Lithium-sulfur battery(LSB)has brought much attention and concern because of high theoretical specific capacity and energy density as one of main competitors for next-generation energy storage systems.The widely comme...Lithium-sulfur battery(LSB)has brought much attention and concern because of high theoretical specific capacity and energy density as one of main competitors for next-generation energy storage systems.The widely commercial application and development of LSB is mainly hindered by serious“shuttle effect”of lithium polysulfides(Li PSs),slow reaction kinetics,notorious lithium dendrites,etc.In various structures of LSB materials,array structured materials,possessing the composition of ordered micro units with the same or similar characteristics of each unit,present excellent application potential for various secondary cells due to some merits such as immobilization of active substances,high specific surface area,appropriate pore sizes,easy modification of functional material surface,accommodated huge volume change,enough facilitated transportation for electrons/lithium ions,and special functional groups strongly adsorbing Li PSs.Thus many novel array structured materials are applied to battery for tackling thorny problems mentioned above.In this review,recent progresses and developments on array structured materials applied in LSBs including preparation ways,collaborative structural designs based on array structures,and action mechanism analyses in improving electrochemical performance and safety are summarized.Meanwhile,we also have detailed discussion for array structured materials in LSBs and constructed the structure-function relationships between array structured materials and battery performances.Lastly,some directions and prospects about preparation ways,functional modifications,and practical applications of array structured materials in LSBs are generalized.We hope the review can attract more researchers'attention and bring more studying on array structured materials for other secondary batteries including LSB.展开更多
Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properti...Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properties of graphitic carbon nitride(g-C_(3)N_(4)),together with unique metal-free characteristic,make them ideal candidates for advanced photocatalysts construction.This review summarizes the up-to-date advances on g-C_(3)N_(4)based photocatalysts from ingenious-design strategies and diversified photocatalytic applications.Notably,the advantages,fabrication methods and limitations of each design strategy are systemically analyzed.In order to deeply comprehend the inner connection of theory–structure–performance upon g-C_(3)N_(4)based photocatalysts,structure/composition designs,corresponding photocatalytic activities and reaction mechanisms are jointly discussed,associated with introducing their photocatalytic applications toward water splitting,carbon dioxide/nitrogen reduction and pollutants degradation,etc.Finally,the current challenges and future perspectives for g-C_(3)N_(4)based materials for photocatalysis are briefly proposed.These design strategies and limitations are also instructive for constructing g-C_(3)N_(4) based materials in other energy and environment-related applications.展开更多
Hydrogen energy has emerged as a pivotal solution to address the global energy crisis and pave the way for a cleaner,low-carbon,secure,and efficient modern energy system.A key imperative in the utilization of hydrogen...Hydrogen energy has emerged as a pivotal solution to address the global energy crisis and pave the way for a cleaner,low-carbon,secure,and efficient modern energy system.A key imperative in the utilization of hydrogen energy lies in the development of high-performance hydrogen storage materials.Magnesium-based hydrogen storage materials exhibit remarkable advantages,including high hydrogen storage density,cost-effectiveness,and abundant magnesium resources,making them highly promising for the hydrogen energy sector.Nonetheless,practical applications of magnesium hydride for hydrogen storage face significant challenges,primarily due to their slow kinetics and stable thermodynamic properties.Herein,we briefly summarize the thermodynamic and kinetic properties of MgH2,encompassing strategies such as alloying,nanoscaling,catalyst doping,and composite system construction to enhance its hydrogen storage performance.Notably,nanoscaling and catalyst doping have emerged as more effective modification strategies.The discussion focuses on the thermodynamic changes induced by nanoscaling and the kinetic enhancements resulting from catalyst doping.Particular emphasis lies in the synergistic improvement strategy of incorporating nanocatalysts with confinement materials,and we revisit typical works on the multi-strategy optimization of MgH2.In conclusion,we conduct an analysis of outstanding challenges and issues,followed by presenting future research and development prospects for MgH2 as hydrogen storage materials.展开更多
