Synergistic Coupling of Sulfide Electrolyte and Integrated 3D FeS_(2)Electrode Toward Long-Cycling All-Solid-State Lithium Batteries

FeS_(2)cathode is promising for all-solid-state lithium batteries due to its ultra-high capacity,low cost,and environmental friendliness.However,the poor performances,induced by limited electrode-electrolyte interface,severe volume expansion,and polysulfide shuttle,hinder the application of FeS_(2)in all-solid-state lithium batteries.Herein,an integrated 3D FeS_(2)electrode with full infiltration of Li6PS5Cl sulfide electrolytes is designed to address these challenges.Such a 3D integrated design not only achieves intimate and maximized interfacial contact between electrode and sulfide electrolytes,but also effectively buffers the inner volume change of FeS_(2)and completely eliminates the polysulfide shuttle through direct solid-solid conversion of Li2S/S.Besides,the vertical 3D arrays guarantee direct electron transport channels and horizontally shortened ion diffusion paths,endowing the integrated electrode with a remarkably reduced interfacial impedance and enhanced reaction kinetics.Benefiting from these synergies,the integrated all-solid-state lithium battery exhibits the largest reversible capacity(667 mAh g^(-1)),best rate performance,and highest capacity retention of 82%over 500 cycles at 0.1 C compared to both a liquid battery and non-integrated all-solid-state lithium battery.The cycling performance is among the best reported for FeS_(2)-based all-solid-state lithium batteries.This work presents an innovative synergistic strategy for designing long-cycling high-energy all-solid-state lithium batteries,which can be readily applied to other battery systems,such as lithium-sulfur batteries.

High‑Entropy Electrode Materials:Synthesis,Properties and Outlook

High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two decades.The definition of high-entropy materials has continuously evolved.In the last ten years,the discovery of an increasing number of high-entropy materials has led to significant advancements in their utilization in energy storage,electrocatalysis,and related domains,accompanied by a rise in techniques for fabricating high-entropy electrode materials.Recently,the research emphasis has shifted from solely improving the performance of high-entropy materials toward exploring their reaction mechanisms and adopting cleaner preparation approaches.However,the current definition of high-entropy materials remains relatively vague,and the preparation method of high-entropy materials is based on the preparation method of single metal/low-or medium-entropy materials.It should be noted that not all methods applicable to single metal/low-or medium-entropy materials can be directly applied to high-entropy materials.In this review,the definition and development of high-entropy materials are briefly reviewed.Subsequently,the classification of high-entropy electrode materials is presented,followed by a discussion of their applications in energy storage and catalysis from the perspective of synthesis methods.Finally,an evaluation of the advantages and disadvantages of various synthesis methods in the production process of different high-entropy materials is provided,along with a proposal for potential future development directions for high-entropy materials.

Advances in Graphene‑Based Electrode for Triboelectric Nanogenerator

With the continuous development of wearable electronics,wireless sensor networks and other micro-electronic devices,there is an increasingly urgent need for miniature,flexible and efficient nanopower generation technology.Triboelectric nanogenerator(TENG)technology can convert small mechanical energy into electricity,which is expected to address this problem.As the core component of TENG,the choice of electrode materials significantly affects its performance.Traditional metal electrode materials often suffer from problems such as durability,which limits the further application of TENG.Graphene,as a novel electrode material,shows excellent prospects for application in TENG owing to its unique structure and excellent electrical properties.This review systematically summarizes the recent research progress and application prospects of TENGs based on graphene electrodes.Various precision processing methods of graphene electrodes are introduced,and the applications of graphene electrode-based TENGs in various scenarios as well as the enhancement of graphene electrodes for TENG performance are discussed.In addition,the future development of graphene electrode-based TENGs is also prospectively discussed,aiming to promote the continuous advancement of graphene electrode-based TENGs.

Dry electrode technology for scalable and flexible high-energy sulfur cathodes in all-solid-state lithium-sulfur batteries

All-solid-state lithium-sulfur batteries(ASSLSBs)employing sulfide solid electrolytes are one of the most promising next-generation energy storage systems due to their potential for higher energy density and safety.However,scalable fabrication of sheet-type sulfur cathodes with high sulfur loading and excellent performances remains challenging.In this work,sheet-type freestanding sulfur cathodes with high sulfur loading were fabricated by dry electrode technology.The unique fibrous morphologies of polytetrafluoroethylene(PTFE)binders in dry electrodes not only provides excellent mechanical properties but also uncompromised ionic/electronic conductance.Even employed with thickened dry cathodes with high sulfur loading of 2 mg cm^(-2),ASSLSBs still exhibit outstanding rate performance and cycle stability.Moreover,the all-solid-state lithium-sulfur monolayer pouch cells(9.2 m Ah)were also demonstrated and exhibited excellent safety under a harsh test situation.This work verifies the potential of dry electrode technology in the scalable fabrication of thickened sulfur cathodes and will promote the practical applications of ASSLSBs.

