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. 2022 May 12;65(9):2540–2552. doi: 10.1007/s40843-021-2022-1

Ultrasensitive, stretchable, and transparent humidity sensor based on ion-conductive double-network hydrogel thin films

基于离子导电双网络水凝胶薄膜的超灵敏、可拉 伸、透明湿度传感器

Zixuan Wu 1,#, Qiongling Ding 1,#, Zhenyi Li 1,#, Zijing Zhou 1, Luqi Luo 1, Kai Tao 2, Xi Xie 1, Jin Wu 1,
PMCID: PMC9109751  PMID: 35600911

Abstract

Ion-conductive hydrogels with intrinsic biocompatibility, stretchability, and stimuli-responsive capability have attracted considerable attention because of their extensive application potential in wearable sensing devices. The miniaturization and integration of hydrogel-based devices are currently expected to achieve breakthroughs in device performance and promote their practical application. However, currently, hydrogel film is rarely reported because it can be easily wrinkled, torn, and dehydrated, which severely hinders its development in microelectronics. Herein, thin, stretchable, and transparent ion-conductive double-network hydrogel films with controllable thickness are integrated with stretchable elastomer substrates, which show good environmental stability and ultrahigh sensitivity to humidity (78,785.5%/% relative humidity (RH)). Benefiting from the ultrahigh surface-area-to-volume ratio, abundant active sites, and short diffusion distance, the hydrogel film humidity sensor exhibits 2 × 105 times increased response to 98% RH, as well as 5.9 and 7.6 times accelerated response and recovery speeds compared with the bulk counterpart, indicating its remarkable thickness-dependent humidity-sensing properties. The humidity-sensing mechanism reveals that the adsorption of water improves the ion migration and dielectric constant, as well as establishes the electrical double layer. Furthermore, the noncontact human-machine interaction and real-time respiratory frequency detection are enabled by the sensors. This work provides an innovative strategy to achieve further breakthroughs in device performance and promote the development of hydrogel-based miniaturized and integrated electronics. graphic file with name 40843_2021_2022_Fig1_HTML.jpg

Electronic Supplementary Material

Supplementary material is available in the online version of this article at 10.1007/s40843-021-2022-1.

Keywords: stretchable hydrogel, humidity sensor, thin-film, ultrasensitive, wearable application

Supplementary Information

40843_2021_2022_MOESM1_ESM.pdf (1.3MB, pdf)

Ultrasensitive, stretchable, and transparent humidity sensor based on ion-conductive double-network hydrogel thin films

Acknowledgements

This work was supported by the National Natural Science Foundation of China (61801525), Guangdong Basic and Applied Basic Research Foundation (2020A1515010693), the Science and Technology Program of Guangzhou (201904010456), and the Fundamental Research Funds for the Central Universities, Sun Yat-sen University (22lgqb17).

Author contributions

Wu J, Wu Z, Ding Q, and Li Z designed the sensors, analyzed the results, and wrote the paper; Wu Z drafted the manuscript; Zhou Z, Luo L, Tao K, and Xie X contributed to the discussion of the results; Wu J revised the paper and supervised the project. All authors contributed to the general discussion.

Footnotes

Jin Wu received his PhD degree from Nanyang Technological University in 2014. After obtaining his PhD degree in 2014, he continued working in the SMART program at Nanyang Technological University as a postdoctoral research fellow. Since 2017, he has been an associate professor at the School of Electronics and Information Technology, Sun Yat-sen University. His research interest includes hydrogel-based sensors, and flexible and stretchable electronics.

Conflict of interest

The authors declare that they have no conflict of interest.

Supplementary information

Supporting data are available in the online version of the paper.

These authors contributed equally to this work.