NaBH_(4) was widely regarded as a low-cost hydrogen storage material due to its high-mass hydrogen capacity of approximately 10.8%(mass)and high volumetric hydrogen capacity of around 115 g·L^(–1).However,it exh...NaBH_(4) was widely regarded as a low-cost hydrogen storage material due to its high-mass hydrogen capacity of approximately 10.8%(mass)and high volumetric hydrogen capacity of around 115 g·L^(–1).However,it exhibits strong stability and requires temperatures above 500℃ for hydrogen release in practical applications.In this study,two polyhydric alcohols,xylitol and erythritol(XE),were prepared as a binary eutectic sugar alcohol through a grinding-melting method.This binary eutectic sugar alcohol was used as a proton-hydrogen carrier to destabilize NaBH_(4).The 19NaBH_(4)-16XE composite material prepared by ball milling could start releasing hydrogen at 57.5℃,and the total hydrogen release can reach over 88.8%(4.45%(mass))of the theoretical capacity.When the 19NaBH_(4)-16XE composite was pressed into solid blocks,the volumetric hydrogen capacity of the block-shaped composite could reach 67.2 g·L^(–1).By controlling the temperature,the hydrogen desorption capacity of the NaBH_(4)-XE composite material was controllable,which has great potential for achieving solid-state hydrogen production from NaBH_(4).展开更多
Cobalt-free,nickel-rich LiNi_(1-x)Al_(x)O_(2)(x≤0.1)is an attractive cathode material because of high energy density and low cost but suffers from severe structural degradation and poor rate performance.In this study...Cobalt-free,nickel-rich LiNi_(1-x)Al_(x)O_(2)(x≤0.1)is an attractive cathode material because of high energy density and low cost but suffers from severe structural degradation and poor rate performance.In this study,we propose a molten salt-assisted synthesis in combination with a Li-refeeding induced aluminum segregation strategy to prepare Li_(5)AlO_(4)-coated single-crystalline slightly Li-rich Li_(1.04)Ni_(0.92)Al_(0.04)O_(2).The symbiotic formation of Li_(5)AlO_(4)from reaction between molten lithium hydroxide and doped aluminum in the bulk ensures a high lattice matching between the Ni-rich oxide and the homogenous conductive Li_(5)AlO_(4)that permits high Li^(+)conductivity.Benefiting from mitigated undesirable side reactions and phase evolution,the Li_(5)AlO_(4)-coated single-crystalline Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)delivers a high specific capacity of220.2 mA h g^(-1)at 0.1 C and considerable rate capability(182.5 mA h g^(-1)at 10 C).Besides,superior capacity retention of 90.8%is obtained at 1/3 C after 100 cycles in a 498.1 mA h pouch full cell.Furthermore,the particulate morphology of Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)remains intact after cycling at a cutoff voltage of 4.3 V,whereas slightly Li-deficient Li_(0.98)Ni_(0.97)Al_(0.05)O_(2)features intragranular cracks and irreversible lattice distortion.The results highlight the value of molten salt-assisted synthesis and Li-refeeding induced elemental segregation strategy to upgrade Ni-based layered oxide cathode materials for advanced Li-ion batteries.展开更多
Constructing heterostructure is considered as an effective strategy to address the sluggish electronic and ionic kinetics of anode materials for sodium ion batteries(SIBs).However,realizing the orientated growth and u...Constructing heterostructure is considered as an effective strategy to address the sluggish electronic and ionic kinetics of anode materials for sodium ion batteries(SIBs).However,realizing the orientated growth and uniform distribution of the heterostructure is still a great challenge.Herein,the regulated novel CoSe_(2)/NiSe_(2)heterostructure confined in N-doped carbon nanofibers(CoSe_(2)/NiSe_(2)@N-C)are prepared by using Co/Ni-ZIF template,in which,the CoSe_(2)/NiSe_(2)heterostructures realize uniform distribution on a micro level.Benefiting from the unique heterostructure and N-doped carbon nanofibers,the CoSe_(2)/NiSe_(2)@N-C deliveries superior rate capability and durable cycle lifespan with a reversible capacity of 400.5 mA h g^(-1)after 5000 cycles at 2 A g^(-1).The Na-ion full battery with CoSe_(2)/NiSe_(2)@N-C anode and layered oxide cathode displays a remarkable energy density of 563 W h kg^(-1)with 241.1 W kg^(-1)at 0.1 A g^(-1).The theoretical calculations disclose that the periodic and directional built-in electric-field along with the heterointerfaces of CoSe_(2)/NiSe_(2)@N-C can accelerate electrochemical reaction kinetics.The in(ex)situ experimental measurements reveal the reversible conversion reaction and stable structure of CoSe_(2)/NiSe_(2)@N-C during Na+insertion/extraction.The study highlights the potential ability of precisely controlled heterostructure to stimulate the electrochemical performances of advanced anode for SIBs.展开更多
