To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as wel...To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well.Herein,we suggest an effective approach to control the micropore structure of silicon oxide(SiO_(x))/artificial graphite(AG)composite electrodes using a perforated current collector.The electrode features a unique pore structure,where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance,leading to a 20%improvement in rate capability at a 5C-rate discharge condition.Using microstructure-resolved modeling and simulations,we demonstrate that the patterned micropore structure enhances lithium-ion transport,mitigating the electrolyte concentration gradient of lithium-ion.Additionally,perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiO_(x)/AG composite electrode,significantly improving adhesion strength.This,in turn,suppresses mechanical degradation and leads to a 50%higher capacity retention.Thus,regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiO_(x)/AG composite electrodes,providing valuable insights into electrode engineering.展开更多
As a negative electrode material for lithium-ion batteries,silicon monoxide(SiO)suffers from dramatic volume changes during cycling,causing excessive stress within the electrode and resulting in electrode deformation ...As a negative electrode material for lithium-ion batteries,silicon monoxide(SiO)suffers from dramatic volume changes during cycling,causing excessive stress within the electrode and resulting in electrode deformation and fragmentation.This ultimately leads to a decrease in cell capacity.The trends of volume expansion and capacity change of the SiO/graphite(SiO/C)composite electrode during cycling were investigated via in situ expansion monitoring.First,a series of expansion test schemes were designed,and the linear relationship between negative electrode expansion and cell capacity degradation was quantitatively analyzed.Then,the effects of different initial pressures on the long-term cycling performance of the cell were evaluated.Finally,the mechanism of their effects was analyzed by scanning electron microscope.The results show that after 50 cycles,the cell capacity decreases from 2.556 mAh to 1.689 mAh,with a capacity retention ratio(CRR)of only 66.08%.A linear relationship between the capacity retention ratio and thickness expansion was found.Electrochemical measurements and scanning electron microscope images demonstrate that intense stress inhibits the lithiation of the negative electrode and that the electrode is more susceptible to irreversible damage during cycling.Overall,these results reveal the relationship between the cycling performance of SiO and the internal pressure of the electrode from a macroscopic point of view,which provides some reference for the application of SiO/C composite electrodes in lithium-ion batteries.展开更多
The silicon-graphite(Si-C)composite electrode is considered a promising candidate for next-generation commercial electrodes due to its high capacity.However,lithium-ion batteries with silicon electrodes often experien...The silicon-graphite(Si-C)composite electrode is considered a promising candidate for next-generation commercial electrodes due to its high capacity.However,lithium-ion batteries with silicon electrodes often experience capacity fading and poor cyclic performance,primarily due to the mechanical degradation of the solid-electrolyte interphase(SEI).In this work,we present a homogenized constitutive model for Si-C composite electrodes under finite deformation,incorporating lithium-ion concentration-dependent properties.We perform a wrinkling analysis and systematically examine the influence of key parameters,such as modulus and thickness ratios,on the critical conditions for instability.Additionally,we investigate the ratcheting effect across varying silicon contents.Our findings reveal that maintaining the silicon content within an optimal range effectively reduces plastic accumulation during charge–discharge cycles.These insights provide crucial guidance for optimizing the design and fabrication of Si–C electrode systems,enhancing their durability and performance.展开更多
All-solid-state lithium metal batteries(ASSLMBs)are widely recognized as promising next-generation energy storage technologies that offer significant advantages in terms of safety and energy density.However,the long-t...All-solid-state lithium metal batteries(ASSLMBs)are widely recognized as promising next-generation energy storage technologies that offer significant advantages in terms of safety and energy density.However,the long-term cycling stability of these batteries is often compromised by interfacial failures driven by coupled mechanical and diffusion effects.This study presents a probabilistic failure prediction model that quantifies interfacial damage and capacity loss in composite electrodes under the coupled influence of mechanical-diffusion-induced processes.We first develop a pseudo3D(P3D)interface failure model for a binary particle system to evaluate interfacial failure during the critical delithiation process.The P3D model is validated through mechanical‒diffusion coupled simulations.Additionally,for multiparticle composite electrode films with heterogeneous particle sizes,we identify a key structural factor that governs the failure of the particle‒solid electrolyte interface,which follows a three-parameter Burr distribution.Building on this,we develop a probabilistic model to predict the capacity fade in multiporject composite films.This work provides a comprehensive understanding of the critical geometric factors that influence interfacial stability,offering valuable theoretical insights and practical guidance for the rapid assessment,optimization,and enhancement of cycling stability in ASSLMBs.展开更多
Anode active materials involving transition metal oxides and sulfides are of great significance for high energy density lithium-ion batteries(LIBs),but the huge volume expansion and inferior electronic conductivity up...Anode active materials involving transition metal oxides and sulfides are of great significance for high energy density lithium-ion batteries(LIBs),but the huge volume expansion and inferior electronic conductivity upon cycling critically constrain their further application.Herein,from a new perspective,a highly conductive and stable 3D flexible composite current collector is rationally designed by facilely electrodepositing metallic Ni thin layer onto the carbon cloth(CC/Ni),which endows the supported active materials with exceptional electronic conductivity and structural stability.In addition,the homogeneously distributed metallic Ni protrusions external CC can strongly bond with the active components,ensuring the structural integrity of electrodes upon cycling.More importantly,the 3D network structure with large specific surface area provides abundant space to alleviate the volume expansion and more active sites for electrochemical reactions.Therefore,taking Ni_(3)S_(2)nanosheet(Ni_(3)S_(2)NS)anode as an example,the prepared Ni_(3)S_(2)NS@CC/Ni electrode shows a high specific capacity of 2.32 mAh/cm^(2)at 1mA/cm^(2)and high capacity retention of 1.68 mAh/cm^(2)at a high rate of 8mA/cm^(2).This study provides a universal approach to obtain highly conductive and stable 3D flexible current collectors towards high performance metal-ion batteries beyond LIBs.展开更多
