Mechanically Excellent, Notch-Insensitive, and Highly Conductive Double-Network Hydrogel for Flexible Strain Sensor.

A novel double-network conductive hydrogel based on lithium acetate/gelatin/polyacrylamide (PAAM) was synthesized by heating-cooling and subsequent γ-ray radiation-induced polymerization and cross-linking. Owing to the hydrogen bonding interaction between lithium acetate, physical cross-linked gelatin, and chemical cross-linked PAAM, the resultant hydrogel exhibited high tensile strength (1260 kPa), high ionic conductivity (35.2 mS cm-1), notch-insensitivity (tensile strength 415 kPa, elongation at break 872% with transverse notch), and extensive strain monitoring range (0.15-800%) under optimum conditions. The lithium acetate/gelatin/polyacrylamide hydrogel strain sensor attached to the skin can sensitively monitor the subtle movements of the human body. The strain sensor based on the resultant hydrogel with transverse notch can still work for 1200 cycles, due to that the covalent-cross-linked PAAm chain bridges the cracks and stabilizes the deformation, while the physical-cross-linked gelatin was unzipped to make the blunting of notch. The conductive hydrogel with high-sensitivity and high stability is expected to be used as materials for the preparation of flexible strain sensors in the future.

Mechanically Robust and Highly Conductive Poly(ionic liquid)/Polyacrylamide Double-Network Hydrogel Electrolytes for Flexible Symmetric Supercapacitors with a Wide Operating Voltage Range.

Flexible electronic devices, such as supercapacitors (SCs), place high demands on the mechanical properties, ionic conductivity, and electrochemical stability of electrolytes. Hydrogels, which combine flexibility and the advantages of both solid and liquid electrolytes, will meet the demand. Here, we report the synthesis of novel poly(ionic liquid)/polyacrylamide double-network (DN) (PIL/PAM DN) hydrogel electrolytes containing different metal salts via a two-step γ-radiation method. The resultant Li2SO4-1.0/PIL/PAM DN hydrogel electrolyte possesses excellent mechanical properties (tensile strength of 3.64 MPa, elongation at break of 446%) and high ionic conductivity (24.1 mS·cm-1). The corresponding flexible SC based on the Li2SO4-1.0/PIL/PAM DN hydrogel electrolyte (SC-Li2SO4) presents improved ion diffusion, ideal electrochemical double-layer capacitor behavior, good rate capability, and excellent cyclic stability. Moreover, symmetric SC-Li2SO4 achieves a wide operating voltage range of up to 1.5 V, with a maximum energy density of 26.0 W h·kg-1 and a capacitance retention of 94.1% after 10,000 galvanostatic charge-discharge cycles, owing to the deactivation of free water molecules by the synergistic effect of PIL, PAM, and SO42-. Above all, the capacitance of SC-Li2SO4 is well-maintained after overcharge, overdischarge, short circuit, extreme temperature, compression, and bending tests, indicating its high security and flexibility. This work reveals the enormous application potential of PIL-based conductive hydrogel electrolytes for flexible electronic devices.

Synthesis and property of superabsorbent polymer based on cellulose grafted 2-acrylamido-2-methyl-1-propanesulfonic acid.

An eco-friendly superabsorbent polymer (SAP) was prepared by grafting 2-acrylamido-2-methyl-1-propanesulfonic acid onto microcrystalline cellulose in lithium chloride/N, N-dimethylacetamide system. The synthesized SAP (cellulose-g-PAMPS) was characterized by FTIR, TGA, SEM, 1H NMR, 13C NMR and XRD. The water absorption equilibrium of cellulose-g-PAMPS could be achieved within 10 min in distilled water. Moreover, the maximum water absorption capacities of cellulose-g-PAMPS in distilled water, 0.9 wt% NaCl solution and 3.2 wt% Na2CO3 solution were 648.9, 298.4 and 207.3 g·g-1, respectively. The water absorption behavior of cellulose-g-PAMPS was interpreted by the pseudo-second-order model. Furthermore, cellulose-g-PAMPS could be used in some extreme conditions due to its high acid and alkali resistance. The water retention rate of cellulose-g-PAMPS could be maintained above 90 % at 25 °C for 6 h. As a consequence, the synthesized SAP can be applied to increase the plant growth and survival time under drought conditions, even under saline alkali conditions.

Ultrastretchable and adhesive agarose/Ti3C2Tx-crosslinked-polyacrylamide double-network hydrogel for strain sensor.