Solid electrolyte-electrode interface based on buffer therapy in solid-state lithium batteries

In the past few years,the all-solid lithium battery has attracted worldwide attentions,the ionic conductivity of some all-solid lithium-ion batteries has reached 10^(-3)-10^(-2) S/cm,indicating that the transport of lithium ions in solid electrolytes is no longer a major problem.However,some interface issues become research hotspots.Examples of these interfacial issues include the electrochemical decomposition reaction at the electrode-electrolyte interface;the low effective contact area between the solid electrolyte and the electrode etc.In order to solve the issues,researchers have pursued many different approaches.The addition of a buffer layer between the electrode and the solid electrolyte has been at the center of this endeavor.In this review paper,we provide a systematic summarization of the problems on the electrode-solid electrolyte interface and detailed reflection on the latest works of buffer-based therapies,and the review will end with a personal perspective on the improvement of buffer-based therapies.

Novel Screen-Printed All-Solid-State Copper(II)-Selective Electrode for Mobile Environmental Analysis

Based on poly(vinyl chloride) membranes, a novel miniaturized screen-printed all-solid-state copper(II)-selective electrode has been developed for applications in environmental monitoring. Performance and applicability of the ion-selective electrode (ISE) have been proved by potentiometric investigations. Conducting polymers were used as intermediate layers and as solid contacts between the ion-selective membrane and the graphite transducer. The ion-complexing reagent 2-mercapto-benzoxazole was incorporated into poly(vinyl chloride) membranes. In the concentration range 10-6 - 10-2 mol/L, the ISE exhibited a linear Nernstian potential response to copper(II) with an average slope value of 28 mV/decade. The detection limit was 3 × 10-7 mol/L. The electrode exhibits a short response time (<10 s) and can be used in the range of pH = 3 - 7. Selectivity coefficents against certain interfering ions are investigated. The life time of the electrode under laboratory conditions was approximately 12-month. The electrode was applied in the investigation of different aqueous environmental samples and the electrode characteristics were described. The copper(II) ASS electrode has also successfully been used in potentiometric, complexometric titrations with ethylenediaminetetraacetic acid.

Elucidation of Abnormal Potential Responses of Cation-Selective Electrodes with Solid-State Membranes to Aqueous Solutions of CuCl2 and CdI2

An empirical solution to abnormal potential responses, showing peaks of emf, of commercial Cu2+- and Cd2+-selective electrodes with solid-state membranes was proposed for aqueous solutions of CuCl2 and CdI2. The two-step processes of Mn+ + Yn? (s: solid phase) MY(s) and MY(s) + 2X? X2MY2?(s) (n = 1, 2) at a test solution/electrode-interface were considered as a model. Here, Mn+, Yn?, and X? refer to a divalent or univalent cation, functional groups of electrode materials, and a halide ion (X? = Cl?, Br?, I?), respectively. By applying electrochemical potentials to these processes at n = 2, we derived an equation. Regression analyses based on the equation reproduced well the plots of emf versus log 2(*[M]t) for the Cd(II) and Cu(II) systems: *[M]t denotes a total concentration of species relevant to M2+ in a bulk of the aqueous solution. Also, we obtained log Ks(CdBr2) = 4.28 ? 0.22, log Ks(CdI2) = 6.98 ? 0.05, log Ks(CuCl2) = 3.96 ? 0.09, and log Ks(CuBr2) = 11.4 at 25?C. The magnitude in ?log Ks reflected that in the logarithmic solubility product, log {*[M2+](*[X?])2}, for bulk water, where *[M2+] or *[X?] denotes a molar concentration of the bulk solu-tion of M2+ or X? at equilibrium, respectively. Moreover, a mixture of CuSO4 with NaCl at the molar ratio of 1:1 yielded a plot similar to that of CuCl2.