The recently reported silicon/graphite(Si/Gr)composite electrode with a layered structure is a promising approach to achieve high capacity and stable cycling of Si-based electrodes in lithium-ion batteries.However,the...The recently reported silicon/graphite(Si/Gr)composite electrode with a layered structure is a promising approach to achieve high capacity and stable cycling of Si-based electrodes in lithium-ion batteries.However,there is still a need to clarify why particular layered structures are effective and why others are ineffective or even detrimental.In this work,an unreported mechanism dominated by the porosity evolution of electrodes is proposed for the degradation behavior of layered Si/Gr electrodes.First,the effect of layering sequence on the overall electrode performance is investigated experimentally,and the results suggest that the cycling performance of the silicon-on-graphite(SG)electrode is much superior to that of the graphite-on-silicon electrode.To explain this phenomenon,a coupled mechanical-electrochemical porous electrode model is developed,in which the porosity is affected by the silicon expansion and the local constraints.The modeling results suggest that the weaker constraint of the silicon layer in the SG electrode leads to a more insignificant decrease in porosity,and consequently,the more stable cycling performance.The findings of this work provide new insights into the structural design of Si-based electrodes.展开更多
In order to investigate the effect of solid particles dopants on physicochemical properties of α-PbO2 electrodes, a-PbO2 composite electrodes doped with nano-TiO2 and nano-CeO2 particles were respectively prepared on...In order to investigate the effect of solid particles dopants on physicochemical properties of α-PbO2 electrodes, a-PbO2 composite electrodes doped with nano-TiO2 and nano-CeO2 particles were respectively prepared on A1/conductive coating electrodes in 4 mol/L NaOH solution with addition of PbO until saturation by anodic codeposition. The electrodeposition mechanism, morphology, composition and structure of the composite electrodes were characterized by cyclic voltarnmogram （CV）, SEM, EDAX and XRD. Results show that the doping solid particles can not change reaction mechanism of α-PbO2 electrode in alkaline or acid plating bath, but can improve deposition rate and reduce oxygen evolution potential. The doping solid particles can inhibit the growth of a-PbO2 unit cell and improve specific surface area. The diffraction peak intensity of a-PbO2-CeO2-TiO2 composite electrode is lower than that of pure a-PbO2 electrode. The electrocatalytic activity of a-PbO2-2.12%CEO2-3.71%TIO2 composite electrode is the best. The Guglielmi model for CeO2 and TiO2 codeposition with a-PbO2 is also pronosed.展开更多
Al/conductive coating/α-Pb O2-Ce O2-Ti O2/β-PbO 2-MnO 2-WC-Zr O2 composite electrode material was prepared on Al/conductive coating/α-PbO 2-Ce O2-Ti O2 substrate by electrochemical oxidation co-deposition technique...Al/conductive coating/α-Pb O2-Ce O2-Ti O2/β-PbO 2-MnO 2-WC-Zr O2 composite electrode material was prepared on Al/conductive coating/α-PbO 2-Ce O2-Ti O2 substrate by electrochemical oxidation co-deposition technique. The effects of current density on the chemical composition, electrocatalytic activity, and stability of the composite anode material were investigated by energy dispersive X-ray spectroscopy（EDXS）, anode polarization curves, quasi-stationary polarization（Tafel） curves, electrochemical impedance spectroscopy（EIS）, scanning electron microscopy（SEM）, and X-ray diffraction（XRD）. Results reveal that the composite electrode obtained at 1 A/dm2 possesses the lowest overpotential（0.610 V at 500 A/m2） for oxygen evolution, the best electrocatalytic activity, the longest service life（360 h at 40 °C in 150 g/L H2SO4 solution under 2 A/cm2）, and the lowest cell voltage（2.75 V at 500 A/m2）. Furthermore, with increasing current density, the coating exhibits grain growth and the decrease of content of Mn O2. Only a slight effect on crystalline structure is observed.展开更多
The synthetic routes of porous carbons and the applications of the functional porous carbon-based composite electrode materials for lithium secondary batteries are reviewed. The synthetic methods have made great break...The synthetic routes of porous carbons and the applications of the functional porous carbon-based composite electrode materials for lithium secondary batteries are reviewed. The synthetic methods have made great breakthroughs to control the pore size and volume, wall thickness, surface area, and connectivity of porous carbons, which result in the development of functional porous carbon-based composite electrode materials. The effects of porous carbons on the electrochemical properties are further discussed. The porous carbons as ideal matrixes to incorporate active materials make a great improvement on the electrochemical properties because of high surface area and pore volume, excellent electronic conductivity, and strong adsorption capacity. Large numbers of the composite electrode materials have been used for the devices of electrochemical energy conversion and storage, such as lithium-ion batteries （LIBs）, Li-S batteries, and Li-O2 batteries. It is believed that functional porous carbon-based composite electrode materials will continuously contribute to the field of lithium secondary batteries.展开更多
