Issue

Vol. 14 (2022)

High-Performance Flexible Microneedle Array as a Low-Impedance Surface Biopotential Dry Electrode for Wearable Electrophysiological Recording and Polysomnography

https://doi.org/10.1007/s40820-022-00870-0
Junshi Li
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Yundong Ma
Peking University Sixth Hospital, Peking University Institute of Mental Health, NHC Key Laboratory of Mental Health (Peking University), National Clinical Research Center for Mental Disorders (Peking University Sixth Hospital), Beijing 100191, People’s Republic of China
Dong Huang
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Zhongyan Wang
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Zhitong Zhang
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Yingjie Ren
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Mengyue Hong
Peking University Sixth Hospital, Peking University Institute of Mental Health, NHC Key Laboratory of Mental Health (Peking University), National Clinical Research Center for Mental Disorders (Peking University Sixth Hospital), Beijing 100191, People’s Republic of China
Yufeng Chen
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Tingyu Li
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Xiaoyi Shi
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Lu Cao
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Jiayan Zhang
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Bingli Jiao
School of Electronics, Peking University, Beijing 100871, People’s Republic of China
Junhua Liu
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China
Hongqiang Sun
Peking University Sixth Hospital, Peking University Institute of Mental Health, NHC Key Laboratory of Mental Health (Peking University), National Clinical Research Center for Mental Disorders (Peking University Sixth Hospital), Beijing 100191, People’s Republic of China
Zhihong Li
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, School of Integrated Circuits, Peking University, Beijing 100871, People’s Republic of China

Corresponding Author: Zhihong Li

zhhli@pku.edu.cn

Nano-Micro Letters, Vol. 14 (2022), Article Number: 132

Abstract

Microneedle array (MNA) electrodes are an effective solution to achieve high-quality surface biopotential recording without the coordination of conductive gel and are thus very suitable for long-term wearable applications. Existing schemes are limited by flexibility, biosafety, and manufacturing costs, which create large barriers for wider applications. Here, we present a novel flexible MNA electrode that can simultaneously achieve flexibility of the substrate to fit a curved body surface, robustness of microneedles to penetrate the skin without fracture, and a simplified process to allow mass production. The compatibility with wearable wireless systems and the short preparation time of the electrodes significantly improves the comfort and convenience of electrophysiological recording. The normalized electrode–skin contact impedance reaches 0.98 kΩ cm2 at 1 kHz and 1.50 kΩ cm2 at 10 Hz, a record low value compared to previous reports and approximately 1/250 of the standard electrodes. The morphology, biosafety, and electrical/mechanical properties are fully characterized, and wearable recordings with a high signal-to-noise ratio and low motion artifacts are realized. The first reported clinical study of microneedle electrodes for surface electrophysiological monitoring was conducted in tens of healthy and sleep-disordered subjects with 44 nights of recording (over 8 h per night), providing substantial evidence that the electrodes can be leveraged to substitute for clinical standard electrodes.


Highlights:


1 Polyimide-based flexible microneedle array (PI-MNA) electrodes realize high electrical/mechanical performance and are compatible with wearable wireless recording systems.
2 The normalized electrode–skin interface impedance (EII) of the PI-MNA electrodes reaches 0.98 kΩ cm2 at 1 kHz and 1.50 kΩ cm2 at 10 Hz, approximately 1/250 of clinical standard electrodes.
3 This is the first report on the clinical study of microneedle electrodes. The PI-MNA electrodes are applied to clinical long-term continuous monitoring for polysomnography.

