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.

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.

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.

A dynamic database of solid-state electrolyte(DDSE)picturing all-solid-state batteries

All-solid-state batteries(ASSBs)are a class of safer and higher-energy-density materials compared to conventional devices,from which solid-state electrolytes(SSEs)are their essential components.To date,investigations to search for high ion-conducting solid-state electrolytes have attracted broad concern.However,obtaining SSEs with high ionic conductivity is challenging due to the complex structural information and the less-explored structure-performance relationship.To provide a solution to these challenges,developing a database containing typical SSEs from available experimental reports would be a new avenue to understand the structureperformance relationships and find out new design guidelines for reasonable SSEs.Herein,a dynamic experimental database containing>600 materials was developed in a wide range of temperatures(132.40–1261.60 K),including mono-and divalent cations(e.g.,Li^(+),Na^(+),K^(+),Ag^(+),Ca^(2+),Mg^(2+),and Zn^(2+))and various types of anions(e.g.,halide,hydride,sulfide,and oxide).Data-mining was conducted to explore the relationships among different variates(e.g.,transport ion,composition,activation energy,and conductivity).Overall,we expect that this database can provide essential guidelines for the design and development of high-performance SSEs in ASSB applications.This database is dynamically updated,which can be accessed via our open-source online system.

Design strategies and recent advancements of solid-state supercapacitor operating in wide temperature range

Solid-state supercapacitors(SSCs)are emerging as one of the promising energy storage devices due to their high safety,superior power density,and excellent cycling life.However,performance degradation and safety issues under extreme conditions are the main challenges for the practical application.With the expansion of human activities,such as space missions,polar exploration,and so on,the investigation of SSC with wide temperature tolerance,high energy density,power density,and sustainability is highly desired.In this review,the effects of temperature on SSC are systematically illustrated and clarified,including the properties of the electrolyte,ion diffusion,and reaction dynamics of the supercapacitor.Subsequently,we summarize the recent advances in wide-temperature-range SSCs from the aspect of electrolyte modification,electrode design,and interface adjustment between electrode and electrolyte,especially with critical concerns on ionic conductivity and cycling stability.In the end,a perspective is presented,expecting to promote the practical application of the SSC in harsh conditions.

SEI/dead Li-turning capacity loss for high-performance anode-free solid-state lithium batteries

Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal batteries.However,the unclear mechanism for the fast capacity decay in AF-SSLBs,either determined by dead Li or solid electrolyte interface(SEI),limits the proposal of effective strategies to prolong cycling life.To clarify the underlying mechanism,herein,the evolution of SEI and dead Li is quantitatively analyzed by a solid-state nuclear magnetic resonance(ss-NMR)technology in a typical LiPF6-based polymer electrolyte.The results show that the initial capacity loss is attributed to the formation of SEI,while the dead Li dominates the following capacity loss and the growth rate is 0.141 mA h cm^(−2)cycle−1.To reduce the active Li loss,the combination of inorganic-rich SEI and self-healing electrostatic shield effect is proposed to improve the reversibility of Li deposition/dissolution behavior,which reduces the capacity loss rate for the initial SEI and following dead Li generation by 2.3 and 20.1 folds,respectively.As a result,the initial Coulombic efficiency(ICE)and stable CE increase by 15.1%and 15.3%in Li-Cu cells,which guides the rational design of high-performance AF-SSLBs.

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.

A Review on Engineering Design for Enhancing Interfacial Contact in Solid-State Lithium–Sulfur Batteries

The utilization of solid-state electrolytes(SSEs)presents a promising solution to the issues of safety concern and shuttle effect in Li–S batteries,which has garnered significant interest recently.However,the high interfacial impedances existing between the SSEs and the electrodes(both lithium anodes and sulfur cathodes)hinder the charge transfer and intensify the uneven deposition of lithium,which ultimately result in insufficient capacity utilization and poor cycling stability.Hence,the reduction of interfacial resistance between SSEs and electrodes is of paramount importance in the pursuit of efficacious solid-state batteries.In this review,we focus on the experimental strategies employed to enhance the interfacial contact between SSEs and electrodes,and summarize recent progresses of their applications in solidstate Li–S batteries.Moreover,the challenges and perspectives of rational interfacial design in practical solid-state Li–S batteries are outlined as well.We expect that this review will provide new insights into the further technique development and practical applications of solid-state lithium batteries.

