We have developed a superhydrophobic and corrosion-resistant LDH-W/PFDTMS composite coating on the surface of Mg alloy.This composite comprised a tungstate-intercalated(LDH-W)underlayer that was grown at low temperatu...We have developed a superhydrophobic and corrosion-resistant LDH-W/PFDTMS composite coating on the surface of Mg alloy.This composite comprised a tungstate-intercalated(LDH-W)underlayer that was grown at low temperature(relative to hydrothermal reaction conditions)under atmospheric pressure and an outer polysiloxane layer created from a solution containing perfluorodecyltrimethoxysilane(PFDTMS)using a simple immersion method.The successful intercalation of tungstate into the LDH phase and the following formation of the polysiloxane layer were confirmed through X-ray diffraction(XRD),Fourier transform infrared(FTIR)spectroscopy,and X-ray photoelectron spectroscopy(XPS).The corrosion resistance of the LDH-W film,both before and after the PFDTMS modification,was evaluated using electrochemical impedance spectroscopy(EIS),Tafel curves,and immersion experiments.The results showed that Mg coated with LDH-W/PFDTMS exhibited significantly enhanced corrosion protection compared to the unmodified LDHW film,with no apparent signs of corrosion after exposure to 3.5wt%NaCl solution for 15 d.Furthermore,the LDH-W/PFDTMS coating demonstrated superior superhydrophobicity and self-cleaning properties against water and several common beverages,as confirmed by static contact angle and water-repellency tests.These results offer valuable insights into preparing superhydrophobic and corrosion-resistant LDH-based composite coatings on Mg alloy surfaces under relatively mild reaction conditions.展开更多
Sodium-ion batteries hold great promise as next-generation energy storage systems.However,the high instability of the electrode/electrolyte interphase during cycling has seriously hindered the development of SIBs.In p...Sodium-ion batteries hold great promise as next-generation energy storage systems.However,the high instability of the electrode/electrolyte interphase during cycling has seriously hindered the development of SIBs.In particular,an unstable cathode–electrolyte interphase(CEI)leads to successive electrolyte side reactions,transition metal leaching and rapid capacity decay,which tends to be exacerbated under high-voltage conditions.Therefore,constructing dense and stable CEIs are crucial for high-performance SIBs.This work reports localized high-concentration electrolyte by incorporating a highly oxidation-resistant sulfolane solvent with non-solvent diluent 1H,1H,5H-octafluoropentyl-1,1,2,2-tetrafluoroethyl ether,which exhibited excellent oxidative stability and was able to form thin,dense and homogeneous CEI.The excellent CEI enabled the O3-type layered oxide cathode NaNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2)(NaNMF)to achieve stable cycling,with a capacity retention of 79.48%after 300 cycles at 1 C and 81.15%after 400 cycles at 2 C with a high charging voltage of 4.2 V.In addition,its nonflammable nature enhances the safety of SIBs.This work provides a viable pathway for the application of sulfolane-based electrolytes on SIBs and the design of next-generation high-voltage electrolytes.展开更多
Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the ...Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the Jahn-Teller(JT)effect associated with Mn-ion,the cathode exhibits poor structural stability.Herein,we propose a strategy to enhance structural stability by introducing robust metal-oxygen(M-O)bonds,which can realize the pinning effect to constrain the distortion in the transition metal(TM)layer.Concurrently,all the elements employed have exceptionally high crustal abundance.As a proof of concept,the designed K_(0.5)Mn_(0.9)Mg_(0.025)Ti_(0.025)Al_(0.05)O_(2)cathode exhibited a discharge capacity of approximately 100 mA h g^(-1)at 20 mA g^(-1)with 79%capacity retention over 50 cycles,and 73%capacity retention over 200 cycles at 200 mA g^(-1),showcased much better battery performance than the designed cathode with less robust M-O bonds.The properties of the formed M-O bonds were investigated using theoretical calculations.The enhanced dynamics,mitigated JT effect,and improved structural stability were elucidated through the in-situ X-ray diffractometer(XRD),in-situ electrochemical impedance spectroscopy(EIS)(and distribution of relaxation times(DRT)method),and ex-situ X-ray absorption fine structure(XAFS)tests.This study holds substantial reference value for the future design of costeffective Mn-based layered cathodes for PIBs.展开更多
Rock slopes with large intersection angles between the strikes of strata and surface(RS-LISS)represent a unique type of layered rock slope.These slopes are usually considered to be well stabilized and less prone to la...Rock slopes with large intersection angles between the strikes of strata and surface(RS-LISS)represent a unique type of layered rock slope.These slopes are usually considered to be well stabilized and less prone to landslides.However,when such slopes contain a significant number of discontinuities,their stability is greatly weakened.This study provided innovative insights into the stability of RS-LISS and conducted an in-depth investigation of their step-path failure mechanisms.The Riyi landslide on the eastern margin of the Qinghai-Tibet Plateau,China,was taken as a typical case and detailed investigations of geological structure and deformation characteristics of the slope were conducted by means of slope mapping,core drilling,and exploratory adits.A large number of steep-dip and gentle-dip joints were discovered in the slope,along with several critical discontinuities such as faults.Analysis shows that the tectonic stresses and river downcutting over geological time played significant roles in the formation of these discontinuities.Based on the investigation results,a numerical model of DFN for the Riyi landslide was developed.The simulation results indicated that the slope could develop a sliding surface characterized by a steep back and a gentle base,formed through the stepped interconnection of various discontinuities.Additionally,the deformation of the rock mass mainly originated from the major fault,progressively extending downward.The sliding mass may slide suddenly as a whole along the stepped bottom surface,with the compressional fracture zones as lateral boundaries,presenting a"drawer-like"movement towards the free surface.展开更多
The spherically layered media theory has wide applications for electromagnetic wave scattering analysis.Due to the involved Bessel functions,the conventional formulations of spherically layered media theory suffer fro...The spherically layered media theory has wide applications for electromagnetic wave scattering analysis.Due to the involved Bessel functions,the conventional formulations of spherically layered media theory suffer from numerical overflow or underflow when the Bessel function’s order is large,the argument is small or the argument has a large imaginary part.The first two issues have been solved recently by employing small-argument asymptotic formulas of Bessel functions,while the third issue remains unsolved.In this paper,the Bessel functions in the conventional formulation of the theory are replaced by scaled Bessel functions which have good numerical properties for high loss media,and stable formulas are derived.Numerical tests show that this approach can work properly with very high lossy media.Also,this approach can be seamlessly combined with the stable computation method for cases of small argument and large order of Bessel functions.展开更多
