Despite extensive investigation on the lattice oxygen redox (LOR) in Li-rich cathodes, significant challenges remain in utilizing LOR activity without compromising structural and electrochemical stability. Related breakthroughs are hindered by the lack of understanding regarding how different LOR activity influences the structural evolution and electrochemical stability, and what is the optimal LOR activity. Herein, the degree of LOR activity is successfully regulated from 22% to 92% in Co-free Li-rich cathodes (LiMnNiO) by controlling local chemical disorder, and the relationship between LOR activity and cycling stability is revealed.
View Article and Find Full Text PDFSolid-state lithium batteries have advantages of high energy density and usage safety and are considered as promising next-generation power sources. Among them, the garnet-type oxide electrolyte has become a widely studied inorganic electrolyte due to its high ionic conductivity and chemical stability. In this paper, nanoscale YO (NYO) particles are introduced as sintering aids for fabricating Ta-doped LiLaZrO (LLZTO) ceramics, and the sintering effects of various NYO ratios on the properties of LLZTO are investigated.
View Article and Find Full Text PDFJ Colloid Interface Sci
November 2024
Binary superparticles formed by self-assembling two different types of nanoparticles may utilize the synergistic interactions and create advanced multifunctional materials. Bi-magnetic superparticles with a core-shell structure have unique properties due to their specific spatial configurations. Herein, we built MnO@Ni core-shell binary superparticles via an emulsion self-assembly technique.
View Article and Find Full Text PDFJ Colloid Interface Sci
September 2024
Sodium (Na) metal anodes receive significant attention due to their high theoretical specific energy and cost-effectiveness. However, the high reactivity of Na foil anodes and the irregular surfaces have posed challenges to the operability and reliability of Na metals in battery applications. In the absence of inert environmental protection conditions, constructing a uniform, dense, and sodiophilic Na metal anode surface is crucial for homogenizing Na deposition, but remains less-explored.
View Article and Find Full Text PDFAll-solid-state thin-film lithium batteries (TFBs) with high voltage are crucial for powering microelectronics systems. However, the issues of interfacial instability and poor solid contact of cathode/electrolyte films have limited their application. In this work, the preferentially orientated LiCoO (LCO) nanocolumns and the LCO/LiPON/Li TFBs are fabricated by in situ heating sputtering.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2024
High electrochemical reversibility is required for the application of high-energy-density lithium (Li) metal batteries; however, inactive Li formation and SEI (solid electrolyte interface)-instability-induced electrolyte consumption cause low Coulombic efficiency (CE). The prior interfacial chemical designs in terms of alloying kinetics have been used to enhance the CE of Li metal anode; however, the role of its redox chemistry at heterointerfaces remains a mystery. Herein, the relationship between heterointerfacial redox chemistry and electrochemical transformation reversibility is investigated.
View Article and Find Full Text PDFHigh-capacity Li-rich layered oxides (LLOs) suffer from severe structure degradation due to the utilization of hybrid anion- and cation-redox activity. The native post-cycled structure, composed of progressively densified defective spinel layer (DSL) and intrinsic cations mixing, is deemed as the hindrance of the rapid and reversible de/intercalation of Li . Herein, the artificial post-cycled structure consisting of artificial DSL and inner cations mixing is in situ constructed, which would act as a shield against the irreversible oxygen emission and undesirable transition metal migration by suppressing anion redox activity and modulating cation mixing.
View Article and Find Full Text PDFThe commercial viability of lithium-sulfur batteries is still challenged by the notorious lithium polysulfides (LiPSs) shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode. Herein, a bi-service host with Co-Fe binary-metal selenide quantum dots embedded in three-dimensional inverse opal structured nitrogen-doped carbon skeleton (3DIO FCSe-QDs@NC) is elaborately designed for both sulfur cathode and Li metal anode. The highly dispersed FCSe-QDs with superb adsorptive-catalytic properties can effectively immobilize the soluble LiPSs and improve diffusion-conversion kinetics to mitigate the polysulfide-shutting behaviors.
View Article and Find Full Text PDFJ Chromatogr B Analyt Technol Biomed Life Sci
March 2023
A monolithic solid-phase extraction (SPE) cartridge packed with a composite adsorbent was fabricated via polymerization using dodecene as the monomer with the porous organic cage (POC) material doped, combing with an analytical column through a high-performance liquid chromatography (HPLC) instrument, which was used for the online extraction and separation of 23-acetyl alismol C, atractylodes lactone II and atractylodes lactone III from Zexie Decoction. The POC-doped adsorbent shows porous structure with a relatively high specific surface area of 85.50 m/g, which was obtained from the characterizations of a scanning electron microscope and an automatic surface area and porosity analyser.
