All-solid-state lithium batteries are expected to achieve high energy density but suffer from the issues of lithium dendrite and anodic interfacial reaction. Herein, a lithiophilic-lithiophobic gradient interlayer of lithium-contained alloy/LiF is in situ constructed on a lithium anode by metal trifluoromethanesulfonate (OTf) salt modification. The upper lithiophobic layer is rich in LiF to avoid deposition of lithium on the solid-state electrolyte/lithiophobic layer interface, while the lithiophilic alloy layer induces uniform lithium deposition.
View Article and Find Full Text PDFThe construction of high-quality solid electrolyte interphase (SEI) on Li metal is one of the key strategies to improve the performance of Li metal anodes. Herein, we propose a novel gas-liquid hybrid source plasma technology to construct composite SEI consisting of organic lithium methyl carbonate (LMC) and inorganic lithium nitride (LiN) and lithium oxide (LiO) on the lithium metal. Supported by the theoretical calculation, the inorganic LiN and LiO phases possess low diffusion barrier potentials, favorable for fast Li transportation, and enhanced lithophilicity.
View Article and Find Full Text PDFJ Colloid Interface Sci
September 2025
The interfacial failure of solid polymer electrolytes (SPEs) with Li anode, particularly those containing succinonitrile (SN) types, has significantly hindered the practical development of solid-state lithium-metal batteries. Herein, we introduce silicified montmorillonite (SiO-MMT) into polyethylene oxide (PEO)/SN-based SPEs to facilitate the in-situ formation of a LiF-rich phase, thereby significantly enhancing the electrolyte/Li anode interface stability. Specifically, the SiO-MMT strongly anchors the SN molecules, preventing their migration to the Li anode side.
View Article and Find Full Text PDFIn situHard carbon (HC) is considered to be the most promising anode material for sodium-ion batteries (SIBs) due to the structural diversity, and low cost. However, limited Na transfer kinetics and structural defects lead to low initial Coulombic efficiency (ICE) and poor rate performance (typically <5 A g) of HC anodes. In this work, an interesting morphology-induced strategy is reported to synthesize 2D HC material.
View Article and Find Full Text PDFNon-flammable butanedinitrile (SN) is recognized as a highly prospective plasticizer for significantly reducing the operating temperature of polyethylene oxide (PEO)-based solid polymer electrolytes. However, the instability of the lithium anode interface severely hinders the practical application of PEO/SN-based solid polymer electrolytes in room-temperature solid-state lithium metal batteries. In this work, we propose fast-ion conductive LiLaZrTaO (LLZTO) nanoparticles as corrosion inhibitors to constructure a multifunctional buffer layer on the surface of PEO/SN-based solid electrolyte (PSE@LLZTO) to stabilize the interface structure of Li anode via a facile spin-coating transfer technique.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2025
The development of high-performance all-solid-state lithium-sulfur batteries (ASSLSBs) has garnered considerable attention due to their potential for high energy density and enhanced safety. However, significant challenges such as poor cycling stability, interface incompatibility, and reaction kinetics hinder severely their practical application. In this work, an all-in-one sulfur/cobalt disulfide (S/CoS) composite cathode is proposed by integrating sulfur and homogenized cobalt disulfide (CoS) as the sulfur-based cathode materials with the sulfide solid electrolyte (LiPSCl) through ball milling.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2024
Selenium (Se) serves as a burgeoning high-energy-density cathode material in lithium-ion batteries. However, the development of Se cathode is strictly limited by low Se utilization and inferior cycling stability arising from intrinsic volume expansion and notorious shuttle effect. Herein, a microbial metabolism strategy is developed to prepare "functional vesicle-like" Se globules via Bacillus subtilis subsp.
View Article and Find Full Text PDFSulfide-based all-solid-state lithium batteries (ASSLBs) have attracted unprecedented attention in the past decade due to their excellent safety performance and high energy storage density. However, the sulfide solid-state electrolytes (SSEs) as the core component of ASSLBs have a certain stiffness, which inevitably leads to the formation of pores and cracks during the production process. In addition, although sulfide SSEs have high ionic conductivity, the electrolytes are unstable to lithium metal and have non-negligible electronic conductivity, which severely limits their practical applications.
View Article and Find Full Text PDFAll-solid-state lithium-sulfur batteries (ASSLSBs) have attracted wide attention due to their ultrahigh theoretical energy density and the ability of completely avoiding the shuttle effect. However, the further development of ASSLSBs is limited by the poor kinetic properties of the solid electrode interface. It remains a great challenge to achieve good kinetic properties, by common strategies to substitute sulfur-transition metal and organosulfur composites for sulfur without reducing the specific capacity of ASSLSBs.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2024
ACS Appl Mater Interfaces
July 2023
Lithium (Li) metal is considered as a promising anode candidate for high-energy-density batteries. However, the high reactivity of Li metal leads to poor air stability, limiting its practical application. Additionally, the interfacial instability, such as dendrite growth and an unstable solid electrolyte interphase layer, further complicates its utilization.
