Explore the vast range of titles available.

HighlightsThe Zn/MnO2 cell with inorganic colloidal electrolyte demonstrates unprecedented durability over 1000 cycles.For the cathode, the presence of the protective film can inhibit the dissolution of manganese element and the formation of irreversible by-products.For the anode, it can reduce the corrosion and de-solvation energy, inhibit the growth of dendrite and irreversible by-products.Zinc-ion batteries (ZIBs) is a promising electrical energy storage candidate due to its eco-friendliness, low cost, and intrinsic safety, but on the cathode the element dissolution and the formation of irreversible products, and on the anode the growth of dendrite as well as irreversible products hinder its practical application. Herein, we propose a new type of the inorganic highly concentrated colloidal electrolytes (HCCE) for ZIBs promoting simultaneous robust protection of both cathode/anode leading to an effective suppression of element dissolution, dendrite, and irreversible products growth. The new HCCE has high Zn2+ ion transference number (0.64) endowed by the limitation of SO42−, the competitive ion conductivity (1.1 × 10–2 S cm−1) and Zn2+ ion diffusion enabled by the uniform pore distribution (3.6 nm) and the limited free water. The Zn/HCCE/α-MnO2 cells exhibit high durability under both high and low current densities, which is almost 100% capacity retention at 200 mA g−1 after 400 cycles (290 mAh g−1) and 89% capacity retention under 500 mA g−1 after 1000 cycles (212 mAh g−1). Considering material sustainability and batteries’ high performances, the colloidal electrolyte may provide a feasible substitute beyond the liquid and all-solid-state electrolyte of ZIBs.

HighlightsThe interfacial engineering strategies of surface and electrolyte modifications for high-performance Zn metal anodes are reviewed.The reaction mechanisms for inhibiting dendrite growth and side reactions in interface engineering are systematically summarized.An outlook on future reference directions for new interface strategies to advance this field is provided.Due to their high safety and low cost, rechargeable aqueous Zn-ion batteries (RAZIBs) have been receiving increased attention and are expected to be the next generation of energy storage systems. However, metal Zn anodes exhibit a limited-service life and inferior reversibility owing to the issues of Zn dendrites and side reactions, which severely hinder the further development of RAZIBs. Researchers have attempted to design high-performance Zn anodes by interfacial engineering, including surface modification and the addition of electrolyte additives, to stabilize Zn anodes. The purpose is to achieve uniform Zn nucleation and flat Zn deposition by regulating the deposition behavior of Zn ions, which effectively improves the cycling stability of the Zn anode. This review comprehensively summarizes the reaction mechanisms of interfacial modification for inhibiting the growth of Zn dendrites and the occurrence of side reactions. In addition, the research progress of interfacial engineering strategies for RAZIBs is summarized and classified. Finally, prospects and suggestions are provided for the design of highly reversible Zn anodes.

The detrimental parasitic reactions and uncontrolled deposition behavior derived from inherently unstable interface have largely impeded the practical application of aqueous zinc batteries. So far, tremendous efforts have been devoted to tailoring interfaces, while stabilization of grain boundaries has received less attention. Here, we demonstrate that preferential distribution of intermetallic compounds at grain boundaries via an alloying strategy can substantially suppress intergranular corrosion. In-depth morphology analysis reveals their thermodynamic stability, ensuring sustainable potency. Furthermore, the hybrid nucleation and growth mode resulting from reduced Gibbs free energy contributes to the spatially uniform distribution of Zn nuclei, promoting the dense Zn deposition. These integrated merits enable a high Zn reversibility of 99.85% for over 4000 cycles, steady charge-discharge at 10 mA cm −2 , and impressive cyclability for roughly 3500 cycles in Zn-Ti//NH 4 V 4 O 10 full cell. Notably, the multi-layer pouch cell of 34 mAh maintains stable cycling for 500 cycles. This work highlights a fundamental understanding of microstructure and motivates the precise tuning of grain boundary characteristics to achieve highly reversible Zn anodes. The electrochemical performance of metal electrodes is significantly influenced by their grain boundary stability. Here, the authors propose a zinc-titanium two-phase alloy via grain boundary engineering to inhibit intergranular corrosion and tailor deposition behavior for stable aqueous zinc batteries.

The optimization of crystalline orientation of a Zn metal substrate to expose more Zn(0002) planes has been recognized as an effective strategy in pursuit of highly reversible Zn metal anodes. However, the lattice mismatch between substrate and overgrowth crystals has hampered the epitaxial sustainability of Zn metal. Herein, we discover that the presence of crystal grains deviating from [0001] orientation within a Zn(0002) metal anode leads to the failure of epitaxial mechanism. The electrodeposited [0001]-uniaxial oriented Zn metal anodes with a single (0002) texture fundamentally eliminate the lattice mismatch and achieve ultra-sustainable homoepitaxial growth. Using high-angle angular dark-filed scanning transmission electron microscopy, we elucidate the homoepitaxial growth of the deposited Zn following the “~ABABAB~” arrangement on the Zn(0002) metal from an atomic-level perspective. Such consistently epitaxial behavior of Zn metal retards dendrite formation and enables improved cycling, even in Zn||NH 4 V 4 O 10 pouch cells, with a high capacity of 220 mAh g −1 for over 450 cycles. The insights gained from this work on the [0001]-oriented Zn metal anode and its persistently homoepitaxial mechanism pave the way for other metal electrodes with high reversibility. The authors present a single [0001]-oriented Zn metal anode with high reversibility and demonstrate the significance of the Zn(0002) metal anode, characterized by a single crystalline orientation, for promoting ultra-sustainable homoepitaxial growth.