A novel agarose/Ti3C2Tx-crosslinked-polyacrylamide (AG/T-PAM) double-network (DN) hydrogel is synthesized by combining heating-cooling and γ-ray radiation-induced polymerization. The AG/T-PAM DN hydrogel possesses excellent mechanical properties with 4250% stretchability, and good adhesion to different substrates, such as an adhesive strength of 1148 kPa to copper at 30 °C. The resultant hydrogel also exhibits excellent tensile and compression sensing properties due to the variation of conductive network within hydrogel. The flexible and wearable strain sensor composed of the AG/T-PAM DN hydrogel presents rapid response to strain withstand 1000 cycles, and can monitor various movements of human body with a high sensibility. The AG/T-PAM DN hydrogel-based strain sensor will have broad application in large-scale strain detection scenarios requiring high sensitivity and adhesion.

Polyacrylamide/Copper-Alginate Double Network Hydrogel Electrolyte with Excellent Mechanical Properties and Strain-Sensitivity.

The double network (DN) hydrogel has attracted great attention due to its wide applications in daily life. However, synthesis DN hydrogel with excellent mechanical properties is still a big challenge. Here, polyacrylamide/copper-alginate double network (PAM/Cu-alg DN) hydrogel electrolyte is successfully synthesized by radiation-induced polymerization and cross-linking process of acrylamide with N, N'-methylene-bis-acrylamide and subsequent cupric ion (Cu2+ ) crosslinking of alginate. The content of sodium alginate, absorbed dose, and the concentration of Cu2+ are investigated in detail for improving the overall properties of PAM/Cu-alg DN hydrogel electrolyte. The PAM/Cu-alg DN hydrogel electrolyte synthesizes by radiation technique and Cu2+ crosslinking shows superior mechanical properties with a tensile strength of 2.25 ± 0.02 MPa, excellent energy dissipation mechanism, and the high ionic conductivity of 4.08 ± 0.17 mS cm-1 . PAM/Cu-alg DN hydrogel is characterized with attenuated total reflection Fourier transform infrared spectroscopy, thermogravimetric analysis, scanning electron microscopy, and X-ray photoelectron spectroscopy analyses and the reason for the improvement of mechanical properties is illustrated. Furthermore, PAM/Cu-alg DN hydrogel electrolyte exhibits excellent strain-sensitivity, cyclic stability, and durability. This work paves for the new way for the preparation of DN hydrogel electrolytes with excellent properties.

One-step radiation synthesis of agarose/polyacrylamide double-network hydrogel with extremely excellent mechanical properties.

A facile one-step radiation method is first developed to synthesize agarose/polyacrylamide (AG/PAM) double-network (DN) hydrogel. Compared to other synthetic methods of DN hydrogels, our synthesis method endows the resultant AG/PAM DN hydrogel with not only top-level tensile properties with a tensile strength of 1263 ± 59 kPa and an elongation at break of 3406 ± 143%, but also highest compression properties with a compression strength of 140 ± 3 MPa and a fracture compression strain of above 99.9%. An expanding-necking phenomenon during compression process of AG/PAM DN hydrogel were observed. We propose a chain pushing-in model to interpret the energy dissipation mechanism accounting for the super-compressibility of AG/PAM DN hydrogel. This novel radiation synthesis strategy provides an insight into the development of DN hydrogels with extremely excellent mechanical properties.

One-Pot Synthesis of a Double-Network Hydrogel Electrolyte with Extraordinarily Excellent Mechanical Properties for a Highly Compressible and Bendable Flexible Supercapacitor.

High-performance hydrogel electrolytes play a crucial role in flexible supercapacitors (SCs). However, the unsatisfactory mechanical properties of widely used polyvinyl alcohol-based electrolytes greatly limit their use in the flexible SCs. Here, a novel Li2SO4-containing agarose/polyacrylamide double-network (Li-AG/PAM DN) hydrogel electrolyte was synthesized by a heating-cooling and subsequent radiation-induced polymerization and cross-linking process. The Li-AG/PAM DN hydrogel electrolyte possesses extremely excellent mechanical properties with a compression strength of 150 MPa, a fracture compression strain of above 99.9%, a tensile strength of 1103 kPa, and an elongation at break of 2780%, greatly superior to those have been reported. It also achieves a high ionic conductivity of 41 mS cm-1 originating from its interconnected three-dimensional porous network structure that provides a three-dimensional channel for ionic migration. Compared to the SC applying Li2SO4 aqueous solution electrolyte, the corresponding flexible Li-AG/PAM DN hydrogel electrolyte-SC presents lower charge-transfer resistance, better ionic diffusion, being closer to ideal capacitive behaviors, superior rate capability, and better cycling stability, owing to the improved ionic transport in the Li-AG/PAM DN hydrogel electrolyte and electrode interfaces. Moreover, after testing with overcharge, short circuit, and high temperature, the capacitance of the Li-AG/PAM DN hydrogel electrolyte-SC can still be well maintained. Furthermore, the electrochemical properties of the Li-AG/PAM DN hydrogel electrolyte-SC remain almost intact under different compression strains/bending angles and even after 1000 compression/bending cycles. It is expected that the Li-AG/PAM DN hydrogel electrolyte may have broad applications in modern flexible and wearable electronics.