Zinc ion batteries are considered as potential energy storage devices due to their advantages of low-cost,high-safety,and high theoretical capacity.However,dendrite growth and chemical corrosion occurring on Zn anode ...Zinc ion batteries are considered as potential energy storage devices due to their advantages of low-cost,high-safety,and high theoretical capacity.However,dendrite growth and chemical corrosion occurring on Zn anode limit their commercialization.These problems can be tackled through the optimization of the electrolyte.However,the screening of electrolyte additives using normal electrochemical methods is time-consuming and labor-intensive.Herein,a fast and simple method based on the digital holography is developed.It can realize the in situ monitoring of electrode/electrolyte interface and provide direct information concerning ion concentration evolution of the diffusion layer.It is effective and time-saving in estimating the homogeneity of the deposition layer and predicting the tendency of dendrite growth,thus able to value the applicability of electrolyte additives.The feasibility of this method is further validated by the forecast and evaluation of thioacetamide additive.Based on systematic characterization,it is proved that the introduction of thioacetamide can not only regulate the interficial ion flux to induce dendrite-free Zn deposition,but also construct adsorption molecule layers to inhibit side reactions of Zn anode.Being easy to operate,capable of in situ observation,and able to endure harsh conditions,digital holography method will be a promising approach for the interfacial investigation of other battery systems.展开更多
Lithium-sulfur(Li-S)batteries are one of the most promising modern-day energy supply systems because of their high theoretical energy density and low cost.However,the development of high-energy density Li-S batteries ...Lithium-sulfur(Li-S)batteries are one of the most promising modern-day energy supply systems because of their high theoretical energy density and low cost.However,the development of high-energy density Li-S batteries with high loading of flammable sulfur faces the challenges of electrochemical performance degradation owing to the shuttle effect and safety issues related to fire or explosion accidents.In this work,we report a three-dimensional(3D)conductive nitrogen-doped carbon foam supported electrostatic self-assembled MXene-ammonium polyphosphate(NCF-MXene-APP)layer as a heat-resistant,thermally-insulated,flame-retardant,and freestanding host for Li-S batteries with a facile and costeffective synthesis method.Consequently,through the use of NCF-MXene-APP hosts that strongly anchor polysulfides,the Li-S batteries demonstrate outstanding electrochemical properties,including a high initial discharge capacity of 1191.6 mA h g^(-1),excellent rate capacity of 755.0 mA h g^(-1)at 1 C,and long-term cycling stability with an extremely low-capacity decay rate of 0.12%per cycle at 2 C.More importantly,these batteries can continue to operate reliably under high temperature or flame attack conditions.Thus,this study provides valuable insights into the design of safe high-performance Li-S batteries.展开更多
The commercialization of silicon-based anodes is affected by their low initial Coulombic efficiency(ICE)and capacity decay,which are attributed to the formation of an unstable solid electrolyte interface(SEI)layer.Her...The commercialization of silicon-based anodes is affected by their low initial Coulombic efficiency(ICE)and capacity decay,which are attributed to the formation of an unstable solid electrolyte interface(SEI)layer.Herein,a feasible and cost-effective prelithiation method under a localized highconcentration electrolyte system(LHCE)for the silicon-silica/graphite(Si-SiO_(2)/C@G)anode is designed for stabilizing the SEI layer and enhancing the ICE.The thin SiO_(2)/C layers with-NH_(2) groups covered on nano-Si surfaces are demonstrated to be beneficial to the prelithiation process by density functional theory calculations and electrochemical performance.The SEI formed under LHCE is proven to be rich in ionic conductivity,inorganic substances,and flexible organic products.Thus,faster Li+transportation across the SEI further enhances the prelithiation effect and the rate performance of Si-SiO_(2)/C@G anodes.LHCE also leads to uniform decomposition and high stability of the SEI with abundant organic components.As a result,the prepared anode shows a high reversible specific capacity of 937.5 mAh g^(-1)after 400 cycles at a current density of 1 C.NCM 811‖Li-SSGLHCE full cell achieves a high-capacity retention of 126.15 mAh g^(-1)at 1 C over 750 cycles with 84.82%ICE,indicating the great value of this strategy for Si-based anodes in large-scale applications.展开更多
