Search Results (375)

Severe polysulfide shuttling and sluggish redox kinetics critically hinder lithium–sulfur (Li-S) battery commercialization. In this study, a multifunctional diatomite (DE)/TiO₂/MoS₂/N-doped carbon nanofiber (NCNF) composite separator was fabricated via hydrothermal synthesis, electrospinning, and carbonization. DE provides dual polysulfide suppression, encompassing microporous confinement and electrostatic repulsion. By integrating synergistic catalytic effects from TiO₂ and MoS₂ nanoparticles, which accelerate polysulfide conversion, and conductive NCNF networks, which facilitate rapid charge transfer, this hierarchical design achieves exceptional electrochemical performance: a 1245.6 mAh g⁻¹ initial capacity at 0.5 C and 65.94% retention after 200 cycles. This work presents a rational multi-component engineering strategy to suppress shuttle effects in high-energy-density Li-S batteries. Full article

Films of functionalised multiwalled carbon nanotubes (MWCNTs) were fabricated as interlayers (interfacial layers between the cathode and separator) in a lithium–sulfur battery (LSB). Phenylsulfonate functionalisation of commercial MWCNTs was achieved via diazotisation to attach lithium phenylsulfonate groups and was characterised by IR and XPS spectroscopies. SEM-EDX showed sulfur and oxygen colocations due to the sulfonate groups on the interlayer surface. However, CHNS elemental microstudies showed a low degree of functionalisation. Without an interlayer, the LSB produced stable cycling at a capacity of 600 mA h g⁻¹_sulfur at 0.05 C for 40 cycles. Using an unfunctionalised interlayer as a control gave a capacity of 1400 mA h g⁻¹_sulfur for the first cycle but rapidly decayed to the same 600 mA h g⁻¹_sulfur at the 40th cycle at 0.05 C, suggesting a high degree of polysulfide shuttling. Adding a lithium phenylsulfonated interlayer gave an initial capacity increase to 1100 mA h g⁻¹_sulfur that lowered to 800 mA h g⁻¹_sulfur at 0.05 C by the 40th cycle, showing an increase in charge storage (33%) relative to the other cells. This performance increase has been attributed to lessened polysulfide shuttling due to repulsion by the phenylsulfonate groups, increased conductivity at the separator-cathode interface and an increase in surface area. Full article

The modification of materials is considered as one of the productive methods to facilitate the better electrochemical behavior of lithium–sulfur battery cathodes and inhibit the shuttle effect. Adopting first-principles calculations in this work, the application potential of pristine and B-, N-, and P-doped thgraphene as anchoring materials was investigated. The results reveal that pristine and doped substrates have an excellent structural stability, conductivity, and electrochemical activity. In the absence of an electric field, four substrates exhibit a strong anchoring effect on the Li₂S cluster, where the adsorption energies fall within 3.10 to 4.48 eV. Even under the external electric field, all substrates exhibit notable structural stability during Li₂S adsorption processes and maintain a high electrical conductivity, with adsorption energies exceeding 2.75 eV. Furthermore, it has been observed that the interfacial diffusion energy barriers for Li on all substrates are below 0.35 eV, which effectively enhances Li migration and facilitates reaction kinetics. Additionally, Li₂S demonstrates a low decomposition energy barrier (varying from 0.84 to 1.55 eV) on pristine and doped substrates, enabling the efficient regeneration of the active material during the battery cycling. These findings offer a scientific guideline for the design of pristine and doped thgraphene as an excellent anchoring material for advanced lithium–sulfur batteries. Full article

The conventional spent lithium-ion batteries (LIBs) recycling method suffers from complex processes and excessive chemical consumption. Hence, this study proposes an electrochemical strategy for achieving reductant-free leaching of high-valence transition metals and efficient separation of valuable components from spent cathode sheets (CSs). An innovatively designed sandwich-structured electrochemical reactor achieved efficient reductive dissolution of cathode materials (CMs) while maintaining the structural integrity of aluminum (Al) foils in a dilute sulfuric acid system. Optimized current enabled leaching efficiencies exceeding 93% for lithium (Li), cobalt (Co), manganese (Mn), and nickel (Ni), with 88% metallic Al foil recovery via cathodic protection. Multi-scale characterization systematically elucidated metal valence evolution and interfacial reaction mechanisms, validating the technology’s tripartite innovation: simultaneous high metal extraction efficiency, high value-added Al foil recovery, and organic removal through single-step electrochemical treatment. The process synergized the dissolution of CM particles and hydrogen bubble-induced physical liberation to achieve clean separation of polyvinylidene difluoride (PVDF) and carbon black (CB) layers from Al foil substrates. This method eliminates crushing pretreatment, high-temperature reduction, and any other reductant consumption, establishing an environmentally friendly and efficient method of comprehensive recycling of battery materials. Full article

