Thermodynamics and Kinetics of Aqueous Zinc Electrolytes in Extreme Temperatures: Challenges, Advances, and Future.

Aqueous zinc batteries have gained prominence in grid-scale energy storage due to their inherent safety and cost-effectiveness. As the core functional medium, electrolytes critically determine battery performance and lifespan across temperature variations. Conventional aqueous zinc electrolytes face dual challenges: low-temperature operation suffers from freezing issues and sluggish ion transport, while high-temperature applications are constrained by electrolyte instability and electrode/electrolyte interfacial deterioration.

Tuning Zn Deposition Kinetics towards Deep-Reversible Zinc Metal Batteries with All-Climate Adaptability.

Uncontrollable Zn dendrites and severe hydrogen evolution reaction (HER) hamper the practical application of aqueous zinc-metal batteries, which closely related to the deposition kinetics and thermodynamic stability of Zn anode. In this work, we returned to the classic perspectives of kinetics and thermodynamics, introducing a small amount of reduced glutathione (RGSH) to reshape the kinetic behavior of Zn deposition and increasing the thermodynamic energy barrier of HER. Specifically, the steric hindrance effect of RGSH tuned the electrochemical reduction kinetics to match Zn migration and increased the proportion of Zn in the bulk phase migration, thereby inducing dendrite-free deposition behavior with ordered (002) texturing.

Interpenetrating Composite Hydrogel Electrolyte with Organic/Inorganic Polar Groups for Stable Zinc Metal Anode.

Hydrogel electrolytes have been widely explored in flexible zinc batteries owing to their considerable mechanical strain and water-retaining properties. However, it is difficult to balance the contradiction between the ionic conductivity and the mechanical strength due to the deterioration of structural stability with the addition of electrolyte salts. To address this, we designed a coassembling organic-inorganic hydrogel (P-P/M) based on poly(vinyl alcohol)-polyacrylamide (P-P) interpenetrating matrix decorated with Zn-based montmorillonite (Zn-MMT).

Tailoring Pseudo-Graphitic Domain by Molybdenum Modification to Boost Sodium Storage Capacity and Durability for Hard Carbon.

Hard carbon (HC) stands out as the most prospective anode for sodium-ion batteries (SIBs) with significant potential for commercial applications. However, some long-standing and intractable obstacles, like low first coulombic efficiency (ICE), poor rate capability, storage capacity, and cycling stability, have severely hindered the conversion process from laboratory to commercialization. The above-mentioned issues are closely related to Na transfer kinetics, surface chemistry, and internal pseudo-graphitic carbon content.

Tailoring the Whole Deposition Process from Hydrated Zn to Zn for Stable and Reversible Zn Anode.

The practical application of aqueous zinc-ion batteries (ZIBs) indeed faces challenges primarily attributed to the inherent side reactions and dendrite growth associated with the Zn anode. In the present work, N-Methylmethanesulfonamide (NMS) is introduced to optimize the transfer, desolvation, and reduction of Zn, achieving highly stable and reversible Zn plating/stripping. The NMS molecule can substitute one HO molecule in the solvation structure of hydrated Zn and be preferentially chemisorbed on the Zn surface to protect Zn anode against corrosion and hydrogen evolution reaction (HER), thereby suppressing byproducts formation.

Intrinsically Decoupled Coordination Chemistries Enable Quasi-Eutectic Electrolytes with Fast Kinetics toward Enhanced Zinc-Ion Capacitors.

Eutectic electrolytes show potential beyond conventional low-concentration electrolytes (LCEs) in zinc (Zn)-ion capacitors (ZICs) yet suffer from high viscosity and sluggish kinetics. Herein, we originally propose a universal theory of intrinsically decoupling to address these issues, producing a novel electrolyte termed "quasi-eutectic" electrolyte (quasi-EE). Joint experimental and theoretical analyses confirm its unique solution coordination structure doped with near-LCE domains.

Water Catchers within Sub-Nano Channels Promote Step-by-Step Zinc-Ion Dehydration Enable Highly Efficient Aqueous Zinc-Metal Batteries.

Zinc metal suffers from violent and long-lasting water-induced side reactions and uncontrollable dendritic Zn growth, which seriously reduce the coulombic efficiency (CE) and lifespan of aqueous zinc-metal batteries (AZMBs). To suppress the corresponding harmful effects of the highly active water, a stable zirconium-based metal-organic framework with water catchers decorated inside its sub-nano channels is used to protect Zn-metal. Water catchers within narrow channels can constantly trap water molecules from the solvated Zn-ions and facilitate step-by-step desolvation/dehydration, thereby promoting the formation of an aggregative electrolyte configuration, which consequently eliminates water-induced corrosion and side reactions.

Zinc-Ion Anchor Induced Highly Reversible Zn Anodes for High Performance Zn-Ion Batteries.

Unstable Zn interface with serious detrimental parasitic side-reactions and uncontrollable Zn dendrites severely plagues the practical application of aqueous zinc-ion batteries. The interface stability was closely related to the electrolyte configuration and Zn depositional behavior. In this work, a unique Zn-ion anchoring strategy is originally proposed to manipulate the coordination structure of solvated Zn-ions and guide the Zn-ion depositional behavior.