Keywords

Flexible microneedle array Dry electrode Low-impedance electrode–skin contact Wearable wireless electrophysiological recording Polysomnography
Li, Junshi, Yundong Ma, Dong Huang, Zhongyan Wang, Zhitong Zhang, Yingjie Ren, Mengyue Hong, Yufeng Chen, Tingyu Li, Xiaoyi Shi, Lu Cao, Jiayan Zhang, Bingli Jiao, Junhua Liu, Hongqiang Sun, and Zhihong Li. 2022. “High-Performance Flexible Microneedle Array As a Low-Impedance Surface Biopotential Dry Electrode for Wearable Electrophysiological Recording and Polysomnography”. Nano-Micro Letters 14 (June):132. https://doi.org/10.1007/s40820-022-00870-0.
Download Citation
Endnote/Zotero/Mendeley (RIS)
BibTeX
References
  1. Y. Ling, T. An, L.W. Yap, B. Zhu, S. Gong et al., Disruptive, soft, wearable sensors. Adv. Mater. 32(18), 1904664 (2020). https://doi.org/10.1002/adma.201904664
  2. T.R. Ray, J. Choi, A.J. Bandodkar, S. Krishnan, P. Gutruf et al., Bio-integrated wearable systems: a comprehensive review. Chem. Rev. 119(8), 5461–5533 (2019). https://doi.org/10.1021/acs.chemrev.8b00573
  3. Y.H. Wang, L. Yin, Y.Z. Bai, S.Y. Liu, L. Wang et al., Electrically compensated, tattoo-like electrodes for epidermal electrophysiology at scale. Sci. Adv. 6(43), abd0996 (2020). https://doi.org/10.1126/sciadv.abd0996
  4. L. Tian, B. Zimmerman, A. Akhtar, K.J. Yu, M. Moore et al., Large-area MRI-compatible epidermal electronic interfaces for prosthetic control and cognitive monitoring. Nat. Biomed. Eng. 3(3), 194–205 (2019). https://doi.org/10.1038/s41551-019-0347-x
  5. L.F. Wang, J.Q. Liu, B. Yang, C.S. Yang, PDMS-based low cost flexible dry electrode for long-term EEG measurement. IEEE Sens. J. 12(9), 2898–2904 (2012). https://doi.org/10.1109/jsen.2012.2204339
  6. Y. Fu, J. Zhao, Y. Dong, X. Wang, Dry electrodes for human bioelectrical signal monitoring. Sensors 20(13), 3651 (2020). https://doi.org/10.3390/s20133651
  7. P. Leleux, C. Johnson, X. Strakosas, J. Rivnay, T. Herve et al., Ionic liquid gel-assisted electrodes for long-term cutaneous recordings. Adv. Healthc. Mater. 3(9), 1377–1380 (2014). https://doi.org/10.1002/adhm.201300614
  8. K.P. Gao, H.J. Yang, X.L. Wang, B. Yang, J.Q. Liu, Soft pin-shaped dry electrode with bristles for EEG signal measurements. Sens. Actuators A Phys. 283, 348–361 (2018). https://doi.org/10.1016/j.sna.2018.09.045
  9. F. Stauffer, M. Thielen, C. Sauter, S. Chardonnens, S. Bachmann et al., Skin conformal polymer electrodes for clinical ECG and EEGrecordings. Adv. Healthc. Mater. 7(7), 1700994 (2018). https://doi.org/10.1002/adhm.201700994
  10. C.T. Lin, L.D. Liao, Y.H. Liu, I.J. Wang, B.S. Lin et al., Novel dry polymer foam electrodes for long-term EEG measurement. IEEE Trans. Biomed. Eng. 58(5), 1200–1207 (2011). https://doi.org/10.1109/TBME.2010.2102353
  11. T.M. Blicharz, P. Gong, B.M. Bunner, L.L. Chu, K.M. Leonard et al., Microneedle-based device for the one-step painless collection of capillary blood samples. Nat. Biomed. Eng. 2(3), 151–157 (2018). https://doi.org/10.1038/s41551-018-0194-1
  12. P. Dardano, I. Rea, L.D. Stefano, Microneedles-based electrochemical sensors: new tools for advanced biosensing. Curr. Opi. Electrochem. 17, 121–127 (2019). https://doi.org/10.1016/j.coelec.2019.05.012
