Rational Design of Antifreezing Organohydrogel Electrolytes for Flexible Supercapacitors

Lü, Nan; Na, Ruiqi; Li, Leibo; Zhang, Chongyang; Chen, Zhuoqi; Zhang, Shuling; Luan, Jingyi; Wang, Guibin

doi:10.1021/acsaem.9b02379

Cited by 107 publications

(55 citation statements)

References 57 publications

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“…The conductivity of the OHE at room temperature in this work is 22.9 mS cm −1 , comparable to or higher than those of reported OHEs. [ 6c,8a,11 ] The good conductivity of the OHE exceeds those of the binary solvent electrolyte with higher water content and hydrogel electrolyte. [ 8a,12 ] The reasons could be ascribed to: i) the high concentration of LiCl; ii) the small atom radius of lithium; iii) OHE with water retention mimicking as “water‐in‐salt” for the fast Li + channels.…”

Section: Resultsmentioning

confidence: 99%

Flexible Supercapacitor Based on Organohydrogel Electrolyte with Long‐Term Anti‐Freezing and Anti‐Drying Property

Lou

Wang

et al. 2020

Adv Funct Materials

187

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Hydrogel electrolytes have spurred the development of flexible energy storage devices by endowing them with liquid-like ion transport and solidlike mechanical elasticity. However, traditional hydrogel electrolytes always lose these functions in climate change because the internal water undergoes freezing and/or dehydration. In this work, a flexible supercapacitor (OHEC) is assembled based on the organohydrogel electrolyte (OHE) and activated carbon electrode material. The OHE is composed of PAMPS/PAAm doublenetwork hydrogel soaked from 4 m LiCl/ethylene glycol and exhibits good conductivities (1.9 and 22.9 mS cm −1 at −20 and 25 °C, respectively). The OHEC exhibits broad temperature adaptability (from −20 to 80 °C) and extraordinary resistance to mechanical damage (above 100 kg crushing). The OHEC avoids the polarization at low temperatures and retains 77.8% capacitance retention after storage at −20 °C for 30 days. Without extra sealed packaging, the OHEC maintains remarkable cycling stability (only 8.7% capacitance decay after 10 000 cycles) and retains 77.3% capacitance at 80 °C after 56 h. The outstanding anti-drying performance and improved interfacial compatibility of OHEC account for the good durability in the hightemperature environments. Additionally, other salts (such as LiClO 4 , NaCl, and KCl) with favorable solubility in ethylene glycol can also serve in OHEs for wide temperature range supercapacitors.

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Section: Resultsmentioning

confidence: 99%

Flexible Supercapacitor Based on Organohydrogel Electrolyte with Long‐Term Anti‐Freezing and Anti‐Drying Property

Lou

Wang

et al. 2020

Adv Funct Materials

187

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“…The ionic conductivity of the PAA-PAH/LiCl gel electrolyte with the extra addition of 1 M LiCl was tested to be 0.050 S·cm −1 , manifesting a high level among hydrogel electrolytes ever reported ( Table S1 and Figure S4 ). In particular, this PAA-PAH/LiCl gel electrolyte holds higher ionic conductivity than most of PVA gel-based electrolytes ( Wang et al., 2016 ; Geng et al., 2019 ; Huang et al., 2019 ; Peng et al., 2019 ; Sun et al., 2019 ; Zhou et al., 2019 ; Liu et al., 2020 ; Lu and Chen, 2020 ; Lu et al., 2020 ) with the same amount of salt addition. This indicates a greater application prospect of PAA-PAH/LiCl than PVA-based gel electrolytes.…”

Section: Resultsmentioning

confidence: 91%

A Regenerable Hydrogel Electrolyte for Flexible Supercapacitors

Zhou

Yang

et al. 2020

iScience

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Summary Easy regenerability of core components such as electrode and electrolyte is highly required in advanced electrochemical devices. This work reports a reliable, regenerable, and stretchable hydrogel electrolyte based on ionic bonds between polyacrylic acid (PAA) and polyallylamine (PAH). PAA-PAH electrolyte (1M LiCl addition) exhibits high ionic conductivity (0.050 S·cm-1) and excellent mechanical property (fracture strain of 1,688%). Notably, the electrolyte can be regenerated to any desired shape under mild conditions and remains 96% and 90% of the initial ionic conductivity after the first and second regeneration, respectively. PAA-PAH/LiCl-based supercapacitor exhibits nearly 100% capacitance retention upon rolling, stretching, and 5,000 charge-discharge cycles, whereas the regenerated device holds 97.6% capacitance of the initial device and 90.9% after 5,000 cycles. This low-cost, high-efficiency, and regenerable hydrogel electrolyte reveals very promising use in solid-state/flexible supercapacitors and possibly becomes a standard commercial hydrogel electrolyte for sustainable electrochemical energy devices.