This work describes the electrochemical behaviour of ibuprofen on two types of multi-walled carbon nanotubes based composite electrodes, i.e., multi-walled carbon nanotubes-epoxy （MWCNT） and silver-modified zeolite-...This work describes the electrochemical behaviour of ibuprofen on two types of multi-walled carbon nanotubes based composite electrodes, i.e., multi-walled carbon nanotubes-epoxy （MWCNT） and silver-modified zeolite-multi-wailed carbon nanotubes-epoxy （AgZMWCNT） composites electrodes. The composite electrodes were obtained using two-roll mill procedure. SEM images of surfaces of the composites revealed a homogeneous distribution of the composite components within the epoxy matrix. AgZMWCNT composite electrode exhibited the better electrical conductivity and larger electroactive surface area. The electrochemical determination of ibuprofen （IBP） was achieved using AgZMWCNT by cyclic voltammetry, differential-pulsed voltammetry, square-wave voltammetry and chronoamperometry. The IBP degradation occurred on both composite electrodes under controlled electrolysis at 1.2 and 1.75 V vs. Ag/AgCl, and IBP concentration was determined comparatively by differential-pulsed voltammetry, under optimized conditions using AgZMWCNT electrode and UV-Vis spectrophotometry methods to determine the IBP degradation performance for each electrode. AgZMWCNT electrode exhibited a dual character allowing a double application in IBP degradation process and its control.展开更多
Composite LaNi5+x wt.% Ti0.10Zr0.16V0.34Cr0.10Ni0.30 (x=0, 1, 5, 10) alloys were prepared by two-step re-melting. X-ray diffractometer (XRD), scanning electron microscopy (FESEM), energy dispersive spectrometry (EDS),...Composite LaNi5+x wt.% Ti0.10Zr0.16V0.34Cr0.10Ni0.30 (x=0, 1, 5, 10) alloys were prepared by two-step re-melting. X-ray diffractometer (XRD), scanning electron microscopy (FESEM), energy dispersive spectrometry (EDS), inductively coupled plasma (ICP) and electrochemical impedance spectroscopy (EIS) analyses showed that the matrix phase of LaNi5 alloy with CaCu5 structure remained unchanged after additive alloy was added, the amount of the second phase increased with increasing x. The synergetic effect withi...展开更多
Taking the nano-sized carbon black and aniline monomer as precursor and （NH4）2S2O6 as oxidant, the well coated C/polyaniline（C/PANI） composite materials were prepared by in situ polymerization of the aniline on th...Taking the nano-sized carbon black and aniline monomer as precursor and （NH4）2S2O6 as oxidant, the well coated C/polyaniline（C/PANI） composite materials were prepared by in situ polymerization of the aniline on the surface of well-dispersed nano-sized carbon black for supercapacitor. The micro-structure of the C/PANI composite electrode materials were analyzed by SEM. The electrochemical properties of C/ PANI and PANI composite electrode were characterized by means of the galvanostatic charge-discharge experiment, cyclic voltammetric measurement and impedance spectroscopy analysis. The results show that by adding the nano-sized carbon black in the process of chemical polymerization of the aniline, the polyaniline can be in situ polymerized and well-coated onto the carbon black particles, which may effectively improve the aggregation of particles and the electrolyte penetration. What’s more , the maximum of specific capacitance of C/PANI electrode 437.6F·g -1 can be attained. Compared with PANI electrode, C/PANI electrode shows more desired capacitance characteristics, smaller internal resistance and better cycle performance.展开更多
PbO2/Co3O4 composites were prepared on a Ti substrate by means of a composite electrodeposition method in Pb2+ plating solution containing dissolved nano-Co3O4 particles. X-ray diffraction（XRD）, scanning electron mi...PbO2/Co3O4 composites were prepared on a Ti substrate by means of a composite electrodeposition method in Pb2+ plating solution containing dissolved nano-Co3O4 particles. X-ray diffraction（XRD）, scanning electron microscopy（SEM）, energy dispersive spectrometry（EDS） and transmission electron microscopy（TEM） were used to characterize the chemical composition and morphology of the PbO2/Co3O4 composites. The electrochemical and capacitance performance of the composites were investigated by cyclic voltammetry（CV）, charge-discharge tests and electrochemical impedance（EIS）. The results indicate that the composites comprise rutile phase Co3O4 and β-PbO2. In addition, the surface of the composite electrode is rough and porous. The PbO2/Co3O4 composites exhibit a high specific capacitance up to 215 F/g, which is ten times higher than that of the pure-PbO2 and two times higher than that of the pure-Co3O4 in 1 mol/L NaOH electrolytes.展开更多
Thick electrodes can increase incorporation of active electrode materials by diminishing the proportion of inactive constituents,improving the overall energy density of batteries.However,thick electrodes fabricated us...Thick electrodes can increase incorporation of active electrode materials by diminishing the proportion of inactive constituents,improving the overall energy density of batteries.However,thick electrodes fabricated using the conventional slurry casting approach frequently exhibit an exacerbated accumulation of carbon additives and binders on their surfaces,invariably leading to compromised electrochemical properties.In this study,we introduce a designed conductive agent/binder composite synthesized from carbon nanotube and polytetrafluoroethylene.This agent/binder composite facilitates production of dry-process-prepared ultra-thick electrodes endowed with a three-dimensional and uniformly distributed percolative architecture,ensuring superior electronic conductivity and remarkable mechanical resilience.Using this approach,ultra-thick LiCoO_(2)(LCO) electrodes demonstrated superior cycling performance and rate capabilities,registering an impressive loading capacity of up to 101.4 mg/cm^(2),signifying a 242% increase in battery energy density.In another analytical endeavor,time-of-flight secondary ion mass spectroscopy was used to clarify the distribution of cathode electrolyte interphase(CEI) in cycled LCO electrodes.The results provide unprecedented evidence explaining the intricate correlation between CEI generation and carbon distribution,highlighting the intrinsic advantages of the proposed dry-process approach in fine-tu ning the CEI,with excellent cycling performance in batteries equipped with ultra-thick electrodes.展开更多
Pt-free counter electrode(CE) composed of La2 MoO(LaO-MoO) was successfully synthesized by simple pyrolysis of lanthanum acetate(CHOLa·xHO) and hexaammonium heptamolybdate tetrahydrate((NH4)6 MoO·4 HO). Furt...Pt-free counter electrode(CE) composed of La2 MoO(LaO-MoO) was successfully synthesized by simple pyrolysis of lanthanum acetate(CHOLa·xHO) and hexaammonium heptamolybdate tetrahydrate((NH4)6 MoO·4 HO). Furthermore,three proportions composites catalysts of La2 MoO@MWCNTs based on La2 MoOand multiwall carbon nanotubes(MWCNTs) were prepared and characterized as Ptfree catalyst for CE in dye-sensitized solar cells(DSSCs). The morphology and structure of La2 MoO@MWCNTs composites were determined by scanning electron microscopy, transmission electron microscope and X-ray diffraction. The electrochemical performance of La2 MoO@MWCNTs composite catalysts for CEs was determined by photocurrent-voltage measurements, cyclic voltammetry,electrochemical impedance spectroscopy, and Tafel polarization. The power conversion efficiencies of4.68%, 4.87% and 5.06% are obtained for La2 MoO:MWCNTs with the mass ratios of 5:1, 3:1 and 1:1 towards the reduction of I~-to I~-under the same conditions,respectively,which are superior to those of MWCNTs(3,94%) and La2 MoO(1.71%) electrodes. The experimental results reveal that the presence of MWCNTs results in an augmented active catalytic surface area and enhanced charge transfer from CE to the electrolyte.展开更多
