Fatigue-less relaxor ferroelectric thin films with high energy storage density via defect engineer

Thin film capacitors with excellent energy storage performances,thermal stability and fatigue endurance are strongly desired in modern electrical and electronic industry.Herein,we design and prepare lead-free0.7Sr_(0.7)Bi_(0.2)TiO_(3)-0.3BiFeO_(3)-x%Mn(x=0,0.5,1.5,2,3)thin films via sol-gel method.Mn ions of divalent valence combine with oxygen vacancies,forming defect complex,which results in marked decline in leakage current and obvious enhancement in breakdown strength.A high energy storage density~47.6 J cm^(-3)and good efficiency~65.68%are simultaneously achieved in 2%Mn doped 0.7Sr_(0.7)Bi_(0.2)TiO_(3)-0.3 BiFeO_(3)thin film capacitor.Moreover,the 2%Mn-doped thin film exhibits excellent thermal stability in wide operating temperature range(35–115℃)and strong fatigue endurance behaviors after 108 cycles.The above results demonstrate that 2%Mn-doped 0.7Sr_(0.7)Bi_(0.2)TiO_(3)-0.3 BiFeO_(3)thin film capacitor with superior energy storage performances is a potential candidate for electrostatic energy storage.

Preparation and investigation on properties of BST-base ceramic with high-energy storage density

The Ba_(0.3)Sr_(0.6)Ca_(0.1)TiO_(3)(BSCT)powder was prepared through the solid-state reaction.And then preparing ceramic samples with quantitative doped-Bi_(2)O_(3)·3TiO_(2) and diferent doped-MgO.X-ray diffractometer(XRD)and scanning electron microscopy(SEM)were used to investigate the phase compositions,distribution and morphology of the ceramic samples.SM-11J49 capacitance measurement instrument and CS2674A pressure tester were used to measure the dieletric properties of the samples.The results show that the compactness and the dielectric constant of the ceramics increases first and then decreases when the doped MgO content was changed from 1.5 to 4.5 wt.%.The trend of breakdown strength is characterized by M-shaped pattern with the increase of doped-MgO content.Calculation results demonstrate that when the doped-MgO content is 2.0%,the samples have the highest energy storage density.

Optimization of synergistic energy storage density and efficiency for eco-friendly (Na_(0.5)Bi_(0.5))_(0.6)Sr_(0.4)TiO_(3)-based relaxor ferroelectric ceramics

Inspired by increasing demand of advanced pulsed power capacitors,the development of lead-free dielectric ceramic capacitors with high energy storage density and temperature-insensitive performance are extremely crucial.Herein,the lead-free relaxor ferroelectric ceramics based on(1-x)(Na_(0.5)Bi_(0.5))0.6Sr_(0.4)TiO_(3-x)Sr_(0.7)La_(0.2)ZrO_(3)[abbreviated as(1-x)NBST-xSLZ]are prepared by the solid-state reaction route.The large recoverable energy density(Wrec)of 3.45 J/cm^(3) and efficiency(h)of 90.1%are simultaneously realized in 0.86NBST-0.14SLZ ceramic due to increased breakdown strength.Furthermore,both the Wrec and h of 0.86NBST-0.14SLZ ceramic display superior of thermal stability(20e180C),frequency stability(1e1000 Hz),and cycle stability(10^(4))within a satisfactory range of variation.In addition,the 0.86NBST-0.14SLZ ceramic can also achieve a large current density(CD)of 625 A/cm^(2),an ultrahigh power density(PD)of 50 MW/cm^(3) and a fast discharge rate(t0.90)of 160.8 ns at 160 kV/cm.These results demonstrate that the 0.86NBST-0.14SLZ ceramic could be a highly competitive and ecofriendly relaxor ferroelectric material for next-generation pulsed power capacitors.

Scaling behavior of different shapes of hysteresis loops and recoverable energy storage density in Na_(0.5)Bi_(0.5)TiO_(3), K_(0.5)Bi_(0.5)TiO_(3), and Na_(0.25)K_(0.25)Bi_(0.5)TiO_(3) ferroelectrics

In this work,the dependency of the polarization(P)-electric field(E)loop area A of lead free ferro-electrics Na_(0.5)Bi_(0.5)TiO_(3)(NBT), K_(0.5)Bi_(0.5)TiO_(3)(KBT),and Na_(0.25)K_(0.25)Bi_(0.5)TiO_(3)(NKBT)on the amplitude(E0)of the electric field is studied.Based on the nature of the hysteresis loop with increasing E0,the lnA versus lnE0 graph is divided into three stages and the scaling exponents of each stage are estimated.In the third stage,NBT,KBT,and NKBT show different shapes of P-E loops(square,slanted and pinched,respectively).Although,almost similar slopes in the third stage are obtained from the lnA versus lnE0 graphs of KBT and NKBT,the formation of pinched P-E loop of NKBT is discussed based on the current-time curve under a complete cycle of the applied electric field.The shape of the P-E loop also affects the recoverable energy storage density(Wrec)of the material.Similar to the scaling of A,the variation of lnWrec with lnE0 of NBT,KBT and NKBT are examined.Interestingly,three stages are only noticed in the lnWrec-lnE0 curve of pinched P-E loop(NKBT),whereas lnWrec linearly increases with lnE0 for square and slanted P-E loop.Such type of behavior of Wrec of NKBT is explained based on the reversible domain switching mechanism of the pinched P-E loop.