Developing artificial solid-state interphase for Li metal electrodes:recent advances and perspective

The failure of Li metal anodes can be attributed to their unstable electrode/electrolyte interface,especially the continuous formation of solid electrolyte interphase(SEI)and dendrite growth.To address this challenge,scholars proposed the construction of artificial SEI(ASEI)as a promising strategy.The ASEI mainly homoge-nizes the distribution of Li+,mitigates dendrite growth,facilitates Li+diffusion,and protects the Li metal anode from electrolyte erosion.This review comprehensively summarizes the recent progress in the construction of ASEI layers in terms of their chemical composition.Fundamental understanding of the mechanisms,design principles,and functions of the main components are analyzed.We also propose future research directions to facilitate the in-depth study of ASEI and its practical applications in Li metal batteries.This review offers perspectives that will greatly contribute to the design of practical Li metal electrodes.

Study on a New Type of All-Solid-StateReference Electrode

A new type of all-solid-state Ag/AgCl reference electrode was constructed by using urea-formaldehyde resin as the frame material and KCl powder as the active component. The properties of the electrode were studied in detail. The electrode exhibited excellent characteristics and could be applied to the electrochemical measurements in syrupy, colloidal and higher temperature solutions as a reference electrode.

Preparation of a New Solid-State Molybdenum-Selective Electrode and Application

A new solid state molybdenum-selective electrode has been developed. The electrode is composed of 20% MoS2, 60% Ag2S, and 20% Cu2S. An analytically useful potential change occurred, from 1 × 10-5 to 1 × 10-1 M molybdenum ion. The slope of the linear portion (1 × 10-1 - 1 × 10-5 M) was about 45 ± 2 mV/10-fold concentration changes in molybdenum. It was found that pH change between 1 and 12 had no effect on the potential of the electrode. There was no interference of most common cations such as K+, Na+, Ca2+, Mg2+, Cu2+ and Fe3+ anions such as Cl-, ,? and . The lifetime of the electrode was more than 2 years, when used at least 4 - 5 times a day, and the response time was about 30 s. This electrode has been used for the determination of molybdenum ion in wine using standard addition method. The validation of the electrode has been made with a commercial molybdenum DP polarography and high consistency was obtained.

Hydrogen production from methane and carbon dioxide mixture using all-solid-state electrochemical cell based on a proton-conducting membrane and redox-robust composite electrodes

In recent years, interest in hydrogen as a fuel has sharply increased in the field of alternative and green energy due to its high energy capability and zero-emission behaviour. As a result, research in the development of new highly efficient methods for producing high-purity hydrogen is relevant. This paper presents, for the first time, the test results of an electrochemical cell with a proton-conducting La_(0.9)Sr_(0.1)ScO_(3-δ) electrolyte and symmetrical Sr_(1.95)Fe_(1.4)Ni_(0.1)Mo_(0.5)O_(6-δ)+ La_(0.9)Sr_(0.1)Sc_(0.9)Co_(0.1)O_(3-δ) electrodes as a hybrid setup for electricity generation in proton ceramic fuel cell mode, for hydrogen separation from H_(2)+ Ar mixture and the production of high-purity hydrogen from methane with simultaneous CO_(2) utilization.It was found that this electrochemical cell generates high flow rates of hydrogen during its separation through a proton-conducting membrane from H_(2)+ Ar mixture, about 500 cm^(3)h^(-1)cm^(-2)at a current density of 0.6 A cm^(-2)as well as about 370 cm^(3) h^(-1)cm^(-2)at a current density of 0.5 A cm^(-2) from CH_(4)+ CO_(2) mixture at 800 ℃ which shows that these cells are promising for hydrogen production.

12.6μm-Thick Asymmetric Composite Electrolyte with Superior Interfacial Stability for Solid-State Lithium-Metal Batteries

Solid-state lithium metal batteries(SSLMBs)show great promise in terms of high-energy-density and high-safety performance.However,there is an urgent need to address the compatibility of electrolytes with high-voltage cathodes/Li anodes,and to minimize the electrolyte thickness to achieve highenergy-density of SSLMBs.Herein,we develop an ultrathin(12.6μm)asymmetric composite solid-state electrolyte with ultralight areal density(1.69 mg cm^(−2))for SSLMBs.The electrolyte combining a garnet(LLZO)layer and a metal organic framework(MOF)layer,which are fabricated on both sides of the polyethylene(PE)separator separately by tape casting.The PE separator endows the electrolyte with flexibility and excellent mechanical properties.The LLZO layer on the cathode side ensures high chemical stability at high voltage.The MOF layer on the anode side achieves a stable electric field and uniform Li flux,thus promoting uniform Li^(+)deposition.Thanks to the well-designed structure,the Li symmetric battery exhibits an ultralong cycle life(5000 h),and high-voltage SSLMBs achieve stable cycle performance.The assembled pouch cells provided a gravimetric/volume energy density of 344.0 Wh kg^(−1)/773.1 Wh L^(−1).This simple operation allows for large-scale preparation,and the design concept of ultrathin asymmetric structure also reveals the future development direction of SSLMBs.