Lithium–sulfur batteries (LSBs), possessing excellent theoretical capacities, advanced theoretical energy densities, low cost, and nontoxicity, are one of the most promising energy storage battery systems. However, some issues, including poor conductivity of elemental S, the “shuttle effect” of high-order lithium polysulfides (LiPSs), and sluggish reaction kinetics, hinder the commercialization of LSBs. To solve these problems, various carbon-based aerogels with developed surface morphology, tunable pores, and electrical conductivity have been examined for immobilizing sulfur, mitigating its volume variation and enhancing its electrochemical kinetics. In this paper, an extensive generalization about the effective preparation methods of carbon-based aerogels comprising the combined method of carbonization with the gelation of precursors and drying processes (ambient pressure drying, freeze-drying, and supercritical drying) is proposed. And we summarize various carbon carbon-based aerogels, mainly including graphene aerogels (Gas) and carbon nanofiber (CNF) and carbon nanotube (CNT) aerogels as cathodes, separators, and interlayers in LSBs. In addition, the mechanism of action of carbon-based aerogels in LSBs is described. Finally, we conclude with an outlook section to provide some insights into the application of carbon-based aerogels in electrochemical energy storage devices. Based on the discussion and proposed recommendations, we provide more approaches on nanomaterials in high-performance liquid or state LSBs with high electrochemical performance in the future. Full article

Lithium–sulfur (Li-S) batteries are hindered by the sluggish electrochemical kinetics and poor reversibility of lithium polysulfides (LiPSs), which limits their practical energy density and cycle life. In order to address this issue, a novel Ni₃N/Nb₄N₅ heterostructure was synthesized via electrospinning and nitridation as a functional coating for polypropylene (PP) separators. Adsorption experiments were conducted in order to ascertain the heterostructure’s superior affinity for LiPSs, thereby effectively mitigating their shuttling. Studies of Li₂S nucleation demonstrated the catalytic role of the substance in accelerating the deposition kinetics of Li₂S. Consequently, Li-S cells that employed the Ni₃N/Nb₄N₅-modified separator were found to achieve significantly enhanced electrochemical performance, with the cells delivering an initial discharge capacity of 1294.4 mAh g⁻¹ at 0.2 C. The results demonstrate that, after 150 cycles, the cells retained a discharge capacity of 796.2 mAh g⁻¹, corresponding to a low capacity decay rate of only 0.25% per cycle. In addition, the rate capability of the cells was found to be improved in comparison to control cells with NiNb₂O₆-modified or pristine separators. Full article

The development of polymer binders with tailored functionalities and green manufacturing processes is highly needed for high-performance lithium–sulfur batteries. In this study, a readily hydrolyzable 3,9-divinyl-2,4,8,10-tetraoxaspiro-[5.5]-undecane is utilized to prepare a water-based binder. Specifically, the acrolein produced by hydrolysis undergoes in situ polymerization to form a linear polymer, while the other hydrolyzed product, pentaerythritol, physically crosslinks these polymer chains via hydrogen bonding, generating a network polymer (BTU). Additionally, gallic acid (GA), a substance derived from waste wood, is further introduced into BTU during slurry preparation, forming a biphenol-containing binder (BG) with a multi-hydrogen-bonded structure. This resilience and robust cathode framework effectively accommodate volumetric changes during cycling while maintaining efficient ion and electron transport pathways. Furthermore, the abundant polar groups in BG enable strong polysulfide adsorption. As a result, sulfur cathode with a high mass loading of 5.3 mg cm⁻² employing the BG (7:3) binder still retains an areal capacity of 4.7 mA h cm⁻² after 50 cycles at 0.1 C. This work presents a sustainable strategy for battery manufacturing by integrating renewable biomass-derived materials and eco-friendly aqueous processing to develop polymer binders, offering a green pathway to high-performance lithium–sulfur batteries. Full article

This study investigated the detrimental effect of graphite on metal recovery during sulfuric acid roasting of lithium-ion battery materials. While sulfuric acid roasting of black mass achieved excellent leaching efficiencies (>99%) for nickel and cobalt at 250 °C, higher roasting temperatures significantly reduced their recovery to 84.9% and 93.1% at 400 °C, respectively. The key finding reveals that graphite accelerates sulfuric acid decomposition during roasting, consuming acid that would otherwise be available for metal sulfate formation. Weight-loss measurements confirmed this mechanism, showing increased acid decomposition with higher graphite content. Despite requiring three times the theoretical acid dosage (0.45 vs. 0.15 mole) for complete conversion, the process remained insufficient at elevated temperatures when graphite was present. These findings demonstrate that graphite interference is a critical factor limiting the efficiency of sulfuric acid roasting for lithium-ion battery recycling, necessitating lower roasting temperatures (around 250 °C) to maintain acceptable metal recovery efficiencies. Full article