References

  • 1.Azevedo S, Costa AMS, Andersen A, et al. Bioinspired ultratough hydrogel with fast recovery, self-healing, injectability and cytocompatibility. Adv Mater. 2017;29:1700759. doi: 10.1002/adma.201700759. [DOI] [PubMed] [Google Scholar]
  • 2.Mo F, Chen Z, Liang G, et al. Zwitterionic sulfobetaine hydrogel electrolyte building separated positive/negative ion migration channels for aqueous Zn-MnO2 batteries with superior rate capabilities. Adv Energy Mater. 2020;10:2000035. doi: 10.1002/aenm.202000035. [DOI] [Google Scholar]
  • 3.Lee J, Tan MWM, Parida K, et al. Water-processable, stretchable, self-healable, thermally stable, and transparent ionic conductors for actuators and sensors. Adv Mater. 2020;32:1906679. doi: 10.1002/adma.201906679. [DOI] [PubMed] [Google Scholar]
  • 4.Farid T, Rafiq MI, Ali A, et al. Transforming wood as next-generation structural and functional materials for a sustainable future. EcoMat. 2022;4:e12154. doi: 10.1002/eom2.12154. [DOI] [Google Scholar]
  • 5.Ding Q, Wu Z, Tao K, et al. Environment tolerant, adaptable and stretchable organohydrogels: Preparation, optimization, and applications. Mater Horiz, 2022, doi: 10.1039/D1MH01871J [DOI] [PubMed]
  • 6.Tao K, Chen Z, Yu J, et al. Ultra-sensitive, deformable, and transparent triboelectric tactile sensor based on micro-pyramid patterned ionic hydrogel for interactive human-machine interfaces. Adv Sci. 2022;9:2104168. doi: 10.1002/advs.202104168. [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 7.Wu J, Wu Z, Xu H, et al. An intrinsically stretchable humidity sensor based on anti-drying, self-healing and transparent organohydrogels. Mater Horiz. 2019;6:595–603. doi: 10.1039/C8MH01160E. [DOI] [Google Scholar]
  • 8.Wu J, Wu Z, Han S, et al. Extremely deformable, transparent, and highperformance gas sensor based on ionic conductive hydrogel. ACS Appl Mater Interfaces. 2018;11:2364–2373. doi: 10.1021/acsami.8b17437. [DOI] [PubMed] [Google Scholar]
  • 9.Ge G, Lu Y, Qu X, et al. Muscle-inspired self-healing hydrogels for strain and temperature sensor. ACS Nano. 2019;14:218–228. doi: 10.1021/acsnano.9b07874. [DOI] [PubMed] [Google Scholar]
  • 10.Wu J, Han S, Yang T, et al. Highly stretchable and transparent thermistor based on self-healing double network hydrogel. ACS Appl Mater Interfaces. 2018;10:19097–19105. doi: 10.1021/acsami.8b03524. [DOI] [PubMed] [Google Scholar]
  • 11.Deng Z, Hu T, Lei Q, et al. Stimuli-responsive conductive nanocomposite hydrogels with high stretchability, self-healing, adhesiveness, and 3D printability for human motion sensing. ACS Appl Mater Interfaces. 2019;11:6796–6808. doi: 10.1021/acsami.8b20178. [DOI] [PubMed] [Google Scholar]
  • 12.Deng Z, Wang H, Ma PX, et al. Self-healing conductive hydrogels: Preparation, properties and applications. Nanoscale. 2020;12:1224–1246. doi: 10.1039/C9NR09283H. [DOI] [PubMed] [Google Scholar]
  • 13.Deng Z, Yu R, Guo B. Stimuli-responsive conductive hydrogels: Design, properties, and applications. Mater Chem Front. 2021;5:2092–2123. doi: 10.1039/D0QM00868K. [DOI] [Google Scholar]