  13. D. Huang, J. Li, T. Li, Z. Wang, Q. Wang et al., Recent advances on fabrication of microneedles on the flexible substrate. J. Micromech. Microeng. 31(7), 0073001 (2021). https://doi.org/10.1088/1361-6439/ac0513
  14. N.W. Kang, S. Kim, J.Y. Lee, K.T. Kim, Y. Choi et al., Microneedles for drug delivery: recent advances in materials and geometry for preclinical and clinical studies. Expert Opin. Drug Deliv. 18(7), 929–947 (2021). https://doi.org/10.1080/17425247.2021.1828860
  15. S. Kusama, K. Sato, Y. Matsui, N. Kimura, H. Abe et al., Transdermal electroosmotic flow generated by a porous microneedle array patch. Nat. Commun. 12, 658 (2021). https://doi.org/10.1038/s41467-021-20948-4
  16. W. Li, R.N. Terry, J. Tang, M.R. Feng, S.P. Schwendeman et al., Rapidly separable microneedle patch for the sustained release of a contraceptive. Nat. Biomed. Eng. 3(3), 220–229 (2019). https://doi.org/10.1038/s41551-018-0337-4
  17. G.S. Liu, Y. Kong, Y. Wang, Y. Luo, X. Fan et al., Microneedles for transdermal diagnostics: recent advances and new horizons. Biomaterials 232, 119740 (2020). https://doi.org/10.1016/j.biomaterials.2019.119740
  18. K.T.M. Tran, T.D. Gavitt, N.J. Farrell, E.J. Curry, A.B. Mara et al., Transdermal microneedles for the programmable burst release of multiple vaccine payloads. Nat. Biomed. Eng. 5(9), 998–1007 (2021). https://doi.org/10.1038/s41551-020-00650-4
  19. Z. Wang, J. Luan, A. Seth, L. Liu, M. You et al., Microneedle patch for the ultrasensitive quantification of protein biomarkers in interstitial fluid. Nat. Biomed. Eng. 5(1), 64–76 (2021). https://doi.org/10.1038/s41551-020-00672-y
  20. G.S. Guvanasen, L. Guo, R.J. Aguilar, A.L. Cheek, C.S. Shafor et al., A stretchable microneedle electrode array for stimulating and measuring intramuscular electromyographic activity. IEEE Trans. Neural Syst. Rehabil. Eng. 25(9), 1440–1452 (2017). https://doi.org/10.1109/TNSRE.2016.2629461
  21. R. Bhandari, S. Negi, F. Solzbacher, Wafer-scale fabrication of penetrating neural microelectrode arrays. Biomed. Microdev. 12(5), 797–807 (2010). https://doi.org/10.1007/s10544-010-9434-1
  22. X. Hong, Z. Wu, L. Chen, F. Wu, L. Wei et al., Hydrogel microneedle arrays for transdermal drug delivery. Nano-Micro Lett. 6, 191–199 (2014). https://doi.org/10.1007/bf03353783
  23. P. Makvandi, R. Jamaledin, G. Chen, Z. Baghbantaraghdari, E.N. Zare et al., Stimuli-responsive transdermal microneedle patches. Mater. Today 47, 206–222 (2021). https://doi.org/10.1016/j.mattod.2021.03.012
  24. P. Makvandi, A. Maleki, M. Shabani, A. Hutton, M. Kirkby et al., Bioinspired microneedle patches: biomimetic designs, fabrication, and biomedical applications. Matter 5(2), 390–429 (2022). https://doi.org/10.1016/j.matt.2021.11.021
  25. L. Ren, B. Liu, W. Zhou, L. Jiang, A mini review of microneedle array electrode for bio-signal recording: a review. IEEE Sens. J. 20(2), 577–590 (2020). https://doi.org/10.1109/jsen.2019.2944847
  26. M. Kim, T. Kim, D.S. Kim, W.K. Chung, Curved microneedle array-based sEMG electrode for robust long-term measurements and high selectivity. Sensors 15(7), 16265–16280 (2015). https://doi.org/10.3390/s150716265