The unstable zinc(Zn)/electrolyte interfaces formed by undesired dendrites and parasitic side reactions greatly hinder the development of aqueous zinc ion batteries.Herein,the hydroxy-rich sorbitol was used as an addi...The unstable zinc(Zn)/electrolyte interfaces formed by undesired dendrites and parasitic side reactions greatly hinder the development of aqueous zinc ion batteries.Herein,the hydroxy-rich sorbitol was used as an additive to reshape the solvation structure and modulate the interface chemistry.The strong interactions among sorbitol and both water molecules and Zn electrode can reduce the free water activity,optimize the solvation shell of water and Zn^(2+)ions,and regulate the formation of local water(H_(2)O)-poor environment on the surface of Zn electrode,which effectively inhibit the decomposition of water molecules,and thus,achieve the thermodynamically stable and highly reversible Zn electrochemistry.As a result,the assembled Zn/Zn symmetric cells with the sorbitol additive realized an excellent cycling life of 2000 h at 1 mA·cm^(-2)and 1 mAh·cm^(-2),and over 250 h at 5 mA.cm^(-2)and 5 mAh.cm^(-2).Moreover,the Zn/Cu asymmetric cells with the sorbitol additive achieved a high Coulombic efficiency of 99.6%,obtaining a better performance than that with a pure 2 mol-L^(-1)ZnSO_(4)electrolyte.And the constructed Zn/poly1,5-naphthalenediamine(PNDA)batteries could be stably discharged for 2300 cycles at 1 A g^(-1)with an excellent capacity retention rate.This result indicates that the addition of 1 mol-L^(-1)non-toxic sorbitol into a conventional ZnSO_(4)electrolyte can successfully protect the Zn anode interface by improving the electrochemical properties of Zn reversible deposition/decomposition,which greatly promotes its cycle performance,providing a new approach in future development of high performance aqueous Zn ion batteries.展开更多
The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clu...The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.展开更多
Anode materials are an essential part of lithium-ion batteries(LIBs),which determine the performance and safety of LIBs.Currently,graphite,as the anode material of commercial LIBs,is limited by its low theoretical cap...Anode materials are an essential part of lithium-ion batteries(LIBs),which determine the performance and safety of LIBs.Currently,graphite,as the anode material of commercial LIBs,is limited by its low theoretical capacity of 372 mA·h·g^(−1),thus hindering further development toward high-capacity and large-scale applications.Alkaline earth metal iron-based oxides are considered a promising candidate to replace graphite because of their low preparation cost,good thermal stability,superior stability,and high electrochemical performance.Nonetheless,many issues and challenges remain to be addressed.Herein,we systematically summarize the research progress of alkaline earth metal iron-based oxides as LIB anodes.Meanwhile,the material and structural properties,synthesis methods,electrochemical reaction mechanisms,and improvement strategies are introduced.Finally,existing challenges and future research directions are discussed to accelerate their practical application in commercial LIBs.展开更多
Rechargeable aqueous zinc-ion batteries are recently gaining incremental attention because of low cost and material abundance, but their development is plagued by limited choice of cathode materials with satisfactory ...Rechargeable aqueous zinc-ion batteries are recently gaining incremental attention because of low cost and material abundance, but their development is plagued by limited choice of cathode materials with satisfactory cycling performance. Here, we report a porous V2O5 nanofibers cathode with high Znstorage performance in an aqueous Zn(CF3SO3)2 electrolyte. We propose a reaction mechanism based on phase transition from orthorhombic V2O5 to zinc pyrovanadate on first discharging and reversible Zn^2+ (de)intercalation in the open-structured hosts during subsequent cycling. This open and stable architecture enables a high reversible capacity of 319 mAh g^-1 at 20 mAg^-1 and a capacity retention of 81% over 500 cycles. The remarkable electrochemical performance makes V2O5 a promising cathode for aqueous zinc-ion batteries.展开更多
In this paper,we report on the preparation of Li2FeSiO4,sintered Li2FeSiO4,and Li2FeSiO4-C composite with spindle-like morphologies and their application as cathode materials of lithium-ion batteries.Spindle-like Li2F...In this paper,we report on the preparation of Li2FeSiO4,sintered Li2FeSiO4,and Li2FeSiO4-C composite with spindle-like morphologies and their application as cathode materials of lithium-ion batteries.Spindle-like Li2FeSi04 was synthesized by a facile hydrothermal method with(NH4)2Fe(SO4)2 as the iron source.The spindle-like Li2FeSiO4 was sintered at 600 ℃ for 6 h in Ar atmosphere.Li2FeSiO4-C composite was obtained by the hydrothermal treatment of spindle-like Li2FeSiO4 in glucose solution at 190 ℃ for 3 h.Electrochemical measurements show that after carbon coating,the electrode performances such as discharge capacity and high-rate capability are greatly enhanced.In particular.Li2FeSiO4-C with carbon content of 7.21 wt%delivers the discharge capacities of 160.9 mAh·g-1 at room temperature and 213 mAh·g-1 at45℃(0.1 C),revealing the potential application in lithium-ion batteries.展开更多
