X, Chen J. Wearable pressure sensors for pulse wave monitoring. Adv Mater, 2022, 34: 2109357,

[3] Wei X, Li H, Yue WJ, Gao S, Chen ZX, Li Y, Shen GZ. A high-accuracy, real-time, intelligent material perception system with a machine-learning-motivated pressure-sensitive electronic skin. Matter, 2022, 5: 1481,

[4] Zhao G, Wu T, Wang R, Li Z, Yang Q, Wang L, Zhou H, Jin B, Liu H, Fang Y, Wang D, Xu F. Hydrogel-assisted microfluidic spinning of stretchable fibers via fluidic and interfacial self-adaptations. Sci Adv, 2023, 9: eaadj5407,

[5] Liu XH, Miao JL, Fan Q, Zhang WX, Zuo XW, Tian MW, Zhu SF, Zhang XJ, Qu LJ. Recent progress on smart fiber and textile based wearable strain sensors: materials fabrications and applications. Adv Fiber Mater, 2022, 4: 361,

[6] Li XX, Chen L, Yuan SL, Tong H, Cheng QL, Zeng HD, Wei L, Zhang Q. Stretchable luminescent perovskite-polymer hydrogels for visual-digital wearable strain sensor textiles. Adv Fiber Mater, 2023, 5: 1671,

[7] Chen GR, Xiao X, Zhao X, Tat T, Bick M, Chen J. Electronic textiles for wearable point-of-care systems. Chem Rev, 2022, 122: 3259,

[8] Hou B, Yi LY, Li C, Zhao H, Zhang R, Zhou B, Liu XG. An interactive mouthguard based on mechanoluminescence-powered optical fibre sensors for bite-controlled device operation. Nat Electron, 2022, 5: 682,

[9] Tian X, Lee PM, Tan YJ, Li Z, Ng KA, Tee BCK, Wu TLY, Yao H, Ho JS. Wireless body sensor networks based on metamaterial textiles. Nat Electron, 2019, 2: 243,

[10] Shveda RA, Rajappan A, Yap TF, Liu Z, Bell MD, Jumet B, Sanchez V, Preston DJ. A wearable textile-based pneumatic energy harvesting system for assistive robotics. Sci Adv, 2022, 8: eabo2418,

[11] Libanori A, Chen GR, Zhao X, Zhou YH, Chen J. Smart textiles for personalized healthcare. Nat Electron, 2022, 5: 142,

[12] Chu ZM, Jiao WC, Huang YF, Zheng YT, Wang RG, He XD. Superhydrophobic gradient wrinkle strain sensor with ultra-high sensitivity and broad strain range for motion monitoring. J Mater Chem A, 2021, 9: 9634,

[13] Kurra N, Ahmed B, Gogotsi Y, Alshareef HN. MXene-on-paper coplanar Microsupercapacitors. Adv Energy Mater, 2016, 6: 1601372,

[14] Horiuchi N. Paper electronics. Nat Photon, 2018, 12: 381,

[15] Liu ZQ, Huang YZ, Shi YX, Tao XL, He HZ, Chen FD, Huang ZX, Wang ZL, Chen XY, Qu JP. Fabrication of triboelectric polymer films via repeated rheological forging for ultrahigh surface charge density. Nat Commun, 2022, 13: 4083,

[16] Tan P, Wang HF, Xiao FR, Lu X, Shang WH, Deng XB, Song HF, Xu ZY, Cao JF, Gan TS, Wang B, Zhou XC. Solution-processable, soft, self-adhesive, and conductive polymer composites for soft electronics. Nat Commun, 2022, 13: 358,

[17] Shan T, Wang YM, Chen QM, Xue ZY, Guo XJ, Li WW, Zhong HL. Achieving efficient flexible and large-area organic solar cells via additive-assisted fluorous solvent soaking. Chem Eng J, 2023, 475,

[18] Chen JM, Zhang J, Hu JL, Luo NQ, Sun FX, Venkatesan H, Zhao N, Zhang YT. Ultrafast-response/recovery flexible piezoresistive sensors with DNA-like double helix yarns for epidermal pulse monitoring. Adv Mater, 2022, 34: 2104313,

[19] Wang L, Fu XM, He JQ, Shi X, Chen TQ, Chen PN, Wang BJ, Peng HS. Application Challenges in Fiber and Textile Electronics. Adv Mater, 2020, 32: 1901971,

[20] Luo YY, Li YZ, Sharma P, Shou W, Wu K, Foshey M, Li B, Palacios T, Torralba A, Matusik W. Learning human–environment interactions using conformal tactile textiles. Nat Electron, 2021, 4: 193,