In nature, the human body is a perfect self-organizing and self-repairing system, with the skin protecting the internal organs and tissues from external damages. In this work, inspired by the human skin, we design a metal electrode skin (MES) to protect the metal interface. MES can increase the flatness of electrode and uniform the electric field distribution, inhibiting the growth of dendrites. In detail, an artificial film made of fluorinated graphene oxide serves as the first protection layer. At molecular level, fluorine is released and in-situ formed a robust SEI as the second protection “skin” for metal anode. As a result, Cu@MES | | K asymmetric cell is able to achieve an unprecedented cycle life (over 1600 cycles). More impressively, the full cell of K@MES | | Prussian blue exhibits a long cycle lifespan over 5000 cycles. This work illustrates a mechanism for metal electrode protection and provides a strategy for the applying bionics in batteries. Metal potassium anodes show great potential in high energy density batteries. However, their practical application is hindered by the unstable nature of the highly active metal surface. Here, authors propose a “metal skin” approach that stabilizes the surface of the metal, resulting in improved cycle life of potassium metal anode-based batteries.

HighlightsMetal-organic frameworks (UiO-66) functionalized glass fiber separator was constructed to accelerate the transport of charge carriers and provide a uniform electric field distribution on the surface of zinc anode.Zinc anode demonstrates preferential orientation of (002) plane under the control of UiO-66-GF, which effectively inhibits dendrites.Density functional theory calculation confirms that the adsorption effect of (002) plane on H is weaker, thus improving corrosion resistance and suppressing the hydrogen evolution reaction.Symmetric cells exhibit highly reversible plating/stripping behavior with long cycle life over 1650 h and full cells demonstrate excellent long-term stability (85%) for 1000 cycles.Aqueous zinc-ion batteries (AZIBs) are one of the promising energy storage systems, which consist of electrode materials, electrolyte, and separator. The first two have been significantly received ample development, while the prominent role of the separators in manipulating the stability of the electrode has not attracted sufficient attention. In this work, a separator (UiO-66-GF) modified by Zr-based metal organic framework for robust AZIBs is proposed. UiO-66-GF effectively enhances the transport ability of charge carriers and demonstrates preferential orientation of (002) crystal plane, which is favorable for corrosion resistance and dendrite-free zinc deposition. Consequently, Zn|UiO-66-GF-2.2|Zn cells exhibit highly reversible plating/stripping behavior with long cycle life over 1650 h at 2.0 mA cm−2, and Zn|UiO-66-GF-2.2|MnO2 cells show excellent long-term stability with capacity retention of 85% after 1000 cycles. The reasonable design and application of multifunctional metal organic frameworks modified separators provide useful guidance for constructing durable AZIBs.

Studies have found that oxygen-rich-containing functional groups in carbon-based materials can be used as active sites for the storage performance of K+, but the basic storage mechanism is still unclear. Herein, we construct and optimize 3D honeycomb-like carbon grafted with plentiful COOH/C = O functional groups (OFGC) as anodes for potassium ion batteries. The OFGC electrode with steady structure and rich functional groups can effectively contribute to the capacity enhancement and the formation of stable solid electrolyte interphase (SEI) film, achieving a high reversible capacity of 230 mAh g−1 at 3000 mA g−1 after 10,000 cycles (almost no capacity decay) and an ultra-long cycle time over 18 months at 100 mA g−1. The study results revealed the reversible storage mechanism between K+ and COOH/C = O functional groups by forming C-O-K compounds. Meanwhile, the in situ electrochemical impedance spectroscopy proved the highly reversible and rapid de/intercalation kinetics of K+ in the OFGC electrode, and the growth process of SEI films. In particular, the full cells assembled by Prussian blue cathode exhibit a high energy density of 113 Wh kg−1 after 800 cycles (calculated by the total mass of anode and cathode), and get the light-emitting diodes lamp and ear thermometer running.