The development of a simple, efficient and sensitive sensor for dissolved oxygen is proposed using a novel type of porous carbon composite membrane/glassy carbon electrode based on the low-cost common filter paper by ...The development of a simple, efficient and sensitive sensor for dissolved oxygen is proposed using a novel type of porous carbon composite membrane/glassy carbon electrode based on the low-cost common filter paper by a simple method. The resulting device exhibited excellent electrocatalytic activities toward the oxygen reduction reaction. Scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy and electrochemical measurements demonstrated that the porous morphology and uniformly dispersed Fe;C nanoparticles of the PCCM play an important role in the oxygen reduction reaction. A linear response range from 2mmol/L up to 110 mmol/L and a detection limit of 1.4 mmol/L was obtained with this sensor. The repeatability of the proposed sensor,evaluated in terms of relative standard deviation, was 3.0%. The successful fabrication of PCCM/GC electrode may promote the development of new porous carbon oxygen reduction reaction material for the oxygen reduction sensor.展开更多
Perovskite solar cells(PSCs)have become the represent-atives of next generation of photovoltaics;nevertheless,their stability is insufficient for large scale deployment,particularly the reverse bias stability.Here,we ...Perovskite solar cells(PSCs)have become the represent-atives of next generation of photovoltaics;nevertheless,their stability is insufficient for large scale deployment,particularly the reverse bias stability.Here,we propose a transparent conducting oxide(TCO)and low-cost metal composite electrode to improve the stability of PSCs without sacrificing the efficiency.The TCO can block ion migrations and chemical reactions between the metal and perovskite,while the metal greatly enhances the conductivity of the composite electrode.As a result,composite electrode-PSCs achieved a power conversion efficiency(PCE)of 23.7%(certified 23.2%)and exhibited excellent stability,maintaining 95%of the initial PCE when applying a reverse bias of 4.0 V for 60 s and over 92%of the initial PCE after 1000 h continuous light soaking.This composite electrode strategy can be extended to different combinations of TCOs and metals.It opens a new avenue for improving the stability of PSCs.展开更多
The direct electron transfer of hemoglobin at the PAMAM-MWNTs-AuNPs composite film modified glassy carbon electrode was studied. In a phosphate buffer solution（PBS, pH=7.0）, the formal potential（E^0） of Hb was -0....The direct electron transfer of hemoglobin at the PAMAM-MWNTs-AuNPs composite film modified glassy carbon electrode was studied. In a phosphate buffer solution（PBS, pH=7.0）, the formal potential（E^0） of Hb was -0.105 V versus SCE, the electron transfer rate constant was 4.66 s-1. E^0＇ of Hb at the modified electrode was linearly varied in a pH range of 5.0-8.0 with a slope of-49.2 mV/pH. The Hb/PAMAM-MWNTs-AuNPs/GCE gave an excellent electrocatalytic response to the reduction of hydrogen peroxide. The catalytic current increased linearly with H2O2 concentration in a range of 1.0× 10^-6 to 2.2× 10^-3 mol/L. The detection limit was 2.0× 10^-7 mol/L at a signal to noise ratio of 3. The Michaelis-Menten constant（Km^app） was 2.95 mmol/L.展开更多
To promote the electrocatalytic activity and stability of traditional(a_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(LSCF)oxygen electrodes in reversible solid oxide cells(RSOCs),conventional physical mixed method was used t...To promote the electrocatalytic activity and stability of traditional(a_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(LSCF)oxygen electrodes in reversible solid oxide cells(RSOCs),conventional physical mixed method was used to prepare the Pd-LSCF composite oxygen electrode.The cell with Pd-LSCF|GDC|YSZ|Ni-YSZ configuration shows perfect electrochemical performance in both solid oxide fuel cell(SOFC)mode and solid oxide electrolysis cell(SOEC)mode.In the SOFC mode,the cell achieves a power density of 1.73 W/cm^(2)at800℃higher than that of the LSCF oxygen electrode with 1.38 W/cm^(2).In the SOEC mode,the current density at 1.5 V is 1.67 A/cm^(2)at 800℃under 50 vol%steam concentration.Moreover,the reversibility and stability of the RSOCs were tested during 192 h long-term reversible operation.The degradation rate of the cell is only 2.2%/100 h and 2.5%/100 h in the SOEC and the SOFC modes,respectively.These results confirm that compositing Pd with the LSCF oxygen electrode can considerably boost the electrochemical performance of LSCF electrode in RSOCs field.展开更多
Composite electrodes prepared by cation exchange resins and activated carbon(AC)were used to adsorb Ⅴ(Ⅳ)in capacitive deionization(CDI).The electrode made of middle resin size(D860/AC M)had the largest specific surf...Composite electrodes prepared by cation exchange resins and activated carbon(AC)were used to adsorb Ⅴ(Ⅳ)in capacitive deionization(CDI).The electrode made of middle resin size(D860/AC M)had the largest specific surface area and mesoporous content than two other composite electrodes.Electrochemical analysis showed that D860/AC M presents higher specific capacitance and electrical double layer capacitor than the others,and significantly lower internal diffusion impedance.Thus,D860/AC M exhibits the highest adsorption capacity and rate of Ⅴ(Ⅳ)among three electrodes.The intra-particle diffusion model fits well in the initial adsorption stage,while the liquid film diffusion model is more suitable for fitting at the later stage.The pseudo-second-order kinetic model is suited for the entire adsorption process.The adsorption of Ⅴ(Ⅳ)on the composite electrode follows that of the Freundlich isotherm.Thermodynamic analysis indicates that the adsorption of Ⅴ(Ⅳ)is an exothermic process with entropy reduction,and the electric field force plays a dominant role in the CDI process.This work aims to improve our understanding of the ion adsorption behaviors and mechanisms on the composite electrodes in CDI.展开更多
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.NRF-2021M3H4A1A02048529)the Ministry of Trade,Industry and Energy(MOTIE)of the Korean government under grant No.RS-2022-00155854support from the DGIST Supercomputing and Big Data Center.