Spontaneous local redox reaction to passivate CNTs as lightweight current collector for high energy density lithium ion batteries

Extensive usage of highly conductive carbon materials with large specific surface area(e.g.,carbon nanotubes,CNTs)in lithium ion batteries(LIBs),especially as current collector of anodes,suffers from low initial coulombic efficiency(ICE),large interfacial resistance,and severe embrittlement,as the large specific surface area often results in severe interfacial decomposition of the electrolyte and the formation of thick and fluffy solid electrolyte interphase(SEI)during cycling of LIBs.Herein,we demonstrate that when the CNT-based current collector and Na foil(which are being stacked intimately upon each other)are being placed in Na+-based organic electrolyte,local redox reaction between the Na foil and the electrolyte would occur spontaneously,generating a thin and homogeneous NaF-based passivating layer on the CNTs.More importantly,we found that owing to the weak solvation behaviors of Na+in the organic electrolyte,the resulting passivation layer,which is rich in NaF,is thin and dense;when used as the anode current collector in LIBs,the pre-existing passivating layer can function effectively in isolating the anode from the solvated Li+,thus suppressing the formation of bulky SEI and the destructive intercalation of solvated Li+.The relevant half-cell(graphite as anode)exhibits a high ICE of 92.1%;the relevant pouch cell with thus passivated CNT film as current collectors for both electrodes(LiCoO_(2)as cathode,graphite as anode)displays a high energy density of 255 Wh kg^(-1),spelling an increase of 50%compared with that using the conventional metal current collectors.

Dielectric and energy storage properties of PbO–SrO–Nb_(2)O_(5)–Na_(2)O–Si thin films by annealing

Dielectric and energy storage properties of PbOSrO-Na_(2)O-Nb_(2)O_(5)-SiO_(2)(PSNNS) thin films with annealing temperature from 700 to 850 ℃ were investigated by measuring their capacitance-electric filed curve and hysteresis loops.The results show that the highest dielectric constant and energy density are 81.2 and 17.0 J·cm^(-3),respectively,which is obtained in the sample with annealing temperature of 800 ℃.Annealed from 700 to800 ℃,the dielectric constant and energy storage performance of PSNNS films are continuously improved.However,with annealing temperature up to 850 ℃,their dielectric constant decreases,which might be related with the removal of interfacial defects as a function of annealing temperature.Defect is one of the causes of space charge phenomenon,resulting in the increase in dielectric constant.Moreover,the micro structure analysis by X-ray diffraction(XRD) and transmission electron microscope(TEM) indicates that the change of crystallization phase and interfacial polarization takes responsibility to the results.

Excellent energy storage performance in Bi_(0.5)Na_(0.5)TiO_(3)-based lead-free high-entropy relaxor ferroelectrics via B-site modification

Next-generation advanced high/pulsed power capacitors urgently require dielectric materials with outstanding energy storage performance.Bi_(0.5)Na_(0.5)TiO_(3)-based lead-free materials exhibit high polarization,but the high remanent polarization and large polarization hysteresis limit their applications in dielectric capacitors.Herein,high-entropy perovskite relaxor ferroelectrics(Na_(0.2)Bi_(0.2)Ba_(0.2)Sr_(0.2)Ca_(0.2))(Ti1-x%Zrx%)O_(3)are designed by adding multiple ions in the A-site and replacing the B-site Ti^(4+)with a certain amount of Zr^(4+).The newly designed system showed high relaxor feature and slim polarization-electric(P-E)loops.Especially,improved relaxor feature and obviously delayed polarization saturation were found with the increasing of Zr^(4+).Of particular importance is that both high recoverable energy storage density of 6.6 J/cm^(3) and energy efficiency of 93.5%were achieved under 550 kV/cm for the ceramics of x=6,accompanying with excellent frequency stability,appreciable thermal stability,and prosperous discharge property.This work not only provides potential dielectric materials for energy storage applications,but also offers an effective strategy to obtain dielectric ceramics with ultrahigh comprehensive energy storage performance to meet the demanding requirements of advanced energy storage applications.

