Supercapacitors based on two-dimensional MXene(Ti_(3)C_(2)T_(z))have shown extraordinary performance in ultrathin electrodes with low mass loading,but usually there is a significant reduction in high-rate performance ...Supercapacitors based on two-dimensional MXene(Ti_(3)C_(2)T_(z))have shown extraordinary performance in ultrathin electrodes with low mass loading,but usually there is a significant reduction in high-rate performance as the thickness increases,caused by increasing ion diffusion limitation.Further limitations include restacking of the nanosheets,which makes it challenging to realize the full potential of these electrode materials.Herein,we demonstrate the design of a vertically aligned MXene hydrogel composite,achieved by thermal-assisted self-assembled gelation,for high-rate energy storage.The highly interconnected MXene network in the hydrogel architecture provides very good electron transport properties,and its vertical ion channel structure facilitates rapid ion transport.The resulting hydrogel electrode show excellent performance in both aqueous and organic electrolytes with respect to high capacitance,stability,and high-rate capability for up to 300μm thick electrodes,which represents a significant step toward practical applications.展开更多
Since 2019,research into MXene derivatives has seen a dramatic rise;further progress requires a rational design for specific functionality.Herein,through a molecular design by selecting suitable functional groups in t...Since 2019,research into MXene derivatives has seen a dramatic rise;further progress requires a rational design for specific functionality.Herein,through a molecular design by selecting suitable functional groups in the MXene coating,we have implemented the dual N doping of the derivatives,nitrogen-doped TiO_(2)@nitrogen-doped carbon nanosheets(N-TiO_(2)@NC),to strike a balance between the active anatase TiO_(2)at low temperatures,and carbon activation at high temperatures.The NH_(3)reduction environment generated at 400℃as evidenced by the in situ pyrolysis SVUV-PIMS process is crucial for concurrent phase engineering.With both electrical conductivity and surface Na+availability,the N-TiO_(2)@NC achieves higher interface capacitive-like sodium storage with long-term stability.More than 100 mAh g^(-1)is achieved at 2 A g^(-1)after 5000 cycles.The proposed design may be extended to other MXenes and solidify the growing family of MXene derivatives for energy storage.展开更多
An emerging practice in the realm of Li-S batteries lies in the employment of single-atom catalysts(SACs)as effective mediators to promote polysulfide conversion,but monometallic SACs affording isolated geometric disp...An emerging practice in the realm of Li-S batteries lies in the employment of single-atom catalysts(SACs)as effective mediators to promote polysulfide conversion,but monometallic SACs affording isolated geometric dispersion and sole electronic configuration limit the catalytic benefits and curtail the cell performance.Here,we propose a class of dual-atom catalytic moieties comprising hetero-or homo-atomic pairs anchored on N-doped graphene(NG)to unlock the liquid–solid redox puzzle of sulfur,readily realizing Li-S full cell under high-rate-charging conditions.As for Fe-Ni-NG,in-depth experimental and theoretical analysis reveal that the hetero-atomic orbital coupling leads to altered energy levels,unique electronic structures,and varied Fe oxidation states in comparison with homo-atomic structures(FeFe-NG or Ni-Ni-NG).This would weaken the bonding energy of polysulfide intermediates and thus enable facile electrochemical kinetics to gain rapid liquid-solid Li_(2)S_(4)?Li_(2)S conversion.Encouragingly,a Li-S battery based on the S@Fe-Ni-NG cathode demonstrates unprecedented fast-charging capability,documenting impressive rate performance(542.7 mA h g^(-1)at 10.0 C)and favorable cyclic stability(a capacity decay of 0.016%per cycle over 3000 cycles at 10.0 C).This finding offers insights to the rational design and application of dual-atom mediators for Li-S batteries.展开更多
The poor rate capability and low capacity are huge barriers to realize the commercial applications of battery-type transition metal compounds(TMCs) cathode.Herein,numerous Se vacancy defects are introduced into the Ni...The poor rate capability and low capacity are huge barriers to realize the commercial applications of battery-type transition metal compounds(TMCs) cathode.Herein,numerous Se vacancy defects are introduced into the Ni_(3)Se_(2)lamellas by pre-lithiation technique,which can be acted as a novel class of battery-type cathode for hybrid supercapacitors.Appropriately modulating the contents of the preembedded lithium(Li) ions can induce a controllable vacancy content in the series of as-prepared products,effectively endowing a fast reaction kinetic and high activity for the cathode.Benefiting from the distinct design,the optimized cathode(Li2-Ni_(3)Se_(2)) presents a high specific capacity of 236 mA h g^(-1)at1 A g^(-1),importantly,it can still possess 117 mA h g^(-1)when the current density is increased up to 100A g^(-1),exhibiting relatively high rate capability.It is much superior to other battery-type TMC cathodes reported in previous studies.Moreover,the cathode also shows the excellent cycling stability with 92%capacity retention after 3,000 cycles.In addition,a hybrid supercapacitor(HSC) is assembled with the obtained Li2-Ni_(3)Se_(2)as the cathode and active carbon(AC) as the anode,which delivers a high energy density of 77 W h kg^(-1)at 4 kW kg^(-1)and long-term durability(90% capacitance retention after 10,000 cycles).Therefore,the strategy not only provides an effective way to realize the controllable vacancy content in TMCs for achieving high-perfo rmance cathodes for HSC,but also further promotes their large-scale applications in the energy storage fields.展开更多
The safe operating voltage and low volume variation of Li_(3)VO_(4)(LVO)make it an ideal anode material for lithium(Li)-ion batteries.However,the insufficient understanding of the inner storage mechanism hinders the d...The safe operating voltage and low volume variation of Li_(3)VO_(4)(LVO)make it an ideal anode material for lithium(Li)-ion batteries.However,the insufficient understanding of the inner storage mechanism hinders the design of LVO-based electrodes.Herein,we investigate,for the first time,the Li-ion storage activity in LVO via Cl doping.Moreover,N-doped C coating was simultaneously achieved in the Cl doping process,resulting in synergistically improved reaction kinetics.As a result,the as-prepared Cl-doped Li_(3)VO_(4) coated with N-doped C(Cl-LVO@NC)electrodes deliver a discharge capacity of 884.1 mAh/g after 200 cycles at 0.2 A/g,which is the highest among all of the LVO-based electrodes.The Cl-LVO@NC electrodes also exhibit high-capacity retention of 331.1 mAh/g at 8.0 A/g and full capacity recovery after 5 periods of rate testing over 400 cycles.After 5000 cycles at 4.0 A/g,the discharge capacity can be maintained at 423.2 mAh/g,which is superior to most LVO-based electrodes.The Li-ion storage activity in LVO via Cl doping and significant improvement in the high-rate Li-ion storage reported in this work can be used as references for the design of advanced LVO-based electrodes for high-power applications.展开更多
