Abstract:Water loss of the gel polymer electrolytes (GPEs) and dendrites growth on Zn anode are overriding obstacles to applying flexible zinc‐air batteries (ZABs) for wearable electronic devices. Nearly all previous efforts aim at developing novel GPEs with enhanced water retention and therefore elongate their lifespan. Herein, a facile interface engineering strategy is proposed to retard the water loss of GPE from the half‐open structured air cathode. In detail, the poly(ethylene vinyl acetate)/carbon powder (PEVA‐C)… Show more
“…The dough electrolyte achieved incredibly high OH − conductivity and promising hygroscopic characteristics at a low RH compared to previously reported KOH-based solid-state hydrogel electrolytes. [5,[40][41][42][43][44][45][46][47][48][49][50][51] The Dough21 and Dough31 samples with and without 5 wt.% of polymer also stably retained their resistances in a device for 170 h at RH 30% (Figure S12, Supporting Information). This distinctive construction was appreciably scalable and malleable enough to be fabricated with a facile kneading method in the form of a film 10 cm × 10 cm in size and could be crafted into desired shapes, as shown in Figure 4g.…”
electronics. The flexible and rechargeable solid-state Zn-air battery (ZAB) has attracted significant attention as a nextgeneration power source given its advantages of its unique "half-open" cell with a high energy density utilizing inexhaustible atmospheric oxygen, affordability, and eco-friendliness. One of the most critical factors related to flexible solid-state ZABs is the use of a highly deformable solid electrolyte. Thus far, there have been extensive studies of elastomeric hydrogel electrolyte substrates. These hydrogels are coated onto an anode metal framework as a thin film [1][2][3][4][5] or constructed as freestanding blocks [6][7][8][9] and molded architectures. [10][11][12] However, despite much effort, resolving certain critical issues related to hydrogel-based electrolytes for use in ZABs remains challenging. Among these issues, interfacial engineering is important to enlarge the triple-phase boundaries (TPBs) and optimize the wettability so as to facilitate ion transport and suppress the flooding phenomenon in the gas-diffusion layer. [13,14] Recently, Tang et al. demonstrated a landmark cycle life up to 120 h at 5 mA cm −2 due to their use of a compact contact between carbon cloth and a PAA-Fe 3+ -CS/NH 4 Cl hydrogel. [15] In addition, a quaternary ammonia-functionalized cellulose electrolyte membrane with a high degree of hydration due to its hydrophilicity and good dimensional stability in a water-swollen state was recently reported. [2] A thermo-reversible alkaline hydrogel electrolyte was also proposed as a material capable of effectively mitigating the poor electrolyte/electrode contact and mechanical degradation caused by deformation. [16] Another critical problem with ZAB electrolytes is that the water in the hydrogel evaporates through the open cathode, thereby reducing the ZAB performance and lifespan. Thus far, many studies have attempted to improve water retention using hydrogels with high hydrophilicity, such as polyacrylic acid (PAA), sodium polyacrylate (PANa), polyacrylamide (PAM), and bacterial cellulose (Table S1, Supporting Information). Though studies have mainly focused on the development of materials to inhibit water evaporation in the hydrogel when the relative humidity (RH) exceeds 40%, there has been few reports of hydrogel for a dry atmosphere with a RH less than 30%. In order to solve this problem, the development of a hydrogel Flexible and rechargeable Zn-air batteries (ZAB) are promising candidates for attaining the high energy density required for next-generation energy storage devices given their half-open cathode configuration. However, the poor interfacial contact between the immobilized solid-state electrolyte and porous cathode, and drying-out of water in the electrolyte at low relative humidity (RH) of 30% or less, cause low performance and short lifespan. Herein, a novel hygroscopic dough-type electrolyte with water-absorbing and malleable free-standing configuration originating from deliquescent KOH and severe gelation of sodium alginate (SA) by facile knead...