Advances in All-Solid-State Lithium-Sulfur Batteries for Commercialization

Solid-state batteries are commonly acknowledged as the forthcoming evolution in energy storage technologies.Recent development progress for these rechargeable batteries has notably accelerated their trajectory toward achieving commercial feasibility.In particular,all-solid-state lithium-sulfur batteries(ASSLSBs)that rely on lithium-sulfur reversible redox processes exhibit immense potential as an energy storage system,surpassing conventional lithium-ion batteries.This can be attributed predominantly to their exceptional energy density,extended operational lifespan,and heightened safety attributes.Despite these advantages,the adoption of ASSLSBs in the commercial sector has been sluggish.To expedite research and development in this particular area,this article provides a thorough review of the current state of ASSLSBs.We delve into an in-depth analysis of the rationale behind transitioning to ASSLSBs,explore the fundamental scientific principles involved,and provide a comprehensive evaluation of the main challenges faced by ASSLSBs.We suggest that future research in this field should prioritize plummeting the presence of inactive substances,adopting electrodes with optimum performance,minimizing interfacial resistance,and designing a scalable fabrication approach to facilitate the commercialization of ASSLSBs.

How Does Stacking Pressure Affect the Performance of Solid Electrolytes and All-Solid-State Lithium Metal Batteries?

All-solid-state lithium metal batteries(ASSLMBs)with solid electrolytes(SEs)have emerged as a promising alternative to liquid electrolyte-based Li-ion batteries due to their higher energy density and safety.However,since ASSLMBs lack the wetting properties of liquid electrolytes,they require stacking pressure to prevent contact loss between electrodes and SEs.Though previous studies showed that stacking pressure could impact certain performance aspects,a comprehensive investigation into the effects of stacking pressure has not been conducted.To address this gap,we utilized the Li_(6)PS_(5)Cl solid electrolyte as a reference and investigated the effects of stacking pressures on the performance of SEs and ASSLMBs.We also developed models to explain the underlying origin of these effects and predict battery performance,such as ionic conductivity and critical current density.Our results demonstrated that an appropriate stacking pressure is necessary to achieve optimal performance,and each step of applying pressure requires a specific pressure value.These findings can help explain discrepancies in the literature and provide guidance to establish standardized testing conditions and reporting benchmarks for ASSLMBs.Overall,this study contributes to the understanding of the impact of stacking pressure on the performance of ASSLMBs and highlights the importance of careful pressure optimization for optimal battery performance.

Implantable probe with integrated reference electrode for in situ neural signal and calcium ion monitoring

Monitoring the electrophysiology activity of neurons and blood calcium signals can enable a better understanding of disease-related neural system circuits.However,currently,in situ calcium ion monitoring tools are scarce and exhibit low integration and limited sensitivity.In this letter,we propose an implantable probe with an integrated in situ Ag/AgCl reference electrode(ISA/ARE)that can monitor action potential(AP)and Ca^(2+) concentrations.

Atom substitution of the solid-state electrolyte Li_(10)GeP_(2)S_(12)for stabilized all-solid-state lithium metal batteries

Solid-state electrolyte Li_(10)GeP_(2)S_(12)(LGPS)has a high lithium ion conductivity of 12 mS cm^(-1)at room temperature,but its inferior chemical stability against lithium metal anode impedes its practical application.Among all solutions,Ge atom substitution of the solid-state electrolyte LGPS stands out as the most promising solution to this interface problem.A systematic screening framework for Ge atom substitution including ionic conductivity,thermodynamic stability,electronic and mechanical properties is utilized to solve it.For fast screening,an enhanced model Dop Net FC using chemical formulas for the dataset is adopted to predict ionic conductivity.Finally,Li_(10)SrP_(2)S_(12)(LSrPS)is screened out,which has high lithium ion conductivity(12.58 mS cm^(-1)).In addition,an enhanced migration of lithium ion across the LSr PS/Li interface is found.Meanwhile,compared to the LGPS/Li interface,LSrPS/Li interface exhibits a larger Schottky barrier(0.134 eV),smaller electron transfer region(3.103?),and enhanced ability to block additional electrons,all of which contribute to the stabilized interface.The applied theoretical atom substitution screening framework with the aid of machine learning can be extended to rapid determination of modified specific material schemes.