文摘To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well.Herein,we suggest an effective approach to control the micropore structure of silicon oxide(SiO_(x))/artificial graphite(AG)composite electrodes using a perforated current collector.The electrode features a unique pore structure,where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance,leading to a 20%improvement in rate capability at a 5C-rate discharge condition.Using microstructure-resolved modeling and simulations,we demonstrate that the patterned micropore structure enhances lithium-ion transport,mitigating the electrolyte concentration gradient of lithium-ion.Additionally,perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiO_(x)/AG composite electrode,significantly improving adhesion strength.This,in turn,suppresses mechanical degradation and leads to a 50%higher capacity retention.Thus,regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiO_(x)/AG composite electrodes,providing valuable insights into electrode engineering.
基金supported by the Fundamental Research Funds for the Central Universities(WK2090000055)Anhui Provincial Natural Science Foundation of China(2308085QG231).
文摘As a negative electrode material for lithium-ion batteries,silicon monoxide(SiO)suffers from dramatic volume changes during cycling,causing excessive stress within the electrode and resulting in electrode deformation and fragmentation.This ultimately leads to a decrease in cell capacity.The trends of volume expansion and capacity change of the SiO/graphite(SiO/C)composite electrode during cycling were investigated via in situ expansion monitoring.First,a series of expansion test schemes were designed,and the linear relationship between negative electrode expansion and cell capacity degradation was quantitatively analyzed.Then,the effects of different initial pressures on the long-term cycling performance of the cell were evaluated.Finally,the mechanism of their effects was analyzed by scanning electron microscope.The results show that after 50 cycles,the cell capacity decreases from 2.556 mAh to 1.689 mAh,with a capacity retention ratio(CRR)of only 66.08%.A linear relationship between the capacity retention ratio and thickness expansion was found.Electrochemical measurements and scanning electron microscope images demonstrate that intense stress inhibits the lithiation of the negative electrode and that the electrode is more susceptible to irreversible damage during cycling.Overall,these results reveal the relationship between the cycling performance of SiO and the internal pressure of the electrode from a macroscopic point of view,which provides some reference for the application of SiO/C composite electrodes in lithium-ion batteries.
基金supported by the National Natural Science Foundation of China(Grants Nos.12172102 and 12372097)the Fundamental Research Funds for the Central Universities(Grant No.HIT.OCEF.2022013).
文摘The silicon-graphite(Si-C)composite electrode is considered a promising candidate for next-generation commercial electrodes due to its high capacity.However,lithium-ion batteries with silicon electrodes often experience capacity fading and poor cyclic performance,primarily due to the mechanical degradation of the solid-electrolyte interphase(SEI).In this work,we present a homogenized constitutive model for Si-C composite electrodes under finite deformation,incorporating lithium-ion concentration-dependent properties.We perform a wrinkling analysis and systematically examine the influence of key parameters,such as modulus and thickness ratios,on the critical conditions for instability.Additionally,we investigate the ratcheting effect across varying silicon contents.Our findings reveal that maintaining the silicon content within an optimal range effectively reduces plastic accumulation during charge–discharge cycles.These insights provide crucial guidance for optimizing the design and fabrication of Si–C electrode systems,enhancing their durability and performance.
基金supported by the Beijing Municipal Education Commission(Grant No.KM202311232008)the National Natural Science Foundation of China(Grant No.12002343).
文摘All-solid-state lithium metal batteries(ASSLMBs)are widely recognized as promising next-generation energy storage technologies that offer significant advantages in terms of safety and energy density.However,the long-term cycling stability of these batteries is often compromised by interfacial failures driven by coupled mechanical and diffusion effects.This study presents a probabilistic failure prediction model that quantifies interfacial damage and capacity loss in composite electrodes under the coupled influence of mechanical-diffusion-induced processes.We first develop a pseudo3D(P3D)interface failure model for a binary particle system to evaluate interfacial failure during the critical delithiation process.The P3D model is validated through mechanical‒diffusion coupled simulations.Additionally,for multiparticle composite electrode films with heterogeneous particle sizes,we identify a key structural factor that governs the failure of the particle‒solid electrolyte interface,which follows a three-parameter Burr distribution.Building on this,we develop a probabilistic model to predict the capacity fade in multiporject composite films.This work provides a comprehensive understanding of the critical geometric factors that influence interfacial stability,offering valuable theoretical insights and practical guidance for the rapid assessment,optimization,and enhancement of cycling stability in ASSLMBs.
基金financially supported by the National Natural Science Foundation of China(Nos.52075351,51604177)the National Key Research and Development Program of China(No.2019YFA0705701)+4 种基金the National Funded Postdoctoral Researcher Program(No.GZC20231762)the Major S&T Infrastructure Construction Project of Sichuan Province(No.2020-510000-73-01441847)the International S&T Innovation Cooperation Program of Sichuan Province(No.2020YFH0039)the Chengdu International S&T Cooperation Funded Project(Nos.2020-GH02-00006HZ,2022-GH02-00027-HZ)the“1000 Talents Plan”of Sichuan Province,and the Talent Introduction Program of Sichuan University(No.YJ201410)。
文摘Anode active materials involving transition metal oxides and sulfides are of great significance for high energy density lithium-ion batteries(LIBs),but the huge volume expansion and inferior electronic conductivity upon cycling critically constrain their further application.Herein,from a new perspective,a highly conductive and stable 3D flexible composite current collector is rationally designed by facilely electrodepositing metallic Ni thin layer onto the carbon cloth(CC/Ni),which endows the supported active materials with exceptional electronic conductivity and structural stability.In addition,the homogeneously distributed metallic Ni protrusions external CC can strongly bond with the active components,ensuring the structural integrity of electrodes upon cycling.More importantly,the 3D network structure with large specific surface area provides abundant space to alleviate the volume expansion and more active sites for electrochemical reactions.Therefore,taking Ni_(3)S_(2)nanosheet(Ni_(3)S_(2)NS)anode as an example,the prepared Ni_(3)S_(2)NS@CC/Ni electrode shows a high specific capacity of 2.32 mAh/cm^(2)at 1mA/cm^(2)and high capacity retention of 1.68 mAh/cm^(2)at a high rate of 8mA/cm^(2).This study provides a universal approach to obtain highly conductive and stable 3D flexible current collectors towards high performance metal-ion batteries beyond LIBs.
基金supported by the National Natural Science Foundation of China(Grant Nos.12072183,12472174,and 12421002).