The polar layered deposits(PLD) of Mars can provide deep insight into paleoclimate changes over the planet's last several million years. Since the 1960s, researchers have studied almost all aspects of Martian PLD ...The polar layered deposits(PLD) of Mars can provide deep insight into paleoclimate changes over the planet's last several million years. Since the 1960s, researchers have studied almost all aspects of Martian PLD properties, searching for patterns that might reveal periodic characteristics of the planet's climate history. Although much progress has been made in our understanding of orbital periodicities reflected in the PLD, questions remain regarding how Martian orbital changes have affected the formation of the PLD and regarding the extent of climate information that is recorded in the PLD. Future studies of PLD should be carried out via integrated research that targets multi-profiles throughout the entire Martian polar regions that would clarify their general features at the hemisphere scale. Numerical modeling, coupled with modern observations of dust and water vapor transportation, should greatly advance our understanding of planetary climate evolution. Furthermore, future landing missions may help to clarify the paleoclimatic characteristics reflected in the PLD by drilling into these layered deposits and measuring mineralogical and geochemical compositions of the drilled samples.展开更多
Hydrogen (H2) production from renewable biomass resources plays a significant role in solving the shortage of fossil energy;hence, there is an interest in investigating alternative, cleaner processes. This work intend...Hydrogen (H2) production from renewable biomass resources plays a significant role in solving the shortage of fossil energy;hence, there is an interest in investigating alternative, cleaner processes. This work intends to study the photocatalytic production of hydrogen from D-(+)-Glucose by using different groups of catalysts that have been prepared (M2+ = Zn, Mg and Ni) M2+/Ti4+ Al3+-LDHs (layered double hydroxides). It is then loaded Pd on the catalyst, and the effect of the composite catalyst, layered double hydroxides, is measured. After calcining, the catalyst for the conversion of Layered Double Hydroxides (LDHs) to Layered Double Oxides (LDOs) is used to produce hydrogen gas from glucose. Photocatalytic reforming of glucose-derived compounds is an efficient method for the production of hydrogen. The purpose is to study the effect of metal ions on layered double oxide (LDO) materials by loading Pd and investigate hydrogen production from glucose. The metal cations in the layer were distributed through the preparation of the catalyst process by ion and atom scale between the layers, which were dispersed systematically, as well as the controlled component catalysis. This process shows that ZnTiAl-LDO had the best effect as a catalyst in producing hydrogen compared to NiTiAl-LDO and MgTiAl-LDO.展开更多
Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capac...Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.展开更多
Lithium-rich layered oxides (LLOs) are increasingly recognized as promising cathode materials for nextgeneration high-energy-density lithium-ion batteries (LIBs).However,they suffer from voltage decay and low initial ...Lithium-rich layered oxides (LLOs) are increasingly recognized as promising cathode materials for nextgeneration high-energy-density lithium-ion batteries (LIBs).However,they suffer from voltage decay and low initial Coulombic efficiency (ICE) due to severe structural degradation caused by irreversible O release.Herein,we introduce a three-in-one strategy of increasing Ni and Mn content,along with Li/Ni disordering and TM–O covalency regulation to boost cationic and anionic redox activity simultaneously and thus enhance the electrochemical activity of LLOs.The target material,Li_(1.2)Ni_(0.168)Mn_(0.558)Co_(0.074)O_(2)(L1),exhibits an improved ICE of 87.2%and specific capacity of 293.2 mA h g^(-1)and minimal voltage decay of less than 0.53 m V cycle-1over 300 cycles at 1C,compared to Li_(1.2)Ni_(0.13)Mn_(0.54)Co_(0.13)O_(2)(Ls)(274.4 mA h g^(-1)for initial capacity,73.8%for ICE and voltage decay of 0.84 mV/cycle over 300 cycles at 1C).Theoretical calculations reveal that the density of states (DOS) area near the Fermi energy level for L1 is larger than that of Ls,indicating higher anionic and cationic redox reactivity than Ls.Moreover,L1 exhibits increased O-vacancy formation energy due to higher Li/Ni disordering of 4.76%(quantified by X-ray diffraction Rietveld refinement) and enhanced TM–O covalency,making lattice O release more difficult and thus improving electrochemical stability.The increased Li/Ni disordering also leads to more Ni^(2+)presence in the Li layer,which acts as a pillar during Li+de-embedding,improving structural stability.This research not only presents a viable approach to designing low-Co LLOs with enhanced capacity and ICE but also contributes significantly to the fundamental understanding of structural regulation in high-performance LIB cathodes.展开更多
The utilization of eco-friendly,lightweight,high-efficiency and high-absorbing electromagnetic interference(EMI)shielding composites is imperative in light of the worldwide promotion of sustainable manufacturing.In th...The utilization of eco-friendly,lightweight,high-efficiency and high-absorbing electromagnetic interference(EMI)shielding composites is imperative in light of the worldwide promotion of sustainable manufacturing.In this work,magnetic poly(butyleneadipate-coterephthalate)(PBAT)microspheres were firstly synthesized via phase separation method,then PBAT composite foams with layered structure was constructed through the supercritical carbon dioxide foaming and scraping techniques.The merits of integrating ferroferric oxideloaded multi-walled carbon nanotubes(Fe3O4@MWCNTs)nanoparticles,a microcellular framework,and a highly conductive silver layer have been judiciously orchestrated within this distinctive layered configuration.Microwaves are consumed throughout the process of“absorption-reflection-reabsorption”as much as possible,which greatly declines the secondary radiation pollution.The biodegradable PBAT composite foams achieved an EMI shielding effectiveness of up to 68 dB and an absorptivity of 77%,and authenticated favorable stabilization after the tape adhesion experiment.展开更多
Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and low-cost.Nevertheless,such cathodes usually suffer from phase transitions,sluggish kinetics and air instabilit...Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and low-cost.Nevertheless,such cathodes usually suffer from phase transitions,sluggish kinetics and air instability,making it difficult to achieve high performance solid-state sodium-ion batteries.Herein,the high-entropy design and Li doping strategy alleviate lattice stress and enhance ionic conductivity,achieving high-rate performance,air stability and electrochemically thermal stability for Na_(0.95)Li_(0.06)Ni_(0.25)Cu_(0.05)Fe_(0.15)Mn_(0.49)O_(2).This cathode delivers a high reversible capacity(141 mAh g^(−1)at 0.2C),excellent rate capability(111 mAh g^(−1)at 8C,85 mAh g^(−1)even at 20C),and long-term stability(over 85%capacity retention after 1000 cycles),which is attributed to a rapid and reversible O3–P3 phase transition in regions of low voltage and suppresses phase transition.Moreover,the compound remains unchanged over seven days and keeps thermal stability until 279℃.Remarkably,the polymer solid-state sodium battery assembled by this cathode provides a capacity of 92 mAh g^(−1)at 5C and keeps retention of 96%after 400 cycles.This strategy inspires more rational designs and could be applied to a series of O3 cathodes to improve the performance of solid-state Na-ion batteries.展开更多