A drug-loaded flexible substrate improves the performance of conformal cortical electrodes

Cortical electrodes are a powerful tool for the stimulation and/or recording of electrical activity in the nervous system.However,the inevitable wound caused by surgical implantation of electrodes presents bacterial infection and inflammatory reaction risks associated with foreign body exposure.Moreover,inflammation of the wound area can dramatically worsen in response to bacterial infection.These consequences can not only lead to the failure of cortical electrode implantation but also threaten the lives of patients.Herein,we prepared a hydrogel made of bacterial cellulose(BC),a flexible substrate for cortical electrodes,and further loaded antibiotic tetracycline(TC)and the anti-inflammatory drug dexamethasone(DEX)onto it.The encapsulated drugs can be released from the BC hydrogel and effectively inhibit the growth of Gram-negative and Gram-positive bacteria.Next,therapeutic cortical electrodes were developed by integrating the drug-loaded BC hydrogel and nine-channel serpentine arrays;these were used to record electrocorticography(ECoG)signals in a rat model.Due to the controlled release of TC and DEX from the BC hydrogel substrate,therapeutic cortical electrodes can alleviate or prevent symptoms associated with the bacterial infection and inflammation of brain tissue.This approach facilitates the development of drug delivery electrodes for resolving complications caused by implantable electrodes.

Ionic Liquid-Enhanced Assembly of Nanomaterials for Highly Stable Flexible Transparent Electrodes

The controlled assembly of nanomaterials has demon-strated significant potential in advancing technological devices.However,achieving highly efficient and low-loss assembly technique for nanomate-rials,enabling the creation of hierarchical structures with distinctive func-tionalities,remains a formidable challenge.Here,we present a method for nanomaterial assembly enhanced by ionic liquids,which enables the fabrication of highly stable,flexible,and transparent electrodes featuring an organized layered structure.The utilization of hydrophobic and non-volatile ionic liquids facilitates the production of stable interfaces with water,effectively preventing the sedimentation of 1D/2D nanomaterials assembled at the interface.Furthermore,the interfacially assembled nanomaterial monolayer exhibits an alternate self-climbing behavior,enabling layer-by-layer transfer and the formation of a well-ordered MXene-wrapped silver nanowire network film.The resulting composite film not only demonstrates exceptional photoelectric performance with a sheet resistance of 9.4Ωsq^(-1) and 93%transmittance,but also showcases remarkable environmental stability and mechanical flexibility.Particularly noteworthy is its application in transparent electromagnetic interference shielding materials and triboelectric nanogenerator devices.This research introduces an innovative approach to manufacture and tailor functional devices based on ordered nanomaterials.

In-situ interfacial passivation and self-adaptability synergistically stabilizing all-solid-state lithium metal batteries

The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state batteries.Specifically,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion transport.While the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li deposition.As expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical passivation.For Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 cycles.Additionally,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical performance.The present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.

Flexible,high-density,laminated ECoG electrode array for high spatiotemporal resolution foci diagnostic localization of refractory epilepsy

High spatiotemporal resolution brain electrical signals are critical for basic neuroscience research and high-precision focus diagnostic localization,as the spatial scale of some pathologic signals is at the submillimeter or micrometer level.This entails connecting hundreds or thousands of electrode wires on a limited surface.This study reported a class of flexible,ultrathin,highdensity electrocorticogram(ECoG)electrode arrays.The challenge of a large number of wiring arrangements was overcome by a laminated structure design and processing technology improvement.The flexible,ultrathin,high-density ECoG electrode array was conformably attached to the cortex for reliable,high spatial resolution electrophysiologic recordings.The minimum spacing between electrodes was 15μm,comparable to the diameter of a single neuron.Eight hundred electrodes were prepared with an electrode density of 4444 mm^(-2).In focal epilepsy surgery,the flexible,high-density,laminated ECoG electrode array with 36 electrodes was applied to collect epileptic spike waves inrabbits,improving the positioning accuracy of epilepsy lesions from the centimeter to the submillimeter level.The flexible,high-density,laminated ECoG electrode array has potential clinical applications in intractable epilepsy and other neurologic diseases requiring high-precision electroencephalogram acquisition.