Developing high-performance anodes for potassium ion batteries(KIBs) is of paramount significance but remains challenging.In the normal sense,electrode materials are prepared by ubiquitous wet chemical routes,which ot...Developing high-performance anodes for potassium ion batteries(KIBs) is of paramount significance but remains challenging.In the normal sense,electrode materials are prepared by ubiquitous wet chemical routes,which otherwise might not be versatile enough to create desired heterostructures and/or form clean interfacial areas for fast transport of K-ions and electrons.Along this line,rate capability/cycling stability of resulting KIBs are greatly handicapped.Herein we present an all-chemical vapor deposition approach to harness the direct synthesis of nitrogen-doped graphene(NG)/rhenium diselenide(ReSe_2)hybrids over three-dimensional MXene supports as superior heterostructure anode material for KIBs.In such an innovative design,1 T'-ReSe2 nanoparticles are sandwiched in between the NG coatings and MXene frameworks via strong interfacial interactions,thereby affording facile K~+ diffusion,enhancing overall conductivity,boosting high-power performance and reinforcing structural stability of electrodes.Thus-constructed anode delivers an excellent rate performance of 138 mAh g^(-1) at 10.0 A g^(-1) and a high reversible capacity of 90 mAh g^(-1) at 5 A g^(-1) after 300 cycles.Furthermore,the potassium storage mechanism has been systematically probed by advanced in situlex situ characterization techniques in combination with first principles computations.展开更多
Scalable fabrication of high-rate micro-supercapacitors(MSCs)is highly desired for on-chip integration of energy storage components.By virtue of the special self-assembly behavior of 2D materials during drying thin fi...Scalable fabrication of high-rate micro-supercapacitors(MSCs)is highly desired for on-chip integration of energy storage components.By virtue of the special self-assembly behavior of 2D materials during drying thin films of their liquid dispersion,a new inkjet printing technique of passivated graphene micro-flakes is developed to directly print MSCs with 3D networked porous microstructure.The presence of macroscale through-thickness pores provides fast ion transport pathways and improves the rate capability of the devices even with solid-state electrolytes.During multiple-pass printing,the porous microstructure effectively absorbs the successively printed inks,allowing full printing of 3D structured MSCs comprising multiple vertically stacked cycles of current collectors,electrodes,and sold-state electrolytes.The all-solid-state heterogeneous 3D MSCs exhibit excellent vertical scalability and high areal energy density and power density,evidently outperforming the MSCs fabricated through general printing techniques.展开更多
Sodium-ion storage devices are highly desirable for large-scale energy storage applications owing to the wide availability of sodium resources and low cost.Transition metal nitrides(TMNs)are promising anode materials ...Sodium-ion storage devices are highly desirable for large-scale energy storage applications owing to the wide availability of sodium resources and low cost.Transition metal nitrides(TMNs)are promising anode materials for sodium-ion storage,while their detailed reaction mechanism remains unexplored.Herein,we synthesize the mesoporous Mo3N2 nanowires(Meso-Mo_(3)N_(2)-NWs).The sodium-ion storage mechanism of Mo3N2 is systematically investigated through in-situ XRD,ex-situ experimental characterizations and detailed kinetics analysis.Briefly,the Mo_(3)N_(2) undergoes a surface pseudocapacitive redox charge storage process.Benefiting from the rapid surface redox reaction,the Meso-Mo_(3)N_(2)-NWs anode delivers high specific capacity(282 m Ah g^(-1) at 0.1 A g^(-1)),excellent rate capability(87 m Ah g^(-1) at 16 A g^(-1))and long cycling stability(a capacity retention of 78.6%after 800 cycles at 1 A g^(-1)).The present work highlights that the surface pseudocapacitive sodium-ion storage mechanism enables to overcome the sluggish sodium-ion diffusion process,which opens a new direction to design and synthesize high-rate sodiumion storage materials.展开更多
The limited lithium resource in earth's crust has stimulated the pursuit of alternative energy storage technologies to lithium-ion battery.Potassium-ion batteries(KIBs)are regarded as a kind of promising candidate...The limited lithium resource in earth's crust has stimulated the pursuit of alternative energy storage technologies to lithium-ion battery.Potassium-ion batteries(KIBs)are regarded as a kind of promising candidate for large-scale energy storage owing to the high abundance and low cost of potassium resources.Nevertheless,further development and wide application of KIBs are still challenged by several obstacles,one of which is their fast capacity deterioration at high rates.A considerable amount of effort has recently been devoted to address this problem by developing advanced carbonaceous anode materials with diverse structures and morphologies.This review presents and highlights how the architecture engineering of carbonaceous anode materials gives rise to high-rate performances for KIBs,and also the beneficial conceptions are consciously extracted from the recent progress.Particularly,basic insights into the recent engineering strategies,structural innovation,and the related advances of carbonaceous anodes for high-rate KIBs are under specific concerns.Based on the achievements attained so far,a perspective on the foregoing,and proposed possible directions,and avenues for designing high-rate anodes,are presented finally.展开更多
Surface-treated MmNi3.55Co0.75Mn0.4Al0.3 alloy as negative electrode material of nickel-metal hydride battery was employed to improve the high-rate dischargeability. Surface treatment was realized by dipping and stirr...Surface-treated MmNi3.55Co0.75Mn0.4Al0.3 alloy as negative electrode material of nickel-metal hydride battery was employed to improve the high-rate dischargeability. Surface treatment was realized by dipping and stirring the alloy into a HCl aqueous solution with various concentrations at room temperature. The microstructure of the alloy before and after surface treatment was analyzed by X-ray diffraction (XRD) and scanning electron microscopy (SEM). The electrochemical properties before and after surface treatment were compared, and the alloy treated in 0.025 mol/L HCl solution showed the optimal high-rate dischargeability.展开更多