“…The dough electrolyte achieved incredibly high OH − conductivity and promising hygroscopic characteristics at a low RH compared to previously reported KOH-based solid-state hydrogel electrolytes. [5,[40][41][42][43][44][45][46][47][48][49][50][51] The Dough21 and Dough31 samples with and without 5 wt.% of polymer also stably retained their resistances in a device for 170 h at RH 30% (Figure S12, Supporting Information). This distinctive construction was appreciably scalable and malleable enough to be fabricated with a facile kneading method in the form of a film 10 cm × 10 cm in size and could be crafted into desired shapes, as shown in Figure 4g.…”
electronics. The flexible and rechargeable solid-state Zn-air battery (ZAB) has attracted significant attention as a nextgeneration power source given its advantages of its unique "half-open" cell with a high energy density utilizing inexhaustible atmospheric oxygen, affordability, and eco-friendliness. One of the most critical factors related to flexible solid-state ZABs is the use of a highly deformable solid electrolyte. Thus far, there have been extensive studies of elastomeric hydrogel electrolyte substrates. These hydrogels are coated onto an anode metal framework as a thin film [1][2][3][4][5] or constructed as freestanding blocks [6][7][8][9] and molded architectures. [10][11][12] However, despite much effort, resolving certain critical issues related to hydrogel-based electrolytes for use in ZABs remains challenging. Among these issues, interfacial engineering is important to enlarge the triple-phase boundaries (TPBs) and optimize the wettability so as to facilitate ion transport and suppress the flooding phenomenon in the gas-diffusion layer. [13,14] Recently, Tang et al. demonstrated a landmark cycle life up to 120 h at 5 mA cm −2 due to their use of a compact contact between carbon cloth and a PAA-Fe 3+ -CS/NH 4 Cl hydrogel. [15] In addition, a quaternary ammonia-functionalized cellulose electrolyte membrane with a high degree of hydration due to its hydrophilicity and good dimensional stability in a water-swollen state was recently reported. [2] A thermo-reversible alkaline hydrogel electrolyte was also proposed as a material capable of effectively mitigating the poor electrolyte/electrode contact and mechanical degradation caused by deformation. [16] Another critical problem with ZAB electrolytes is that the water in the hydrogel evaporates through the open cathode, thereby reducing the ZAB performance and lifespan. Thus far, many studies have attempted to improve water retention using hydrogels with high hydrophilicity, such as polyacrylic acid (PAA), sodium polyacrylate (PANa), polyacrylamide (PAM), and bacterial cellulose (Table S1, Supporting Information). Though studies have mainly focused on the development of materials to inhibit water evaporation in the hydrogel when the relative humidity (RH) exceeds 40%, there has been few reports of hydrogel for a dry atmosphere with a RH less than 30%. In order to solve this problem, the development of a hydrogel Flexible and rechargeable Zn-air batteries (ZAB) are promising candidates for attaining the high energy density required for next-generation energy storage devices given their half-open cathode configuration. However, the poor interfacial contact between the immobilized solid-state electrolyte and porous cathode, and drying-out of water in the electrolyte at low relative humidity (RH) of 30% or less, cause low performance and short lifespan. Herein, a novel hygroscopic dough-type electrolyte with water-absorbing and malleable free-standing configuration originating from deliquescent KOH and severe gelation of sodium alginate (SA) by facile knead...
“…In stark contrast, the XRD patterns of the Zn anode with the PVA and PANa electrolytes denote a much higher content of ZnO after cycling. The formation of ZnO with low ionic conductivity and cycling reversibility greatly shortens the cell life of the FZABS. , With improved mechanical flexibility and water absorption/retention of the HAcc@HPPAN-COONa/PANa electrolyte, the deformation of the Zn anode can be well accommodated, and the volume shrinkage of the electrolyte induced by water loss can be mitigated. Besides, the abundant hydrophilic hydroxyl groups of HAcc@HPPAN-COONa nanofibers regulate the interfacial ion flux, , which collectively inhibits Zn dendrite growth and ZnO passivation.…”
The low ionic conductivity and poor mechanical property of quasi-solid electrolytes (QSEs) have hindered the practical implementation of flexible zinc−air batteries (FZABs) with a higher energy density and a longer working time. Herein, inspired by the robust natural extracellular matrix and good waterretention vacuoles of plant cells, semi-interpenetrating networkstructured QSEs composed of rigid quaternary ammonium salt of chitosan-decorated hollow porous polyacrylonitrile-based nanofibers and a soft hydrophilic sodium acrylate (PANa) polymer are fabricated. The cross-linked semi-interpenetrating network structure endows the QSEs with enhanced electrolyte absorption/ retention capacity, increased ionic conductivity, and improved mechanical strength. Moreover, the introduction of interconnected hollow porous nanofibers offers favorable water reservoirs and ion-conduction channels to further regulate the OH − flux. As a result, the FZABs assembled with the bioinspired QSEs exhibit a high power density (126 mW cm −2 ), a long lifespan (100 h), as well as good flexibility. The demonstrated bionic and in situ crosslinking strategies provide enlightening pathways for the design of advanced QSEs for high-performance flexible energy conversion and storage systems.
“…In addition to enhancing the water retention capacity of the electrolyte itself, modifying the electrode is also an effective way to inhibit water loss of electrolyte. He et al [97] fabricated a composite layer at carbon cloth via electrospinning technique for ZAB cathode (Figure 10d). The poly (ethylene vinylacetate)/carbon powder (PEVA-C) with reliable hydrophobic properties was employed to reduce the loss of water in the electrolyte through the semi-open structure of the cathode.…”
Section: Fabricate the Hydrophobic Coating On The Air Cathodementioning
Aqueous zinc batteries are promising candidates for energy storage and conversion devices in the “post‐lithium” era due to their high energy density, high safety, and low cost. The electrolyte plays an important role in zinc batteries by conducting and separating the positive and negative electrodes. However, the issues of zinc dendrites growth, corrosion, by‐product formation, hydrogen evolution and leakage, and evaporation of the aqueous electrolytes affect the commercialization of the batteries. Moreover, the widely used aqueous electrolytes result in large battery sizes, which are not conducive to the emerging smart devices. The intrinsic properties of gel polymer electrolytes (GPEs) can solve the above problems. In order to promote the wider application of GPEs‐based zinc batteries, in this review, the working principle and the current problems of zinc batteries are first introduced, andthe merits of GPEs compared to aqueous electrolytes are then summarized. Subsequently, a series of challenges and corresponding strategies faced by GPE is discussed, and an outlook for its future development is finally proposed.
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