Chelating Additive Regulating Zn-Ion Solvation Chemistry for Highly Efficient Aqueous Zinc-Metal Battery.

Aqueous zinc-metal batteries (AZMBs) usually suffered from poor reversibility and limited lifespan because of serious water induced side-reactions, hydrogen evolution reactions (HER) and rampant zinc (Zn) dendrite growth. Reducing the content of water molecules within Zn-ion solvation sheaths can effectively suppress those inherent defects of AZMBs. In this work, we originally discovered that the two carbonyl groups of N-Acetyl-ϵ-caprolactam (N-ac) chelating ligand can serve as dual solvation sites to coordinate with Zn, thereby minimizing water molecules within Zn-ion solvation sheaths, and greatly inhibit water-induced side-reactions and HER.

Unleashing the high energy potential of zinc-iodide batteries: high-loaded thick electrodes designed with zinc iodide as the cathode.

The realization of high energy is of great importance to unlock the practical potential of zinc-iodine batteries. However, significant challenges, such as low iodine loading (mostly less than 50 wt%), restricted iodine reutilization, and severe structural pulverization during cycling, compromise its intrinsic features. This study introduces an optimized, fully zincified zinc iodide loaded onto a hierarchical carbon scaffold with high active component loading and content (82 wt%) to prepare a thick cathode for enabling high-energy Zn-I batteries.

Solid-State Electrolytes and Electrode/Electrolyte Interfaces in Rechargeable Batteries.

Solid-state batteries (SSBs) are considered to be one of the most promising candidates for next-generation energy storage systems due to the high safety, high energy density and wide operating temperature range of solid-state electrolytes (SSEs) they use. Unfortunately, the practical application of SSEs has rarely been successful, which is largely attributed to the low chemical stability and ionic conductivity, ineluctable solid-solid interface issues including limited ion transport channels, high energy barriers, and poor interface contact. A comprehensive understanding of ion transport mechanisms of various SSEs, interactions between fillers and polymer matrixes and the role of the interface in SSBs are indispensable for rational design and performance optimization of novel electrolytes.

Highly Stable Aqueous Zinc Metal Batteries Enabled by an Ultrathin Crack-Free Hydrophobic Layer with Rigid Sub-Nanochannels.

Aqueous zinc-metal batteries (AZMBs) have received tremendous attentions due to their high safety, low cost, environmental friendliness, and simple process. However, zinc-metal still suffer from uncontrollable dendrite growth and surface parasitic reactions that reduce the Coulombic efficiency (CE) and lifetime of AZMBs. These problems which are closely related to the active water are not well-solved.

Aligned Dipoles Induced Electric-Field Promoting Zinc-Ion De-Solvation toward Highly Stable Dendrite-Free Zinc-Metal Batteries.

Water-induced parasitic reactions and uncontrolled dendritic Zn growth are long-lasting tricky problems that severely hinder the development of aqueous zinc-metal batteries. Those notorious issues are closely related to electrolyte configuration and zinc-ion transport behavior. Herein, through constructing aligned dipoles induced electric-field on Zn surface, both the solvation structure and transport behavior of zinc-ions are fundamentally changed.

Unique ion rectifier intermediate enabled by ultrathin vermiculite sheets for high-performance Zn metal anodes.

Metallic Zn represents as a primary choice in fabricating various aqueous Zn-ion batteries (ZIBs), however challenging issues including dendrite growth and parasitic reactions at the anode/electrolyte interface, considerably hamper its practical implementation in large-scale energy storage. Herein, we report a low-cost multifunctional ion rectifier (IRT) as an artificial intermediate to reform Zn anode, which can practically eliminate the above issues. The hydrophobic shell (polyvinylidene difluoride) can suppress Zn interfacial corrosion with an inhibition efficiency of 94.

Lithiophilic Magnetic Host Facilitates Target-Deposited Lithium for Practical Lithium-Metal Batteries.

Lithium-metal shows promising prospects in constructing various high-energy-density lithium-metal batteries (LMBs) while long-lasting tricky issues including the uncontrolled dendritic lithium growth and infinite lithium volume expansion seriously impede the application of LMBs. In this work, it is originally found that a unique lithiophilic magnetic host matrix (Co O -CCNFs) can simultaneously eliminate the uncontrolled dendritic lithium growth and huge lithium volume expansion that commonly occur in typical LMBs. The magnetic Co O nanocrystals which inherently embed on the host matrix act as nucleation sites and can also induce micromagnetic field and facilitate a targeted and ordered lithium deposition behavior thus, eliminating the formation of dendritic Li.

Enzyme-Triggered Size-Switchable Nanosystem for Deep Tumor Penetration and Hydrogen Therapy.