Lithium-sulfur batteries suffer from poor cycling stability because of the intrinsic shuttling effect of intermediate polysulfides and sluggish reaction kinetics,especially at high rates and high sulfur loading.Herein...Lithium-sulfur batteries suffer from poor cycling stability because of the intrinsic shuttling effect of intermediate polysulfides and sluggish reaction kinetics,especially at high rates and high sulfur loading.Herein,we report the construction of a CoP-CO_(2)N@N-doped carbon polyhedron uniformly anchored on three-dimensional carbon nanotubes/graphene(CoP-CO_(2)N@NC/CG)scaffold as a sulfur reservoir to achieve the trapping-diffusion-conversion of polysulfides.Highly active CoP-CO_(2)N shows marvelous catalytic effects by effectively accelerating the reduction of sulfur and the oxidation of Li_(2)S during the discharging and charging process,respectively,while the conductive NC/CG network with massive mesoporous channels ensures fast and continuous long-distance electron/ion transportation.DFT calculations demonstrate that the CoP-CO_(2)N with excellent intrinsic conductivity serves as job-synergistic immobilizing-conversion sites for polysulfides through the formation of P…Li/N…Li and Co…S bonds.As a result,the S@CoP-CO_(2)N@NC/CG cathode(sulfur content 1.7 mg cm^(-2))exhibits a high capacity of988 mAh g^(-1)at 2 C after 500 cycles,which is superior to most of the electrochemical performance reported.Even under high sulfur content(4.3 mg cm^(-2)),it also shows excellent cyclability with high capacity at 1 C.展开更多
Sulfurized polyacrylonitrile(SPAN)as a promising cathode material for lithium sulfur(Li-S)batteries has drawn increasing attention for its improved electrochemical performance in carbonate-based electrolyte.However,th...Sulfurized polyacrylonitrile(SPAN)as a promising cathode material for lithium sulfur(Li-S)batteries has drawn increasing attention for its improved electrochemical performance in carbonate-based electrolyte.However,the relatively poor electronic and ionic conductivities of SPAN limit its high-rate and lowtemperature performances.In this work,a novel one-dimensional nanofiber SPAN(SFPAN)composite is developed as the cathode material for Li-S batteries.Benefitting from its one-dimensional nanostructure,the SFPAN composite cathode provides fast channels for the migration of ions and electronics,thus effectively improving its electrochemical performance at high rates and low temperature.As a result,the SFPAN maintains a high reversible specific capacity^1200 mAh g−1 after 400 cycles at 0.3 A g−1 and can deliver a high capacity of^850 mAh g−1 even at a high current density of 12.5 A g−1.What is more,the SFPAN can achieve a capacity of^800 mAh g−1 at 0℃and^1550 mAh g−1 at 60℃,thus providing a wider temperature range of applications.This work provides new perspectives on the cathode design for high-rate lithium-sulfur batteries.展开更多
Nano-LiMn2O4 cathode materials with nano-sized particles are synthesized via a citric acid assisted sol-gel route. The structure, the morphology and the electrochemical properties of the nano-LiMn204 are investigated....Nano-LiMn2O4 cathode materials with nano-sized particles are synthesized via a citric acid assisted sol-gel route. The structure, the morphology and the electrochemical properties of the nano-LiMn204 are investigated. Compared with the micro-sized LiMn2O4, the nano-LiMn2O4 possesses a high initial capacity (120 mAh/g) at a discharge rate of 0.2 C (29.6 mA/g). The nano-LiMn2O4 also has a good high-rate discharge capability, retaining 91% of its capacity at a discharge rate of 10 C and 73~ at a discharge rate of 40 C. In particular, the nano-LiMn2O4 shows an excellent high-rate pulse discharge capability. The cut-off voltage at the end of 50-ms pulse discharge with a discharge rate of 80 C is above 3.40 V, and the voltage returns to over 4.10 V after the pulse discharge. These results show that the prepared nano-LiMn2O4 could be a potential cathode material for the power sources with the capability to deliver very high-rate pulse currents.展开更多
In order to successively compete with supercapacitors, an ability of fast discharge is a must for lithium-ion batteries. From this point of view, stoichiometric and substituted lithium manganese spinels as cathode mat...In order to successively compete with supercapacitors, an ability of fast discharge is a must for lithium-ion batteries. From this point of view, stoichiometric and substituted lithium manganese spinels as cathode materials are one of the most prospective candidates, especially in their nanosized form. In this article, an overview of the most recent data regarding physico-chemical and electrochemical properties of lithium manganese spinels, especially, LiMn2O4 and LiNi0.5Mn1.5O4, synthesized by means of various methods is presented, with special emphasis of their use in high-rate electrochemical applications. In particular, specific capacities and rate capabilities of spinel materials are analyzed. It is suggested that reduced specific capacity is determined primarily by the aggregation of material particles, whereas good high-rate capability is governed not only by the size of crystallites but also by the perfectness of crystals. The most technologically advantageous solutions are described, existing gaps in the knowledge of spinel materials are outlined, and the ways of their filling are suggested, in a hope to be helpful in keeping lithium batteries afloat in the struggle for a worthy place among electrochemical energy systems of the 21st century.展开更多
Manganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries(ZIBs)because of the low price and high security.However,the practical application of Mn2O3 in ZIBs ...Manganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries(ZIBs)because of the low price and high security.However,the practical application of Mn2O3 in ZIBs is still plagued by the low specific capacity and poor rate capability.Herein,highly crystalline Mn2O3 materials with interconnected mesostructures and controllable pore sizes are obtained via a ligand-assisted self-assembly process and used as high-performance electrode materials for reversible aqueous ZIBs.The coordination degree between Mn2+and citric acid ligand plays a crucial role in the formation of the mesostructure,and the pore sizes can be easily tuned from 3.2 to 7.3 nm.Ascribed to the unique feature of nanoporous architectures,excellent zinc-storage performance can be achieved in ZIBs during charge/discharge processes.The Mn2O3 electrode exhibits high reversible capacity(233 mAh g−1 at 0.3 A g−1),superior rate capability(162 mAh g−1 retains at 3.08 A g−1)and remarkable cycling durability over 3000 cycles at a high current rate of 3.08 A g−1.Moreover,the corresponding electrode reaction mechanism is studied in depth according to a series of analytical methods.These results suggest that rational design of the nanoporous architecture for electrode materials can effectively improve the battery performance.展开更多
