Lithium-sulfur batteries undergo solid-liquid-solid phase transitions based on a dissolution-deposition reaction mechanism. To effectively suppress the shuttling of soluble polysulfides, catalysts should be incorporated into the cathode to enhance both the adsorption and conversion processes. The formation of a triphasic interface among the catalyst, conductive material, and electrolyte plays a key role in facilitating these reactions.
View Article and Find Full Text PDFPrussian blue (PB) is a promising low-cost cathode material for sodium-ion batteries (SIBs), but the impact of crystal water on performance degradation remains unclear. This study explores how PB's crystal water interacts with different electrolyte salts-NaClO and NaTFSI-affecting solvation structure and interfacial stability. Based on the Hofmeister series, it is demonstrated that the strong hydration of ClO sustains water reactivity, promoting Fe oxidation and solvent decomposition at high voltages.
View Article and Find Full Text PDFLi- and Mn-rich layered oxides (LLOs) with a Co-free composition are promising candidates for next-generation cathodes in low-cost and high-energy-density lithium-ion batteries. Despite their potential, the commercialization of Co-free LLOs encounters several electrochemical challenges, such as low activity and initial coulombic efficiency of the first activation cycle and compromised cycle retention, which are primarily attributed to the poor phase integrity between LiTMO and LiMnO domains. In this study, we identified that the compromised phase integrity in Co-free LLOs can be driven by the sticking Ni compositional design, which induces Li-Ni site-exchange defects in the LiTMO domain, leading to severe TMO slab mismatches between phases and resulting in a penalty in enthalpy mixing energy.
View Article and Find Full Text PDFNanomicro Lett
April 2025
Energy harvesting storage hybrid devices have garnered considerable attention as self-rechargeable power sources for wireless and ubiquitous electronics. Triboelectric nanogenerators (TENGs), a common type of energy harvester, generate alternating current-based, irregular short pulses, posing a challenge for storing the generated electrical energy in energy storage systems that typically operate with direct current (DC)-based low-frequency response. In this study, we propose a new strategy that leverages high-frequency response to develop efficient chargeable TENG-supercapacitor (SC) hybrid devices.
View Article and Find Full Text PDFLiFePO (Li-rich LFP) has been proposed as an alternative to address low ionic and electronic conductivity of stoichiometric LiFePO (LFP). However, comprehensive studies investigating the impact of the carbon coating process on crystal structure and electrochemical performance during the synthesis of Li-rich LFP are still lacking. In particular, the characteristics of carbon precursor and calcination atmosphere significantly influence formation of crystal structure and electrochemical properties of the Li-rich LFP, underlining the necessity for further investigation.
View Article and Find Full Text PDFJ Mater Chem A Mater
April 2025
Titanium niobium oxides (TNOs) are attractive anode materials for high power density Li-ion batteries. However, the details of capacity storage in TNOs are not fully understood today as it depends on the Ti and Nb composition and their changes in the oxidation state. This is further complicated by a wide variation in gravimetric capacities reported in the literature for TNO anodes.
View Article and Find Full Text PDFLattice volume changes in Li-ion batteries active materials are unavoidable during electrochemical cycling, posing significant engineering challenges from the particle to the electrode level. In this study, we present an elastic framework coating designed to absorb and reversibly release strain energy associated with particle volume changes, thereby enhancing mechanical resilience at both the particle and electrode levels. This framework, composed of multiwalled carbon nanotubes (MWCNTs), is applied to nickel-rich LiNiCoMnO (NCM9055) cathodes at a low loading of 0.
View Article and Find Full Text PDFMesoporous metal oxides exhibit excellent physicochemical properties and are widely used in various fields, including energy storage/conversion, catalysis, and sensors. Although several soft-template approaches are reported, high-temperature calcination for both metal oxide formation and template removal is necessary, which limits direct synthesis on a plastic substrate for flexible devices. Here, a universal synthetic approach that combines thermal activation and oxygen plasma to synthesize diverse mesoporous metal oxides (VO, VO, TiO, NbO, WO and MoO) at low temperatures (150-200 °C), which can be applicable to a flexible polymeric substrate is introduced.
View Article and Find Full Text PDFHierarchical superstructures have novel shape-dependent properties, but well-defined anisotropic carbon superstructures with controllable size, shape, and building block dimensionality have rarely been accomplished thus far. Here, a hierarchical assembly technique is presented that uses spinodal decomposition (SD) to synthesize anisotropic oblate particles of mesoporous carbon superstructure (o-MCS) with nanorod arrays by integrating block-copolymer (BCP) self-assembly and polymer-polymer interface behaviors in binary blends. The interaction of major and minor phases in binary polymer blends leads to the formation of an anisotropic oblate particle, and the BCP-rich phase enables ordered packing and unidirectional alignment of carbon nanorods.
View Article and Find Full Text PDFTo increase the energy density of lithium-ion batteries (LIBs), high-capacity anodes which alloy with Li ions at a low voltage against Li/Li have been actively pursued. So far, Si has been studied the most extensively because of its high specific capacity and cost efficiency; however, Ge is an interesting alternative. While the theoretical specific capacity of Ge (1600 mAh g) is only half that of Si, its density is more than twice as high (Ge, 5.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2023
The rapid transport of alkali ions in electrodes is a long-time dream for fast-charging batteries. Though electrode nanostructuring has increased the rate-capability, its practical use is limited because of the low tap density and severe irreversible reactions. Therefore, development of a strategy to design fast-charging micron-sized electrodes without nanostructuring is of significant importance.
