A High-Performance Quasi-Solid-State Aqueous Zinc–Dual Halogen Battery

Abstract

Aqueous zinc-based batteries are promising candidates for the grid-scale energy storage owing to their nonflammability, ecofriendliness, and low cost. Nevertheless, their practical applications are hindered by the relatively low capacity and energy density. Herein, we develop a quasi-solid-state aqueous zinc–dual halogen battery composed of freestanding carbon cloth–iodine cathode and in situ prepared concentrated aqueous gel electrolyte. The freestanding composite cathode and aqueous gel electrolyte can afford iodine source and bromide ions, respectively, thus activating the I–/I0/I+ reaction by forming [IBr2]− interhalogen. Furthermore, the conversion reaction of Br–/Br0 in [IBr2]− interhalogen is stimulated due to the catalytic effect of iodine. Therefore, this rationally designed aqueous dual halogen conversion chemistry enables three successive redox reactions (i.e., I–/I0, I0/I+, and Br–/Br0). Additionally, the LiNO3 additive and acrylamide (AM)-based polymer matrix not only stabilizes the anode/electrolyte interface but also restrains the side reactions and dissolution/diffusion of active species. Consequently, the as-assembled aqueous zinc–dual halogen battery exhibits high areal capacity and energy density.

Optimized Charge Storage in Aza-Based Covalent Organic Frameworks by Tuning Electrolyte Proton Activity

“…In addition, FTIR was employed to probe the dipolar situation. As shown in Figure h, the vibration at 1600–1700 cm –1 is assigned to the scissor vibration of H–O in water molecules . The strong interaction between K + ions and water oxygen atoms in 1.0 m KCl electrolyte would cause the dipole between oxygen and hydrogen to increase, which causes a blue shift (makes the vibration energy decrease).…”

“…As shown in Figure 4h, the vibration at 1600−1700 cm −1 is assigned to the scissor vibration of H−O in water molecules. 32 The strong interaction between K + ions and water oxygen atoms in 1.0 m KCl electrolyte would cause the dipole between oxygen and hydrogen to increase, which causes a blue shift (makes the vibration energy decrease). On the contrary, the weak dipole among free water molecules in 20 m KOAc electrolyte causes a red shift (the vibration energy increases), indicating more stable water molecules.…”

Bifunctional Dynamic Adaptive Interphase Reconfiguration for Zinc Deposition Modulation and Side Reaction Suppression in Aqueous Zinc Ion Batteries

“…Graphene quantum dots (GQDs) have attracted much attention in recent years due to their excellent optical properties and chemical stability, and they have been widely used in photodetectors and energy storage devices. − More importantly, the well-defined structure of GQDs can be modified to achieve precise control over their components and load charge, which provides the possibility for the design of customizable additives. Previous studies have shown that the addition of positively charged competitive cations, such as NH 4 + , , Li + , Na + , Cs + , Ca 2+ , and Ce 3+ , to the electrolyte can spontaneously create a dynamic electrostatic shielding layer on the anode surface, promoting even Zn deposition. Additionally, ZnF 2 and SnCl 2 additives that contain halogen groups have also been reported to build a hydrophobic characteristic interphase in the outer Helmholtz layer to prevent corrosion of the Zn anode by water molecules. , Inspired by these studies, positively charged chlorinated graphene quantum dots (Cl-GQDs) were introduced into AZBs to construct a bifunctional dynamic adaptive interphase on the anode surface for Zn deposition modulation and side reaction suppression.…”

“…18−21 More importantly, the well-defined structure of GQDs can be modified to achieve precise control over their components and load charge, which provides the possibility for the design of customizable additives. Previous studies have shown that the addition of positively charged competitive cations, such as NH 4 + , 22,23 Li + , 24 Na + , 25 Cs + , 26 Ca 2+ , 27 and Ce 3+ , 28 to the electrolyte can spontaneously create a dynamic electrostatic shielding layer on the anode surface, promoting even Zn deposition. Additionally, ZnF 2 and SnCl 2 additives that contain halogen groups have also been reported to build a hydrophobic characteristic interphase in the outer Helmholtz layer to prevent corrosion of the Zn anode by water molecules.…”

Quasi-Solid Electrolyte Interphase Boosting Charge and Mass Transfer for Dendrite-Free Zinc Battery

“…Tremendous efforts have been performed to enhance the durability and reversibility of Zn anodes, including modifying the Zn electrode structure [10], building artificial protective layers [11][12][13][14], and introducing electrolyte additives [15][16][17]. Among them, metal-organic frameworks (MOFs) have emerged as one of the most promising materials to mitigate the Zn dendrite growth [18,19].…”