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“…At present, there are two main solutions to solve these problems, one is to reduce the freezing point of the system by using a solvent, [41,42] and the other is to reduce the freezing point by using an inorganic salt. [43,44] The strategy of using an EG/H 2 O binary solvent instead of a distilled water solvent endowed the hydrogel with superb anti-freezing properties. Compared with the composite preparation process of replacing a solvent by solvent soaking after the hydrogel was formed, the one-pot method used to prepare the PVA/agar-EG organic hydrogel was facile and avoided solvent waste.…”

Section: Resultsmentioning

confidence: 99%

PVA/Agar Interpenetrating Network Hydrogel with Fast Healing, High Strength, Antifreeze, and Water Retention

Han

Fan

et al. 2020

Macro Chemistry & Physics

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concentration to achieve a self-healing ability and mechanical properties. [20] Among them, the main design methods are physical and chemical design concepts. The hydrogels prepared based on physical crosslinking interact through hydrogen bonding, [21,22] hydrophobic association, electrostatic interaction, [23] segment entanglement, [24] and other noncovalent [25,26] interactions, while the traditional chemical cross-linking method mainly takes advantage of the interaction mode of dynamic binding. [27] That is, the dynamic exchange process occurs when the chain is broken, contributing to the self-healing effect. At the same time, owing to the high water content, it is difficult for traditional hydrogels to avoid high water loss and early degradation during use. Additionally, their inherent properties such as light transmittance will be destroyed under freezing conditions. However, compared with the traditional hydrogel preparation methods, the multifunctional hydrogel requires more steps to synthesize, increasing the difficulty of preparation. Thus, it is a great challenge for traditional hydrogels to operate under complex working conditions such as high-and low-temperature fluctuations. Therefore, to improve the applicability of hydrogels under complex working conditions, various methods have been suggested, such as network interpenetrating structure hydrogels, [28] double network hydrogels, [29-31] nanocomposite structure hydrogels, [32-35] and host-guest supermolecule hydrogels. [36,37] Different from other methods, network interpenetrating structure hydrogels are multifunctionally designed to avoid the disadvantages of pure water loss and degradation of hydrogels due to the higher fault tolerance and compatibility. Polyvinyl alcohol (PVA) matrices can be utilized to achieve a balance of self-healing ability and mechanical properties and can be multifunctionalized by modification with a variety of composite products. PVA hydrogels are formed in a variety of ways. Moreover, hydrogen bond cross-linking or external dynamic binding can be introduced to achieve self-healing properties. The PVA hydrogel has a uniform network structure and large energy consumption capacity that make it extremely light transmissive and give it an outstanding comprehensive performance. These reversible and breakable high-density hydrogenbonded cross networks provide PVA hydrogels with self-healing effects at room temperature without any irritation or healing Traditional self-healing hydrogels have great application prospects in biological engineering because of their extremely high water content, but their durability cannot be easily guaranteed. Therefore, developing a rapid self-healing hydrogel with long-lasting water retention capacity is still a significant challenge. A highstrength and fast self-healing hydrogel with an interpenetrating double network based on polyvinyl alcohol/agar-ethylene glycol (PVA/agar-EG) is proposed. Polyvinyl alcohol (PVA) and agar are designed for the construction of the interpenetrating network. Further...

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Rational Design of Antifreezing Organohydrogel Electrolytes for Flexible Supercapacitors

Cited by 107 publications

References 57 publications

Flexible Supercapacitor Based on Organohydrogel Electrolyte with Long‐Term Anti‐Freezing and Anti‐Drying Property

Flexible Supercapacitor Based on Organohydrogel Electrolyte with Long‐Term Anti‐Freezing and Anti‐Drying Property

A Regenerable Hydrogel Electrolyte for Flexible Supercapacitors

PVA/Agar Interpenetrating Network Hydrogel with Fast Healing, High Strength, Antifreeze, and Water Retention

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