This study presents a facile and rapid method for synthesizing novel Layered Double Hydroxide(LDH)nanoflakes,exploring their application as a photocatalyst,and investigating the influence of condensed phosphates'g...This study presents a facile and rapid method for synthesizing novel Layered Double Hydroxide(LDH)nanoflakes,exploring their application as a photocatalyst,and investigating the influence of condensed phosphates'geometric linearity on their photocatalytic properties.Herein,the Mg O film,obtained by plasma electrolysis of AZ31 Mg alloys,was modified by growing an LDH film,which was further functionalized using cyclic sodium hexametaphosphate(CP)and linear sodium tripolyphosphate(LP).CP acted as an enhancer for flake spacing within the LDH structure,while LP changed flake dispersion and orientation.Consequently,CP@LDH demonstrated exceptional efficiency in heterogeneous photocatalysis,effectively degrading organic dyes like Methylene blue(MB),Congo red(CR),and Methyl orange(MO).The unique cyclic structure of CP likely enhances surface reactions and improves the catalyst's interaction with dye molecules.Furthermore,the condensed phosphate structure contributes to a higher surface area and reactivity in CP@LDH,leading to its superior photocatalytic performance compared to LP@LDH.Specifically,LP@LDH demonstrated notable degradation efficiencies of 93.02%,92.89%,and 88.81%for MB,MO,and CR respectively,over a 40 min duration.The highest degradation efficiencies were observed in the case of the CP@LDH sample,reporting 99.99%for MB,98.88%for CR,and 99.70%for MO.This underscores the potential of CP@LDH as a highly effective photocatalyst for organic dye degradation,offering promising prospects for environmental remediation and water detoxification applications.展开更多
Energy-storage systems and their production have attracted significant interest for practical applications.Batteries are the foundation of sustainable energy sources for electric vehicles(EVs),portable electronic devi...Energy-storage systems and their production have attracted significant interest for practical applications.Batteries are the foundation of sustainable energy sources for electric vehicles(EVs),portable electronic devices(PEDs),etc.In recent decades,Lithium-ion batteries(LIBs) have been extensively utilized in largescale energy storage devices owing to their long cycle life and high energy density.However,the high cost and limited availability of Li are the two main obstacles for LIBs.In this regard,sodium-ion batteries(SIBs) are attractive alternatives to LIBs for large-scale energy storage systems because of the abundance and low cost of sodium materials.Cathode is one of the most important components in the battery,which limits cost and performance of a battery.Among the classified cathode structures,layered structure materials have attracted attention because of their high ionic conductivity,fast diffusion rate,and high specific capacity.Here,we present a comprehensive review of the classification of layered structures and the preparation of layered materials.Furthermore,the review article discusses extensively about the issues of the layered materials,namely(1) electrochemical degradation,(2) irreversible structural changes,and(3) structural instability,and also it provides strategies to overcome the issues such as elemental phase composition,a small amount of elemental doping,structural design,and surface alteration for emerging SIBs.In addition,the article discusses about the recent research development on layered unary,binary,ternary,quaternary,quinary,and senary-based O3-and P2-type cathode materials for high-energy SIBs.This review article provides useful information for the development of high-energy layered sodium transition metal oxide P2 and O3-cathode materials for practical SIBs.展开更多
Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the...Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the degradation of layered oxides and the decomposition of electrolyte at high voltage,as well as the high reactivity of metallic Li.The key is the development of stable electrolytes against both highvoltage cathodes and Li with the formation of robust interphase films on the surfaces.Herein,we report a highly fluorinated ether,1,1,1-trifluoro-2-[(2,2,2-trifluoroethoxy)methoxy]ethane(TTME),as a cosolvent,which not only functions as a diluent forming a localized high concentration electrolyte(LHCE),but also participates in the construction of the inner solvation structure.The TTME-based electrolyte is stable itself at high voltage and induces the formation of a unique double-layer solid electrolyte interphase(SEI)film,which is embodied as one layer rich in crystalline structural components for enhanced mechanical strength and another amorphous layer with a higher concentration of organic components for enhanced flexibility.The Li||Cu cells display a noticeably high Coulombic efficiency of 99.28%after 300 cycles and Li symmetric cells maintain stable cycling more than 3200 h at 0.5 mA/cm^(2) and 1.0m Ah/cm^(2).In addition,lithium metal cells using LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) and Li CoO_(2) cathodes(both loadings~3.0 m Ah/cm^(2))realize capacity retentions of>85%over 240 cycles with a charge cut-off voltage of 4.4 V and 90%for 170 cycles with a charge cut-off voltage of 4.5 V,respectively.This study offers a bifunctional ether-based electrolyte solvent beneficial for high-voltage Li metal batteries.展开更多
Full concentration gradient lithium-rich layered oxides are catching lots of interest as the next generation cathode for lithium-ion batteries due to their high discharge voltage,reduced voltage decay and enhanced rat...Full concentration gradient lithium-rich layered oxides are catching lots of interest as the next generation cathode for lithium-ion batteries due to their high discharge voltage,reduced voltage decay and enhanced rate performance,whereas the high lithium residues on its surface impairs the structure stability and long-term cycle performance.Herein,a facile multifunctional surface modification method is implemented to eliminate surface lithium residues of full concentration gradient lithium-rich layered oxides by a wet chemistry reaction with tetrabutyl titanate and the post-annealing process.It realizes not only a stable Li_(2)TiO_(3)coating layer with 3D diffusion channels for fast Li^(+)ions transfer,but also dopes partial Ti^(4+)ions into the sub-surface region of full concentration gradient lithium-rich layered oxides to further strengthen its crystal structure.Consequently,the modified full concentration gradient lithium-rich layered oxides exhibit improved structure stability,elevated thermal stability with decomposition temperature from 289.57℃to 321.72℃,and enhanced cycle performance(205.1 mAh g^(-1)after 150 cycles)with slowed voltage drop(1.67 mV per cycle).This work proposes a facile and integrated modification method to enhance the comprehensive performance of full concentration gradient lithium-rich layered oxides,which can facilitate its practical application for developing higher energy density lithium-ion batteries.展开更多