  27. P. Makvandi, M. Kirkby, A.R.J. Hutton, M. Shabani, C.K.Y. Yiu et al., Engineering microneedle patches for improved penetration: analysis, skin models and factors affecting needle insertion. Nano-Micro Lett. 13, 93 (2021). https://doi.org/10.1007/s40820-021-00611-9
  28. Y. Hou, Z. Li, Z. Wang, H. Yu, Miura-ori structured flexible microneedle array electrode for biosignal recording. Microsyst. Nanoeng. 7, 53 (2021). https://doi.org/10.1038/s41378-021-00259-w
  29. R. Wang, X. Jiang, W. Wang, Z. Li, A microneedle electrode array on flexible substrate for long-term EEG monitoring. Sens. Actuators B Chem. 244, 750–758 (2017). https://doi.org/10.1016/j.snb.2017.01.052
  30. R. Wang, W. Zhao, W. Wang, Z. Li, A flexible microneedle electrode array with solid silicon needles. J. Microelectromech. Syst. 21(5), 1084–1089 (2012). https://doi.org/10.1109/jmems.2012.2203790
  31. L. Ren, Q. Jiang, Z. Chen, K. Chen, S. Xu et al., Flexible microneedle array electrode using magnetorheological drawing lithography for bio-signal monitoring. Sens. Actuators A Phys. 268, 38–45 (2017). https://doi.org/10.1016/j.sna.2017.10.042
  32. L. Ren, S. Xu, J. Gao, Z. Lin, Z. Chen et al., Fabrication of flexible microneedle array electrodes for wearable bio-signal recording. Sensors 18(4), 1191 (2018). https://doi.org/10.3390/s18041191
  33. M. Mahmood, S. Kwon, H. Kim, Y.S. Kim, P. Siriaraya et al., Wireless soft scalp electronics and virtual reality system for motor imagery-based brain–machine interfaces. Adv. Sci. 8(19), 2101129 (2021). https://doi.org/10.1002/advs.202101129
  34. L.F. Wang, J.Q. Liu, X.X. Yan, B. Yang, C.S. Yang, A MEMS-based pyramid micro-needle electrode for long-term EEG measurement. Microsyst. Technol. 19(2), 269–276 (2012). https://doi.org/10.1007/s00542-012-1638-2
  35. R. Wang, W. Wang, Z. Li, An improved manufacturing approach for discrete silicon microneedle arrays with tunable height-pitch ratio. Sensors 16(10), 1628 (2016). https://doi.org/10.3390/s16101628
  36. H. Roh, Y.J. Yoon, J.S. Park, D.H. Kang, S.M. Kwak et al., Fabrication of high-density out-of-plane microneedle arrays with various heights and diverse cross-sectional shapes. Nano-Micro Lett. 14, 24 (2021). https://doi.org/10.1007/s40820-021-00778-1
  37. K. Badnikar, S.N. Jayadevi, S. Pahal, S. Sripada, M.M. Nayak et al., Generic molding platform for simple, low-cost fabrication of polymeric microneedles. Macromol. Mater. Eng. 305(5), 2000072 (2020). https://doi.org/10.1002/mame.202000072
  38. R. He, Y. Niu, Z. Li, A. Li, H. Yang et al., A hydrogel microneedle patch for point-of-care testing based on skin interstitial fluid. Adv. Healthc. Mater. 9(4), 1901201 (2020). https://doi.org/10.1002/adhm.201901201
  39. K.J. Krieger, N. Bertollo, M. Dangol, J.T. Sheridan, M.M. Lowery et al., Simple and customizable method for fabrication of high-aspect ratio microneedle molds using low-cost 3D printing. Microsyst. Nanoeng. 5, 42 (2019). https://doi.org/10.1038/s41378-019-0088-8
  40. J. Madden, C. O’Mahony, M. Thompson, A. O’Riordan, P. Galvin, Biosensing in dermal interstitial fluid using microneedle based electrochemical devices. Sens. Bio. Sens. Res. 29, 100348 (2020). https://doi.org/10.1016/j.sbsr.2020.100348
