电生理信号的长期稳定采集有助于疾病早期诊断康复和对人体的各种生理认知研究,与皮肤相接触的电极决定了所采集的电生理信号的质量水平。导电水凝胶由于其与生物组织相似的低杨氏模量,可调节的机械性能和高生物相容性的特点在生理电信号无创采集电极中得到了广泛应用研究。综述了近年来在提升导电水凝胶导电性能、机械性能、黏附性能、保湿性能和自愈性能的研究进展,介绍了导电水凝胶在心电、肌电和脑电无创生理电信号采集电极上的应用。
The long-term stable acquisition of electrophysiological signals contributes significantly to early disease diagnosis,rehabilitation,and various physiological cognition studies in humans.The quality of collected electrophysiological signals depends on the electrodes in contact with the skin.Conductive hydrogels,due to their low Young's modulus resembling biological tissues,adjustable mechanical properties,and high biocompatibility,have been widely applied in non-invasive physiological signal collection electrodes.This review summarized recent progress in enhancing the conductivity,mechanical properties,adhesion,moisturizing,and self-healing capabilities of conductive hydrogels.Additionally,it introduced their applications in non-invasive physiological signal collection electrodes for electrocardiography (ECG),electromyography (EMG),and electroencephalography (EEG) based on recent research developments.
[1] Liu J C,Lin S,Li W Z,et al.Ten-hour stable noninvasive brain-computer interface realized by semidry hydrogel-based electrodes[J].Research,2022,2022:12.
[2] Wu B Y,Mai Z F,Ji Z C,et al.Self-compounded,tough biohydrogels for robust self-adhesive biointerfaces[J].Materials Today Physics,2022,29:9.
[3] Shen G C,Gao K P,Zhao N,et al.A fully flexible hydrogel electrode for daily EEG monitoring[J].Ieee Sensors Journal,2022,22(13):12522-12529.
[4] Zhang Y,Mao J C,Jiang W K,et al.Lignin sulfonate induced ultrafast polymerization of double network hydrogels with anti-freezing,high strength and conductivity and their sensing applications at extremely cold conditions[J].Composites Part B-Engineering,2021,217:9.
[5] Gao Y,Wang Y R,Xia S,et al.An environment-stable hydrogel with skin-matchable performance for human-machine interface[J].Science China-Materials,2021,64(9):2313-2324.
[6] Quan L,Tie J F,Wang Y M,et al.Mussel-inspired chitosan-based hydrogel sensor with pH-responsive and adjustable adhesion,toughness and self-healing capability[J].Polymers for Advanced Technologies,2022,33(6):1867-1880.
[7] Tan Y,Zhang Y Y,Zhang Y J,et al.Dual cross-linked ion-based temperature-responsive conductive hydrogels with multiple sensors and steady electrocardiogram monitoring[J].Chemistry of Materials,2020,32(18):7670-7678.
[8] Pan L,Cai P Q,Mei L,et al.A compliant ionic adhesive electrode with ultralow bioelectronic impedance[J].Advanced Materials,2020,32(38):9.
[9] Xing R Z,Huang R L,Su R X,et al.Facile fabrication of a printable conductive self-healing hydrogel for human motion and electrocardiogram monitoring[J].New Journal of Chemistry,2023,47(23):11063-11070.
[10] Ingtipi K,Choudhury B J,Moholkar V S.Ultrasound assisted lignin-decorated MWCNT doped flexible PVA-chitosan composite hydrogel[J].Materials Today Communications,2023,35:11.
[11] Xu J X,Zhang H Y,Guo Z Y,et al.Fully physical crosslinked BSA-based conductive hydrogels with high strength and fast self-recovery for human motion and wireless electrocardiogram sensing[J].International Journal of Biological Macromolecules,2023,230:11.
[12] Kateb P,Fan J,Kim J,et al.Printable,adhesive,and self-healing dry epidermal electrodes based on PEDOT∶PSS and polyurethane diol[J].Flexible and Printed Electronics,2023,8:045006.
[13] Liu L L,Liu Y F,Tang R T,et al.Stable and low-resistance polydopamine methacrylamide-polyacrylamide hydrogel for brain-computer interface[J].Science China-Materials,2022,65(8):2298-2308.
[14] Liu J T,Zhou Y Y,Lu J W,et al.Injectable,tough and adhesive zwitterionic hydrogels for 3D-printed wearable strain sensors[J].Chemical Engineering Journal,2023,475:12.
[15] Shi Y F,Wang W Z,Lei Z X,et al.A transparent,anti-fatigue,flexible multifunctional hydrogel with self-adhesion and conductivity for biosensors[J].Polymer,2023,281:8.
[16] Tan Y,Zhang Y Y,Ge Z Y,et al.Physical cross-linkage constructed supramolecular conductive hydrogel as sustainable and remolded epidermal electronics[J].ACS Applied Polymer Materials,2022,4(4):2585-2594.
[17] Wang F S,Yang L,Sun Y,et al.A nanoclay-enhanced hydrogel for self-adhesive wearable electrophysiology electrodes with high sensitivity and stability[J].Gels,2023,9(4):15.
[18] Yang W J,Zhang R,Guo X,et al.Supramolecular polyelectrolyte hydrogel based on conjoined double-networks for multifunctional applications[J].Journal of Materials Chemistry A,2022,10(44):23649-23665.