Face stability is an essential issue in tunnel design and construction.Layered rock masses are typical and ubiquitous;uncertainties in rock properties always exist.In view of this,a comprehensive method,which combines...Face stability is an essential issue in tunnel design and construction.Layered rock masses are typical and ubiquitous;uncertainties in rock properties always exist.In view of this,a comprehensive method,which combines the Upper bound Limit analysis of Tunnel face stability,the Polynomial Chaos Kriging,the Monte-Carlo Simulation and Analysis of Covariance method(ULT-PCK-MA),is proposed to investigate the seismic stability of tunnel faces.A two-dimensional analytical model of ULT is developed to evaluate the virtual support force based on the upper bound limit analysis.An efficient probabilistic analysis method PCK-MA based on the adaptive Polynomial Chaos Kriging metamodel is then implemented to investigate the parameter uncertainty effects.Ten input parameters,including geological strength indices,uniaxial compressive strengths and constants for three rock formations,and the horizontal seismic coefficients,are treated as random variables.The effects of these parameter uncertainties on the failure probability and sensitivity indices are discussed.In addition,the effects of weak layer position,the middle layer thickness and quality,the tunnel diameter,the parameters correlation,and the seismic loadings are investigated,respectively.The results show that the layer distributions significantly influence the tunnel face probabilistic stability,particularly when the weak rock is present in the bottom layer.The efficiency of the proposed ULT-PCK-MA is validated,which is expected to facilitate the engineering design and construction.展开更多
This study explores the impact of introducing vacancy in the transition metal layer of rationally designed Na_(0.6)[Ni_(0.3)Ru_(0.3)Mn_(0.4)]O_(2)(NRM)cathode material.The incorporation of Ru,Ni,and vacancy enhances t...This study explores the impact of introducing vacancy in the transition metal layer of rationally designed Na_(0.6)[Ni_(0.3)Ru_(0.3)Mn_(0.4)]O_(2)(NRM)cathode material.The incorporation of Ru,Ni,and vacancy enhances the structural stability during extensive cycling,increases the operation voltage,and induces a capacity increase while also activating oxygen redox,respectively,in Na_(0.7)[Ni_(0.2)V_(Ni0.1)Ru_(0.3)Mn_(0.4)]O_(2)(V-NRM)compound.Various analytical techniques including transmission electron microscopy,X-ray absorption near edge spectroscopy,operando X-ray diffraction,and operando differential electrochemical mass spectrometry are employed to assess changes in the average oxidation states and structural distortions.The results demonstrate that V-NRM exhibits higher capacity than NRM and maintains a moderate capacity retention of 81%after 100 cycles.Furthermore,the formation of additional lone-pair electrons in the O 2p orbital enables V-NRM to utilize more capacity from the oxygen redox validated by density functional calculation,leading to a widened dominance of the OP4 phase without releasing O_(2) gas.These findings offer valuable insights for the design of advanced high-capacity cathode materials with improved performance and sustainability in sodium-ion batteries.展开更多
Ni-rich layered oxides are potential cathode materials for next-generation high energy density Li-ion batteries due to their high capacity and low cost.However,the inherently unstable surface properties,including high...Ni-rich layered oxides are potential cathode materials for next-generation high energy density Li-ion batteries due to their high capacity and low cost.However,the inherently unstable surface properties,including high levels of residual Li compounds,dissolution of transition metal cations,and parasitic side reactions,have not been effectively addressed,leading to significant degradation in their electrochemical performance.In this study,we propose a simple and effective lactic acid-assisted interface engineering strategy to regulate the surface chemistry and properties of Ni-rich LiNi_(0.8)Co_(0.1)Mr_(0.1)O_(2) cathode.This novel surface treatment method successfully eliminates surface residual Li compounds,inhibits structural collapse,and mitigates cathode-electrolyte interface film growth.As a result,the lactic acidtreated LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) achieved a remarkable capacity retention of 91.7% after 100 cycles at 0.5 C(25℃) and outstanding rate capability of 149.5 mA h g^(-1) at 10 C,significantly outperforming the pristine material.Furthermore,a pouch-type full cell incorporating the modified LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) cathode demonstrates impressive long-term cycle life,retaining 81.5% of its capacity after 500 cycles at 1 C.More importantly,the thermal stability of the modified cathode is also dramatically improved.This study offers a valuable surface modification strategy for enhancing the overall performance of Ni-rich cathode materials.展开更多
Modulating metal-organic framework’s(MOF)crystallinity and size using a polymer,in conjunction with a high surface area of layered double hydroxide,yields an effective strategy for concurrently enhancing the electroc...Modulating metal-organic framework’s(MOF)crystallinity and size using a polymer,in conjunction with a high surface area of layered double hydroxide,yields an effective strategy for concurrently enhancing the electrochemical and photocatalytic performance.In this study,we present the development of an optimized nanocomposite,denoted as 0.5PVP/ZIF-67,developed on AZ31 magnesium alloy,serving as an efficient and durable multifunctional coating.This novel strategy aims to enhance the overall performance of the porous coating through the integration of microarc oxidation(MAO),ZnFe LDH backbone,and ZIF-67 formation facilitated by the addition of polyvinylpyrrolidone(PVP),resulting in a three-dimensional,highly efficient,and multifunctional material.The incorporation of 0.5 g of PVP proved to be effective in the size modulation of ZIF-67,which formed a corrosion-resistant top layer,improving the total polarization resistance(R_(p)=8.20×10^(8)).The dual functionality exhibited by this hybrid architecture positions it as a promising candidate for mitigating environmental pollution,degrading 97.93%of Rhodamine B dye in 45 min.Moreover,the sample displayed exceptional degradation efficiency(96.17%)after 5 cycles.This study illuminates the potential of nanocomposites as electrochemically stable and photocatalytically active materials,laying the foundation for the advancements of next-generation multifunctional frameworks.展开更多
High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)M...High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.展开更多
基金supported by the National Natural Science Foundation of China(No.52271073)the Sichuan Provincial Natural Science Foundation for Distinguished Young Scholars,China(No.2024NSFJQ0034)the Innovation Team Funds of China West Normal University(No.KCXTD2024-1)。
文摘We have developed a superhydrophobic and corrosion-resistant LDH-W/PFDTMS composite coating on the surface of Mg alloy.This composite comprised a tungstate-intercalated(LDH-W)underlayer that was grown at low temperature(relative to hydrothermal reaction conditions)under atmospheric pressure and an outer polysiloxane layer created from a solution containing perfluorodecyltrimethoxysilane(PFDTMS)using a simple immersion method.The successful intercalation of tungstate into the LDH phase and the following formation of the polysiloxane layer were confirmed through X-ray diffraction(XRD),Fourier transform infrared(FTIR)spectroscopy,and X-ray photoelectron spectroscopy(XPS).The corrosion resistance of the LDH-W film,both before and after the PFDTMS modification,was evaluated using electrochemical impedance spectroscopy(EIS),Tafel curves,and immersion experiments.The results showed that Mg coated with LDH-W/PFDTMS exhibited significantly enhanced corrosion protection compared to the unmodified LDHW film,with no apparent signs of corrosion after exposure to 3.5wt%NaCl solution for 15 d.Furthermore,the LDH-W/PFDTMS coating demonstrated superior superhydrophobicity and self-cleaning properties against water and several common beverages,as confirmed by static contact angle and water-repellency tests.These results offer valuable insights into preparing superhydrophobic and corrosion-resistant LDH-based composite coatings on Mg alloy surfaces under relatively mild reaction conditions.