Sludge blanket height (SBH) is an important parameter in the clarifier design, operation and control. Based on an overview and classification of SBH algorithms, a modified SBH algorithm is proposed by incorporating ...Sludge blanket height (SBH) is an important parameter in the clarifier design, operation and control. Based on an overview and classification of SBH algorithms, a modified SBH algorithm is proposed by incorporating a threshold concentration limit into a relative concentration sharp change algorithm to eliminate the disturbance of compression interfaces on the correct simulation of SBH. Pilot-scale test data are adopted to compare reliability of three SBH algorithms reported in literature and the modified SBH algorithm developed in this paper. Calculated results demonstrate that the three SBH algorithms give results with large deviation (〉 50%) from measured SBH, especially under low solid flux conditions. The modified algorithm is computationally efficient and reliable in matching the measured data. It is incorporated into a one- dimensional clarifier model for stable simulation of pilot-scale experimental clarifier data and into dynamic simulation of a full-scale wastewater treatment plant (WWTP) clarifier data.展开更多
The April 25, 2015 Mw7.8 Nepal earthquake was successfully recorded by Crustal Movement Observation Network of China (CMONOC) and Nepal Geodetic Array (NGA). We processed the high-rate GPS data (1 Hz and 5 Hz) b...The April 25, 2015 Mw7.8 Nepal earthquake was successfully recorded by Crustal Movement Observation Network of China (CMONOC) and Nepal Geodetic Array (NGA). We processed the high-rate GPS data (1 Hz and 5 Hz) by using relative kinematic positioning and derived dynamic ground motions caused by this large earthquake. The dynamic displacements time series clearly indicated the displacement amplitude of each station was related to the rupture directivity. The stations which located in the di- rection of rupture propagation had larger displacement amplitudes than others. Also dynamic ground displacement exceeding 5 cm was detected by the GPS station that was 2000 km away from the epicenter. Permanent coseismic displacements were resolved from the near-field high-rate GPS stations with wavelet decomposition-reconstruction method and P-wave arrivals were also detected with S transform method. The results of this study can be used for earthquake rupture process and Earthquake Early Warning studies.展开更多
The effluent quality from a secondary clarifier in an activated sludge process depends on the performance in the secondary clarifier at great extent. Several models have been developed based on the Kynch solid flux th...The effluent quality from a secondary clarifier in an activated sludge process depends on the performance in the secondary clarifier at great extent. Several models have been developed based on the Kynch solid flux theory to improve the clarifier performance at last decades. This paper proposed a model which is established according to the basis sedimentation process of the secondary clarifier and Kynch flux theory for a clarifier with feedwell in upper of tank and the diffusion effective are combined into the model, which benefts the further improvement of the model and makes the solutions fit to the measurement data in secondary clarifier,展开更多
The M_(W)7.1 Anchorage earthquake is the most destructive earthquake since the 1964 M_(W)9.2 great Alaska earthquake in the United States.In this study,high-rate GPS data and near-field broadband seismograms are used ...The M_(W)7.1 Anchorage earthquake is the most destructive earthquake since the 1964 M_(W)9.2 great Alaska earthquake in the United States.In this study,high-rate GPS data and near-field broadband seismograms are used in separate and joint inversions by the generalized Cut-and-Paste(gCAP)method to estimate the focal mechanism.In order to investigate the influence of crustal velocity structure on the focal mechanism inversion results,two velocity models(Crustl.0 and Alaska Earthquake Center(AEC))are used for detailed comparison and analysis.The results show that:(1)The two nodal planes of the optimal double-couple solution are nearly north-south striking,with dip angles of about 30°and 60°respectively,and the centroid focal depth is 54-55 km,which is an intraplate normal fault event.(2)The inversion results for the two types of data and the two velocity models are consistent with some previous studies,which indicates that the results are stable and reliable.The more accurate velocity structure model is helpful for focal mechanism inversion of the complex earthquake.(3)The inclusion of high-rate GPS data in joint inversion provides a more effective constraint on centroid depth.展开更多
To alleviate the main limitations of lithium ion diffusion rate and poor electronic conductivity for LiFePO4 cathode material, it is desirable to synthesize nano-size LiFePO4 material due to its enhanced electronic an...To alleviate the main limitations of lithium ion diffusion rate and poor electronic conductivity for LiFePO4 cathode material, it is desirable to synthesize nano-size LiFePO4 material due to its enhanced electronic and lithium ion transport rates and thus an improved high-rate performance. However, our previous synthesized LiFePO4 nanorods only exhibited low high-rate and slightly unstable cycle performance. Possible reasons are the poor crystallization and Fe2+ oxidation of LiFePO4 nanorods prepared by hydrothermal method. In this paper, LiFePO4 nanorods were simply dealt with at 700 ℃ for 4 h under the protection of Ar and H2 mixture gas. The electrochemical properties of LiFePO4/Li cells were investigated by galvanostatic test and cyclic voltammetry(CV). The experimental results indicated that the annealed LiFePO4 nanorods delivered an excellent cycling stability and obviously improved capacity of 150 mA·h·g-1 at 1C, and even 122 mA·h·g-1 at 5C.展开更多
基金financed by the National Natural Science Foundation of China(52103212)Jiangxi Provincial Natural Science Foundation(20224BAB214022)+7 种基金the SSF Synergy Program(EM16-0004)Swedish Energy Agency(EM 42033-1)the Knut and Alice Wal enberg(KAW)Foundation through a Fellowship Grant and a Project Grant(KAW2020.0033)Support from the National Natural Science Foundation of China(61774077)the Youth Projects of Joint Fund of Basic and Applied Basic Research Fund of Guangdong Province(2020A1515110738)the Key Projects of Joint Fund of Basic and Applied Basic Research Fund of Guangdong Province(2019B1515120073)the High-End Foreign Experts Project(G20200019046)the Guangzhou Key laboratory of Vacuum Coating Technologies and New Energy Materials Open Projects Fund(KFVE20200006)
文摘Supercapacitors based on two-dimensional MXene(Ti_(3)C_(2)T_(z))have shown extraordinary performance in ultrathin electrodes with low mass loading,but usually there is a significant reduction in high-rate performance as the thickness increases,caused by increasing ion diffusion limitation.Further limitations include restacking of the nanosheets,which makes it challenging to realize the full potential of these electrode materials.Herein,we demonstrate the design of a vertically aligned MXene hydrogel composite,achieved by thermal-assisted self-assembled gelation,for high-rate energy storage.The highly interconnected MXene network in the hydrogel architecture provides very good electron transport properties,and its vertical ion channel structure facilitates rapid ion transport.The resulting hydrogel electrode show excellent performance in both aqueous and organic electrolytes with respect to high capacitance,stability,and high-rate capability for up to 300μm thick electrodes,which represents a significant step toward practical applications.