Hierarchical Sb_2S_3 hollow microspheres assembled by nanowires have been successfully synthesized by a simple and practical hydrothermal reaction. The possible formation process of this architecture was investigated ...Hierarchical Sb_2S_3 hollow microspheres assembled by nanowires have been successfully synthesized by a simple and practical hydrothermal reaction. The possible formation process of this architecture was investigated by X-ray diffraction, focused-ion beam-scanning electron microscopy dual-beam system, and transmission electron microscopy. When used as the anode material for lithium-ion batteries, Sb_2S_3 hollow microspheres manifest excellent rate property and enhanced lithium-storage capability and can deliver a discharge capacity of 674 m Ah g^(-1) at a current density of 200 m A g^(-1) after 50 cycles. Even at a high currentdensity of 5000 m A g^(-1), a discharge capacity of541 m Ah g^(-1) is achieved. Sb_2S_3 hollow microspheres also display a prominent sodium-storage capacity and maintain a reversible discharge capacity of 384 m Ah g^(-1) at a current density of 200 m A g^(-1) after 50 cycles. The remarkable lithium/sodium-storage property may be attributed to the synergetic effect of its nanometer size and three-dimensional hierarchical architecture, and the outstanding stability property is attributed to the sufficient interior void space,which can buffer the volume expansion.展开更多
The development of novel organic electrode materials is of great significance for improving the reversible capacity and cycle stability of rechargeable batteries.Before practical application,it is essential to charact...The development of novel organic electrode materials is of great significance for improving the reversible capacity and cycle stability of rechargeable batteries.Before practical application,it is essential to characterize the electrode materials to study their structures,redox mechanisms and electrochemical performances.In this review,the common characterization methods that have been adopted so far are summarized from two aspects:experimental characterization and theoretical calculation.The experimental characterization is introduced in detail from structural characterization,electrochemical characterization and electrode reaction chara cterization.The experimental purposes and working principles of various experimental characterization methods are briefly illustrated.As the auxilia ry means,theoretical calculation provides the theoretical basis for characterizing the electrochemical reaction mechanism of organic electrode materials.Through these characterizations,we will have a deep understanding about the material structures,electrochemical redox mechanisms,electrochemical properties and the relationships of structure-property.It is hoped that this review would help researchers to select the suitable characterization methods to analyze the structures and performances of organic electrode materials quickly and effectively.展开更多
Na0.44MnO2 nanorods have been prepared by a hydrothermal method.The experimental parameters have been systematically investigated and optimized.The results show that Na0.44MnO2 nanorods obtained via the hydrothermal t...Na0.44MnO2 nanorods have been prepared by a hydrothermal method.The experimental parameters have been systematically investigated and optimized.The results show that Na0.44MnO2 nanorods obtained via the hydrothermal treatment at 200℃for 16 h show the best electrochemical properties,which deliver the high initial discharge capacity of 110.7 mA·h/g at 50 mA/g in potential window 2.0-4.0 V.To further improve their electrochemical properties,a ball milling process with graphene has been carried out to obtain Na0.44MnO2/graphene composite.The initial discharge capacity of Na0.44MnO2/graphene composite is 106.9 mA·h/g at a current density of 50 mA/g.After 100 cycles,the residual discharge capacity is 91.8 mA·h/g and the capacity retention rate is 85.9%,which is much higher than that of pristine Na0.44MnO2 nanorods(74.7%)at the same condition.What is more,when the current density reaches 500 and 1000 mA/g,the corresponding discharge capacities of Na0.44MnO2/graphene composite are about 89 and 78 mA·h/g,respectively,indicating outstanding rate capability.展开更多