Preparation and energy storage properties of <001>-textured NaNbO_(3)-based ceramics

Dielectric materials with high energy storage density(Wrec)and efficiency(η)are expected for energy storage capacitors.In this work,<001>-textured Na0.7Bi0.1NbO_(3)(NBN)ceramics were prepared by a templated grain growth technique.The effects of microstructure and orientation degree on dielectric properties,polarization and energy storage performance were investigated.The textured ceramic with an optimized orientation degree(70%)showed a high Wrec of 2.4 J/cm^(3) andηof 85.6%.The excellent energy storage properties of textured ceramic originate from the co-effect of interfacial polarization and clamping effect.The results indicate that texture development is a potential candidate to optimize the energy storage properties of functional ceramics.

Phase engineering in NaNbO_(3) antiferroelectrics for high energystorage density

The NaNbO_(3) antiferroelectrics have been considered as a potential candidate for dielectric capacitorsapplications. However, the high-electric-field-unstable antiferroelectric phase resulted in low energystorage density and efficiency. Herein, good energy storage properties were realized in (1-x)NaNbO_(3)- xNaTaO_(3) ceramics, by building a new phase boundary. As a result, a high recoverable energy density(Wrec) of 2.2 J/cm3 and efficiency (h) of 80.1% were achieved in 0.50NaNbO_(3)-0.50NaTaO_(3) ceramic at300 kV/cm. The excellent energy storage performance originates from an antiferroelectric-paraelectricphase boundary with simultaneously high polarization and low hysteresis, by tailoring the ratio ofantiferroelectric and paraelectric phases. Moreover, the 0.50NaNbO_(3)-0.50NaTaO_(3) ceramic also exhibitedgood temperature and frequency stability, together with excellent charge-discharge performance. Theresults pave a good way of designing new NaNbO_(3)-based antiferroelectrics with good energy storageperformance.

Improved breakdown strength and energy density of polyimide composites by interface engineering between BN and BaTiO3 fibers

Conventionally,interface effects between polymers and fillers are essential for determining the breakdown strength and energy storage density of polymer-based dielectric composites.In this study,we found that interface effects between different fillers have similar behavior.BN and Ba TiO3 fiber composite fillers with three different interface bonding strengths were successfully achieved by controlling composite processes(BT-fiber/BN<BT-fiber@BN<BT-fiber&BN),and introduced into a polyimide(PI)matrix to form composite films.Considerably enhanced breakdown strength and energy storage density were obtained in BT-fiber&BN/PI composites owing to strong interface bonding,compared to other two composite fillers,which are well supported by the data from the finite element simulation.Specifically,PI composites with only 3 wt%BT-fiber&BN possess an optimized energy storage density of approximately 4.25 J/cm^(3)at 4343 k V/cm.These results provide an effective way for adjusting and improving the energy storage properties of polymer-based composites.

Sodium bismuth titanate-based perovskite ceramics with high energy storage efficiency and discharge performance

Designing dielectric materials with the tremendous energy storage density is fundamentally important for developing pulse power capacitors.An effective approach was proposed to favorably modify the dielectric energy storage properties(ESP)of Bi_(0.5)Na_(0.5)TiO_(3) ceramics using CaTiO_(3) incorporation.The dielectric breakdown strength was effectively enhanced,and simultaneously the relaxor behavior was optimized to lower the remnant polarization,which is resulted from the decreased grains size with the introduction of Ca^(2+)ion.Remarkably,at a CaTiO_(3) doping level of 0.2,a 0.8Bi_(0.5)Na_(0.5)TiO_(3)-0.2CaTiO_(3)(0.8BNT-0.2CT)ceramic obtained both high energy storage density(Wtotal)of~1.38 J/cm^(3) together with excellent efficiency(h)of~91.3%.Furthermore,an ultrafast discharge response speed(t0:9)~94 ns was achieved in 0.8BNT-0.2CT ceramic,as well as tremendous current density(C_(D)~1520 A/cm2)and power density(P_(D)~115 MW/cm^(3)).This study not only revealed the superior ESP mechanism as regards Bi_(0.5)Na_(0.5)TiO_(3) based ceramics but also provided candidate materials in pulse power capacitor devices.

Excellent energy storage performance of niobate-based glass-ceramics via introduction of nucleating agent

For glass-ceramics, how to realize the collaborative optimization of BDS and permittivity is the key toimprove the energy storage density. In this work, ZrO2 is introduced into BPKNAS glass-ceramics asnucleating agent to promote crystal development of glass-ceramics and then achieve high permittivity.When 1.5 mol% ZrO2 is added, the glass-ceramics have the highest permittivity (~128.59) and meanwhilepossess high BDS (1948.90 kV/cm) due to the dense microstructure. Therefore, BPKNAS-1.5ZrO2 glass-ceramics has the highest theoretical energy storage density (21.62 J/cm3). Moreover, the permittivityvariation of BPKNAS-1.5ZrO2 glass-ceramics is less than 6 % in the wide temperature range from 80 to300 C, showing excellent temperature stability. In addition, BPKNAS-1.5ZrO2 glass-ceramics possessesultrahigh power density, which reaches up to 382.40 MW/cm3 in overdamped circuit. The above evi-dence shows that BPKNAS-1.5ZrO2 glass-ceramics with ultrahigh energy storage density and powerdensity is very competitive in the field of energy storage applications.