文摘The recently reported silicon/graphite(Si/Gr)composite electrode with a layered structure is a promising approach to achieve high capacity and stable cycling of Si-based electrodes in lithium-ion batteries.However,there is still a need to clarify why particular layered structures are effective and why others are ineffective or even detrimental.In this work,an unreported mechanism dominated by the porosity evolution of electrodes is proposed for the degradation behavior of layered Si/Gr electrodes.First,the effect of layering sequence on the overall electrode performance is investigated experimentally,and the results suggest that the cycling performance of the silicon-on-graphite(SG)electrode is much superior to that of the graphite-on-silicon electrode.To explain this phenomenon,a coupled mechanical-electrochemical porous electrode model is developed,in which the porosity is affected by the silicon expansion and the local constraints.The modeling results suggest that the weaker constraint of the silicon layer in the SG electrode leads to a more insignificant decrease in porosity,and consequently,the more stable cycling performance.The findings of this work provide new insights into the structural design of Si-based electrodes.
基金Project(51004056) supported by the National Natural Science Foundation of ChinaProject(KKZ6201152009) supported by the Opening Foundation of Key Laboratory of Inorganic Coating Materials,Chinese Academy of Sciences+2 种基金Project(2010ZC052) supported by the Applied Basic Research Foundation of Yunnan Province,ChinaProject(20125314110011) supported by the Specialized Research Fund for the Doctoral Program of Higher EducationProject(2010247) supported by Analysis & Testing Foundation of Kunming University of Science and Technology,China
文摘In order to investigate the effect of solid particles dopants on physicochemical properties of α-PbO2 electrodes, a-PbO2 composite electrodes doped with nano-TiO2 and nano-CeO2 particles were respectively prepared on A1/conductive coating electrodes in 4 mol/L NaOH solution with addition of PbO until saturation by anodic codeposition. The electrodeposition mechanism, morphology, composition and structure of the composite electrodes were characterized by cyclic voltarnmogram （CV）, SEM, EDAX and XRD. Results show that the doping solid particles can not change reaction mechanism of α-PbO2 electrode in alkaline or acid plating bath, but can improve deposition rate and reduce oxygen evolution potential. The doping solid particles can inhibit the growth of a-PbO2 unit cell and improve specific surface area. The diffraction peak intensity of a-PbO2-CeO2-TiO2 composite electrode is lower than that of pure a-PbO2 electrode. The electrocatalytic activity of a-PbO2-2.12%CEO2-3.71%TIO2 composite electrode is the best. The Guglielmi model for CeO2 and TiO2 codeposition with a-PbO2 is also pronosed.
基金Projects(51004056,51004057)supported by the National Natural Science Foundation of ChinaProject(KKZ6201152009)supported by the Opening Foundation of Key Laboratory of Inorganic Coating Materials,Chinese Academy of Sciences+2 种基金Project(2010ZC052)supported by the Applied Basic Research Foundation of Yunnan Province,ChinaProject(20125314110011)supported by the Specialized Research Fund for the Doctoral Program of Higher Education,ChinaProject(2010247)supported by Analysis&Testing Foundation of Kunming University of Science and Technology,China
文摘Al/conductive coating/α-Pb O2-Ce O2-Ti O2/β-PbO 2-MnO 2-WC-Zr O2 composite electrode material was prepared on Al/conductive coating/α-PbO 2-Ce O2-Ti O2 substrate by electrochemical oxidation co-deposition technique. The effects of current density on the chemical composition, electrocatalytic activity, and stability of the composite anode material were investigated by energy dispersive X-ray spectroscopy（EDXS）, anode polarization curves, quasi-stationary polarization（Tafel） curves, electrochemical impedance spectroscopy（EIS）, scanning electron microscopy（SEM）, and X-ray diffraction（XRD）. Results reveal that the composite electrode obtained at 1 A/dm2 possesses the lowest overpotential（0.610 V at 500 A/m2） for oxygen evolution, the best electrocatalytic activity, the longest service life（360 h at 40 °C in 150 g/L H2SO4 solution under 2 A/cm2）, and the lowest cell voltage（2.75 V at 500 A/m2）. Furthermore, with increasing current density, the coating exhibits grain growth and the decrease of content of Mn O2. Only a slight effect on crystalline structure is observed.
基金supported by the Programs of National 973 (2011CB935900)NSFC (51231003 and 21231005)+1 种基金111 Project (B12015)Tianjin High-Tech (10SYSYJC27600)
文摘The synthetic routes of porous carbons and the applications of the functional porous carbon-based composite electrode materials for lithium secondary batteries are reviewed. The synthetic methods have made great breakthroughs to control the pore size and volume, wall thickness, surface area, and connectivity of porous carbons, which result in the development of functional porous carbon-based composite electrode materials. The effects of porous carbons on the electrochemical properties are further discussed. The porous carbons as ideal matrixes to incorporate active materials make a great improvement on the electrochemical properties because of high surface area and pore volume, excellent electronic conductivity, and strong adsorption capacity. Large numbers of the composite electrode materials have been used for the devices of electrochemical energy conversion and storage, such as lithium-ion batteries （LIBs）, Li-S batteries, and Li-O2 batteries. It is believed that functional porous carbon-based composite electrode materials will continuously contribute to the field of lithium secondary batteries.
基金supported by the strategic grant POSDRU/88/1.5/S/50783POSDRU/21/1.5/G/13798+1 种基金POSDRU/89/1.5/S/57649 co-financed by the European Social Fund - Investing in People,within the Sectoral Operational Programme Human Resources Development 2007-2013partially by the PN II-RU-PD129/2010 and PN II Ideas 165/2011
文摘This work describes the electrochemical behaviour of ibuprofen on two types of multi-walled carbon nanotubes based composite electrodes, i.e., multi-walled carbon nanotubes-epoxy （MWCNT） and silver-modified zeolite-multi-wailed carbon nanotubes-epoxy （AgZMWCNT） composites electrodes. The composite electrodes were obtained using two-roll mill procedure. SEM images of surfaces of the composites revealed a homogeneous distribution of the composite components within the epoxy matrix. AgZMWCNT composite electrode exhibited the better electrical conductivity and larger electroactive surface area. The electrochemical determination of ibuprofen （IBP） was achieved using AgZMWCNT by cyclic voltammetry, differential-pulsed voltammetry, square-wave voltammetry and chronoamperometry. The IBP degradation occurred on both composite electrodes under controlled electrolysis at 1.2 and 1.75 V vs. Ag/AgCl, and IBP concentration was determined comparatively by differential-pulsed voltammetry, under optimized conditions using AgZMWCNT electrode and UV-Vis spectrophotometry methods to determine the IBP degradation performance for each electrode. AgZMWCNT electrode exhibited a dual character allowing a double application in IBP degradation process and its control.
