A Bio-Inspired Multifunctional Hydrogel Network with Toughly Interfacial Chemistry for Dendrite-Free Flexible Zinc Ion Battery.

Flexible and high-performance aqueous zinc-ion batteries (ZIBs), coupled with low cost and safe, are considered as one of the most promising energy storage candidates for wearable electronics. Hydrogel electrolytes present a compelling alternative to liquid electrolytes due to their remarkable flexibility and clear advantages in mitigating parasitic side reactions. However, hydrogel electrolytes suffer from poor mechanical properties and interfacial chemistry, which limits them to suppressed performance levels in flexible ZIBs, especially under harsh mechanical strains. Herein, a bio-inspired multifunctional hydrogel electrolyte network (polyacrylamide (PAM)/trehalose) with improved mechanical and adhesive properties was developed via a simple trehalose network-repairing strategy to stabilize the interfacial chemistry for dendrite-free and long-life flexible ZIBs. As a result, the trehalose-modified PAM hydrogel exhibits a superior strength and stretchability up to 100 kPa and 5338 %, respectively, as well as strong adhesive properties to various substrates. Also, the PAM/trehalose hydrogel electrolyte provides superior anti-corrosion capability for Zn anode and regulates Zn nucleation/growth, resulting in achieving a high Coulombic efficiency of 98.8 %, and long-term stability over 2400 h. Importantly, the flexible Zn//MnO2 pouch cell exhibits excellent cycling performance under different bending conditions, which offers a great potential in flexible energy-related applications and beyond.

Achieving High Ionic Conductivity and Mechanical Strength by a Leather Gel Electrolyte for Flexible Zinc-Ion Batteries.

The continuous advancement in the field of flexible and wearable electronics has led to increased research interest in safe, low-cost, and flexible zinc-ion batteries, particularly with a focus on flexible electrolytes. In this study, we present a leather gel electrolyte (LGE) that offers robust mechanical properties and an excellent electrochemical performance. LGE exhibits an ionic conductivity of 1.36 × 10-2 S cm-1 and achieves a capacity of 303.7 mAh g-1 in flexible zinc-manganese dioxide batteries. Even after 1000 cycles, the capacity retention remains above 90%, demonstrating outstanding performance in protecting the zinc anode. Furthermore, such a flexible battery shows good resistance to damage due to the strong mechanical strength originating from leather. Notably, LGE utilizes green and sustainable leather as a raw material, making it a promising option for sustainable flexible devices.

Heterostructure Engineering of NiCo-LDHs for Enhanced Energy Storage Performance in Aqueous Zinc-Ion Batteries.

Aqueous zinc-ion batteries (AZIBs) are considered a promising device for next-generation energy storage due to their high safety and low cost. However, developing high-performance cathodes that can be matched with zinc metal anodes remains a challenge in unlocking the full potential of AZIBs. In this study, a typical transition metal layered double hydroxides (NiCo-LDHs) can be in situ reconstructed to NiCo-LDHs/Ni(Co)OOH heterostructure using an electrochemical cycling activation (ECA) method, serving as a novel cathode material for AZIBs. The optimized ECA-NiCo-LDHs cathode demonstrates a high capacity of 181.5 mAh g-1 at 1 A g-1 and retains 75% of initial capacity after 700 cycles at 5 A g-1. The abundant heterointerfaces of the NiCo-LDHs/Ni(Co)OOH material can activate additional active sites for zinc-ion storage and accelerate ion diffusion. Theoretical calculations also suggest the heterostructure can boost charge transfer and regulate ion-adsorption capability, thereby improving the electrochemical performance. Additionally, the flexible AZIBs device exhibits good service performance. This study on interface engineering introduces a new possibility for utilizing LDHs in AZIBs and offers a novel strategy for designing electrode materials.

A Hydrogel Electrolyte with High Adaptability over a Wide Temperature Range and Mechanical Stress for Long-Life Flexible Zinc-Ion Batteries.

Flexible zinc-ion batteries have garnered significant attention in the realm of wearable technology. However, the instability of hydrogel electrolytes in a wide-temperature range and uncontrollable side reactions of the Zn electrode have become the main problems for practical applications. Herein, N,N-dimethylformamide (DMF) to design a binary solvent (H2O-DMF) is introduced and combined it with polyacrylamide (PAM) and ZnSO4 to synthesize a hydrogel electrolyte (denoted as PZD). The synergistic effect of DMF and PAM not only guides Zn2+ deposition on Zn(002) crystal plane and isolates H2O from the Zn anode, but also breaks the hydrogen bonding network between water to improve the wide-temperature range stability of hydrogel electrolytes. Consequently, the symmetric cell utilizing PZD can stably cycle over 5600 h at 0.5 mA cm- 2@0.5 mAh cm-2. Furthermore, the Zn//PZD//MnO2 full cell exhibits favorable wide-temperature range adaptability (for 16000 cycles at 3 A g-1 under 25 °C, 750 cycles with 98 mAh g-1 at 0.1 A g-1 under -20 °C) and outstanding mechanical properties (for lighting up the LEDs under conditions of pressure, bending, cutting, and puncture). This work proposes a useful modification for designing a high-performance hydrogel electrolyte, which provides a reference for investigating the practical flexible aqueous batteries.