Low-temperature compression-assisted absorption thermal energy storage using ionic liquids

Thermal energy storage technologies play a significant role in building energy efficiency by balancing the mis-match between renewable energy supply and building energy demand.The absorption thermal energy storage(ATES)stands out due to its high energy storage density(ESD),high coefficient of performance(COP),low charg-ing temperature and wider application flexibility.A hybrid compression-assisted ATES(CATES)using ionic liquid(IL)-based working fluids is investigated to address the problems of the existing ATES cycle.Models for mixture property and cycle performance are established with verified accuracies.Four ILs([DMIM][DMP],[EMIM][Ac],[EMIM][DEP],and[EMIM][EtSO_(4)])are compared with H_(2)O/LiBr.Results show that the CATES effectively avoid the crystallization,decreases the circulation ratio,lowers the charging temperature,and improves the COP/ESD.H_(2)O/[DMIM][DMP]has the highest COP and performs better than H_(2)O/LiBr with generation temperatures above 86℃,while H_(2)O/[EMIM][EtSO_(4)]shows the highest COP with generation temperatures below 75℃.Among the H_(2)O/IL mixtures,H_(2)O/[EMIM][Ac]shows the highest ESD with generation temperatures above 86℃,otherwise H_(2)O/[EMIM][EtSO_(4)]shows the highest.The optimal compression ratio is 1.6-2.8 for H_(2)O/[DMIM][DMP]under the generation temperatures of 90-70℃with the maximum COP of 0.758-0.727.The ESD increases significantly with the compression ratio.

The First Principles Study of Li, Al and Ca Doped Zigzag(7,0) Single Walled Carbon Nanotube

We use the ab initio density functional theory to calculate the band structure, density of states, charge transfer, charge density difference, binding energy and vibration frequency. We can see that the conduction band through the Fermi level include SWNT/H_2/Li, SWNT/H_2/Al and SWNT/H_2/Ca, which shows a kind of metallic character. The charge distribution and contour plots of charge difference density of ion/H_2/SWNT show charge transfer between ion and H_2 molecules rather than between H_2 and H_2. Meanwhile, the interaction between Al, Ca and H_2 is weaker than that of Li. We can also prove that the ion is the primary reason to the increase of adsorption energy of hydrogen molecule in SWNT. Finally, we calculate the vibration frequency and don＇t find any imaginary frequency, which proves that the（7,0） SWNT is more stable.

A review of solid electrolytes for safe lithium-sulfur batteries

Due to the high specific capacity, low cost, and environmental friendliness, lithium-sulfur batteries hold great potential to become the mainstay of next-generation energy storage system. Regarding the composition of sulfur/carbon in cathode, flammable organic liquid electrolyte, and lithium metal anode, great concerns about the safety have been raised. Hence solid-electrolyte-based lithium-sulfur batteries, as one alternative route for safe batteries, are highly interested. This review highlights the recent research progress of lithium-sulfur batteries with solid electrolytes. Both sulfide solid electrolytes and oxide solid electrolytes are included.The sulfide solid electrolytes are mainly employed in all-solid-state lithium-sulfur batteries, while the oxide solid electrolytes are applied in hybrid electrolyte for lithium-sulfur batteries. The challenges and perspectives in this field are also featured on the basis of its current progress.

A non-aqueous Li/organosulfur semi-solid flow battery

Non-aqueous flow batteries have attracted extensive attention due to the advantages of wide voltagewindow, high energy density and wide operating temperature and so on. Herein, tetramethylthiuramdisulfide （TMTD） with high intrinsic capacity （223 mAh/g） and high solubility （-1 mol/L in chloroform） isinvestigated as the positive active material of the non-aqueous LiJdisulfide semi-solid flow battery. Theelectrochemical activity and reversibility are investigated by cyclic voltammetry and linear scanvoltammetry. This Li/TMTD battery with a high cell voltage of 3.36 V achieves coulombic efficiency of 99%,voltage efficiency of 73% and energy efficiency of 72% at the current density of 5 mA/cm2 with activematerial concentration of 0.1 mol/L. Moreover, the LiJTMTD battery can operate for 100 cycles withoutobvious efficiency decay, indicating good stability.