Nitrogen-doped TiO_2–C composite nanofibers(TiO_2/N–C NFs) were manufactured by a convenient and green electrospinning technique in which urea acted as both the nitrogen source and a pore-forming agent. The TiO_2/N...Nitrogen-doped TiO_2–C composite nanofibers(TiO_2/N–C NFs) were manufactured by a convenient and green electrospinning technique in which urea acted as both the nitrogen source and a pore-forming agent. The TiO_2/N–C NFs exhibit a large specific surface area(213.04 m^2 g^(-1)) and a suitable nitrogen content(5.37 wt%). The large specific surface area can increase the contribution of the extrinsic pseudocapacitance, which greatly enhances the rate capability. Further, the diffusion coefficient of sodium ions(DNa_+) could be greatly improved by the incorporation of nitrogen atoms. Thus, the TiO_2/N–C NFs display excellent electrochemical properties in Na-ion batteries. A TiO_2/N–C NF anode delivers a high reversible discharge capacity of 265.8 mAh g^(-1) at 0.05 A g^(-1) and an outstanding long cycling performance even at a high current density(118.1 m Ah g^(-1)) with almost no capacity decay at 5 A g^(-1) over 2000 cycles. Therefore, this work sheds light on the application of TiO_2-based materials in sodium-ion batteries.展开更多
Exploring the production and application of clean energy has always been the core of sustainable development.As a clean and sustainable technology,electrocatalysis has been receiving widespread attention.It is crucial...Exploring the production and application of clean energy has always been the core of sustainable development.As a clean and sustainable technology,electrocatalysis has been receiving widespread attention.It is crucial to achieve efficient,stable and cheap electrocatalysts.However,the traditional“trial and error”method is time-consuming,laborious and costly.In recent years,with the significant increase in computing power,computations have played an important role in electrocatalyst design.Nevertheless,it is still difficult to search for advanced electrocatalysts in the vast chemical space through traditional density functional theory(DFT)computations.Fortunately,the development of machine learning and interdisciplinary integration will inject new impetus into targeted design of electrocatalysts.Machine learning is able to predict electrochemical performances with an accuracy close to DFT.Here we provide an overview of the application of machine learning in electrocatalyst design,including the prediction of structure,thermodynamic properties and kinetic barriers.We also discuss the potential of explicit solvent model combined with machine learning molecular dynamics in this field.Finally,the favorable circumstances and challenges are outlined for the future development of machine learning in electrocatalysis.The studies on electrochemical processes by machine learning will further realize targeted design of high-efficiency electrocatalysts.展开更多
Rational design of hybrid carbon host with high electrical conductivity and strong adsorption toward soluble lithium polysulfides is the main challenge for achieving high-performance lithium-sulfur batteries(LSBs).Her...Rational design of hybrid carbon host with high electrical conductivity and strong adsorption toward soluble lithium polysulfides is the main challenge for achieving high-performance lithium-sulfur batteries(LSBs).Herein,novel binder-free Ni@N-doped carbon nanospheres(N-CNSs)films as sulfur host are firstly synthesized via a facile combined hydrothermal-atomic layer deposition method.The cross-linked multilayer N-CNSs films can effectively enhance the electrical conductivity of electrode and provide physical blocking“dams”toward the soluble long-chain polysulfides.Moreover,the doped N heteroatoms and superficial NiO layer on Ni layer can work synergistically to suppress the shuttle of lithium polysulfides by effective chemical interaction/adsorption.In virtue of the unique composite architecture and reinforced dual physical and chemical adsorption to the soluble polysulfides,the obtained Ni@N-CNSs/S electrode is demonstrated with enhanced rate performance(816 mAh g?1 at 2 C)and excellent long cycling life(87%after 200 cycles at 0.1 C),much better than N-CNSs/S electrode and other carbon/S counterparts.Our proposed design strategy offers a promising prospect for construction of advanced sulfur cathodes for applications in LSBs and other energy storage systems.展开更多
基金This work was supported by the National Natural Science Foundation of China(52203066,51973157,61904123)the Tianjin Natural Science Foundation(18JCQNJC02900)+3 种基金the National innovation and entrepreneurship training program for college students(202310058007)the Tianjin Municipal college students’innovation and entrepreneurship training program(202310058088)the Science&Technology Development Fund of Tianjin Education Commission for Higher Education(Grant No.2018KJ196)the State Key Laboratory of Membrane and Membrane Separation,Tiangong University.