Polysaccharide hydrogel electrolytes with robust interfacial contact to electrodes for quasi-solid state flexible aqueous zinc ion batteries with efficient suppressing of dendrite growth.

Flexible aqueous zinc-ion batteries (AZIBs) require high conductive and adhesive hydrogel electrolytes. However, high adhesion tends to hinder ion conduction rate. Herein, we designed a water/glycerol binary solvent coordinating the hydrophilic polymers to reconstruct the water molecules' environment in the hydrogel. As a consequence, the interface adhesion strength between Zn and the hydrogel reached 3.0 kPa and the ionic conductivity was up to 16.8 mS cm-1. In addition, inspired by the slurry electrode preparation method, we developed a simple blade coating technique using a non-Newtonian polysaccharide liquid solution to construct an ultra-thin hydrogel electrolyte in situ on the cathode. The thickness of the obtained hydrogel reached 70 µm, and the ultrathin flexible AZIBs were easily constructed by pasting a Zn anode directly on the adhesive hydrogel, showing the potential of flexible AZIBs scalable assembly. In addition, the Zn//Zn symmetrical cells with the hydrogel electrolyte provided stable cycling performance for over 400 h at 0.1 mA cm-2 with suppressed dendrite growth. The assembled Zn//Polyaniline battery and Zn//V2O5 battery also exhibited excellent capacity retention after cycles. This work has realized the hydrogel electrolyte with high adhesion and conductivity, which has good adaptability to metal electrodes and opened up a new practical way for large-scale assembly of flexible energy storage devices.

Comparative Review on the Aqueous Zinc-Ion Batteries (AZIBs) and Flexible Zinc-Ion Batteries (FZIBs).

Lithium-ion batteries (LIBs) have been considered an easily accessible battery technology because of their low weight, cheapness, etc. Unfortunately, they have significant drawbacks, such as flammability and scarcity of lithium. Since the components of zinc-ion batteries are nonflammable, nontoxic, and cheap, AZIBs could be a suitable replacement for LIBs. In this article, the advantages and drawbacks of AZIBs over other energy storage devices are briefly discussed. This review focused on the cathode materials and electrolytes for AZIBs. In addition, we discussed the approaches to improve the electrochemical performance of zinc batteries. Here, we also discussed the polymer gel electrolytes and the electrodes for flexible zinc-ion batteries (FZIBs). Moreover, we have outlined the importance of temperature and additives in a flexible zinc-ion battery. Finally, we have discussed anode materials for both AZIBs and FZIBs. This review has summarized the advantages and disadvantages of AZIBs and FZIBs for future applications in commercial battery technology.

Ionic Liquid-Softened Polymer Electrolyte for Anti-Drying Flexible Zinc Ion Batteries.

Using solid polymer electrolytes has been proven to be an efficient strategy to address the metal dendrites and pursuing high-voltage performance. Polyethylene oxide (PEO), as a popular polymer matrix, hardly works for zinc ion batteries due to its poor zinc ionic conductivity and the poor interfacial adhesion. Here, an ionic liquid, 1-ethyl-3-methylimidazolium trifluoromethanesulfonate ([Emim]OTF), was applied as a plasticizer to tune the room-temperature ionic conductivity and mechanical properties of PEO membrane electrolyte. Additional nanofillers ZnO were utilized to enhance the plasticity and modulus. With an optimized composition, the membrane exhibits a high modulus and soft mechanics, which can facilitate the reversible stripping/plating of Zn without formation of Zn dendrites. The optimized polymer electrolyte achieved an ionic conductivity of 2.3 × 10-3 S cm-1 at room temperature with a softness of 5.1 mm. By applying the resulted soft membrane electrolyte for a Zn-MnO2 battery, a capacity of 137 mAh g-1 is achieved at 30 mA g-1 even without the contribution from H+. Such an electrolyte also works for Prussian blue analogue cathodes. Importantly, the addition of [Emim]OTF can enhance the soft contact with the electrodes, and a stable output is delivered under severe deformations for the assembled flexible devices.

Mild synthesis of superadhesive hydrogel electrolyte with low interfacial resistance and enhanced ionic conductivity for flexible zinc ion battery.

Flexible aqueous battery is considered to be one of the most promising energy storage devices for powering flexible electronics. However, inferior interfacial compatibility in electrode-electrolyte interfaces and inefficient ionic channel of electrolytes usually result in potential troubles when applied in practical applications. Herein, we report a mild synthetic route to a sodium lignosulfonate-polyacrylamide hydrogel electrolyte with a high adhesiveness to achieve low electrode-electrolyte interfacial resistance and fast ionic conduction. Comprehensive experiments show that the catechol groups from sodium lignosulfonate demonstrate strong interactions with both cathode and anode materials, and thus greatly reduce the contact resistances across the electrodes. Meanwhile, the existence of sulfonate groups significantly enhances the ionic conductivity of the hydrogel electrolyte. Benefiting from this design, a low ohmic resistance of 3.8 Ω (i.e., 11.4 Ω cm2 ), a low charge transfer resistance of 22.5 Ω (i.e., 67.5 Ω cm2 ), a high ionic conductivity of 31.1 mS cm-1 as well as a 100% capacity retention upon harsh bending deformation can be realized in the flexible zinc ion battery, which are significantly superior to those in the traditional candidates. The present investigation provides new insight into addressing the interfacial issue plaguing flexible energy storage devices.