View Article and Find Full Text PDFThe construction of a protective layer for stabilizing anion redox reaction is the key to obtaining long cycling stability for Li-rich Mn-based cathode materials. However, the protection of the exposed surface/interface of the primary particles inside the secondary particles is usually ignored and difficult, let alone the investigation of the impact of the surface engineering of the internal primary particles on the cycling stability. In this work, an efficient method to regulate cycling stability is proposed by simply adjusting the distribution state of the boron nickel complexes coating layer.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
March 2023
Passivation of stainless steel by additives forming mass-transport blocking layers is widely practiced, where Cr element is added into bulk Fe-C forming the Cr O -rich protective layer. Here we extend the long-practiced passivation concept to Si anodes for lithium-ion batteries, incorporating the passivator of LiF/Li CO into bulk Si. The passivation mechanism is studied by various ex situ characterizations, redox peak contour maps, thickness evolution tests, and finite element simulations.
View Article and Find Full Text PDFThe high capacity of Li-rich and Mn-based (LRM) cathode materials is originally due to the unique hybrid anion- and cation redox, which also induces detrimental oxygen escape. Furthermore, the counter diffusion of released oxygen (into electrolyte) and induced oxygen vacancies (into the interior bulk phase) that occurs at the interface will cause uncontrolled phase collapse and other issues. Therefore, due to its higher working voltage (>4.
View Article and Find Full Text PDFMetal-sulfur batteries exhibit great potential as next-generation rechargeable batteries due to the low sulfur cost and high theoretical energy density. Sodium-sulfur (Na-S) batteries present higher feasibility of long-term development than lithium-sulfur (Li-S) batteries in technoeconomic and geopolitical terms. Both lithium and sodium are alkali metal elements with body-centered cubic structures, leading to similar physical and chemical properties and exposing similar issues when employed as the anode in metal-sulfur batteries.
View Article and Find Full Text PDFLithium-sulfur (Li-S) batteries are regarded as the most promising next-generation energy storage systems due to their high energy density and cost-effectiveness. However, their practical applications are seriously hindered by several inevitable drawbacks, especially the shuttle effects of soluble lithium polysulfides (LiPSs) which lead to rapid capacity decay and short cycling lifespan. This review specifically concentrates on the shuttle path of LiPSs and their interaction with the corresponding cell components along the moving way, systematically retrospect the recent advances and strategies toward polysulfides diffusion suppression.
View Article and Find Full Text PDFLithium cobalt oxide (LCO) is the most widely used cathode materials in electronic devices due to the high working potential and dense tap density, but the performance is limited by the unstable interfaces at high potential. Herein, LiF thin film is sputtered on the surface of LCO electrodes for enhancing the electrochemical performance and reducing the voltage polarization. The polarization components are discussed and quantified by analyzing the relationship between electrochemical polarization and charger transfer resistance, as well as that between concentration polarization and Li-ion diffusion coefficients.
View Article and Find Full Text PDFA solid-phase extraction cartridge was fabricated using diallyl isophthalate as the monomer with the addition of porous organic cage material via in situ free-radical polymerization in a stainless-steel column. The resulting monolithic adsorbent exhibited a relatively uniform porous structure, a high specific surface area of 113.98 m /g, and multiple functional chemical groups according to the characterization results.
View Article and Find Full Text PDFThere are plenty of issues need to be solved before the practical application of Li- and Mn-rich cathodes, including the detrimental voltage decay and mediocre rate capability, etc. Element doping can effectively solve the above problems, but cause the loss of capacity. The introduction of appropriate defects can compensate the capacity loss; however, it will lead to structural mismatch and stress accumulation.
View Article and Find Full Text PDFLi-rich cathode materials have attracted increasing attention because of their high reversible discharge capacity (>250 mA h g ), which originates from transition metal (TM) ion redox reactions and unconventional oxygen anion redox reactions. However, many issues need to be addressed before their practical applications, such as their low kinetic properties and inefficient voltage fading. The development of cutting-edge technologies has led to cognitive advances in theory and offer potential solutions to these problems.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2021
Lithium-rich manganese-based (LRM) layered oxides are considered as one of the most promising cathode materials for next-generation high-energy-density lithium-ion batteries (LIBs) because of their high specific capacity (>250 mAh g). However, they also go through severe capacity decay, serious voltage fading, and poor rate capability during cycling. Herein, a multiscale deficiency integration, including surface coating, subsurface defect construction, and bulk doping, is realized in a LiMnNiCoO cathode material by facile Na-rich engineering through a sol-gel method.
View Article and Find Full Text PDFCombining MoSe with other transition metal dichalcogenides to form a hybrid nanostructure is an effective route to enhance the electrocatalytic activities for hydrogen evolution reaction (HER). In this study, MoSe-NiSe hybrid nanoelectrocatalysts with a flower-like morphology are synthesized by a seed-induced solution approach. Instead of independently nucleating to form separate nanocrystals, the NiSe component tends to nucleate and grow on the surfaces of ultrathin nanoflakes of MoSe to form a hybrid nanostructure.
View Article and Find Full Text PDF