Exploring advanced sulfur cathode materials is important for the development of lithium-sulfur batteries (LSBs), but they still present challenges. Herein, zinc oxide dots-modified vanadium nitride flower-like heterojunctions (Zn-QDs-VN) as sulfur hosts are prepared by a phase separation strategy. Characterizations confirm that the flower structure with high specific surface area and pores improves active site exposure and electron/mass transfer. In situ phase separation enriches the Zn-QDs-VN interface, addressing the issues of uneven distribution and interface reduction of Zn-QDs-VN. Further theoretical computations reveal that ZnO-QDs-VN with optimized intermediate spin states can constitute a stable LiS* bond sequence, which can conspicuously facilitate the adsorption and conversion of LiPSs and reduce the battery reaction energy barrier. Therefore, the ZnO-QDs-VN@S cathode shows a high initial specific capacity of 1109.6 mAh g⁻¹ at 1.0 C and long cycle stability (maintaining 984.2 mAh g⁻¹ after 500 cycles). Under high S loading (8.5 mg cm⁻²) and lean electrolyte conditions (E/S = 6.5 μL mg⁻¹), it also exhibits a high initial area capacity (10.26 mAh cm⁻²) at 0.2 C. The interfacial synergistic effect accelerates the adsorption and conversion of LiPSs and reduces the energy barriers in cell reactions. The study provides a new method for designing heterojunctions to achieve high-performance LSBs. Full article

The “shuttle effect” caused by the shuttling of soluble long-chain polysulfides between the anode and cathode electrodes has persistently hindered lithium–sulfur batteries (LSBs) from achieving stable and high-capacity performance. Numerous materials have been explored to mitigate the adverse effects of this phenomenon, among which metal oxides and metal sulfides are regarded as promising solutions due to their strong adsorption capability toward lithium polysulfides (LiPSs). However, the poor electrical conductivity of the metal oxides and sulfides, coupled with their inherent morphological limitations, makes it challenging to sustainably suppress LiPS shuttling. In this study, we designed a heterostructured catalyst composed of a metal oxide–metal sulfide heterostructure integrated with carbon nanotubes (CNTs). This design addresses the low conductivity issue of metal oxides/sulfides while optimizing the material’s morphology, enabling persistent LiPSs adsorption. Furthermore, the composite successfully facilitates three-dimensional (3D) Li₂S deposition. The assembled battery exhibits stable and high-capacity performance, delivering an initial discharge capacity of 622.45 mAh g⁻¹ at 2C and retaining 569.5 mAh g⁻¹ after 350 cycles, demonstrating exceptional cycling stability. Full article

Lithium- and sodium-ion batteries (LIBs and SIBs) suffer from the significant degradation of electrochemical performance at low temperatures. This work presents promising hybrid anodes synthesized by the rapid thermolysis of ammonium tetrathiomolybdate and graphene oxide (GO) at 600 and 700 °C. Transmission electron microscopy revealed the formation of MoS₂ crystallites oriented along or perpendicular to the surface of reduced GO (rGO) layers. X-ray photoelectron spectroscopy found the covalent C–S bonds connecting components in the MoS₂/rGO hybrids. The MoS₂/rGO_600 hybrid showed higher specific capacities in LIBs of 1370 mAh/g, 835 mAh/g, and 711 mAh/g at a current density of 0.1 A/g and temperatures of 25 °C, 0 °C, and −20 °C, respectively, due to the presence of excess sulfur in the sample. Increasing the current density to 2 A/g retained 78 and 34% of the capacity at 25 °C and −20 °C. In SIBs, the MoS₂/rGO_700 hybrid showed more promising results, achieving 550 mAh/g at 0.1 A/g and 400 mAh/g at 2 A/g, while lowering the temperature to −20 °C retained 48 and 17% of the capacity. Such good SIB performance is attributed to the enrichment of the sample with vertically oriented MoS₂ layers covalently bonded to the rGO surface. Full article