The poor penetration of nanocarriers within tumor dense extracellular matrices (ECM) greatly restricts the access of anticancer drugs to the deep tumor cells, resulting in low therapeutic efficacy. Moreover, the high toxicity of the traditional chemotherapeutics inevitably causes undesirable side effects. Herein, taking the advantages of biosafe H and small-sized nanoparticles in diffusion within tumor ECM, we develop a matrix metalloprotease 2 (MMP-2) responsive size-switchable nanoparticle (UAMSN@Gel-PEG) that is composed of ultrasmall amino-modified mesoporous silica nanoparticles (UAMSN) wrapped within a PEG-conjugated gelatin to deliver H to the deep part of tumors for effective gas therapy.

In/Ce Co-doped LiVO and Nitrogen-modified Carbon Nanofiber Composites as Advanced Anode Materials for Lithium-ion Batteries.

LiVO (LVO) is considered as a novel alternative anode material for lithium-ion batteries (LIBs) due to its high capacity and good safety. However, the inferior electronic conductivity impedes its further application. Here, nanofibers (LICVO/NC) with In/Ce co-doped LiVO strengthened by nitrogen-modified carbon are prepared.

An improved 9 micron thick separator for a 350 Wh/kg lithium metal rechargeable pouch cell.

The use of separators that are thinner than conventional separators (> 20 µm) would improve the energy densities and specific energies of lithium batteries. However, thinner separators increase the risk of internal short circuits from lithium dendrites formed in both lithium-ion and lithium metal batteries. Herein, we grow metal-organic frameworks (MOFs) inside the channels of a polypropylene separator (8 µm thick) using current-driven electrosynthesis, which aggregates the electrolyte in the MOF channels.

Multichannel Ca Generator for Synergistic Tumor Therapy via Intracellular Ca Overload and Chemotherapy.

Ca overload has attracted an increasing attention due to its benefit of precise cancer therapy, but its efficacy is limited by the strong Ca excretion of cancer cells. Moreover, monotherapy of Ca overload usually fails to treat tumors satisfactorily. Herein, we develop a multifunctional nanosystem that could induce Ca overload by multipathway and simultaneously produce chemotherapy for synergistic tumor therapy.

Mesoporous peroxidase nanozyme for synergistic chemodynamic therapy and chemotherapy.

Peroxidase nanozyme, enabling decomposition of hydrogen peroxide (HO) into highly toxic hydroxyl radical (•OH), is an emerging technology for tumor treatment. However, limited by the low HO level in the tumor microenvironment, the standalone peroxidase nanozyme-mediated therapy usually fails to achieve desirable therapeutic outcomes. Herein, we presented a mesoporous nanozyme that not only had peroxidase-like activity but also could deliver anticancer drug for synergistic tumor therapy.

Building Ultra-Stable and Low-Polarization Composite Zn Anode Interface via Hydrated Polyzwitterionic Electrolyte Construction.

Aqueous zinc metal batteries are noted for their cost-effectiveness, safety and environmental friendliness. However, the water-induced notorious issues such as continuous electrolyte decomposition and uneven Zn electrochemical deposition remarkably restrict the development of the long-life zinc metal batteries. In this study, zwitterionic sulfobetaine is introduced to copolymerize with acrylamide in zinc perchlorate (Zn(ClO)) solution.

Autocatalytic oncotherapy nanosystem with glucose depletion for the cascade amplification of hypoxia-activated chemotherapy and HO-dependent chemodynamic therapy.

Employing hypoxia-activated prodrugs is an appealing oncotherapy strategy, but limited by insufficient tumor hypoxia. Moreover, a standalone prodrug fails to treat tumors satisfactorily due to tumor complexity. Herein, a nanosystem (TPZ@FeMSN-GOX) was established for triple synergetic cancer starvation therapy, hypoxia-activated chemotherapy and chemodynamic therapy (CDT).

Intelligent Nanoplatform with Multi Therapeutic Modalities for Synergistic Cancer Therapy.

Chemodynamic therapy (CDT) has attracted increasing attention in tumor treatment but is limited by insufficient endogenous HO. Moreover, it is challenging for monotherapy to achieve a satisfactory outcome due to tumor complexity. Herein, we developed an intelligent nanoplatform that could respond to a tumor microenvironment to induce efficient CDT without complete dependence on HO and concomitantly generate chemotherapy and oncosis therapy (OT).

pH-Responsive size-shrinkable mesoporous silica-based nanocarriers for improving tumor penetration and therapeutic efficacy.

Poor tumor penetration is a major obstacle to nanomedicine for achieving effective anticancer therapy. Tumor microenvironment-induced nanomedicine size shrinkage is a promising strategy to overcome the drug penetration barrier across the dense tumor matrix. Herein, we design a size-shrinkable nanocarrier that uses acid as a means of triggering a change in particle size for co-achievement of efficient tumor accumulation followed by deep tumor penetration and rapid clearance from the body.

Organic-Inorganic Hybrid Cathode with Dual Energy-Storage Mechanism for Ultrahigh-Rate and Ultralong-Life Aqueous Zinc-Ion Batteries.

The exploitation of cathode materials with high capacity as well as high operating voltage is extremely important for the development of aqueous zinc-ion batteries (ZIBs). Yet, the classical high-capacity materials (e.g.