基金Project supported by Foundation of State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences (CAS)
文摘Composite LaNi5+x wt.% Ti0.10Zr0.16V0.34Cr0.10Ni0.30 (x=0, 1, 5, 10) alloys were prepared by two-step re-melting. X-ray diffractometer (XRD), scanning electron microscopy (FESEM), energy dispersive spectrometry (EDS), inductively coupled plasma (ICP) and electrochemical impedance spectroscopy (EIS) analyses showed that the matrix phase of LaNi5 alloy with CaCu5 structure remained unchanged after additive alloy was added, the amount of the second phase increased with increasing x. The synergetic effect withi...
基金Project(2005CB623703) supported by the National Basic Research Program of China project(5JJ30103) supported bythe Natural Science Foundation of Hunan Province
文摘Taking the nano-sized carbon black and aniline monomer as precursor and （NH4）2S2O6 as oxidant, the well coated C/polyaniline（C/PANI） composite materials were prepared by in situ polymerization of the aniline on the surface of well-dispersed nano-sized carbon black for supercapacitor. The micro-structure of the C/PANI composite electrode materials were analyzed by SEM. The electrochemical properties of C/ PANI and PANI composite electrode were characterized by means of the galvanostatic charge-discharge experiment, cyclic voltammetric measurement and impedance spectroscopy analysis. The results show that by adding the nano-sized carbon black in the process of chemical polymerization of the aniline, the polyaniline can be in situ polymerized and well-coated onto the carbon black particles, which may effectively improve the aggregation of particles and the electrolyte penetration. What’s more , the maximum of specific capacitance of C/PANI electrode 437.6F·g -1 can be attained. Compared with PANI electrode, C/PANI electrode shows more desired capacitance characteristics, smaller internal resistance and better cycle performance.
基金Supported by the National Natural Science Foundation of China(No.51502117,No.21671084)Key Research&Development Plan of Zhenjiang City(No.SH2017051)+1 种基金Foundation from Marine Equipment and Technology Institute for Jiangsu University of Science and Technology(No.HZ20170015)Six Talent Peaks Project in Jiangsu Province(No.2014-XCL-008)
文摘PbO2/Co3O4 composites were prepared on a Ti substrate by means of a composite electrodeposition method in Pb2+ plating solution containing dissolved nano-Co3O4 particles. X-ray diffraction（XRD）, scanning electron microscopy（SEM）, energy dispersive spectrometry（EDS） and transmission electron microscopy（TEM） were used to characterize the chemical composition and morphology of the PbO2/Co3O4 composites. The electrochemical and capacitance performance of the composites were investigated by cyclic voltammetry（CV）, charge-discharge tests and electrochemical impedance（EIS）. The results indicate that the composites comprise rutile phase Co3O4 and β-PbO2. In addition, the surface of the composite electrode is rough and porous. The PbO2/Co3O4 composites exhibit a high specific capacitance up to 215 F/g, which is ten times higher than that of the pure-PbO2 and two times higher than that of the pure-Co3O4 in 1 mol/L NaOH electrolytes.
基金supported by the National Key Research and Development Program of China,China(2019YFA0705102)the National Natural Science Foundation of China,China(22179144,22005332)。
文摘Thick electrodes can increase incorporation of active electrode materials by diminishing the proportion of inactive constituents,improving the overall energy density of batteries.However,thick electrodes fabricated using the conventional slurry casting approach frequently exhibit an exacerbated accumulation of carbon additives and binders on their surfaces,invariably leading to compromised electrochemical properties.In this study,we introduce a designed conductive agent/binder composite synthesized from carbon nanotube and polytetrafluoroethylene.This agent/binder composite facilitates production of dry-process-prepared ultra-thick electrodes endowed with a three-dimensional and uniformly distributed percolative architecture,ensuring superior electronic conductivity and remarkable mechanical resilience.Using this approach,ultra-thick LiCoO_(2)(LCO) electrodes demonstrated superior cycling performance and rate capabilities,registering an impressive loading capacity of up to 101.4 mg/cm^(2),signifying a 242% increase in battery energy density.In another analytical endeavor,time-of-flight secondary ion mass spectroscopy was used to clarify the distribution of cathode electrolyte interphase(CEI) in cycled LCO electrodes.The results provide unprecedented evidence explaining the intricate correlation between CEI generation and carbon distribution,highlighting the intrinsic advantages of the proposed dry-process approach in fine-tu ning the CEI,with excellent cycling performance in batteries equipped with ultra-thick electrodes.
基金Project supported by the National Natural Science Foundation of China(21473048 and 21303039)the Natural Science Foundation of Hebei Province(B2015205163,B2016205161)the 2015 Hebei Province Undergraduate Training Programs for Innovation and Entrepreneurship
文摘Pt-free counter electrode(CE) composed of La2 MoO(LaO-MoO) was successfully synthesized by simple pyrolysis of lanthanum acetate(CHOLa·xHO) and hexaammonium heptamolybdate tetrahydrate((NH4)6 MoO·4 HO). Furthermore,three proportions composites catalysts of La2 MoO@MWCNTs based on La2 MoOand multiwall carbon nanotubes(MWCNTs) were prepared and characterized as Ptfree catalyst for CE in dye-sensitized solar cells(DSSCs). The morphology and structure of La2 MoO@MWCNTs composites were determined by scanning electron microscopy, transmission electron microscope and X-ray diffraction. The electrochemical performance of La2 MoO@MWCNTs composite catalysts for CEs was determined by photocurrent-voltage measurements, cyclic voltammetry,electrochemical impedance spectroscopy, and Tafel polarization. The power conversion efficiencies of4.68%, 4.87% and 5.06% are obtained for La2 MoO:MWCNTs with the mass ratios of 5:1, 3:1 and 1:1 towards the reduction of I~-to I~-under the same conditions,respectively,which are superior to those of MWCNTs(3,94%) and La2 MoO(1.71%) electrodes. The experimental results reveal that the presence of MWCNTs results in an augmented active catalytic surface area and enhanced charge transfer from CE to the electrolyte.