HighlightsSmall cobalt nanoparticles are carefully encapsulated into a N-doped carbon shell (Co-NC) by calcining a Prussian blue analogue precursor.The presence of cobalt nanoparticles and Co-N bonds not only promotes adsorption behavior, but also reduces the diffusion energy barrier, enabling fast diffusion kinetics of K+ ions.The good diffusion kinetics and capacitive adsorption behavior of the Co-NC material synergistically contributes to enhanced potassium storage performances.Potassium-ion batteries (KIBs) have great potential for applications in large-scale energy storage devices. However, the larger radius of K+ leads to sluggish kinetics and inferior cycling performance, severely restricting its practical applicability. Herein, we propose a rational strategy involving a Prussian blue analogue-derived graphitized carbon anode with fast and durable potassium storage capability, which is constructed by encapsulating cobalt nanoparticles in nitrogen-doped graphitized carbon (Co-NC). Both experimental and theoretical results show that N-doping effectively promotes the uniform dispersion of cobalt nanoparticles in the carbon matrix through Co–N bonds. Moreover, the cobalt nanoparticles and strong Co–N bonds synergistically form a three-dimensional conductive network, increase the number of adsorption sites, and reduce the diffusion energy barrier, thereby facilitating the adsorption and the diffusion kinetics. These multiple effects lead to enhanced reversible capacities of 305 and 208.6 mAh g−1 after 100 and 300 cycles at 0.05 and 0.1 A g−1, respectively, demonstrating the applicability of the Co-NC anode for KIBs.

HighlightsAnimal models are applied to evaluate the biosecurity and biocompatibility of the zinc-ion batteries with the electrolytes of different zinc salts.Leakage scene simulations and histological analysis are employed in investigating the tissue response after battery implantations, in which ZnSO4 exhibits higher biosecurity.Sn hetero nucleus is introduced to stabilize the zinc anode, which not only facilitates the planar zinc deposition, but also contributes to higher hydrogen evolution overpotential.Biocompatible devices are widely employed in modernized lives and medical fields in the forms of wearable and implantable devices, raising higher requirements on the battery biocompatibility, high safety, low cost, and excellent electrochemical performance, which become the evaluation criteria toward developing feasible biocompatible batteries. Herein, through conducting the battery implantation tests and leakage scene simulations on New Zealand rabbits, zinc sulfate electrolyte is proved to exhibit higher biosecurity and turns out to be one of the ideal zinc salts for biocompatible zinc-ion batteries (ZIBs). Furthermore, in order to mitigate the notorious dendrite growth and hydrogen evolution in mildly acidic electrolyte as well as improve their operating stability, Sn hetero nucleus is introduced to stabilize the zinc anode, which not only facilitates the planar zinc deposition, but also contributes to higher hydrogen evolution overpotential. Finally, a long lifetime of 1500 h for the symmetrical cell, the specific capacity of 150 mAh g−1 under 0.5 A g−1 for the Zn–MnO2 battery and 212 mAh g−1 under 5 A g−1 for the Zn—NH4V4O10 battery are obtained. This work may provide unique perspectives on biocompatible ZIBs toward the biosecurity of their cell components.

HighlightsThe large-sheet holey graphene framework/SiO (LHGF/SiO) composite displays notably high recoverable strain, suggesting considerably improved mechanical flexibility and robustnessThe LHGF/SiO anode with a mass loading of 44 mg cm−2 delivers a high areal capacity of 35.4 mAh cm−2 at current density of 8.8 mA cm−2 and retains a capacity of 10.6 mAh cm−2 at 17.6 mA cm−2The LHGF/SiO anode with an ultra-high mass loading of 94 mg cm−2 delivers an extraordinary areal capacity up to 140.8 mAh cm−2, about 1–2 order of magnitude higher than those in typical commercial devicesSilicon monoxide (SiO) is an attractive anode material for next-generation lithium-ion batteries for its ultra-high theoretical capacity of 2680 mAh g−1. The studies to date have been limited to electrodes with a relatively low mass loading (< 3.5 mg cm−2), which has seriously restricted the areal capacity and its potential in practical devices. Maximizing areal capacity with such high-capacity materials is critical for capitalizing their potential in practical technologies. Herein, we report a monolithic three-dimensional (3D) large-sheet holey graphene framework/SiO (LHGF/SiO) composite for high-mass-loading electrode. By specifically using large-sheet holey graphene building blocks, we construct LHGF with super-elasticity and exceptional mechanical robustness, which is essential for accommodating the large volume change of SiO and ensuring the structure integrity even at ultrahigh mass loading. Additionally, the 3D porous graphene network structure in LHGF ensures excellent electron and ion transport. By systematically tailoring microstructure design, we show the LHGF/SiO anode with a mass loading of 44 mg cm−2 delivers a high areal capacity of 35.4 mAh cm−2 at a current of 8.8 mA cm−2 and retains a capacity of 10.6 mAh cm−2 at 17.6 mA cm−2, greatly exceeding those of the state-of-the-art commercial or research devices. Furthermore, we show an LHGF/SiO anode with an ultra-high mass loading of 94 mg cm−2 delivers an unprecedented areal capacity up to 140.8 mAh cm−2. The achievement of such high areal capacities marks a critical step toward realizing the full potential of high-capacity alloy-type electrode materials in practical lithium-ion batteries.