A Novel Framework to Construct S-Box Quantum Circuits Using System Modeling: Application to 4-Bit S-Boxes

Quantum computers accelerate many algorithms based on the superposition principle of quantum mechanics.The Grover algorithm provides significant performance to malicious users attacking symmetric key systems.Since the performance of attacks using quantum computers depends on the efficiency of the quantum circuit of the encryption algorithms,research research on the implementation of quantum circuits is essential.This paper presents a new framework to construct quantum circuits of substitution boxes(S-boxes)using system modeling.We model the quantum circuits of S-boxes using two layers:Toffoli and linear layers.We generate vector spaces based on the values of qubits used in the linear layers and apply them to find quantum circuits.The framework finds the circuit bymatching elements of vector spaces generated fromthe input and output of a given S-box,using the forward search or themeet-in-the-middle strategy.We developed a tool to apply this framework to 4-bit S-boxes.While the 4-bit S-box quantum circuit construction tool LIGHTER-R only finds circuits that can be implemented with four qubits,the proposed tool achieves the circuits with five qubits.The proposed tool can find quantum circuits of 4-bit odd permutations based on the controlled NOT,NOT,and Toffoli gates,whereas LIGHTER-R is unable to perform this task in the same environment.We expect this technique to become a critical step toward optimizing S-box quantum circuits.

MET receptor tyrosine kinase promotes the generation of functional synapses in adult cortical circuits

Loss of synapse and functional connectivity in brain circuits is associated with aging and neurodegeneration,however,few molecular mechanisms are known to intrinsically promote synaptogenesis or enhance synapse function.We have previously shown that MET receptor tyrosine kinase in the developing cortical circuits promotes dendritic growth and dendritic spine morphogenesis.To investigate whether enhancing MET in adult cortex has synapse regenerating potential,we created a knockin mouse line,in which the human MET gene expression and signaling can be turned on in adult(10–12 months)cortical neurons through doxycycline-containing chow.We found that similar to the developing brain,turning on MET signaling in the adult cortex activates small GTPases and increases spine density in prefrontal projection neurons.These findings are further corroborated by increased synaptic activity and transient generation of immature silent synapses.Prolonged MET signaling resulted in an increasedα-amino-3-hydroxy-5-methyl-4-isoxazolepropionic acid/N-methyl-Daspartate(AMPA/NMDA)receptor current ratio,indicative of enhanced synaptic function and connectivity.Our data reveal that enhancing MET signaling could be an interventional approach to promote synaptogenesis and preserve functional connectivity in the adult brain.These findings may have implications for regenerative therapy in aging and neurodegeneration conditions.

Nullors, and Nullor Circuits;There Applications in Symbolic Circuit Analysis and Design

The objective in this presentation is to introduce some of the unique properties and applications of nullors in active circuit analysis and designs. The emphasis is to discuss the role nullors can play in symbolic representation of transfer functions. To show this we adopt the topological platform for the circuit analysis and use a recently developed Admittance Method (AM) to achieve the Sum of Tree Products (STP), replacing the determinant and cofactors of the Nodal Admittance Matrix (NAM) of the circuit. To construct a transfer function, we start with a given active circuit and convert all its controlled sources and I/O-ports to nullors. Now, with a solid nullor circuit (passive elements and nullors) we first eliminate the passive elements through AM operations. This produces the STPs. Second, the all-nullor circuit is then used to find the signs or the STPs. Finally, the transfer function (in symbolic, if chosen) is obtained from the ratio between the STPs.

Lithiophilic Li-Si alloy-solid electrolyte interface enabled by high-concentration dual salt-reinforced quasi-solid-state electrolyte

Solid polymer electrolytes(SPEs)are urgently required to achieve practical solid-state lithium metal batteries(LMBs)and lithium-ion batteries(LIBs),Herein,we proposed a mechanism for modulating interfacial conduction and anode interfaces in high-concentration SPEs by LiDFBOP.Optimized electrolyte exhibits superior ionic conductivity and remarkable interface compatibility with salt-rich clusters:(1)polymer-plastic crystal electrolyte(P-PCE,TPU-SN matrix)dissociates ion pairs to facilitate Li+transport in the electrolyte and regulates Li^(+)diffusion in the SEI.The crosslinking structure of the matrix compensates for the loss of mechanical strength at high-salt concentrations;(2)dual-anion TFSI^(-)_(n)-DFBOP^(-)_(m)in the Li^(+)solvation sheath facilitates facile Li^(+)desolvation and formation of salt-rich clusters and is conducive to the formation of Li conductive segments of TPU-SN matrix;(3)theoretical calculations indicate that the decomposition products of LiDFBOP form SEI with lower binding energy with LiF in the SN system,thereby enhancing the interfacial electrochemical redox kinetics of SPE and creating a solid interface SEI layer rich in LiF.As a result,the optimized electrolyte exhibits an excellent ionic conductivity of9.31×10^(-4)S cm^(-1)at 30℃and a broadened electrochemical stability up to 4.73 V.The designed electrolyte effectively prevents the formation of Li dendrites in Li symmetric cells for over 6500 h at0.1 mA cm^(-2).The specific Li-Si alloy-solid state half-cell capacity shows 711.6 mAh g^(-1)after 60 cycles at 0.3 A g^(-1).Excellent rate performance and cycling stability are achieved for these solid-state batteries with Li-Si alloy anodes and NCM 811 cathodes.NCM 811‖Prelithiated silicon-based anode solid-state cell delivers a discharge capacity of 195.55 mAh g^(-1)and a capacity retention of 97.8%after 120 cycles.NCM 811‖Li solid-state cell also delivers capacity retention of 84.2%after 450 cycles.