  41. K.J. Krieger, J. Liegey, E.M. Cahill, N. Bertollo, M.M. Lowery et al., Development and evaluation of 3D-printed dry microneedle electrodes for surface electromyography. Adv. Mater. Technol. 5(10), 2000518 (2020). https://doi.org/10.1002/admt.202000518
  42. L. Ren, Z. Chen, H. Wang, Z. Dou, B. Liu et al., Fabrication of bendable microneedle-array electrode by magnetorheological drawing lithography for electroencephalogram recording. IEEE Trans. Instrum. Meas. 69(10), 8328–8334 (2020). https://doi.org/10.1109/tim.2020.2990523
  43. R. Soltanzadeh, E. Afsharipour, C. Shafai, N. Anssari, B. Mansouri et al., Molybdenum coated SU-8 microneedle electrodes for transcutaneous electrical nerve stimulation. Biomed. Microdev. 20, 1 (2017). https://doi.org/10.1007/s10544-017-0241-9
  44. A.K. Srivastava, B. Bhartia, K. Mukhopadhyay, A. Sharma, Long term biopotential recording by body conformable photolithography fabricated low cost polymeric microneedle arrays. Sens. Actuators A Phys. 236, 164–172 (2015). https://doi.org/10.1016/j.sna.2015.10.041
  45. K. Moussi, A. Bukhamsin, T. Hidalgo, J. Kosel, Biocompatible 3D printed microneedles for transdermal, intradermal, and percutaneous applications. Adv. Eng. Mater. 22(2), 1901358 (2019). https://doi.org/10.1002/adem.201901358
  46. J.H. Lee, H. Kim, J.H. Kim, S.H. Lee, Soft implantable microelectrodes for future medicine: prosthetics, neural signal recording and neuromodulation. Lab Chip 16(6), 959–976 (2016). https://doi.org/10.1039/c5lc00842e
  47. S. Venkatraman, J. Hendricks, Z.A. King, A.J. Sereno, S. Richardson-Burns et al., In vitro and in vivo evaluation of pedot microelectrodes for neural stimulation and recording. IEEE Trans. Neural Syst. Rehabil. Eng. 19(3), 307–316 (2011). https://doi.org/10.1109/tnsre.2011.2109399
  48. N. Rossetti, P. Luthra, J.E. Hagler, A.H.J. Lee, C. Bodart et al., Poly(3,4-ethylenedioxythiophene) (PEDOT) coatings for high-quality electromyography recording. ACS Appl. Bio Mater. 2(11), 5154–5163 (2019). https://doi.org/10.1021/acsabm.9b00809
  49. C. Bodart, N. Rossetti, J.E. Hagler, P. Chevreau, D. Chhin et al., Electropolymerized poly(3,4-ethylenedioxythiophene) (PEDOT) coatings for implantable deep-brain-stimulating microelectrodes. ACS Appl. Mater. Interfaces 11(19), 17226–17233 (2019). https://doi.org/10.1021/acsami.9b03088
  50. P. Fattahi, G. Yang, G. Kim, M.R. Abidian, A review of organic and inorganic biomaterials for neural interfaces. Adv. Mater. 26(12), 1846–1885 (2014). https://doi.org/10.1002/adma.201304496
  51. K.M. Szostak, L. Grand, T.G. Constandinou, Neural interfaces for intracortical recording: requirements, fabrication methods, and characteristics. Front. Neurosci. 11, 665 (2017). https://doi.org/10.3389/fnins.2017.00665
  52. C.A. Goldstein, R.D. Chervin, Use of clinical tools and tests in sleep medicine, in Principles and Practice of Sleep Medicine. (Elsevier, 2017), pp. 607–617. https://doi.org/10.1016/B978-0-323-24288-2.00060-X
  53. Products: sleep diagnostics. (Compumedics). https://www.compumedics.com.au/en/product-category/sleep-diagnostics/
  54. What is EEGLAB? (Swartz Center for Computational Neuroscience). https://sccn.ucsd.edu/eeglab/
Read More
Author biographies are not available.
Download this PDF file
PDF SUPPLEMENTARY MATERIAL
Statistic
Read Counter : 4670 Download : 3509