基金financially supported by the National Key R&D Program of China(2021YFA1501502)National Natural Science Foundation of China(22075263,52002366)+2 种基金Fundamental Research Funds for the Central Universities(WK2060000039)USTC Research Funds(KY2060000165,GG2060007008)Natural Science Foundation of Jiangsu Province(BK20200386)
文摘Since 2019,research into MXene derivatives has seen a dramatic rise;further progress requires a rational design for specific functionality.Herein,through a molecular design by selecting suitable functional groups in the MXene coating,we have implemented the dual N doping of the derivatives,nitrogen-doped TiO_(2)@nitrogen-doped carbon nanosheets(N-TiO_(2)@NC),to strike a balance between the active anatase TiO_(2)at low temperatures,and carbon activation at high temperatures.The NH_(3)reduction environment generated at 400℃as evidenced by the in situ pyrolysis SVUV-PIMS process is crucial for concurrent phase engineering.With both electrical conductivity and surface Na+availability,the N-TiO_(2)@NC achieves higher interface capacitive-like sodium storage with long-term stability.More than 100 mAh g^(-1)is achieved at 2 A g^(-1)after 5000 cycles.The proposed design may be extended to other MXenes and solidify the growing family of MXene derivatives for energy storage.
基金supported by the National Natural Science Foundation of China(22179089)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX23_3245)support from Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies,Suzhou,China。
文摘An emerging practice in the realm of Li-S batteries lies in the employment of single-atom catalysts(SACs)as effective mediators to promote polysulfide conversion,but monometallic SACs affording isolated geometric dispersion and sole electronic configuration limit the catalytic benefits and curtail the cell performance.Here,we propose a class of dual-atom catalytic moieties comprising hetero-or homo-atomic pairs anchored on N-doped graphene(NG)to unlock the liquid–solid redox puzzle of sulfur,readily realizing Li-S full cell under high-rate-charging conditions.As for Fe-Ni-NG,in-depth experimental and theoretical analysis reveal that the hetero-atomic orbital coupling leads to altered energy levels,unique electronic structures,and varied Fe oxidation states in comparison with homo-atomic structures(FeFe-NG or Ni-Ni-NG).This would weaken the bonding energy of polysulfide intermediates and thus enable facile electrochemical kinetics to gain rapid liquid-solid Li_(2)S_(4)?Li_(2)S conversion.Encouragingly,a Li-S battery based on the S@Fe-Ni-NG cathode demonstrates unprecedented fast-charging capability,documenting impressive rate performance(542.7 mA h g^(-1)at 10.0 C)and favorable cyclic stability(a capacity decay of 0.016%per cycle over 3000 cycles at 10.0 C).This finding offers insights to the rational design and application of dual-atom mediators for Li-S batteries.
基金supported by the National Natural Science Foundation of China(Grant No.51672144,51572137,51702181,52072196,52002199,52002200)the Major Basic Research Program of Natural Science Foundation of Shandong Province(Grant No.ZR2020ZD09)+6 种基金the Shandong Provincial Key Research and Development Program(SPKR&DP)(Grant No.2019GGX102055)the Natural Science Foundation of Shandong Province(Grant No.ZR2019BEM042,ZR2020QE063)the Innovation and Technology Program of Shandong Province(Grant No.2020KJA004)the Guangdong Basic and Applied Basic Research Foundation(Grant No.2019A1515110933)the China Postdoctoral Science Foundation(Grant No.2020M683450)the Taishan Scholars Program of Shandong Province(No.ts201511034)the Postdoctoral Innovation Project of Shandong Province(Grant no.202101020)。
文摘The poor rate capability and low capacity are huge barriers to realize the commercial applications of battery-type transition metal compounds(TMCs) cathode.Herein,numerous Se vacancy defects are introduced into the Ni_(3)Se_(2)lamellas by pre-lithiation technique,which can be acted as a novel class of battery-type cathode for hybrid supercapacitors.Appropriately modulating the contents of the preembedded lithium(Li) ions can induce a controllable vacancy content in the series of as-prepared products,effectively endowing a fast reaction kinetic and high activity for the cathode.Benefiting from the distinct design,the optimized cathode(Li2-Ni_(3)Se_(2)) presents a high specific capacity of 236 mA h g^(-1)at1 A g^(-1),importantly,it can still possess 117 mA h g^(-1)when the current density is increased up to 100A g^(-1),exhibiting relatively high rate capability.It is much superior to other battery-type TMC cathodes reported in previous studies.Moreover,the cathode also shows the excellent cycling stability with 92%capacity retention after 3,000 cycles.In addition,a hybrid supercapacitor(HSC) is assembled with the obtained Li2-Ni_(3)Se_(2)as the cathode and active carbon(AC) as the anode,which delivers a high energy density of 77 W h kg^(-1)at 4 kW kg^(-1)and long-term durability(90% capacitance retention after 10,000 cycles).Therefore,the strategy not only provides an effective way to realize the controllable vacancy content in TMCs for achieving high-perfo rmance cathodes for HSC,but also further promotes their large-scale applications in the energy storage fields.
基金supported by the National Natural Science Foundation of China(No.52101262)Distinguished Youth Foundation of Hubei Province(2019CFA084)+1 种基金Educational offi ce of Hubei Province(Q20201201)the 111 project(D20015).