  • 14.Liang Y, Wu Z, Wei Y, et al. Self-healing, self-adhesive and stable organohydrogel-based stretchable oxygen sensor with high performance at room temperature. Nano-Micro Lett. 2022;14:52. doi: 10.1007/s40820-021-00787-0. [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 15.Ding H, Wu Z, Wang H, et al. An ultrastretchable, high-performance, and crosstalk-free proximity and pressure bimodal sensor based on ionic hydrogel fibers for human-machine interfaces. Mater Horiz, 2022, doi: 10.1039/D2MH00281G [DOI] [PubMed]
  • 16.Wei Y, Wang H, Ding Q, et al. Hydrogel- and organohydrogel-based stretchable, ultrasensitive, transparent, room-temperature and real-time NO2 sensors and the mechanism. Mater Horiz, 2022, doi: 10.1039/D2MH00284A [DOI] [PubMed]
  • 17.Zhang C, Wu B, Zhou Y, et al. Mussel-inspired hydrogels: From design principles to promising applications. Chem Soc Rev. 2020;49:3605–3637. doi: 10.1039/C9CS00849G. [DOI] [PubMed] [Google Scholar]
  • 18.Yang C, Suo Z. Hydrogel ionotronics. Nat Rev Mater. 2018;3:125–142. doi: 10.1038/s41578-018-0018-7. [DOI] [Google Scholar]
  • 19.Le HH, Tran VT, Mredha MTI, et al. Thin-film hydrogels with superior stiffness, strength, and stretchability. Extreme Mech Lett. 2020;37:100720. doi: 10.1016/j.eml.2020.100720. [DOI] [Google Scholar]
  • 20.Wu Z, Yang X, Wu J. Conductive hydrogel- and organohydrogel-based stretchable sensors. ACS Appl Mater Interfaces. 2021;13:2128–2144. doi: 10.1021/acsami.0c21841. [DOI] [PubMed] [Google Scholar]
  • 21.Mo F, Liang G, Wang D, et al. Biomimetic organohydrogel electrolytes for high-environmental adaptive energy storage devices. EcoMat. 2019;1:e12008. doi: 10.1002/eom2.12008. [DOI] [Google Scholar]
  • 22.Wu S, Alsaid Y, Yao B, et al. Rapid and scalable fabrication of ultra-stretchable, anti-freezing conductive gels by cononsolvency effect. EcoMat. 2021;3:e12085. [Google Scholar]
  • 23.Lu L, Jiang C, Hu G, et al. Flexible noncontact sensing for human-machine interaction. Adv Mater. 2021;33:2100218. doi: 10.1002/adma.202100218. [DOI] [PubMed] [Google Scholar]
  • 24.Jeong W, Song J, Bae J, et al. Breathable nanomesh humidity sensor for real-time skin humidity monitoring. ACS Appl Mater Interfaces. 2019;11:44758–44763. doi: 10.1021/acsami.9b17584. [DOI] [PubMed] [Google Scholar]
  • 25.Massaroni C, Nicolò A, Schena E, et al. Remote respiratory monitoring in the time of COVID-19. Front Physiol. 2020;11:635. doi: 10.3389/fphys.2020.00635. [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 26.Zhu P, Liu Y, Fang Z, et al. Flexible and highly sensitive humidity sensor based on cellulose nanofibers and carbon nanotube composite film. Langmuir. 2019;35:4834–4842. doi: 10.1021/acs.langmuir.8b04259. [DOI] [PubMed] [Google Scholar]
  • 27.Li B, Xiao G, Liu F, et al. A flexible humidity sensor based on silk fabrics for human respiration monitoring. J Mater Chem C. 2018;6:4549–4554. doi: 10.1039/C8TC00238J. [DOI] [Google Scholar]
  • 28.Lan L, Le X, Dong H, et al. One-step and large-scale fabrication of flexible and wearable humidity sensor based on laser-induced graphene for real-time tracking of plant transpiration at bio-interface. Biosens Bioelectron. 2020;165:112360. doi: 10.1016/j.bios.2020.112360. [DOI] [PubMed] [Google Scholar]