Lithium–sulfur batteries (LSBs) are favorable candidates for advanced energy storage, boasting a remarkable theoretical energy density of 2600 Wh kg⁻¹. Moreover, several challenges hinder their practical implementation, including sulfur’s intrinsic electrical insulation, the shuttle effect of lithium polysulfides (LiPSs), sluggish redox kinetics of Li₂S₂/Li₂S, and the uncontrolled growth of Li dendrites. These issues pose significant obstacles to the commercialization of LSBs. A viable strategy to address these challenges involves using MXene materials, 2D transition metal carbides, and nitrides (TMCs/TMNs) as hosts, functional separators, or interlayers. MXenes offer exceptional electronic conductivity, adjustable structural properties, and abundant polar functional groups, enabling strong interactions with both S cathodes and Li anodes. Despite their advantages, current MXene synthesis methods predominantly rely on acid etching, which is associated with environmental concerns, low production efficiency, and limited structural versatility, restricting their potential in LSBs. This review provides a comprehensive overview of traditional and environmentally sustainable MXene synthesis techniques, emphasizing their applications in developing S cathodes, Li anodes, and functional separators for LSBs. Additionally, it discusses the challenges and outlines future directions for advancing MXene-based solutions in LSBs technology. Full article

With the rapid development of electrical energy storage technologies, traditional battery systems are limited in practical applications by insufficient energy density and short cycle life. This review provides a comprehensive and critical summary of MXene or MXene-based composites as electrode materials for high-performance energy storage devices. By integrating the synthesis techniques of MXenes that have been studied, this paper systematically illustrates the physicochemical properties, synthesis strategies, and mechanisms of MXenes, and analyzes the bottlenecks in their large-scale preparation. Meanwhile, it collates the latest research achievements of MXenes in the field of metal–ion batteries in recent years, focusing on integrating their latest progress in lithium–ion, sodium–ion, lithium–sulfur, and multivalent ion (Zn²⁺, Mg²⁺, Al³⁺) batteries, and reveals their action mechanisms in different electrode material cases. Combining DFT analysis of the effects of surface functional groups on adsorption energy with experimental studies clarifies the structure–activity relationships of MXene-based composites. However, the development of energy storage electrode materials using MXenes and their hybrid compounds remains in its infancy. Future development directions for MXene-based batteries should focus on understanding and regulating surface chemistry, investigating specific energy storage mechanisms in electrodes, and exploring and developing electrode materials related to bimetallic MXenes. Full article

Layered double hydroxides (LDHs), notable for their unique two-dimensional layered structures, have attracted significant research attention due to their exceptional versatility and promising performance in energy storage and conversion applications. This comprehensive review systematically addresses the fundamentals and diverse synthesis strategies for LDHs, including co-precipitation, hydrothermal synthesis, electrochemical deposition, sol-gel processes, ultrasonication, and exfoliation techniques. The synthesis methods profoundly influence the physicochemical properties, morphology, and electrochemical performance of LDHs, necessitating a detailed understanding to optimize their applications. In this paper, the role of LDHs in batteries, supercapacitors, and hydrogen production is critically evaluated. We discuss their incorporation in various battery systems, such as lithium-ion, lithium–sulfur, sodium-ion, chloride-ion, zinc-ion, and zinc–air batteries, highlighting their structural and electrochemical advantages. Additionally, the superior pseudocapacitive behavior and high energy densities offered by LDHs in supercapacitors are elucidated. The effectiveness of LDHs in hydrogen production, particularly through electrocatalytic water splitting, underscores their significance in renewable energy systems. This review paper uniquely integrates these three pivotal energy technologies, outlining current innovations and challenges, thus fulfilling a critical need for the scientific community by providing consolidated insights and guiding future research directions. Full article

The imperative for sustainable energy has driven the demand for efficient energy storage systems that can harness renewable resources and store surplus energy for off-peak usage. Among the numerous advancements in energy storage technology, polymeric nanofibers have emerged as promising nanomaterials, offering high specific surface areas that facilitate increased charge storage and enhanced energy density, thereby improving electrochemical performance. This review delves into the pivotal role of nanofibers in determining the optimal functionality of energy storage systems. Electrospinning emerged as a facile and cost-effective method for generating nanofibers with customizable nanostructures, making it attractive for energy storage applications. Our comprehensive review article examines the latest developments in electrospun nanofibers for electrochemical storage devices, highlighting their use as separators and electrode materials. We provide an in-depth analysis of their application in various battery technologies, including supercapacitors, lithium-ion batteries, sodium-ion batteries, potassium-ion batteries, lithium–sulfur batteries, and lithium–oxygen batteries, with a focus on their electrochemical performance. Furthermore, we summarize the diverse fabrication techniques, optimization of key influencing factors, and environmental implications of nanofiber production and their properties. This review aims to offer an inclusive understanding of electrospinning’s role in advancing electrochemical energy storage, providing insights into the factors that drive the performance of these critical materials. Full article