文摘The safe operating voltage and low volume variation of Li_(3)VO_(4)(LVO)make it an ideal anode material for lithium(Li)-ion batteries.However,the insufficient understanding of the inner storage mechanism hinders the design of LVO-based electrodes.Herein,we investigate,for the first time,the Li-ion storage activity in LVO via Cl doping.Moreover,N-doped C coating was simultaneously achieved in the Cl doping process,resulting in synergistically improved reaction kinetics.As a result,the as-prepared Cl-doped Li_(3)VO_(4) coated with N-doped C(Cl-LVO@NC)electrodes deliver a discharge capacity of 884.1 mAh/g after 200 cycles at 0.2 A/g,which is the highest among all of the LVO-based electrodes.The Cl-LVO@NC electrodes also exhibit high-capacity retention of 331.1 mAh/g at 8.0 A/g and full capacity recovery after 5 periods of rate testing over 400 cycles.After 5000 cycles at 4.0 A/g,the discharge capacity can be maintained at 423.2 mAh/g,which is superior to most LVO-based electrodes.The Li-ion storage activity in LVO via Cl doping and significant improvement in the high-rate Li-ion storage reported in this work can be used as references for the design of advanced LVO-based electrodes for high-power applications.
基金supported by the National Natural Science Foundation of China (51702225)the National Key Research and Development Program (2016YFA0200103)+2 种基金the Natural Science Foundation of Jiangsu Province (BK20170336)the support from Suzhou Key Laboratory for Advanced Carbon MaterialsWearable Energy Technologies, Suzhou, China。
文摘Developing high-performance anodes for potassium ion batteries(KIBs) is of paramount significance but remains challenging.In the normal sense,electrode materials are prepared by ubiquitous wet chemical routes,which otherwise might not be versatile enough to create desired heterostructures and/or form clean interfacial areas for fast transport of K-ions and electrons.Along this line,rate capability/cycling stability of resulting KIBs are greatly handicapped.Herein we present an all-chemical vapor deposition approach to harness the direct synthesis of nitrogen-doped graphene(NG)/rhenium diselenide(ReSe_2)hybrids over three-dimensional MXene supports as superior heterostructure anode material for KIBs.In such an innovative design,1 T'-ReSe2 nanoparticles are sandwiched in between the NG coatings and MXene frameworks via strong interfacial interactions,thereby affording facile K~+ diffusion,enhancing overall conductivity,boosting high-power performance and reinforcing structural stability of electrodes.Thus-constructed anode delivers an excellent rate performance of 138 mAh g^(-1) at 10.0 A g^(-1) and a high reversible capacity of 90 mAh g^(-1) at 5 A g^(-1) after 300 cycles.Furthermore,the potassium storage mechanism has been systematically probed by advanced in situlex situ characterization techniques in combination with first principles computations.
基金financial support of the Swedish Research Council through the Marie Sklodowska-Curie International Career Grant (No.2015-00395,co-funded by Marie Sklodowska-Curie Actions, through the Project INCA 600398)the Formas Foundation through the Future Research Leaders Grant (No.2016-00496)+3 种基金the AForsk Foundation (Grant No.17-352)the Olle Engkvist Byggmastare Foundation (Grant No.2014/799)the Academy of Finland (Grant No.288945 and 319408)Academy of Finland Research Infrastructure "Printed Intelligence Infrastructure" (PII-FIRI,Grant No. 320019)
文摘Scalable fabrication of high-rate micro-supercapacitors(MSCs)is highly desired for on-chip integration of energy storage components.By virtue of the special self-assembly behavior of 2D materials during drying thin films of their liquid dispersion,a new inkjet printing technique of passivated graphene micro-flakes is developed to directly print MSCs with 3D networked porous microstructure.The presence of macroscale through-thickness pores provides fast ion transport pathways and improves the rate capability of the devices even with solid-state electrolytes.During multiple-pass printing,the porous microstructure effectively absorbs the successively printed inks,allowing full printing of 3D structured MSCs comprising multiple vertically stacked cycles of current collectors,electrodes,and sold-state electrolytes.The all-solid-state heterogeneous 3D MSCs exhibit excellent vertical scalability and high areal energy density and power density,evidently outperforming the MSCs fabricated through general printing techniques.
基金supported by the National Natural Science Foundation of China(51832004,51521001)the National Key Research and Development Program of China(2016YFA0202603)+2 种基金the Program of Introducing Talents of Discipline to Universities(B17034)the Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory(XHT2020-003)the “Double-First Class”Foundation of Materials and Intelligent Manufacturing Discipline of Xiamen University。
文摘Sodium-ion storage devices are highly desirable for large-scale energy storage applications owing to the wide availability of sodium resources and low cost.Transition metal nitrides(TMNs)are promising anode materials for sodium-ion storage,while their detailed reaction mechanism remains unexplored.Herein,we synthesize the mesoporous Mo3N2 nanowires(Meso-Mo_(3)N_(2)-NWs).The sodium-ion storage mechanism of Mo3N2 is systematically investigated through in-situ XRD,ex-situ experimental characterizations and detailed kinetics analysis.Briefly,the Mo_(3)N_(2) undergoes a surface pseudocapacitive redox charge storage process.Benefiting from the rapid surface redox reaction,the Meso-Mo_(3)N_(2)-NWs anode delivers high specific capacity(282 m Ah g^(-1) at 0.1 A g^(-1)),excellent rate capability(87 m Ah g^(-1) at 16 A g^(-1))and long cycling stability(a capacity retention of 78.6%after 800 cycles at 1 A g^(-1)).The present work highlights that the surface pseudocapacitive sodium-ion storage mechanism enables to overcome the sluggish sodium-ion diffusion process,which opens a new direction to design and synthesize high-rate sodiumion storage materials.