View Article and Find Full Text PDFIn this study, sodium cobalt fluoride (NaCoF)/reduced graphene oxide (NCF/rGO) nanocomposites were fabricated through a simple one-pot solvothermal process and their electrochemical performance as cathodes for Li-ion batteries (LIBs) was investigated. The NCF nanoclusters (NCs) on the composites (300-500 nm in size) were formed by the assembly of primary nanoparticles (~20 nm), which were then incorporated on the surface of rGO. This morphology provided NCF NCs with a large surface area for efficient ion diffusion and also allowed for close contact with the conductive matrix to promote rapid electron transfer.
View Article and Find Full Text PDFMaterials (Basel)
October 2020
Lithium metal batteries are considered "rough diamonds" in electrochemical energy storage systems. Li-metal anodes have the versatile advantages of high theoretical capacity, low density, and low reaction potential, making them feasible candidates for next-generation battery applications. However, unsolved problems, such as dendritic growths, high reactivity of Li-metal, low Coulombic efficiency, and safety hazards, still exist and hamper the improvement of cell performance and reliability.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
September 2020
Ultrathick battery electrodes are appealing as they reduce the fraction of inactive battery parts such as current collectors and separators. However, thick electrodes are difficult to dry and tend to crack or flake during production. Moreover, the electrochemical performance of thick electrodes is constrained by ion and electron transport as well as fast capacity degradation.
View Article and Find Full Text PDFOff-grid energy storage devices are becoming increasingly important to power distributed applications, such as the Internet of things, and smart city ubiquitous sensor systems. To date, this has been achieved by combining an energy storage device, e.g.
View Article and Find Full Text PDFLithium (Li) metal is a promising anode material for next-generation batteries because of its low standard reduction potential (-3.04 V vs. SHE) and high specific capacity (3860 mA h g-1).
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2020
Herein, we show a facile surfactant-free synthetic platform for the synthesis of nanostructured vanadium pentoxide (VO) using reline as a green and eco-friendly deep eutectic solvent. This new approach overcomes the dependence of the current synthetic methods on shape directing agents such as surfactants with potential detrimental effects on the final applications. Excellent morphological control is achieved by simply varying the water ratio in the reaction leading to the selective formation of VO 3D microbeads, 2D nanosheets, and 1D randomly arranged nanofleece.
View Article and Find Full Text PDFIn this work we show for the first time that a continuous plasma process can synthesize materials from bulk industrial powders to produce hierarchical structures for energy storage applications. The plasma production process's unique advantages are that it is fast, inexpensive, and scalable due to its high energy density that enables low-cost precursors. The synthesized hierarchical material is comprised of iron oxide and aluminum oxide aggregate particles and carbon nanotubes grown in situ from the iron particles.
View Article and Find Full Text PDFThe development of better Li-ion battery (LIB) electrodes requires an orchestrated effort to improve the active materials as well as the electron and ion transport in the electrode. In this paper, iron silicide is studied as an anode material for LIBs because of its higher conductivity and lower volume expansion compared to pure Si particles. In addition, carbon nanotubes (CNTs) can be synthesized from the surface of iron-silicides using a continuous flow coating process where precursors are first spray dried into micrometer-scale secondary particles and are then flown through a chemical vapor deposition (CVD) reactor.
View Article and Find Full Text PDFAn array of amorphous tin oxide (a-SnO) nanohelixes (NHs) was fabricated on copper foil as an electrode for Na-ion batteries via the oblique angle deposition method, a solution- and surfactant-free process. The combination of the amorphous phase SnO with a low oxidation number and its vertically aligned NH geometry with a large surface area and high porosity, which facilitate Na-ion dynamics and accommodate the volume changes, enabled a reversible capacity of up to 915 mA h g after 50 cycles, fast rate capability with 48.1% retention at 2 A g, and high stability, which are superior to those of crystalline nanoparticle-based electrodes.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2019
Lithium-sulfur batteries (LSBs) are cost-effective and high-energy-density batteries. However, the insulating nature of active materials, the shuttle effect, and slow redox kinetics lead to severe capacity decay and low rate capabilities. Numerous multimodal approaches have been attempted to tackle these issues and have pushed the cycle stability and energy density to higher levels.
View Article and Find Full Text PDFThe benefits of nanosize active particles in Li-ion batteries are currently ambiguous. They are acclaimed for enhancing the cyclability of certain electrode materials and for improving rate performance. However, at the same time, nanoparticles are criticized for causing side reactions as well as for their low packing density and, therefore, poor volumetric battery performance.
View Article and Find Full Text PDFPorous architectures are important in determining the performance of lithium-sulfur batteries (LSBs). Among them, multiscale porous architecutures are highly desired to tackle the limitations of single-sized porous architectures, and to combine the advantages of different pore scales. Although a few carbonaceous materials with multiscale porosity are employed in LSBs, their nonpolar surface properties cause the severe dissolution of lithium polysulfides (LiPSs).
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