基金financial support by National Natural Science Foundation(NNSF)of China(Nos.52202269,52002248,U23B2069,22309162)Shenzhen Science and Technology program(No.20220810155330003)+1 种基金Shenzhen Basic Research Project(No.JCYJ20190808163005631)Xiangjiang Lab(22XJ01007).
文摘Sodium-ion batteries hold great promise as next-generation energy storage systems.However,the high instability of the electrode/electrolyte interphase during cycling has seriously hindered the development of SIBs.In particular,an unstable cathode–electrolyte interphase(CEI)leads to successive electrolyte side reactions,transition metal leaching and rapid capacity decay,which tends to be exacerbated under high-voltage conditions.Therefore,constructing dense and stable CEIs are crucial for high-performance SIBs.This work reports localized high-concentration electrolyte by incorporating a highly oxidation-resistant sulfolane solvent with non-solvent diluent 1H,1H,5H-octafluoropentyl-1,1,2,2-tetrafluoroethyl ether,which exhibited excellent oxidative stability and was able to form thin,dense and homogeneous CEI.The excellent CEI enabled the O3-type layered oxide cathode NaNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2)(NaNMF)to achieve stable cycling,with a capacity retention of 79.48%after 300 cycles at 1 C and 81.15%after 400 cycles at 2 C with a high charging voltage of 4.2 V.In addition,its nonflammable nature enhances the safety of SIBs.This work provides a viable pathway for the application of sulfolane-based electrolytes on SIBs and the design of next-generation high-voltage electrolytes.
基金financially supported by the National Natural Science Foundation of China(NSFC)(52274295)the Natural Science Foundation of Hebei Province(E2021501029)+3 种基金the Fundamental Research Funds for the Central Universities(N2423051,N2423053,N2302016,N2423019,N2323013,N2423005)the Science and Technology Project of Hebei Education Department(QN2024238)the Basic Research Program Project of Shijiazhuang City for Universities Stationed in Hebei Province(241790937A)the Science and Technology Project of Qinhuangdao City in 2023.
文摘Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the Jahn-Teller(JT)effect associated with Mn-ion,the cathode exhibits poor structural stability.Herein,we propose a strategy to enhance structural stability by introducing robust metal-oxygen(M-O)bonds,which can realize the pinning effect to constrain the distortion in the transition metal(TM)layer.Concurrently,all the elements employed have exceptionally high crustal abundance.As a proof of concept,the designed K_(0.5)Mn_(0.9)Mg_(0.025)Ti_(0.025)Al_(0.05)O_(2)cathode exhibited a discharge capacity of approximately 100 mA h g^(-1)at 20 mA g^(-1)with 79%capacity retention over 50 cycles,and 73%capacity retention over 200 cycles at 200 mA g^(-1),showcased much better battery performance than the designed cathode with less robust M-O bonds.The properties of the formed M-O bonds were investigated using theoretical calculations.The enhanced dynamics,mitigated JT effect,and improved structural stability were elucidated through the in-situ X-ray diffractometer(XRD),in-situ electrochemical impedance spectroscopy(EIS)(and distribution of relaxation times(DRT)method),and ex-situ X-ray absorption fine structure(XAFS)tests.This study holds substantial reference value for the future design of costeffective Mn-based layered cathodes for PIBs.
基金supported by the National Natural Science Foundation of China(No.U23A2047,No.42277187,No.42307248)Natural Science Foundation of Hebei Province(No.D2022202005)。
文摘Rock slopes with large intersection angles between the strikes of strata and surface(RS-LISS)represent a unique type of layered rock slope.These slopes are usually considered to be well stabilized and less prone to landslides.However,when such slopes contain a significant number of discontinuities,their stability is greatly weakened.This study provided innovative insights into the stability of RS-LISS and conducted an in-depth investigation of their step-path failure mechanisms.The Riyi landslide on the eastern margin of the Qinghai-Tibet Plateau,China,was taken as a typical case and detailed investigations of geological structure and deformation characteristics of the slope were conducted by means of slope mapping,core drilling,and exploratory adits.A large number of steep-dip and gentle-dip joints were discovered in the slope,along with several critical discontinuities such as faults.Analysis shows that the tectonic stresses and river downcutting over geological time played significant roles in the formation of these discontinuities.Based on the investigation results,a numerical model of DFN for the Riyi landslide was developed.The simulation results indicated that the slope could develop a sliding surface characterized by a steep back and a gentle base,formed through the stepped interconnection of various discontinuities.Additionally,the deformation of the rock mass mainly originated from the major fault,progressively extending downward.The sliding mass may slide suddenly as a whole along the stepped bottom surface,with the compressional fracture zones as lateral boundaries,presenting a"drawer-like"movement towards the free surface.
文摘The spherically layered media theory has wide applications for electromagnetic wave scattering analysis.Due to the involved Bessel functions,the conventional formulations of spherically layered media theory suffer from numerical overflow or underflow when the Bessel function’s order is large,the argument is small or the argument has a large imaginary part.The first two issues have been solved recently by employing small-argument asymptotic formulas of Bessel functions,while the third issue remains unsolved.In this paper,the Bessel functions in the conventional formulation of the theory are replaced by scaled Bessel functions which have good numerical properties for high loss media,and stable formulas are derived.Numerical tests show that this approach can work properly with very high lossy media.Also,this approach can be seamlessly combined with the stable computation method for cases of small argument and large order of Bessel functions.
基金supported financially by the Key Research Program of the Institute of Geology and Geophysics, CAS (Grant No. IGGCAS-202102 and IGGCAS-201905)。
文摘The polar layered deposits(PLD) of Mars can provide deep insight into paleoclimate changes over the planet's last several million years. Since the 1960s, researchers have studied almost all aspects of Martian PLD properties, searching for patterns that might reveal periodic characteristics of the planet's climate history. Although much progress has been made in our understanding of orbital periodicities reflected in the PLD, questions remain regarding how Martian orbital changes have affected the formation of the PLD and regarding the extent of climate information that is recorded in the PLD. Future studies of PLD should be carried out via integrated research that targets multi-profiles throughout the entire Martian polar regions that would clarify their general features at the hemisphere scale. Numerical modeling, coupled with modern observations of dust and water vapor transportation, should greatly advance our understanding of planetary climate evolution. Furthermore, future landing missions may help to clarify the paleoclimatic characteristics reflected in the PLD by drilling into these layered deposits and measuring mineralogical and geochemical compositions of the drilled samples.
