Zn batteries are considered as potential candidates in future power sources, however suffer problems of rampant dendrite/by-product on Zn anodes, torpid Zn2+ transfer/diffusion and poor energy density. Inspired by the host-guest interaction chemistry, an anion-trap agent β-cyclodextrin (β-CD) is introduced into the Zn(ClO4)2 electrolyte to induce dominant Zn (002) deposition and improve Zn2+ migration behaviors. The anion ClO4- is revealed to be trapped inside the cavity of β-CD, impairing barriers for Zn2+ migration and significantly elevate the Zn2+ transference number to 0.878. Meanwhile, the β-CD@ClO4- complex shows the function in preferential growth of the Zn (002), blocking the approach of dendrite growth. Above combined functions lead to substantial enhancement in long-term stability and cell capacity, as proved by 10 times longer life of Zn||Zn symmetric cells and 57% capacity increasement of Zn-MnO2 full cells (at 0.1 A g-1) compared with that of pure Zn(ClO4)2 electrolyte.

Anion-trap Engineering toward Remarkable Crystallographic Reorientation and Efficient Cation Migration of Zn Ion Batteries.

Aqueous zinc (Zn)-ion batteries are regarded as promising candidates for large-scale energy storage systems because of their high safety, low cost, and environmental benignity. However, the dendrite issue of Zn anode hinders their practical application. Herein, a freestanding, lightweight, and zincophilic MXene/nanoporous oxide heterostructure engineered separator is designed to stabilize a Zn metal anode. The nanoporous oxides prepared by a one-step vacuum distillation technique afford the advantages of large surface area, high porosity, and homogeneous porous structure. The zincophilic MXene@oxides layer can homogenize the electric field distribution, facilitate ion diffusion kinetics, reduce local current density, and promote even Zn ionic flux, which will regulate uniform Zn deposition and suppress side reactions. Accordingly, dendrite-free Zn anodes with stable cyclability are achieved for over 500 h at an ultrahigh area capacity of 10 mAh cm-2. Besides, flexible, long-lifespan, and high-rate N/S-doped three-dimensional MXene@MnO2||Zn full cells are constructed with the engineered separator. Moreover, this strategy can be successfully extended to lithium, sodium, potassium, and magnesium metal batteries, indicating that separator regulation is a universal approach to overcome the challenges of metal batteries.

Highly Reversible Zn Metal Anodes Enabled by Freestanding, Lightweight, and Zincophilic MXene/Nanoporous Oxide Heterostructure Engineered Separator for Flexible Zn-MnO2 Batteries.

The advent of 5G and the Internet of Things has spawned a demand for wearable electronic devices. However, the lack of a suitable flexible energy storage system has become the "Achilles' Heel" of wearable electronic devices. Additional problems during the transformation of the battery structure from conventional to flexible also present a severe challenge to the battery design. Flexible Zn-based batteries, including Zn-ion batteries and Zn-air batteries, have long been considered promising candidates due to their high safety, eco-efficiency, substantial reserve, and low cost. In the past decade, researchers have come up with elaborate designs for each portion of flexible Zn-based batteries to improve the ionic conductivities, mechanical properties, environment adaptabilities, and scalable productions. It would be helpful to summarize the reported strategies and compare their pros and cons to facilitate further research toward the commercialization of flexible Zn-based batteries. In this review, the current progress in developing flexible Zn-based batteries is comprehensively reviewed, including their electrolytes, cathodes, and anodes, and discussed in terms of their synthesis, characterization, and performance validation. By clarifying the challenges in flexible Zn-based battery design, we summarize the methodology from previous investigations and propose challenges for future development. In the end, a research paradigm of Zn-based batteries is summarized to fit the burgeoning requirement of wearable electronic devices in an iterative process, which will benefit the future development of Zn-based batteries.

Rational Design of Flexible Zn-Based Batteries for Wearable Electronic Devices.

Rechargeable aqueous zinc‐ion batteries are of great potential as one of the next‐generation energy‐storage devices due to their low cost and high safety. However, the development of long‐term stable electrodes and electrolytes still suffers from great challenges. Herein, a self‐separation strategy is developed for an interface layer design to optimize both electrodes and electrolytes simultaneously. Specifically, the coating with an organometallics (sodium tricyanomethanide) evolves into an electrically responsive shield layer composed of nitrogen, carbon‐enriched polymer network, and sodium ions, which not only modulates the zinc‐ion migration pathways to inhibit interface side reactions but also adsorbs onto Zn perturbations to induce planar zinc deposition. Additionally, the separated ions from the coating can diffuse to the electrolyte to affect the Zn2+ solvation structure and maintain the cathode structural stability by forming a stable cathode–electrolyte interface and sodium ions’ equilibrium, confirmed by in situ spectroscopy and electrochemical analysis. Due to these unique advantages, the symmetric zinc batteries exhibit an extralong cycling lifespan of 3000 h and rate performance at 20 mA cm−2 at wide temperatures. The efficiency of the self‐separation strategy is further demonstrated in practical full batteries with an ultralong lifespan over 10 000 cycles from −35 to 60 °C.

