An Environment-Tolerant Ion-Conducting Double-Network Composite Hydrogel for High-Performance Flexible Electronic Devices

doi:10.1007/s40820-023-01311-2

Abstract

Abstract:

High-performance ion-conducting hydrogels (ICHs) are vital for developing flexible electronic devices. However, the robustness and ion-conducting behavior of ICHs deteriorate at extreme temperatures, hampering their use in soft electronics. To resolve these issues, a method involving freeze-thawing and ionizing radiation technology is reported herein for synthesizing a novel double-network (DN) ICH based on a poly(ionic liquid)/MXene/poly(vinyl alcohol) (PMP DN ICH) system. The well-designed ICH exhibits outstanding ionic conductivity (63.89 mS cm⁻¹ at 25 °C), excellent temperature resistance (− 60-80 °C), prolonged stability (30 d at ambient temperature), high oxidation resistance, remarkable antibacterial activity, decent mechanical performance, and adhesion. Additionally, the ICH performs effectively in a flexible wireless strain sensor, thermal sensor, all-solid-state supercapacitor, and single-electrode triboelectric nanogenerator, thereby highlighting its viability in constructing soft electronic devices. The highly integrated gel structure endows these flexible electronic devices with stable, reliable signal output performance. In particular, the all-solid-state supercapacitor containing the PMP DN ICH electrolyte exhibits a high areal specific capacitance of 253.38 mF cm⁻² (current density, 1 mA cm⁻²) and excellent environmental adaptability. This study paves the way for the design and fabrication of high-performance multifunctional/flexible ICHs for wearable sensing, energy-storage, and energy-harvesting applications.

Key words: Ionic liquids, Double-network hydrogels, Temperature tolerance, Multifunctionality, Flexible electronic devices

Wenchao Zhao, Haifeng Zhou, Wenkang Li, Manlin Chen, Min Zhou, Long Zhao. An Environment-Tolerant Ion-Conducting Double-Network Composite Hydrogel for High-Performance Flexible Electronic Devices[J]. Nano-Micro Letters, 2024, 16(1): 99-.

Wenchao Zhao, Haifeng Zhou, Wenkang Li, Manlin Chen, Min Zhou, Long Zhao. [J]. Nano-Micro Letters, 2024, 16(1): 99-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-023-01311-2

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/99

Figures/Tables 8

Fig. 1 Preparation and characterization of the PIL/MXene/PVA (PMP)-based double-network (DN) ion-conducting hydrogel (ICH). Schematics illustrating the a construction of PMP DN ICH and its b multiple hydrogen bond interactions. c, d FTIR and XRD spectra of VBImBr, Ph-3MVIm-Br, the MXene, PVA, and PMP DN ICH. e SEM image of PMP DN ICH

Fig. 2 a, b Photographs of PMP DN ICH undergoing stretching and compression. c, d Cyclic tensile and compressive loading-unloading curves of PMP DN ICH at strains of up to 100% and 70% for 10 successive cycles. e Photographs showing the temperature resistance behavior of PMP DN ICH. f, g Tensile and compressive stress-strain curves of PMP DN ICH acquired from − 60-80 °C. h Conductivities of Pre-PMP DN ICH and PMP DN ICH from − 60-80 °C. i, j Changes in weight and conductivity of Pre-PMP DN ICH and PMP DN ICH during 30 d of storage in an ambient environment. The error bars represent standard deviation; sample size n = 3

Fig. 3 a-c Antibacterial schematic illustration of the PMP DN ICH. d-f The antibacterial activity against E. coli and S. aureus of the PMP DN ICH

Fig. 4 Time-dependent changes in relative resistance of the PMP DN ICH-based strain sensor subjected to cyclic stretching at various a tensile rates and b tensile strains. c Cyclic sensing response of the PMP DN ICH-based strain sensor at 25% strain for ~ 300 stretching cycles (inset: magnified data over a representative timeframe). d Schematic of the monitored sensing sites. Variations in relative resistance of the sensor attached to the e belly (during normal breathing, deep breathing, and breathing after exercise) and f knee (during walking, running, and jumping). g Photographs of the wireless transmission device and setup of the practical application. Changes in relative resistance during h nodding and looking up movements, i finger bending, and j wrist bending. k Schematic showing the definition of Morse codes. Coding the words l “GO,” m “SOS,” and n “HELP” by short- and long-duration finger bending

Fig. 5 Thermal sensing properties of a PMP DN ICH-based thermistor. Changes in relative resistance of the PMP DN ICH-based thermistor with step increases in temperature from 30 to 100 °C with respect to a time and b temperature. c Dynamic resistance responses of the thermistor during successive heating-cooling cycles between 25 and 30 °C. d Dynamic resistance responses of the thermistor to detect the addition or removal of water at different temperatures (38.3, 59.2, and 75.2 °C); inset: infrared images of the added water. e Dynamic resistance responses of the thermistor to temperature changes while breathing; inset: the temperature changes of a mask during inhalation and exhalation. f Dynamic resistance responses of the thermistor to variations in skin temperature while simulating a fever; inset: changes in the skin temperature before and after the fever

Fig. 6 Electrochemical properties of the PMP DM ICH-based SC. a Illustration of the assembled SC. b CV curves of the fabricated SC at scan rates of 5-100 mV s⁻¹). c GCD curves and d the corresponding areal capacitance and coulombic efficiency of the SC at current densities of 1-8 mA cm⁻². e EIS curve and the corresponding equivalent circuit diagram of the devised SC. f Ragone plot comparing the energy and power densities of the SC with those reported previously. g Cycling stability of the SC at 6 mA cm⁻². h Photographs illustrating the ability of the SC to power an electronic meter and LED bulb

Fig. 7 CV curves (scan rate, 20 mV s⁻¹); capacitance retention and coulombic efficiency (current density, 6 mA cm⁻²); and EIS curves of a PMP DN ICH-based SC for different a-c storage durations, d-f temperatures, g-i pressures, and j-l bending angles

Fig. 8 Schematics of the a PMP DN ICH-based TENG and its b working principle. c Output V_oc, I_sc, and Q_sc values of the TENG. d V_oc values of the TENG for different frequencies (1-3 Hz). e Electrical output properties of the TENG with different external resistors. f Long-term stability test of the TENG. g Equivalent circuit diagram of a self-charging power system based on the TENG. h Charging behavior of capacitors (4.7 and 22 μF) at a working frequency of 2 Hz. i Photograph of 68 commercial green LEDs illuminated by the TENG

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