基金National Natural Science Foundation of China,Grant/Award Numbers:51972121,51972270,51702262Tip-top Scientific and Technical Innovative Youth Talents of Guangdong Special Support Program,Grant/Award Number:2017TQ04C419Key Research and Development Program of Shaanxi Province,Grant/Award Number:2019TSLGY07-03。
文摘The limited lithium resource in earth's crust has stimulated the pursuit of alternative energy storage technologies to lithium-ion battery.Potassium-ion batteries(KIBs)are regarded as a kind of promising candidate for large-scale energy storage owing to the high abundance and low cost of potassium resources.Nevertheless,further development and wide application of KIBs are still challenged by several obstacles,one of which is their fast capacity deterioration at high rates.A considerable amount of effort has recently been devoted to address this problem by developing advanced carbonaceous anode materials with diverse structures and morphologies.This review presents and highlights how the architecture engineering of carbonaceous anode materials gives rise to high-rate performances for KIBs,and also the beneficial conceptions are consciously extracted from the recent progress.Particularly,basic insights into the recent engineering strategies,structural innovation,and the related advances of carbonaceous anodes for high-rate KIBs are under specific concerns.Based on the achievements attained so far,a perspective on the foregoing,and proposed possible directions,and avenues for designing high-rate anodes,are presented finally.
基金supported by Hi-Tech Research and Development Program (863) of China (2006AA11A159)
文摘Surface-treated MmNi3.55Co0.75Mn0.4Al0.3 alloy as negative electrode material of nickel-metal hydride battery was employed to improve the high-rate dischargeability. Surface treatment was realized by dipping and stirring the alloy into a HCl aqueous solution with various concentrations at room temperature. The microstructure of the alloy before and after surface treatment was analyzed by X-ray diffraction (XRD) and scanning electron microscopy (SEM). The electrochemical properties before and after surface treatment were compared, and the alloy treated in 0.025 mol/L HCl solution showed the optimal high-rate dischargeability.
基金supported by the National Natural Science Foundation of China(21903051 and 22073061))the award of Future Fellowship from the Australian Research Council(FT170100224)。
文摘Lithium-sulfur batteries suffer from poor cycling stability because of the intrinsic shuttling effect of intermediate polysulfides and sluggish reaction kinetics,especially at high rates and high sulfur loading.Herein,we report the construction of a CoP-CO_(2)N@N-doped carbon polyhedron uniformly anchored on three-dimensional carbon nanotubes/graphene(CoP-CO_(2)N@NC/CG)scaffold as a sulfur reservoir to achieve the trapping-diffusion-conversion of polysulfides.Highly active CoP-CO_(2)N shows marvelous catalytic effects by effectively accelerating the reduction of sulfur and the oxidation of Li_(2)S during the discharging and charging process,respectively,while the conductive NC/CG network with massive mesoporous channels ensures fast and continuous long-distance electron/ion transportation.DFT calculations demonstrate that the CoP-CO_(2)N with excellent intrinsic conductivity serves as job-synergistic immobilizing-conversion sites for polysulfides through the formation of P…Li/N…Li and Co…S bonds.As a result,the S@CoP-CO_(2)N@NC/CG cathode(sulfur content 1.7 mg cm^(-2))exhibits a high capacity of988 mAh g^(-1)at 2 C after 500 cycles,which is superior to most of the electrochemical performance reported.Even under high sulfur content(4.3 mg cm^(-2)),it also shows excellent cyclability with high capacity at 1 C.
基金supported by the National Natural Science Foundation of China(Grant nos.21773077,51632001,and 51532005)the Ministry of Science and Technology“973”program(Grant No.2015CB258400)the National Key R&D Program of China(2018YFB0905400)。
文摘Sulfurized polyacrylonitrile(SPAN)as a promising cathode material for lithium sulfur(Li-S)batteries has drawn increasing attention for its improved electrochemical performance in carbonate-based electrolyte.However,the relatively poor electronic and ionic conductivities of SPAN limit its high-rate and lowtemperature performances.In this work,a novel one-dimensional nanofiber SPAN(SFPAN)composite is developed as the cathode material for Li-S batteries.Benefitting from its one-dimensional nanostructure,the SFPAN composite cathode provides fast channels for the migration of ions and electronics,thus effectively improving its electrochemical performance at high rates and low temperature.As a result,the SFPAN maintains a high reversible specific capacity^1200 mAh g−1 after 400 cycles at 0.3 A g−1 and can deliver a high capacity of^850 mAh g−1 even at a high current density of 12.5 A g−1.What is more,the SFPAN can achieve a capacity of^800 mAh g−1 at 0℃and^1550 mAh g−1 at 60℃,thus providing a wider temperature range of applications.This work provides new perspectives on the cathode design for high-rate lithium-sulfur batteries.
基金supported by the National Natural Science Foundation for Postdoctoral Scientists of China (Grant No. 20090451554)
文摘Nano-LiMn2O4 cathode materials with nano-sized particles are synthesized via a citric acid assisted sol-gel route. The structure, the morphology and the electrochemical properties of the nano-LiMn204 are investigated. Compared with the micro-sized LiMn2O4, the nano-LiMn2O4 possesses a high initial capacity (120 mAh/g) at a discharge rate of 0.2 C (29.6 mA/g). The nano-LiMn2O4 also has a good high-rate discharge capability, retaining 91% of its capacity at a discharge rate of 10 C and 73~ at a discharge rate of 40 C. In particular, the nano-LiMn2O4 shows an excellent high-rate pulse discharge capability. The cut-off voltage at the end of 50-ms pulse discharge with a discharge rate of 80 C is above 3.40 V, and the voltage returns to over 4.10 V after the pulse discharge. These results show that the prepared nano-LiMn2O4 could be a potential cathode material for the power sources with the capability to deliver very high-rate pulse currents.
文摘In order to successively compete with supercapacitors, an ability of fast discharge is a must for lithium-ion batteries. From this point of view, stoichiometric and substituted lithium manganese spinels as cathode materials are one of the most prospective candidates, especially in their nanosized form. In this article, an overview of the most recent data regarding physico-chemical and electrochemical properties of lithium manganese spinels, especially, LiMn2O4 and LiNi0.5Mn1.5O4, synthesized by means of various methods is presented, with special emphasis of their use in high-rate electrochemical applications. In particular, specific capacities and rate capabilities of spinel materials are analyzed. It is suggested that reduced specific capacity is determined primarily by the aggregation of material particles, whereas good high-rate capability is governed not only by the size of crystallites but also by the perfectness of crystals. The most technologically advantageous solutions are described, existing gaps in the knowledge of spinel materials are outlined, and the ways of their filling are suggested, in a hope to be helpful in keeping lithium batteries afloat in the struggle for a worthy place among electrochemical energy systems of the 21st century.