Simultaneously Stabilizing Both Electrodes and Electrolytes by a Self‐Separating Organometallics Interface for High‐Performance Zinc‐Ion Batteries at Wide Temperatures

MXenes for advanced separator in rechargeable batteries

An active and durable molecular catalyst for aqueous polysulfide-based redox flow batteries

The performances of rechargeable batteries are strongly affected by the operating environmental temperature. In particular, low temperatures (e.g., ≤0 °C) are detrimental to efficient cell cycling. To circumvent this issue, we propose a few-layer Bi2Se3 (a topological insulator) as cathode material for Zn metal batteries. When the few-layer Bi2Se3 is used in combination with an anti-freeze hydrogel electrolyte, the capacity delivered by the cell at -20 °C and 1 A g-1 is 1.3 larger than the capacity at 25 °C for the same specific current. Also, at 0 °C the Zn | |few-layer Bi2Se3 cell shows capacity retention of 94.6% after 2000 cycles at 1 A g-1. This behaviour is related to the fact that the Zn-ion uptake in the few-layer Bi2Se3 is higher at low temperatures, e.g., almost four Zn2+ at 25 °C and six Zn2+ at -20 °C. We demonstrate that the unusual performance improvements at low temperatures are only achievable with the few-layer Bi2Se3 rather than bulk Bi2Se3. We also show that the favourable low-temperature conductivity and ion diffusion capability of few-layer Bi2Se3 are linked with the presence of topological surface states and weaker lattice vibrations, respectively. 

/pdf/few-layer-bismuth-selenide-cathode-for-low-temperature-quasi-64vlx6wd.pdf

Few-layer bismuth selenide cathode for low-temperature quasi-solid-state aqueous zinc metal batteries

High rate tolerance and long cycle life represent the critical demand of the market for energy storage devices, known as one of major challenges for the development of rechargeable aqueous batteries. Herein, a layered Mo4/3B2T2 (where “T” denotes ‐O, ‐OH, and ‐F terminations) MBene (a transition metal boride) with in‐plane ordered metal vacancies is first proposed as an iodine species host of an aqueous Zn‖I2 battery, delivering a discharge capacity of 106.8 mAh g−1 at 25 A g−1 after 230 000 cycles and 80 mAh g−1 at 100 A g−1, far exceeding those of all Zn‖I2 batteries ever reported. The high performance is attributed to the strong affinity with iodine species and accelerated the redox kinetics by the conductive MBene with metal vacancies, as evidenced by the one‐step conversion of I‒/I0 without the generation of I3‒ ions. This work unlocks a new route for the construction of other halide or sulfur electrode batteries with superior durability and kinetics.

Ultralong Cycle Life and High Rate of Zn‖I2 Battery Enabled by MBene‐Hosted I2 Cathode

Exploring the potential of MXene nanoslit for water desalination through molecular dynamics simulations

Hydrogels are widely used as quasi-solid-state electrolytes in aqueous batteries. However, they are not applicable in high-voltage batteries because the hydrogen evolution reaction cannot be effectively suppressed even when water is incorporated into the polymer network. Herein, by profoundly investigating the states of water molecules in hydrogels, we designed supramolecular hydrogel electrolytes featuring much more nonfreezable bound water and much less free water than that found in conventional hydrogels. Specifically, two strategies are developed to achieve this goal. One strategy is adopting monomers with a variety of hydrophilic groups to enhance the hydrophilicity of polymer chains. The other strategy is incorporating zwitterionic polymers or polymers with counterions as superhydrophilic units. In particular, the nonfreezable bound water content increased from 0.129 in the conventional hydrogel to >0.4 mg mg-1 in the fabricated hydrogels, while the free water content decreased from 1.232 to ∼0.15 mg mg-1. As a result, a wide electrochemical stability window of up to 3.25 V was obtained with the fabricated hydrogels with low concentrations of incorporated salts and enhanced hydrophilic groups or superhydrophilic groups. The ionic conductivities achieved with our developed hydrogel electrolytes were much higher than those in the conventional highly concentrated salt electrolytes, and their cost is also much lower. The designed supramolecular hydrogel electrolytes endowed an aqueous K-ion battery (AKIB) system with a high voltage plateau of 1.9 V and contributed to steady cycling of the AKIB for over 3000 cycles. The developed supramolecular hydrogel electrolytes are also applicable to other batteries, such as aqueous lithium-ion batteries, hybrid sodium-ion batteries, and multivalent-ion aqueous batteries, and can achieve high voltage output.

Fine Tuning Water States in Hydrogels for High Voltage Aqueous Batteries.

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