View Article and Find Full Text PDFA stable anode-free all-solid-state battery (AF-ASSB) with sulfide-based solid-electrolyte (SE) (argyrodite Li PS Cl) is achieved by tuning wetting of lithium metal on "empty" copper current-collector. Lithiophilic 1 µm Li Te is synthesized by exposing the collector to tellurium vapor, followed by in situ Li activation during the first charge. The Li Te significantly reduces the electrodeposition/electrodissolution overpotentials and improves Coulombic efficiency (CE).
View Article and Find Full Text PDFSelenium-sulfur solid solutions (Se S ) are considered to be a new class of promising cathodic materials for high-performance rechargeable lithium batteries owing to their superior electric conductivity than S and higher theoretical specific capacity than Se. In this work, high-performance Li-Se S batteries employed freestanding cathodes by encapsulating Se S in a N-doped carbon framework with three-dimensional (3D) interconnected porous structure (NC@SWCNTs) are proposed. Se S is uniformly dispersed in 3D porous carbon matrix with the assistance of supercritical CO (SC-CO) technique.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2021
The integration of Li S within a poly(ethylene oxide) (PEO)-based polymer electrolyte is demonstrated to improve the polymer electrolyte's ionic conductivity because the strong interplay between O and Li from Li S reduces the crystalline volume within the PEO. The Li/electrolyte interface is stabilized by the in situ formation of an ultra-thin Li S/Li S layer via the reaction between Li S and lithium metal, which increases the ionic transport at the interface and suppresses lithium dendrite growth. A symmetric Li/Li cell with the Li S -integrated composite electrolyte has excellent cyclability and a high critical current density of 0.
View Article and Find Full Text PDFThe application of flexible, robust, and low-cost solid polymer electrolytes in next-generation all-solid-state lithium metal batteries has been hindered by the low room-temperature ionic conductivity of these electrolytes and the small critical current density of the batteries. Both issues stem from the low mobility of Li ions in the polymer and the fast lithium dendrite growth at the Li metal/electrolyte interface. Herein, Mg(ClO) is demonstrated to be an effective additive in the poly(ethylene oxide) (PEO)-based composite electrolyte to regulate Li ion transport and manipulate the Li metal/electrolyte interfacial performance.
View Article and Find Full Text PDFEnviron Sci Technol
February 2020
Development of low-cost, high-efficiency, and environmentally benign adsorbents for mercury removal is of significant importance for environmental remediation. Herein, we report a novel porous puffed rice carbon (PRC) with co-implanted metal iron and sulfur, forming a high-quality PRC/Fe@S composite as a high-efficiency adsorbent for mercury removal from aqueous solution. The in situ-formed Fe nanoparticles in PRC are strongly coupled with sulfur via a supercritical CO fluid approach and dispersed homogeneously in the cross-linked hierarchical porous architecture.
View Article and Find Full Text PDFTransition metal carbides and/or nitrides (MXenes), a burgeoning group of 2 D layer-structure compounds, have multiple merits, such as high electrical conductivity, tunable layer structure, small band gap, and functionalized redox-active surface, and are receiving significant attention as one of the most promising class of energy storage materials. The synthesis methods, structural configuration, and surface chemistry of MXenes directly influence their performance. This Minireview focuses on interfacial structure design and functionalization of MXenes and MXene-based energy storage materials and the effect of structural configuration and surface chemistry on their electrochemical performance.
View Article and Find Full Text PDFSilicon oxycarbides (SiOC) are regarded as potential anode materials for lithium-ion batteries, although inferior cycling stability and rate performance greatly limit their practical applications. Herein, amorphous SiOC is synthesized from Chlorella by means of a biotemplate method based on supercritical fluid technology. On this basis, tin particles with sizes of several nanometers are introduced into the SiOC matrix through the biosorption feature of Chlorella.
View Article and Find Full Text PDFACS Appl Mater Interfaces
July 2017
Lithium-sulfur (Li-S) battery is one of the most attractive candidates for the next-generation energy storage system. However, the intrinsic insulating nature of sulfur and the notorious polysulfide shuttle are the major obstacles, which hinder the commercial application of Li-S battery. Confining sulfur into conductive porous carbon matrices with designed polarized surfaces is regarded as a promising and effective strategy to overcome above issues.
View Article and Find Full Text PDF