[21] Zhang MC, Wang CY, Wang HM, Jian MQ, Hao XY, Zhang YY. Carbonized cotton fabric for high-performance wearable strain sensors. Adv Funct Mater, 2016, 27: 1604795,

[22] Gao ZY, Xiao X, Carlo AD, Yin JY, Wang YX, Huang LJ, Tang JG, Chen J. Advances in wearable strain sensors based on electrospun fibers. Adv Funct Mater, 2023, 33: 2214265,

[23] Aeby X, Poulin A, Siqueira G, Hausmann MK, Nyström G. Fully 3D printed and disposable paper supercapacitors. Adv Mater, 2021, 33: 2101328,

[24] Lee S, Seong H, Im SG, Moon H, Yoo S. Organic flash memory on various flexible substrates for foldable and disposable electronics. Nat Commun, 2017, 8: 725,

[25] Zheng C, Li W, Shi YX, Wei SS, Liu KQ, Cheng J, Ji LH, Lu YJ. Stretchable self-adhesive and self-powered smart bandage for motion perception and motion intention recognition. Nano Energy, 2023, 109,

[26] Wang QZ, Li YY, Xu Q, Yu HX, Zhang DJ, Zhou QH, Dhakal R, Li Y, Yao Z. Finger–coding intelligent human-machine interaction system based on all-fabric ionic capacitive pressure sensors. Nano Energy, 2023, 116,

[27] Lee G, Zarei M, Wei QS, Zhu Y, Lee SG. Surface wrinkling for flexible and stretchable sensors. Small, 2022, 18: 2203491,

[28] Bhuyan P, Wei Y, Cho D, Nakate UT, Kim S, Lee S, Choe M, Jeon H, Park S. Multifunctional ultrastretchable and ultrasoft electronics enabled by uncrosslinked polysiloxane elastomers patterned with rheologically modified liquid metal electrodes: Beyond current soft and stretchable electronics. Chem Eng J, 2023, 453,

[29] Kang D, Pikhitsa PV, Choi YW, Lee C, Shin SS, Piao L, Park B, Suh K-Y, Kim T-I, Choi M. Ultrasensitive mechanical crack-based sensor inspired by the spider sensory system. Nature, 2014, 516: 222,

[30] Zhou J, Yu H, Xu XZ, Han F, Lubineau G. Ultrasensitive, stretchable strain sensors based on fragmented carbon nanotube papers. ACS Appl Mater Interfaces, 2017, 9: 4835,

[31] Wang S, Xiao P, Liang Y, Zhang JW, Huang YJ, Wu S, Kuo SW, Chen T. Network cracks-based wearable strain sensors for subtle and large strain detection of human motions. J Mater Chem C, 2018, 6: 5140,

[32] Shen TY, Liu S, Yue XY, Wang ZQ, Liu H, Yin R, Liu CT, Shen CY. High-performance fibrous strain sensor with synergistic sensing layer for human motion recognition and robot control. Adv Compos Hybrid Mater, 2023, 6: 127,

[33] Zhou YJ, Zhan PF, Ren MN, Zheng GQ, Dai K, Mi LW, Liu CT, Shen CY. Significant stretchability enhancement of a crack-based strain sensor combined with high sensitivity and superior durability for motion monitoring. ACS Appl Mater Interfaces, 2019, 11: 7405,

[34] Pu JH, Zhao X, Zha XJ, Li WD, Ke K, Bao RY, Liu ZY, Yang MB, Yang W. A strain localization directed crack control strategy for designing MXene-based customizable sensitivity and sensing range strain sensors for full-range human motion monitoring. Nano Energy, 2020, 74,

[35] Chao MY, Wang YG, Ma D, Wu XX, Zhang WX, Zhang LQ, Wan PB. Wearable MXene nanocomposites-based strain sensor with tile-like stacked hierarchical microstructure for broad-range ultrasensitive sensing. Nano Energy, 2020, 78,

[36] He YX, Wu DY, Zhou MY, Zheng YJ, Wang TF, Lu C, Zhang L, Liu H, Liu CT. Wearable strain sensors based on a porous polydimethylsiloxane hybrid with carbon nanotubes and graphene. ACS Appl Mater Interfaces, 2021, 13: 15572,

[37] He YX, Zhou MY, Mahmoud MHH, Lu XS, He GY, Zhang L, Huang MN, Elnaggar AY, Lei Q, Liu H, Liu CT, Azab IHE. Multifunctional wearable strain/pressure sensor based on conductive carbon nanotubes/silk nonwoven fabric with high durability and low detection limit. Adv Compos Hybrid Mater, 2022, 5: 1939,

[38] Bock N, Dargaville TR, Woodruff MA. Electrospraying of polymers with therapeutic molecules: State of the art. Prog Polym Sci, 2012, 37: 1510,