  • 29.Park R, Kim H, Lone S, et al. One-step laser patterned highly uniform reduced graphene oxide thin films for circuit-enabled tattoo and flexible humidity sensor application. Sensors. 2018;18:1857. doi: 10.3390/s18061857. [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 30.Songkeaw P, Onlaor K, Thiwawong T, et al. Transparent and flexible humidity sensor based on graphene oxide thin films prepared by electrostatic spray deposition technique. J Mater Sci-Mater Electron. 2020;31:12206–12215. doi: 10.1007/s10854-020-03766-0. [DOI] [Google Scholar]
  • 31.Zhang X, Maddipatla D, Bose AK, et al. Printed carbon nanotubes-based flexible resistive humidity sensor. IEEE Sens J. 2020;20:12592–12601. doi: 10.1109/JSEN.2020.3002951. [DOI] [Google Scholar]
  • 32.Zhou C, Zhang X, Tang N, et al. Rapid response flexible humidity sensor for respiration monitoring using nano-confined strategy. Nanotechnology. 2020;31:125302. doi: 10.1088/1361-6528/ab5cda. [DOI] [PubMed] [Google Scholar]
  • 33.Wu J, Wu Z, Ding H, et al. Multifunctional and high-sensitive sensor capable of detecting humidity, temperature, and flow stimuli using an integrated microheater. ACS Appl Mater Interfaces. 2019;11:43383–43392. doi: 10.1021/acsami.9b16336. [DOI] [PubMed] [Google Scholar]
  • 34.Wu J, Sun YM, Wu Z, et al. Carbon nanocoil-based fast-response and flexible humidity sensor for multifunctional applications. ACS Appl Mater Interfaces. 2019;11:4242–4251. doi: 10.1021/acsami.8b18599. [DOI] [PubMed] [Google Scholar]
  • 35.Cai J, Lv C, Aoyagi E, et al. Laser direct writing of a high-performance all-graphene humidity sensor working in a novel sensing mode for portable electronics. ACS Appl Mater Interfaces. 2018;10:23987–23996. doi: 10.1021/acsami.8b07373. [DOI] [PubMed] [Google Scholar]
  • 36.Hajian S, Zhang X, Maddipatla D, et al. Development of a fluorinated graphene-based flexible humidity sensor. In: 2019 IEEE International Conference on Flexible and Printable Sensors and Systems (FLEPS), Glasgow, 2019, 1–3
  • 37.Zhang D, Zong X, Wu Z, et al. Hierarchical self-assembled SnS2 nanoflower/Zn2SnO4 hollow sphere nanohybrid for humidity-sensing applications. ACS Appl Mater Interfaces. 2018;10:32631–32639. doi: 10.1021/acsami.8b08493. [DOI] [PubMed] [Google Scholar]
  • 38.Guo J, Wen R, Liu Y, et al. Piezotronic effect enhanced flexible humidity sensing of monolayer MoS2. ACS Appl Mater Interfaces. 2018;10:8110–8116. doi: 10.1021/acsami.7b17529. [DOI] [PubMed] [Google Scholar]
  • 39.Jenjeti RN, Kumar R, Sampath S. Two-dimensional, few-layer NiPS3 for flexible humidity sensor with high selectivity. J Mater Chem A. 2019;7:14545–14551. doi: 10.1039/C9TA03214B. [DOI] [Google Scholar]
  • 40.Duy LT, Baek JY, Mun YJ, et al. Patternable production of SrTiO3 nanoparticles using 1-W laser directly on flexible humidity sensor platform based on ITO/SrTiO3/CNT. J Mater Sci Tech. 2021;71:186–194. doi: 10.1016/j.jmst.2020.07.024. [DOI] [Google Scholar]
  • 41.Feng Y, Gong S, Du E, et al. TaS2 nanosheet-based ultrafast response and flexible humidity sensor for multifunctional applications. J Mater Chem C. 2019;7:9284–9292. doi: 10.1039/C9TC02785H. [DOI] [Google Scholar]
  • 42.Jeong H, Noh Y, Lee D. Highly stable and sensitive resistive flexible humidity sensors by means of roll-to-roll printed electrodes and flowerlike TiO2 nanostructures. Ceramics Int. 2019;45:985–992. doi: 10.1016/j.ceramint.2018.09.276. [DOI] [Google Scholar]