文摘Hydrogen (H2) production from renewable biomass resources plays a significant role in solving the shortage of fossil energy;hence, there is an interest in investigating alternative, cleaner processes. This work intends to study the photocatalytic production of hydrogen from D-(+)-Glucose by using different groups of catalysts that have been prepared (M2+ = Zn, Mg and Ni) M2+/Ti4+ Al3+-LDHs (layered double hydroxides). It is then loaded Pd on the catalyst, and the effect of the composite catalyst, layered double hydroxides, is measured. After calcining, the catalyst for the conversion of Layered Double Hydroxides (LDHs) to Layered Double Oxides (LDOs) is used to produce hydrogen gas from glucose. Photocatalytic reforming of glucose-derived compounds is an efficient method for the production of hydrogen. The purpose is to study the effect of metal ions on layered double oxide (LDO) materials by loading Pd and investigate hydrogen production from glucose. The metal cations in the layer were distributed through the preparation of the catalyst process by ion and atom scale between the layers, which were dispersed systematically, as well as the controlled component catalysis. This process shows that ZnTiAl-LDO had the best effect as a catalyst in producing hydrogen compared to NiTiAl-LDO and MgTiAl-LDO.
基金financially supported by the National Natural Science Foundation of China(No.12304077)the Natural Science Foundation of Science and Technology Department of Sichuan Province(No.23NSFSC6224)+3 种基金Sichuan Science and Technology Program(No.2024NSFSC0989)the Key Laboratory of Computational Physics of Sichuan Province(No.YBUJSWL-YB-2022-03)the Material Corrosion and Protection Key Laboratory of Sichuan Province(No.2023CL14 and No.2023CL01)the National Innovation Practice Project(No.202411079005S).
文摘Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.
基金National Natural Science Foundation of China (No.52202046)Natural Science Foundation of Shaanxi Province (No.2021JQ-034)。
文摘Lithium-rich layered oxides (LLOs) are increasingly recognized as promising cathode materials for nextgeneration high-energy-density lithium-ion batteries (LIBs).However,they suffer from voltage decay and low initial Coulombic efficiency (ICE) due to severe structural degradation caused by irreversible O release.Herein,we introduce a three-in-one strategy of increasing Ni and Mn content,along with Li/Ni disordering and TM–O covalency regulation to boost cationic and anionic redox activity simultaneously and thus enhance the electrochemical activity of LLOs.The target material,Li_(1.2)Ni_(0.168)Mn_(0.558)Co_(0.074)O_(2)(L1),exhibits an improved ICE of 87.2%and specific capacity of 293.2 mA h g^(-1)and minimal voltage decay of less than 0.53 m V cycle-1over 300 cycles at 1C,compared to Li_(1.2)Ni_(0.13)Mn_(0.54)Co_(0.13)O_(2)(Ls)(274.4 mA h g^(-1)for initial capacity,73.8%for ICE and voltage decay of 0.84 mV/cycle over 300 cycles at 1C).Theoretical calculations reveal that the density of states (DOS) area near the Fermi energy level for L1 is larger than that of Ls,indicating higher anionic and cationic redox reactivity than Ls.Moreover,L1 exhibits increased O-vacancy formation energy due to higher Li/Ni disordering of 4.76%(quantified by X-ray diffraction Rietveld refinement) and enhanced TM–O covalency,making lattice O release more difficult and thus improving electrochemical stability.The increased Li/Ni disordering also leads to more Ni^(2+)presence in the Li layer,which acts as a pillar during Li+de-embedding,improving structural stability.This research not only presents a viable approach to designing low-Co LLOs with enhanced capacity and ICE but also contributes significantly to the fundamental understanding of structural regulation in high-performance LIB cathodes.
基金This work was supported by the National Natural Science Foundation of China(No.U21A2093)the Anhui Provincial Natural Science Foundation(No.2308085QE146)the National Natural Science Foundation of Jiangsu Province(No.BK20210894).
文摘The utilization of eco-friendly,lightweight,high-efficiency and high-absorbing electromagnetic interference(EMI)shielding composites is imperative in light of the worldwide promotion of sustainable manufacturing.In this work,magnetic poly(butyleneadipate-coterephthalate)(PBAT)microspheres were firstly synthesized via phase separation method,then PBAT composite foams with layered structure was constructed through the supercritical carbon dioxide foaming and scraping techniques.The merits of integrating ferroferric oxideloaded multi-walled carbon nanotubes(Fe3O4@MWCNTs)nanoparticles,a microcellular framework,and a highly conductive silver layer have been judiciously orchestrated within this distinctive layered configuration.Microwaves are consumed throughout the process of“absorption-reflection-reabsorption”as much as possible,which greatly declines the secondary radiation pollution.The biodegradable PBAT composite foams achieved an EMI shielding effectiveness of up to 68 dB and an absorptivity of 77%,and authenticated favorable stabilization after the tape adhesion experiment.
基金National Natural Science Foundation of China(52202327)Science and Technology Commission of Shanghai Municipality(22ZR1471300)+2 种基金National Science Foundation of China(Grant 51972326)Youth Innovation Promotion Association CAS,Foundation Strengthening ProjectProgram of Shanghai Academic Research Leader(Grant 22XD1424300).
文摘Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and low-cost.Nevertheless,such cathodes usually suffer from phase transitions,sluggish kinetics and air instability,making it difficult to achieve high performance solid-state sodium-ion batteries.Herein,the high-entropy design and Li doping strategy alleviate lattice stress and enhance ionic conductivity,achieving high-rate performance,air stability and electrochemically thermal stability for Na_(0.95)Li_(0.06)Ni_(0.25)Cu_(0.05)Fe_(0.15)Mn_(0.49)O_(2).This cathode delivers a high reversible capacity(141 mAh g^(−1)at 0.2C),excellent rate capability(111 mAh g^(−1)at 8C,85 mAh g^(−1)even at 20C),and long-term stability(over 85%capacity retention after 1000 cycles),which is attributed to a rapid and reversible O3–P3 phase transition in regions of low voltage and suppresses phase transition.Moreover,the compound remains unchanged over seven days and keeps thermal stability until 279℃.Remarkably,the polymer solid-state sodium battery assembled by this cathode provides a capacity of 92 mAh g^(−1)at 5C and keeps retention of 96%after 400 cycles.This strategy inspires more rational designs and could be applied to a series of O3 cathodes to improve the performance of solid-state Na-ion batteries.