基金the National Natural Science Foundation of China (No.21273097)the project from the State Key Laboratory of Electroanalytical Chemistry (No.2013)the Science Foundation of Jilin Province (No.20130204003GX)
文摘The development of a simple, efficient and sensitive sensor for dissolved oxygen is proposed using a novel type of porous carbon composite membrane/glassy carbon electrode based on the low-cost common filter paper by a simple method. The resulting device exhibited excellent electrocatalytic activities toward the oxygen reduction reaction. Scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy and electrochemical measurements demonstrated that the porous morphology and uniformly dispersed Fe;C nanoparticles of the PCCM play an important role in the oxygen reduction reaction. A linear response range from 2mmol/L up to 110 mmol/L and a detection limit of 1.4 mmol/L was obtained with this sensor. The repeatability of the proposed sensor,evaluated in terms of relative standard deviation, was 3.0%. The successful fabrication of PCCM/GC electrode may promote the development of new porous carbon oxygen reduction reaction material for the oxygen reduction sensor.
基金supported by National Natural Science Foundation of China(No.21872080)National Key Research and Development Program of China(2022YFB3803304)+2 种基金supported by Tsinghua University Initiative Scientific Research Program(20221080065,20223080044)The State Key Laboratory of Power System and Generation Equipment(Nos.SKLD21Z03 and SKLD20M03)the Chinese Thousand Talents Program for Young Professionals.
文摘Perovskite solar cells(PSCs)have become the represent-atives of next generation of photovoltaics;nevertheless,their stability is insufficient for large scale deployment,particularly the reverse bias stability.Here,we propose a transparent conducting oxide(TCO)and low-cost metal composite electrode to improve the stability of PSCs without sacrificing the efficiency.The TCO can block ion migrations and chemical reactions between the metal and perovskite,while the metal greatly enhances the conductivity of the composite electrode.As a result,composite electrode-PSCs achieved a power conversion efficiency(PCE)of 23.7%(certified 23.2%)and exhibited excellent stability,maintaining 95%of the initial PCE when applying a reverse bias of 4.0 V for 60 s and over 92%of the initial PCE after 1000 h continuous light soaking.This composite electrode strategy can be extended to different combinations of TCOs and metals.It opens a new avenue for improving the stability of PSCs.
基金Supported by the National Natural Science Foundation of China(No.20605009)
文摘The direct electron transfer of hemoglobin at the PAMAM-MWNTs-AuNPs composite film modified glassy carbon electrode was studied. In a phosphate buffer solution（PBS, pH=7.0）, the formal potential（E^0） of Hb was -0.105 V versus SCE, the electron transfer rate constant was 4.66 s-1. E^0＇ of Hb at the modified electrode was linearly varied in a pH range of 5.0-8.0 with a slope of-49.2 mV/pH. The Hb/PAMAM-MWNTs-AuNPs/GCE gave an excellent electrocatalytic response to the reduction of hydrogen peroxide. The catalytic current increased linearly with H2O2 concentration in a range of 1.0× 10^-6 to 2.2× 10^-3 mol/L. The detection limit was 2.0× 10^-7 mol/L at a signal to noise ratio of 3. The Michaelis-Menten constant（Km^app） was 2.95 mmol/L.
基金Project supported by the National Key Research&Development Project(2020YFB1506304)the National Natural Science Foundation of China(52172199,52072135,52002121)。
文摘To promote the electrocatalytic activity and stability of traditional(a_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(LSCF)oxygen electrodes in reversible solid oxide cells(RSOCs),conventional physical mixed method was used to prepare the Pd-LSCF composite oxygen electrode.The cell with Pd-LSCF|GDC|YSZ|Ni-YSZ configuration shows perfect electrochemical performance in both solid oxide fuel cell(SOFC)mode and solid oxide electrolysis cell(SOEC)mode.In the SOFC mode,the cell achieves a power density of 1.73 W/cm^(2)at800℃higher than that of the LSCF oxygen electrode with 1.38 W/cm^(2).In the SOEC mode,the current density at 1.5 V is 1.67 A/cm^(2)at 800℃under 50 vol%steam concentration.Moreover,the reversibility and stability of the RSOCs were tested during 192 h long-term reversible operation.The degradation rate of the cell is only 2.2%/100 h and 2.5%/100 h in the SOEC and the SOFC modes,respectively.These results confirm that compositing Pd with the LSCF oxygen electrode can considerably boost the electrochemical performance of LSCF electrode in RSOCs field.
基金financially supported by the National Natural Science Foundation of China(No.51874222).
文摘Composite electrodes prepared by cation exchange resins and activated carbon(AC)were used to adsorb Ⅴ(Ⅳ)in capacitive deionization(CDI).The electrode made of middle resin size(D860/AC M)had the largest specific surface area and mesoporous content than two other composite electrodes.Electrochemical analysis showed that D860/AC M presents higher specific capacitance and electrical double layer capacitor than the others,and significantly lower internal diffusion impedance.Thus,D860/AC M exhibits the highest adsorption capacity and rate of Ⅴ(Ⅳ)among three electrodes.The intra-particle diffusion model fits well in the initial adsorption stage,while the liquid film diffusion model is more suitable for fitting at the later stage.The pseudo-second-order kinetic model is suited for the entire adsorption process.The adsorption of Ⅴ(Ⅳ)on the composite electrode follows that of the Freundlich isotherm.Thermodynamic analysis indicates that the adsorption of Ⅴ(Ⅳ)is an exothermic process with entropy reduction,and the electric field force plays a dominant role in the CDI process.This work aims to improve our understanding of the ion adsorption behaviors and mechanisms on the composite electrodes in CDI.