[39] Liu H, Li MX, Liu SB, Jia PP, Guo XJ, Feng SS, Lu TJ, Yang HY, Li F, Xu F. Spatially modulated stiffness on hydrogels for soft and stretchable integrated electronics. Mater Horiz, 2020, 7: 203,

[40] Zhao C, Wang YJ, Tang GQ, Ru J, Zhu ZC, Li B, Guo CF, Li LJ, Zhu DL. Ionic flexible sensors: mechanisms, materials, structures, and applications. Adv Funct Mater, 2022, 32: 2110417,

[41] Sanchez V, Mahadevan K, Ohlson G, Graule MA, Yuen MC, Teeple CB, Weaver JC, McCann J, Bertoldi K, Wood RJ. 3D knitting for pneumatic soft robotics. Adv Funct Mater, 2023, 33: 2212541,

[42] Niu Y, Liu H, He RY, Luo MQ, Shu MG, Xu F. Environmentally compatible wearable electronics based on ionically conductive organohydrogels for health monitoring with thermal compatibility, anti-dehydration, and underwater adhesion. Small, 2021, 17: 2101151,

[43] Zhao Y, Gao WC, Dai K, Wang S, Yuan ZQ, Li JN, Zhai W, Zheng GQ, Pan CF, Liu CT, Shen CY. Bioinspired multifunctional photonic-electronic smart skin for ultrasensitive health monitoring, for visual and self-powered sensing. Adv Mater, 2021, 33: 2102332,

[44] Liu RY, Lai Y, Li SX, Wu F, Shao JM, Liu D, Dong X, Wang J, Wang ZL. Ultrathin, transparent, and robust self-healing electronic skins for tactile and non-contact sensing. Nano Energy, 2022, 95,

[45] Li Y, Yin JY, Liu SY, Xue B, Shokoohi C, Ge G, Hu ML, Li TH, Tao X, Rao Z, Meng FY, Shi HF, Ji XQ, Servati P, Xiao X, Chen J. Learning hand kinematics for Parkinson's disease assessment using a multimodal sensor glove. Adv Sci, 2023, 10: 2206982,

[46] Zhao XX, Guo H, Ding P, Zhai W, Liu CT, Shen CY, Dai K. Hollow-porous fiber-shaped strain sensor with multiple wrinkle-crack microstructure for strain visualization and wind monitoring. Nano Energy, 2023, 108,

[47] Niu HS, Li H, Li Y, Yue WJ, Gao S, Wei X, Shen GZ. Cocklebur-inspired “branch-seed-spininess” 3D hierarchical structure bionic electronic skin for intelligent perception. Nano Energy, 2023, 107,

[48] Kim KH, Hong SK, Ha SH, Li L, Lee HW, Kim JM. Enhancement of linearity range of stretchable ultrasensitive metal crack strain sensor via superaligned carbon nanotube-based strain engineering. Mater Horiz, 2020, 7: 2662,

[49] Ji J, Zhang CP, Yang SH, Liu YZ, Wang JL, Shi ZY. High sensitivity and a wide sensing range flexible strain sensor based on the V-groove/wrinkles hierarchical array. ACS Appl Mater Interfaces, 2022, 14: 24059,

[50] He J, Zhou RH, Zhang YF, Gao WC, Chen T, Mai WJ, Pan CF. 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,

[51] Luo GX, Xie JQ, Liu JL, Zhang QK, Luo YY, Li M, Zhou WK, Chen K, Li ZK, Yang P, Zhao LB, Teh KS, Wang XZ, Dong LX, Maeda R, Jiang ZD. Highly conductive, stretchable, durable, breathable electrodes based on electrospun polyurethane mats superficially decorated with carbon nanotubes for multifunctional wearable electronics. Chem Eng J, 2022, 451,

[52] Yoon C, Ippili S, Jella V, Thomas AM, Jung JS, Han YR, Yang TY, Yoon SG, Yoon G. Synergistic contribution of flexoelectricity and piezoelectricity towards a stretchable robust nanogenerator for wearable electronics. Nano Energy, 2022, 91,

[53] Huang LB, Dai XY, Sun ZH, Wong MC, Pang SY, Han JC, Zheng QQ, Zhao CH, Jie Kongb JH. Environment-resisted flexible high performance triboelectric nanogenerators based on ultrafast self-healing non-drying conductive organohydrogel. Nano Energy, 2021, 82,

Funding

National Natural Science Foundation of China(32260244); Hainan Provincial Natural?Science Foundation of China(524YXQN416); Hainan Provincial Natural?Science Foundation of China(824CXTD424); Science and Technology Special Fund of Hainan Province(ZDYF2022SHFZ289)