基金the National Research Foundation of Korea(NRF)funded by the Korean Government(MSIT)(No.2022R1A2C1006743)。
文摘This study presents a facile and rapid method for synthesizing novel Layered Double Hydroxide(LDH)nanoflakes,exploring their application as a photocatalyst,and investigating the influence of condensed phosphates'geometric linearity on their photocatalytic properties.Herein,the Mg O film,obtained by plasma electrolysis of AZ31 Mg alloys,was modified by growing an LDH film,which was further functionalized using cyclic sodium hexametaphosphate(CP)and linear sodium tripolyphosphate(LP).CP acted as an enhancer for flake spacing within the LDH structure,while LP changed flake dispersion and orientation.Consequently,CP@LDH demonstrated exceptional efficiency in heterogeneous photocatalysis,effectively degrading organic dyes like Methylene blue(MB),Congo red(CR),and Methyl orange(MO).The unique cyclic structure of CP likely enhances surface reactions and improves the catalyst's interaction with dye molecules.Furthermore,the condensed phosphate structure contributes to a higher surface area and reactivity in CP@LDH,leading to its superior photocatalytic performance compared to LP@LDH.Specifically,LP@LDH demonstrated notable degradation efficiencies of 93.02%,92.89%,and 88.81%for MB,MO,and CR respectively,over a 40 min duration.The highest degradation efficiencies were observed in the case of the CP@LDH sample,reporting 99.99%for MB,98.88%for CR,and 99.70%for MO.This underscores the potential of CP@LDH as a highly effective photocatalyst for organic dye degradation,offering promising prospects for environmental remediation and water detoxification applications.
基金supported by a grant from the Subway Fine Dust Reduction Technology Development Project of the Ministry of Land Infrastructure and Transport,Republic of Korea(21QPPWB152306-03)the Basic Science Research Capacity Enhancement Project through a Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Education of the Republic of Korea(2019R1A6C1010016)。
文摘Energy-storage systems and their production have attracted significant interest for practical applications.Batteries are the foundation of sustainable energy sources for electric vehicles(EVs),portable electronic devices(PEDs),etc.In recent decades,Lithium-ion batteries(LIBs) have been extensively utilized in largescale energy storage devices owing to their long cycle life and high energy density.However,the high cost and limited availability of Li are the two main obstacles for LIBs.In this regard,sodium-ion batteries(SIBs) are attractive alternatives to LIBs for large-scale energy storage systems because of the abundance and low cost of sodium materials.Cathode is one of the most important components in the battery,which limits cost and performance of a battery.Among the classified cathode structures,layered structure materials have attracted attention because of their high ionic conductivity,fast diffusion rate,and high specific capacity.Here,we present a comprehensive review of the classification of layered structures and the preparation of layered materials.Furthermore,the review article discusses extensively about the issues of the layered materials,namely(1) electrochemical degradation,(2) irreversible structural changes,and(3) structural instability,and also it provides strategies to overcome the issues such as elemental phase composition,a small amount of elemental doping,structural design,and surface alteration for emerging SIBs.In addition,the article discusses about the recent research development on layered unary,binary,ternary,quaternary,quinary,and senary-based O3-and P2-type cathode materials for high-energy SIBs.This review article provides useful information for the development of high-energy layered sodium transition metal oxide P2 and O3-cathode materials for practical SIBs.
基金the financial supports from the KeyArea Research and Development Program of Guangdong Province (2020B090919001)the National Natural Science Foundation of China (22078144)the Guangdong Natural Science Foundation for Basic and Applied Basic Research (2021A1515010138 and 2023A1515010686)。
文摘Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the degradation of layered oxides and the decomposition of electrolyte at high voltage,as well as the high reactivity of metallic Li.The key is the development of stable electrolytes against both highvoltage cathodes and Li with the formation of robust interphase films on the surfaces.Herein,we report a highly fluorinated ether,1,1,1-trifluoro-2-[(2,2,2-trifluoroethoxy)methoxy]ethane(TTME),as a cosolvent,which not only functions as a diluent forming a localized high concentration electrolyte(LHCE),but also participates in the construction of the inner solvation structure.The TTME-based electrolyte is stable itself at high voltage and induces the formation of a unique double-layer solid electrolyte interphase(SEI)film,which is embodied as one layer rich in crystalline structural components for enhanced mechanical strength and another amorphous layer with a higher concentration of organic components for enhanced flexibility.The Li||Cu cells display a noticeably high Coulombic efficiency of 99.28%after 300 cycles and Li symmetric cells maintain stable cycling more than 3200 h at 0.5 mA/cm^(2) and 1.0m Ah/cm^(2).In addition,lithium metal cells using LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) and Li CoO_(2) cathodes(both loadings~3.0 m Ah/cm^(2))realize capacity retentions of>85%over 240 cycles with a charge cut-off voltage of 4.4 V and 90%for 170 cycles with a charge cut-off voltage of 4.5 V,respectively.This study offers a bifunctional ether-based electrolyte solvent beneficial for high-voltage Li metal batteries.
基金financially supported by the Natural Science Foundation of Shandong Province(ZR2022QB166,ZR2020KE032)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA22010600)+3 种基金the Youth Innovation Promotion Association of CAS(2021210)the Foundation of Qingdao Postdoctoral Application Program(Y63302190F)the Natural Science Foundation of Qingdao Institute ofBioenergy and Bioprocess Technology(QIBEBT SZ202101)support from the Max Planck-POSTECH-Hsinchu Center for Complex Phase Materials
文摘Full concentration gradient lithium-rich layered oxides are catching lots of interest as the next generation cathode for lithium-ion batteries due to their high discharge voltage,reduced voltage decay and enhanced rate performance,whereas the high lithium residues on its surface impairs the structure stability and long-term cycle performance.Herein,a facile multifunctional surface modification method is implemented to eliminate surface lithium residues of full concentration gradient lithium-rich layered oxides by a wet chemistry reaction with tetrabutyl titanate and the post-annealing process.It realizes not only a stable Li_(2)TiO_(3)coating layer with 3D diffusion channels for fast Li^(+)ions transfer,but also dopes partial Ti^(4+)ions into the sub-surface region of full concentration gradient lithium-rich layered oxides to further strengthen its crystal structure.Consequently,the modified full concentration gradient lithium-rich layered oxides exhibit improved structure stability,elevated thermal stability with decomposition temperature from 289.57℃to 321.72℃,and enhanced cycle performance(205.1 mAh g^(-1)after 150 cycles)with slowed voltage drop(1.67 mV per cycle).This work proposes a facile and integrated modification method to enhance the comprehensive performance of full concentration gradient lithium-rich layered oxides,which can facilitate its practical application for developing higher energy density lithium-ion batteries.