  • 43.Kim H, Park S, Park Y, et al. Fabrication of a semi-transparent flexible humidity sensor using kinetically sprayed cupric oxide film. Sens Actuat B-Chem. 2018;274:331–337. doi: 10.1016/j.snb.2018.07.127. [DOI] [Google Scholar]
  • 44.Zhou G, Byun JH, Oh Y, et al. Highly sensitive wearable textile-based humidity sensor made of high-strength, single-walled carbon nanotube/poly(vinyl alcohol) filaments. ACS Appl Mater Interfaces. 2017;9:4788–4797. doi: 10.1021/acsami.6b12448. [DOI] [PubMed] [Google Scholar]
  • 45.Wang Y, Zhang L, Zhou J, et al. Flexible and transparent cellulose-based ionic film as a humidity sensor. ACS Appl Mater Interfaces. 2020;12:7631–7638. doi: 10.1021/acsami.9b22754. [DOI] [PubMed] [Google Scholar]
  • 46.Zhang D, Jiang C, Sun Y, et al. Layer-by-layer self-assembly of tricobalt tetroxide-polymer nanocomposite toward high-performance humidity-sensing. J Alloys Compd. 2017;711:652–658. doi: 10.1016/j.jallcom.2017.03.365. [DOI] [Google Scholar]
  • 47.Zhang D, Zong X, Wu Z. Fabrication of tin disulfide/graphene oxide nanoflower on flexible substrate for ultrasensitive humidity sensing with ultralow hysteresis and good reversibility. Sens Actuat B-Chem. 2019;287:398–407. doi: 10.1016/j.snb.2019.01.123. [DOI] [Google Scholar]
  • 48.Qi P, Zhang T, Shao J, et al. A QCM humidity sensor constructed by graphene quantum dots and chitosan composites. Sens Actuat A-Phys. 2019;287:93–101. doi: 10.1016/j.sna.2019.01.009. [DOI] [Google Scholar]
  • 49.Ying B, Wu Q, Li J, et al. An ambient-stable and stretchable ionic skin with multimodal sensation. Mater Horiz. 2020;7:477–488. doi: 10.1039/C9MH00715F. [DOI] [Google Scholar]
  • 50.Li T, Li L, Sun H, et al. Porous ionic membrane based flexible humidity sensor and its multifunctional applications. Adv Sci. 2017;4:1600404. doi: 10.1002/advs.201600404. [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 51.Lim C, Hong YJ, Jung J, et al. Tissue-like skin-device interface for wearable bioelectronics by using ultrasoft, mass-permeable, and low-impedance hydrogels. Sci Adv. 2021;7:eabd3716. doi: 10.1126/sciadv.abd3716. [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 52.Chen X, He M, Zhang X, et al. Metal-free and stretchable conductive hydrogels for high transparent conductive film and flexible strain sensor with high sensitivity. Macromol Chem Phys. 2020;221:2000054. doi: 10.1002/macp.202000054. [DOI] [Google Scholar]
  • 53.Wu Z, Ding H, Tao K, et al. Ultrasensitive, stretchable, and fast-response temperature sensors based on hydrogel films for wearable applications. ACS Appl Mater Interfaces. 2021;13:21854–21864. doi: 10.1021/acsami.1c05291. [DOI] [PubMed] [Google Scholar]
  • 54.Buchberger A, Peterka S, Coclite AM, et al. Fast optical humidity sensor based on hydrogel thin film expansion for harsh environment. Sensors. 2019;19:999. doi: 10.3390/s19050999. [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 55.Huang Y, Zhang X, Ma Z, et al. Hydrogen-bond relaxation dynamics: Resolving mysteries of water ice. Coord Chem Rev. 2015;285:109–165. doi: 10.1016/j.ccr.2014.10.003. [DOI] [Google Scholar]
  • 56.Wu Z, Shi W, Ding H, et al. Ultrastable, stretchable, highly conductive and transparent hydrogels enabled by salt-percolation for high-performance temperature and strain sensing. J Mater Chem C. 2021;9:13668–13679. doi: 10.1039/D1TC02506F. [DOI] [Google Scholar]