基金the Young Thousand Talented Program and the National Natural Science Foundation of China (21671073 and 21621001)the “111” Project of the Ministry of Education of China (B17020)Program for JLU Science and Technology Innovative Research Team
文摘Manganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries(ZIBs)because of the low price and high security.However,the practical application of Mn2O3 in ZIBs is still plagued by the low specific capacity and poor rate capability.Herein,highly crystalline Mn2O3 materials with interconnected mesostructures and controllable pore sizes are obtained via a ligand-assisted self-assembly process and used as high-performance electrode materials for reversible aqueous ZIBs.The coordination degree between Mn2+and citric acid ligand plays a crucial role in the formation of the mesostructure,and the pore sizes can be easily tuned from 3.2 to 7.3 nm.Ascribed to the unique feature of nanoporous architectures,excellent zinc-storage performance can be achieved in ZIBs during charge/discharge processes.The Mn2O3 electrode exhibits high reversible capacity(233 mAh g−1 at 0.3 A g−1),superior rate capability(162 mAh g−1 retains at 3.08 A g−1)and remarkable cycling durability over 3000 cycles at a high current rate of 3.08 A g−1.Moreover,the corresponding electrode reaction mechanism is studied in depth according to a series of analytical methods.These results suggest that rational design of the nanoporous architecture for electrode materials can effectively improve the battery performance.
基金supported by the National Natural Science Foundation of China (Grant No.501380107)
文摘Sludge blanket height (SBH) is an important parameter in the clarifier design, operation and control. Based on an overview and classification of SBH algorithms, a modified SBH algorithm is proposed by incorporating a threshold concentration limit into a relative concentration sharp change algorithm to eliminate the disturbance of compression interfaces on the correct simulation of SBH. Pilot-scale test data are adopted to compare reliability of three SBH algorithms reported in literature and the modified SBH algorithm developed in this paper. Calculated results demonstrate that the three SBH algorithms give results with large deviation (〉 50%) from measured SBH, especially under low solid flux conditions. The modified algorithm is computationally efficient and reliable in matching the measured data. It is incorporated into a one- dimensional clarifier model for stable simulation of pilot-scale experimental clarifier data and into dynamic simulation of a full-scale wastewater treatment plant (WWTP) clarifier data.
基金supported by Director Foundation of Institute of Seismology,China Earthquake Administration(IS201426142)National Natural Science Foundation of China(41541029,41574017, 41274027)+1 种基金Natural Science Foundation of HuBei Province (2015CFB642)provided by Crustal Movement Observation Network of China(CMONOC) and UNAVCO
文摘The April 25, 2015 Mw7.8 Nepal earthquake was successfully recorded by Crustal Movement Observation Network of China (CMONOC) and Nepal Geodetic Array (NGA). We processed the high-rate GPS data (1 Hz and 5 Hz) by using relative kinematic positioning and derived dynamic ground motions caused by this large earthquake. The dynamic displacements time series clearly indicated the displacement amplitude of each station was related to the rupture directivity. The stations which located in the di- rection of rupture propagation had larger displacement amplitudes than others. Also dynamic ground displacement exceeding 5 cm was detected by the GPS station that was 2000 km away from the epicenter. Permanent coseismic displacements were resolved from the near-field high-rate GPS stations with wavelet decomposition-reconstruction method and P-wave arrivals were also detected with S transform method. The results of this study can be used for earthquake rupture process and Earthquake Early Warning studies.
文摘The effluent quality from a secondary clarifier in an activated sludge process depends on the performance in the secondary clarifier at great extent. Several models have been developed based on the Kynch solid flux theory to improve the clarifier performance at last decades. This paper proposed a model which is established according to the basis sedimentation process of the secondary clarifier and Kynch flux theory for a clarifier with feedwell in upper of tank and the diffusion effective are combined into the model, which benefts the further improvement of the model and makes the solutions fit to the measurement data in secondary clarifier,
基金co-supported by the National Natural Science Foundation of China under Grants No.41721003,No.42074007the National Key Research and Development Program of China under Grant No.2018YFC1503604。
文摘The M_(W)7.1 Anchorage earthquake is the most destructive earthquake since the 1964 M_(W)9.2 great Alaska earthquake in the United States.In this study,high-rate GPS data and near-field broadband seismograms are used in separate and joint inversions by the generalized Cut-and-Paste(gCAP)method to estimate the focal mechanism.In order to investigate the influence of crustal velocity structure on the focal mechanism inversion results,two velocity models(Crustl.0 and Alaska Earthquake Center(AEC))are used for detailed comparison and analysis.The results show that:(1)The two nodal planes of the optimal double-couple solution are nearly north-south striking,with dip angles of about 30°and 60°respectively,and the centroid focal depth is 54-55 km,which is an intraplate normal fault event.(2)The inversion results for the two types of data and the two velocity models are consistent with some previous studies,which indicates that the results are stable and reliable.The more accurate velocity structure model is helpful for focal mechanism inversion of the complex earthquake.(3)The inclusion of high-rate GPS data in joint inversion provides a more effective constraint on centroid depth.
基金Funded by the National Natural Science Foundation of China(51208396 and 21277017)the Fundamental Research Funds for the Central Universities(2013-Ia-36 and 2013-Ia-39)the Selfdetermined and Innovative Research Funds of WUT(136814016)
文摘To alleviate the main limitations of lithium ion diffusion rate and poor electronic conductivity for LiFePO4 cathode material, it is desirable to synthesize nano-size LiFePO4 material due to its enhanced electronic and lithium ion transport rates and thus an improved high-rate performance. However, our previous synthesized LiFePO4 nanorods only exhibited low high-rate and slightly unstable cycle performance. Possible reasons are the poor crystallization and Fe2+ oxidation of LiFePO4 nanorods prepared by hydrothermal method. In this paper, LiFePO4 nanorods were simply dealt with at 700 ℃ for 4 h under the protection of Ar and H2 mixture gas. The electrochemical properties of LiFePO4/Li cells were investigated by galvanostatic test and cyclic voltammetry(CV). The experimental results indicated that the annealed LiFePO4 nanorods delivered an excellent cycling stability and obviously improved capacity of 150 mA·h·g-1 at 1C, and even 122 mA·h·g-1 at 5C.