基金supported by Science and Technology Project of Yunnan Provincial Transportation Department(Grant No.25 of 2018)the National Natural Science Foundation of China(Grant No.52279107)The authors are grateful for the support by the China Scholarship Council(CSC No.202206260203 and No.201906690049).
文摘Face stability is an essential issue in tunnel design and construction.Layered rock masses are typical and ubiquitous;uncertainties in rock properties always exist.In view of this,a comprehensive method,which combines the Upper bound Limit analysis of Tunnel face stability,the Polynomial Chaos Kriging,the Monte-Carlo Simulation and Analysis of Covariance method(ULT-PCK-MA),is proposed to investigate the seismic stability of tunnel faces.A two-dimensional analytical model of ULT is developed to evaluate the virtual support force based on the upper bound limit analysis.An efficient probabilistic analysis method PCK-MA based on the adaptive Polynomial Chaos Kriging metamodel is then implemented to investigate the parameter uncertainty effects.Ten input parameters,including geological strength indices,uniaxial compressive strengths and constants for three rock formations,and the horizontal seismic coefficients,are treated as random variables.The effects of these parameter uncertainties on the failure probability and sensitivity indices are discussed.In addition,the effects of weak layer position,the middle layer thickness and quality,the tunnel diameter,the parameters correlation,and the seismic loadings are investigated,respectively.The results show that the layer distributions significantly influence the tunnel face probabilistic stability,particularly when the weak rock is present in the bottom layer.The efficiency of the proposed ULT-PCK-MA is validated,which is expected to facilitate the engineering design and construction.
基金supported by Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education,Science and Technology(NRF-2020R1A6A1A03043435,NRF-2023R1A2C2003210,and NRF-2022M3H4A1A04096478)by Technology Innovation Program(Alchemist Project,20012196,Al based supercritical materials discovery)funded by the Ministry of Trade,Industry&Energy,Korea.support from the“Bundesministerium fur Bildung und Forschung”(BMBF)and the computing time granted through JARA-HPC on the supercomputer JURECA at Forschungszentrum Julich.
文摘This study explores the impact of introducing vacancy in the transition metal layer of rationally designed Na_(0.6)[Ni_(0.3)Ru_(0.3)Mn_(0.4)]O_(2)(NRM)cathode material.The incorporation of Ru,Ni,and vacancy enhances the structural stability during extensive cycling,increases the operation voltage,and induces a capacity increase while also activating oxygen redox,respectively,in Na_(0.7)[Ni_(0.2)V_(Ni0.1)Ru_(0.3)Mn_(0.4)]O_(2)(V-NRM)compound.Various analytical techniques including transmission electron microscopy,X-ray absorption near edge spectroscopy,operando X-ray diffraction,and operando differential electrochemical mass spectrometry are employed to assess changes in the average oxidation states and structural distortions.The results demonstrate that V-NRM exhibits higher capacity than NRM and maintains a moderate capacity retention of 81%after 100 cycles.Furthermore,the formation of additional lone-pair electrons in the O 2p orbital enables V-NRM to utilize more capacity from the oxygen redox validated by density functional calculation,leading to a widened dominance of the OP4 phase without releasing O_(2) gas.These findings offer valuable insights for the design of advanced high-capacity cathode materials with improved performance and sustainability in sodium-ion batteries.
基金This work was supported by the Anhui Provincial Natural Science Foundation(Grant No.2308085QB69)the Institute of Energy,Hefei Comprehensive National Science Center(Grant No.21KZS210).
文摘Ni-rich layered oxides are potential cathode materials for next-generation high energy density Li-ion batteries due to their high capacity and low cost.However,the inherently unstable surface properties,including high levels of residual Li compounds,dissolution of transition metal cations,and parasitic side reactions,have not been effectively addressed,leading to significant degradation in their electrochemical performance.In this study,we propose a simple and effective lactic acid-assisted interface engineering strategy to regulate the surface chemistry and properties of Ni-rich LiNi_(0.8)Co_(0.1)Mr_(0.1)O_(2) cathode.This novel surface treatment method successfully eliminates surface residual Li compounds,inhibits structural collapse,and mitigates cathode-electrolyte interface film growth.As a result,the lactic acidtreated LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) achieved a remarkable capacity retention of 91.7% after 100 cycles at 0.5 C(25℃) and outstanding rate capability of 149.5 mA h g^(-1) at 10 C,significantly outperforming the pristine material.Furthermore,a pouch-type full cell incorporating the modified LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) cathode demonstrates impressive long-term cycle life,retaining 81.5% of its capacity after 500 cycles at 1 C.More importantly,the thermal stability of the modified cathode is also dramatically improved.This study offers a valuable surface modification strategy for enhancing the overall performance of Ni-rich cathode materials.
基金supported by the National Research Foundation of Korea(NRF)funded by the Korean government(MSIT)(No.2022R1A2C1006743).
文摘Modulating metal-organic framework’s(MOF)crystallinity and size using a polymer,in conjunction with a high surface area of layered double hydroxide,yields an effective strategy for concurrently enhancing the electrochemical and photocatalytic performance.In this study,we present the development of an optimized nanocomposite,denoted as 0.5PVP/ZIF-67,developed on AZ31 magnesium alloy,serving as an efficient and durable multifunctional coating.This novel strategy aims to enhance the overall performance of the porous coating through the integration of microarc oxidation(MAO),ZnFe LDH backbone,and ZIF-67 formation facilitated by the addition of polyvinylpyrrolidone(PVP),resulting in a three-dimensional,highly efficient,and multifunctional material.The incorporation of 0.5 g of PVP proved to be effective in the size modulation of ZIF-67,which formed a corrosion-resistant top layer,improving the total polarization resistance(R_(p)=8.20×10^(8)).The dual functionality exhibited by this hybrid architecture positions it as a promising candidate for mitigating environmental pollution,degrading 97.93%of Rhodamine B dye in 45 min.Moreover,the sample displayed exceptional degradation efficiency(96.17%)after 5 cycles.This study illuminates the potential of nanocomposites as electrochemically stable and photocatalytically active materials,laying the foundation for the advancements of next-generation multifunctional frameworks.
基金supported by the National Natural Science Foundation of China(52162030)the Yunnan Major Scientific and Technological Projects(202202AG050003)+4 种基金the Key Research and Development Program of Yunnan Province(202103AA080019)the Scientific Research Foundation of Kunming University of Science and Technology(20220122)the Graduate Student Top Innovative Talent Program of Kunming University of Science and Technology(CA23107M139A)the Analysis and Testing Foundation of Kunming University of Science and Technology(2023T20220122)the Shenzhen Science and Technology Program(KCXST20221021111201003)。
文摘High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.