In-situ deposited anti-aging TiN capping layer for Nb superconducting quantum circuits

The performance of Nb superconducting quantum devices is predominantly limited by dielectric loss at the metal–air interface,where Nb2O5 is considered the main loss source.Here,we suppress the formation of native oxides by in-situ deposition of a TiN capping layer on the Nb film.With TiN capping layers,no Nb2O5 forms on the surface of the Nb film.The quality factor Qi of the Nb resonator increases from 5.6×10^(5) to 7.9×10^(5) at low input power and from 6.8×10^(6) to 1.1×10^(7)at high input power.Furthermore,the TiN capping layer also shows good aging resistance in Nb resonator devices,with no significant performance fluctuations after one month of aging.These findings highlight the effectiveness of TiN capping layers in enhancing the performance and longevity of Nb superconducting quantum devices.

Correction of microwave pulse reflection by digital filters in superconducting quantum circuits

Reducing the control error is vital for high-fidelity digital and analog quantum operations.In superconducting circuits,one disagreeable error arises from the reflection of microwave signals due to impedance mismatch in the control chain.Here,we demonstrate a reflection cancelation method when considering that there are two reflection nodes on the control line.We propose to generate the pre-distortion pulse by passing the envelopes of the microwave signal through digital filters,which enables real-time reflection correction when integrated into the field-programmable gate array(FPGA).We achieve a reduction of single-qubit gate infidelity from 0.67%to 0.11%after eliminating microwave reflection.Real-time correction of microwave reflection paves the way for precise control and manipulation of the qubit state and would ultimately enhance the performance of algorithms and simulations executed on quantum processors.

Interplay between topology and localization on superconducting circuits

Topological insulators occupy a prominent position in the realm of condensed matter physics. Nevertheless, the presence of strong disorder has the potential to disrupt the integrity of topological states, leading to the localization of all states.This study delves into the intricate interplay between topology and localization within the one-dimensional Su–Schrieffer–Heeger(SSH) model, which incorporates controllable off-diagonal quasi-periodic modulations on superconducting circuits.Through the application of external alternating current(ac) magnetic fluxes, each transmon undergoes controlled driving,enabling independent tuning of all coupling strengths. Within a framework of this model, we construct comprehensive phase diagrams delineating regions characterized by extended topologically nontrivial states, critical localization, and coexisting topological and critical localization phases. The paper also addresses the dynamics of qubit excitations, elucidating distinct quantum state transfers resulting from the intricate interplay between topology and localization. Additionally, we propose a method for detecting diverse quantum phases utilizing existing experimental setups.

A gel polymer electrolyte based on IL@NH_(2)-MIL-53(Al)for high-performance all-solid-state lithium metal batteries

Solid polymer composite electrolytes possess the benefits of superior compatibility with electrodes and good thermal characteristics for more secure energy storage equipment.Herein,a new gel polymer electrolyte(GPE)containing NH_(2)-MIL-53(Al),[PP_(13)][TFSI],LiTFSI,and PVDF-HFP was prepared using a simple method of solution casting.The effects of encapsulating different ratios of ionic liquid([PP_(13)][TFSI])into the micropores of functionalized metal-organic frameworks(NH_(2)-MIL-53(Al))on the electrochemical properties were compared.XRD,SEM,nitrogen adsorption-desorption isotherms,and electrochemical measurements were conducted.This GPE demonstrates a superior ionic conductivity of 8.08×10^(-4)S·cm^(-1)at 60℃and can sustain a discharge specific capacity of 156.6 mA·h·g^(-1)at 0.2 C for over 100 cycles.This work might offer a potential approach to alleviate the solid-solid contact with the solid-state electrolyte and electrodes and broaden a new window for the creation of all-solid-state batteries.