[19] Tang L,Li Y W,Liu F,et al.Ultrastretchable,highly conductive,rapid self-recovery,and antiswelling hydrogels as multifunctional wearable electronic devices[J].ACS Applied Electronic Materials,2023,5(10):5651-5660.
[20] Zhao Y H,Zhao Q B,Peng S H,et al.A robust conductive organohydrogel with adhesive and low-hysteresis properties for all-weather human motion and wireless electrocardiogram sensing[J].Journal of Materials Chemistry C,2023,11(46):16135-16142.
[21] Lu Y J,Li Z H,Li Z W,et al.Fabrication of a tough,long-lasting adhesive hydrogel patch via the synergy of interfacial entanglement and adhesion group densification[J].Nanoscale,2024,16(2):645-656.
[22] Xue H L,Wang D Y,Jin M Y,et al.Hydrogel electrodes with conductive and substrate-adhesive layers for noninvasive long-term EEG acquisition[J].Microsystems & Nanoengineering,2023,9(1):14.
[23] Shen G C,Zheng K Y,Jiang C P,et al.A gelatin-based hydrogel electrode with high moisturizing ability for wearable EEG recording[J].Ieee Sensors Journal,2023,23(21):25689-25697.
[24] Shen G C,Gao K P,Zhao N,et al.A novel flexible hydrogel electrode with a strong moisturizing ability for long-term EEG recording[J].Journal of Neural Engineering,2021,18(6):12.
[25] Zhang Q,Liu X,Zhang J W,et al.A highly conductive hydrogel driven by phytic acid towards a wearable sensor with freezing and dehydration resistance[J].Journal of Materials Chemistry A,2021,9(39):22615-22625.
[26] Li J J,Ge S J,Niu Y F,et al.Intrinsically adhesive,conductive organohydrogel with high stretchable,moisture retention,anti-freezing and healable properties for monitoring of human motions and electrocardiogram[J].Sensors and Actuators B-Chemical,2023,377:10.
[27] Xu L J,Chen Y,Yu M L,et al.NIR light-induced rapid self-healing hydrogel toward multifunctional applications in sensing[J].Nano Energy,2023,107:14.
[28] Panwar V,Babu A,Sharma A,et al.Tunable,conductive,self-healing,adhesive and injectable hydrogels for bioelectronics and tissue regeneration applications[J].Journal of Materials Chemistry B,2021,9(31):6260-6270.
[29] Han K,Bai Q,Wu W D,et al.Gelatin-based adhesive hydrogel with self-healing,hemostasis,and electrical conductivity[J].International Journal of Biological Macromolecules,2021,183:2142-2151.
[30] Park J,Kim J Y,Heo J H,et al.Intrinsically nonswellable multifunctional hydrogel with dynamic nanoconfinement networks for robust tissue-adaptable bioelectronics[J].Advanced Science,2023,10(12):15.
[31] Shi Y F,Fu X L,Wang W,et al.Stretchable,adhesive and low impedance hydrogel prepared by one-pot method used as ECG electrodes[J].Colloids and Surfaces A-Physicochemical and Engineering Aspects,2023,662:10.
[32] Hao P,Gao X,Li Z,et al.Multi-branch fusion network for myocardial infarction screening from 12-lead ECG images[J].Computer Methods and Programs in Biomedicine,2020,DOI:10.1016/j.cmpb.2019.105286.
[33] Aufan M R,Jost Z T,Miller N J,et al.Electrocardiogram to determine mitral and aortic valve opening and closure[J].Cardiovascular Engineering and Technology,2023,14(3):447-456.
[34] Nahak S,Pathak A,Saha G.Fragment-level classification of ECG arrhythmia using wavelet scattering transform[J].Expert Systems with Applications,2023,224:16.
[35] Lee Y,Yim S G,Lee G W,et al.Self-adherent biodegradable gelatin-based hydrogel electrodes for electrocardiography monitoring[J].Sensors,2020,20(20):12.
[36] Hou Y,Li Y Z,Li Y Q,et al.Tuning water-resistant networks in mussel-inspired hydrogels for robust wet tissue and bioelectronic adhesion[J].ACS Nano,2023,17(3):2745-2760.
[37] Yu J W,Wan R T,Tian F J,et al.3D printing of robust high-performance conducting polymer hydrogel-based electrical bioadhesive interface for soft bioelectronics[J].Small,2024,20(19):2308778.
[38] Zhang Y R,Chen L,Xie M Z,et al.Ultra-fast programmable human-machine interface enabled by 3D printed degradable conductive hydrogel[J].Materials Today Physics,2022,27:9.
[39] Wang C Y,Wang H Y,Wang B H,et al.On-skin paintable biogel for long-term high-fidelity electroencephalogram recording[J].Science Advances,2022,8(20):11.
[40] Luo J B,Sun C Y,Chang B Y,et al.MXene-enabled self-adaptive hydrogel interface for active electroencephalogram interactions[J].ACS Nano,2022,16(11):19373-19384.
基金资助
中国医学科学院医学与健康科技创新工程(重大协同创新项目)(2021-I2M-1-058,2021-I2M-1-042);天津市杰出青年基金项目(20JCJQIC00230);CAMS医学科学创新基金项目(CIFMS)(2022-I2M-C&T-B-012)