  • 57.Trung TQ, Duy LT, Ramasundaram S, et al. Transparent, stretchable, and rapid-response humidity sensor for body-attachable wearable electronics. Nano Res. 2017;10:2021–2033. doi: 10.1007/s12274-016-1389-y. [DOI] [Google Scholar]
  • 58.Guo H, Lan C, Zhou Z, et al. Transparent, flexible, and stretchable WS2 based humidity sensors for electronic skin. Nanoscale. 2017;9:6246–6253. doi: 10.1039/C7NR01016H. [DOI] [PubMed] [Google Scholar]
  • 59.Huang X, Li B, Wang L, et al. Superhydrophilic, underwater superoleophobic, and highly stretchable humidity and chemical vapor sensors for human breath detection. ACS Appl Mater Interfaces. 2019;11:24533–24543. doi: 10.1021/acsami.9b04304. [DOI] [PubMed] [Google Scholar]
  • 60.Guo YN, Gao ZY, Wang XX, et al. A highly stretchable humidity sensor based on spandex covered yarns and nanostructured polyaniline. RSC Adv. 2018;8:1078–1082. doi: 10.1039/C7RA10474J. [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 61.Ho DH, Sun Q, Kim SY, et al. Stretchable and multimodal all graphene electronic skin. Adv Mater. 2016;28:2601–2608. doi: 10.1002/adma.201505739. [DOI] [PubMed] [Google Scholar]
  • 62.Li Y, Pham JQ, Johnston KP, et al. Contact angle of water on polystyrene thin films: Effects of CO2 environment and film thickness. Langmuir. 2007;23:9785–9793. doi: 10.1021/la0636311. [DOI] [PubMed] [Google Scholar]
  • 63.Islam T, Ur Rahman MZ. Investigation of the electrical characteristics on measurement frequency of a thin-film ceramic humidity sensor. IEEE Trans Instrum Meas. 2016;65:694–702. doi: 10.1109/TIM.2015.2506302. [DOI] [Google Scholar]
  • 64.Ju M, Wu B, Sun S, et al. Redox-active iron-citrate complex regulated robust coating-free hydrogel microfiber net with high environmental tolerance and sensitivity. Adv Funct Mater. 2020;30:1910387. doi: 10.1002/adfm.201910387. [DOI] [Google Scholar]
  • 65.Lei Z, Wu P. A highly transparent and ultra-stretchable conductor with stable conductivity during large deformation. Nat Commun. 2019;10:3429. doi: 10.1038/s41467-019-11364-w. [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 66.Huang J. Diffusion impedance of electroactive materials, electrolytic solutions and porous electrodes: Warburg impedance and beyond. Electrochim Acta. 2018;281:170–188. doi: 10.1016/j.electacta.2018.05.136. [DOI] [Google Scholar]
  • 67.Bi H, Yin K, Xie X, et al. Ultrahigh humidity sensitivity of graphene oxide. Sci Rep. 2013;3:2714. doi: 10.1038/srep02714. [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 68.Li N, Chen X, Chen X, et al. Ultrahigh humidity sensitivity of graphene oxide combined with Ag nanoparticles. RSC Adv. 2017;7:45988–45996. doi: 10.1039/C7RA06959F. [DOI] [Google Scholar]
  • 69.Zammit C, Liddicoat H, Moonsie I, et al. Obesity and respiratory diseases. Int J Gen Med. 2010;3:335. doi: 10.2147/IJGM.S11926. [DOI] [PMC free article] [PubMed] [Google Scholar]

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Supplementary Materials

40843_2021_2022_MOESM1_ESM.pdf (1.3MB, pdf)

Ultrasensitive, stretchable, and transparent humidity sensor based on ion-conductive double-network hydrogel thin films


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