Structural analysis of silk using solid-state NMR

Silkworms and spiders are capable of generating fibers that are both highly durable and elastic in a short span of time,using a silk solution stored within their bodies at room temperature and normal atmospheric pressure.The dragline silk fiber,which is essentially a spider's lifeline,surpasses the strength of a steel wire of equivalent thickness.Regrettably,humans have yet to replicate this process to produce fibers with similar high strength and elasticity in an eco-friendly manner.Therefore,it is of utmost importance to thoroughly comprehend the extraordinary structure and fibrillation mechanism of silk,and leverage this understanding in the manufacturing of high-strength,high-elasticity fibers.This review will delve into the recent progress in comprehending the structure of silks derived from silkworms and spiders,emphasizing the distinctive attributes of solidstate NMR.

Enhanced High-Temperature Cycling Stability of Garnet-Based All Solid-State Lithium Battery Using a Multi-Functional Catholyte Buffer Layer

The pursuit of safer and high-performance lithium-ion batteries(LIBs)has triggered extensive research activities on solid-state batteries,while challenges related to the unstable electrode-electrolyte interface hinder their practical implementation.Polymer has been used extensively to improve the cathode-electrolyte interface in garnet-based all-solid-state LIBs(ASSLBs),while it introduces new concerns about thermal stability.In this study,we propose the incorporation of a multi-functional flame-retardant triphenyl phos-phate additive into poly(ethylene oxide),acting as a thin buffer layer between LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode and garnet electro-lyte.Through electrochemical stability tests,cycling performance evaluations,interfacial thermal stability analysis and flammability tests,improved thermal stability(capacity retention of 98.5%after 100 cycles at 60℃,and 89.6%after 50 cycles at 80℃)and safety characteristics(safe and stable cycling up to 100℃)are demonstrated.Based on various materials characterizations,the mechanism for the improved thermal stability of the interface is proposed.The results highlight the potential of multi-functional flame-retardant additives to address the challenges associated with the electrode-electrolyte interface in ASSLBs at high temperature.Efficient thermal modification in ASSLBs operating at elevated temperatures is also essential for enabling large-scale energy storage with safety being the primary concern.

Green recycling of short-circuited garnet-type electrolyte for high-performance solid-state lithium batteries

Solid-state lithium batteries(SSLBs)solve safety issues and are potentially energy-dense alternatives to next-generation energy storage systems.Battery green recycling routes are responsible for the widespread use of SSLBs due to minimizing environmental contamination,reducing production costs,and providing a sustainable solution for resources,e.g.,saving rare earth elements(La,Ta,etc.).Herein,a solid-state recycling strategy is proposed to achieve green recycling of the crucial component solidstate electrolytes(SSEs)in spent SSLBs.The short-circuited garnet Li_(6.5)La_(3)Zr_(1.5)Ta_(0.5)O_(12)(LLZTO)is broken into fine particles and mixed with fresh particles to improve sintering activity and achieve high packing density.The continuous Li absorption process promotes sufficient grain fusion and guarantees the transformation from tetragonal phase to pure cubic phase for high-performance recycled LLZTO.The Li-ion conductivity reaches 5.80×10^(-4)S cm-1with a relative density of 95.9%.Symmetric Li cell with asrecycled LLZTO shows long-term cycling stability for 700 h at 0.3 mA cm^(-2)without any voltage hysteresis.Full cell exhibits an excellent cycling performance with a discharge capacity of 141.5 mA h g^(-1)and a capacity retention of 92.1%after 400 cycles(0.2C).This work develops an environmentally friendly and economically controllable strategy to recycle SSE from spent SSLBs,guiding future directions of SSLBs large-scale industrial application and green recycling study.

Recent advances in solving Li_(2)CO_(3) problems in garnet-based solid-state battery: A systematic review(2020-2023)

Garnet solid electrolytes are one of the most promising electrolytes for solid-state batteries.However,Li_(2)CO_(3) is a critical issue that hinders the practical application of garnet-based solid-state lithium-ion batteries.There are two sources of Li_(2)CO_(3) contamination.The main one is the aging of garnet electrolytes in the atmosphere.Garnet electrolytes can react with H_(2)O and CO_(2) in the air to form Li_(2)CO_(3),which reduces ion conductivity,increases electrode/garnet electrolyte interface resistance,and deteriorates the electrochemical performance of the battery.Various strategies,such as elemental doping,grain boundary manipulation,and interface engineering,have been suggested to address these issues.The other is the passivation layer(Li_(2)CO_(3),Li_3N,LiOH,Li_(2)O) formed on the surface of the lithium foil after long-term storage,which is ignored by most researchers.To better understand the current strategies and future trends to address the Li_(2)CO_(3) problem,this perspective provides a systematic review of journals published in this field from 2020-2023.