Bi-Functional Electrolyte Additive Leading to a Highly Reversible and Stable Zinc Anode.

A stable stripping/plating process of the zinc anode is extremely critical for the practical application of aqueous zinc metal batteries. However, obstacles, including parasitic reactions and dendrite growth, notoriously deteriorate the stability and reversibility of zinc anode. Herein, Methyl l-α-aspartyl-l-phenylalaninate (Aspartame) is proposed as an effective additive in the ZnSO4 system to realize high stability and reversibility. Aspartame molecule with rich polar functional groups successfully participates in the solvation sheath of Zn2+ to suppress water-induced side reactions. The self-driven adsorption of Aspartame on zinc anode improves uniform deposition with a dose of 10 mm. These synergetic functions endow the zinc anode with a significantly long cycling lifespan of 4500 h. The cell coupled with a vanadium-based cathode also exhibited a high-capacity retention of 71.8% after 1000 cycles, outperforming the additive-free counterparts.

Tackling the Challenges of Aqueous Zn-Ion Batteries via Polymer-Derived Strategies.

Zn-ion batteries (ZIBs) have gathered unprecedented interest recently benefiting from their intrinsic safety, affordability, and environmental benignity. Nevertheless, their practical implementation is hampered by low rate performance, inferior Zn2+ diffusion kinetics, and undesired parasitic reactions. Innovative solutions are put forth to address these issues by optimizing the electrodes, separators, electrolytes, and interfaces. Remarkably, polymers with inherent properties of low-density, high processability, structural flexibility, and superior stability show great promising in tackling the challenges. Herein, the recent progress in the synthesis and customization of functional polymers in aqueous ZIBs is outlined. The recent implementations of polymers into each component are summarized, with a focus on the inherent mechanisms underlying their unique functions. The challenges of incorporating polymers into practical ZIBs are also discussed and possible solutions to circumvent them are proposed. It is hoped that such a deep analysis could accelerate the design of polymer-derived approaches to boost the performance of ZIBs and other aqueous battery systems as they share similarities in many aspects.

Anti-Fatigue Hydrogel Electrolyte for All-Flexible Zn-Ion Batteries.

Hydrogel electrolytes are widely explored in Zn metal batteries for application in wearable electronics. While extensive studies have been conducted on optimizing the chemical structure and boosting the tensile elasticity, the mechanical stability of the hydrogel under repeated deformation is largely overlooked, leading to unsatisfactory performance at large cycling capacity. This work systematically analyzes the compressive fatigue-resistance properties of the hydrogel electrolyte, revealing the critical roles of the salt and copolymer matrix on crack initiation and propagation. It shows that, on the premise of homogeneous Zn deposition, an improved anti-fatigue property is essential to achieve high-capacity Zn metal anodes. The optimal Zn(ClO4 )2 -polyacrylamide/chitosan hydrogel electrolyte (C-PAMCS) exhibits an unprecedented lifespan of 1500 h for Zn//Zn cells at a current density of 10 mA cm-2 and a high areal capacity of 10 mAh cm-2 . The potential application of C-PAMCS is exemplified in all-flexible Zn-ion batteries enabled by a flexible current collector consisting of a Ag nanowires embedded elastomer. This study provides the rationale under hydrogel electrolyte engineering toward advanced Zn-ion battereis and the application in flexible devices.

Synthesis and Mechanism of High Structural Stability of Nickel-Rich Cathode Materials by Adjusting Li-Excess.

It has been a long-term challenge to improve the phase stability of Ni-rich LiNixMnyCo1-x-yO2 (x ≥ 0.6) transition metal (TM) oxides for large-scale applications. Herein, a new structure engineering strategy is utilized to optimize the structural arrangement of Li1+x(Ni0.88Mn0.06Co0.06)1-xO2 (NMC88) with a different Li-excess content. It was found that structure stability and particle sizes can be tuned with suitable Li-excess contents. NMC88 with an actual Li-excess of 2.7% (x = 0.027, Li/TM = 1.055) exhibits a high discharge capacity (209.1 mAh g-1 at 3.0-4.3 V, 0.1 C) and maintains 91.7% after the 100th cycle at 1 C compared with the NMC88 sample free of Li-excess. It also performs a delayed voltage decay and a good rate capacity, delivering 145.8 mAh g-1 at a high rate of 10 C. Multiscale characterization technologies including ex/in situ X-ray diffraction (XRD), focused ion beam (FIB) cutting-scanning electronic microscopy (SEM), and transmission electron microscopy (TEM) results show that a proper Li-excess (2.7%) content contributes to the formation of a broader Li slab, optimized cation mixing ratio, and even particle sizes. Therefore, NMC88 with a proper Li-excess is a good choice for next-generation cathode materials.

Synthesis and Redox Mechanism of Cation-Disordered, Rock-Salt Cathode-Material Li-Ni-Ti-Nb-O Compounds for a Li-Ion Battery.

Cation-disordered oxide materials working as cathodes for Li-ion batteries have been at a standstill because of their structurally limited specific capacities (below 175 mAh g-1 in most cases). In this work, we have introduced 4d0 Nb5+ into host material LiNi0.5Ti0.5O2 to synthesize Ni-based cation-disordered Fm3̅m Li-Ni-Ti-Nb-O compounds of Li1+x/100Ni1/2-x/100Ti1/2-x/100Nbx/100O2 (x = 0, 5, 10, 15, 20) through a sol-gel method, showing particle sizes of less than 200 nm. Taking Li1.2Ni0.3Ti0.3Nb0.2O2 with the best performance (an average voltage of ∼2.7 V and high discharge capacity of 221.5 mAh g-1) among oxides as a model, we study the relationship between the structure, morphology, redox mechanism, and electrochemical performance of cation-disordered oxides through a combination of X-ray diffraction (XRD), scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and X-ray absorption near-edge spectroscopy tests and in situ XRD with electrochemistry. The obtained results indicate that the improved capacity is mainly ascribed to Nb5+, which optimizes the Ni2+/Ni4+ practical capacity and effectively stabilizes the O2-/O- redox reaction. The results emphasize that Li-Ni-Ti-Nb-O compounds are promising members in the family of cation-disordered transition-metal oxide materials.