文摘Lithium-sulfur battery(LSB)has brought much attention and concern because of high theoretical specific capacity and energy density as one of main competitors for next-generation energy storage systems.The widely commercial application and development of LSB is mainly hindered by serious“shuttle effect”of lithium polysulfides(Li PSs),slow reaction kinetics,notorious lithium dendrites,etc.In various structures of LSB materials,array structured materials,possessing the composition of ordered micro units with the same or similar characteristics of each unit,present excellent application potential for various secondary cells due to some merits such as immobilization of active substances,high specific surface area,appropriate pore sizes,easy modification of functional material surface,accommodated huge volume change,enough facilitated transportation for electrons/lithium ions,and special functional groups strongly adsorbing Li PSs.Thus many novel array structured materials are applied to battery for tackling thorny problems mentioned above.In this review,recent progresses and developments on array structured materials applied in LSBs including preparation ways,collaborative structural designs based on array structures,and action mechanism analyses in improving electrochemical performance and safety are summarized.Meanwhile,we also have detailed discussion for array structured materials in LSBs and constructed the structure-function relationships between array structured materials and battery performances.Lastly,some directions and prospects about preparation ways,functional modifications,and practical applications of array structured materials in LSBs are generalized.We hope the review can attract more researchers'attention and bring more studying on array structured materials for other secondary batteries including LSB.
基金supported by the National Natural Science Foundation of China(21875118,22111530112)the support from the Smart Sensing Interdisciplinary Science Center,Nankai University。
文摘Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properties of graphitic carbon nitride(g-C_(3)N_(4)),together with unique metal-free characteristic,make them ideal candidates for advanced photocatalysts construction.This review summarizes the up-to-date advances on g-C_(3)N_(4)based photocatalysts from ingenious-design strategies and diversified photocatalytic applications.Notably,the advantages,fabrication methods and limitations of each design strategy are systemically analyzed.In order to deeply comprehend the inner connection of theory–structure–performance upon g-C_(3)N_(4)based photocatalysts,structure/composition designs,corresponding photocatalytic activities and reaction mechanisms are jointly discussed,associated with introducing their photocatalytic applications toward water splitting,carbon dioxide/nitrogen reduction and pollutants degradation,etc.Finally,the current challenges and future perspectives for g-C_(3)N_(4)based materials for photocatalysis are briefly proposed.These design strategies and limitations are also instructive for constructing g-C_(3)N_(4) based materials in other energy and environment-related applications.
基金supported by National Key Research and Development Program of China(2021YFB4000604)National Natural Science Foundation of China(52271220)111 Project(B12015)and the Fundamental Research Funds for the Central Universities.
文摘Hydrogen energy has emerged as a pivotal solution to address the global energy crisis and pave the way for a cleaner,low-carbon,secure,and efficient modern energy system.A key imperative in the utilization of hydrogen energy lies in the development of high-performance hydrogen storage materials.Magnesium-based hydrogen storage materials exhibit remarkable advantages,including high hydrogen storage density,cost-effectiveness,and abundant magnesium resources,making them highly promising for the hydrogen energy sector.Nonetheless,practical applications of magnesium hydride for hydrogen storage face significant challenges,primarily due to their slow kinetics and stable thermodynamic properties.Herein,we briefly summarize the thermodynamic and kinetic properties of MgH2,encompassing strategies such as alloying,nanoscaling,catalyst doping,and composite system construction to enhance its hydrogen storage performance.Notably,nanoscaling and catalyst doping have emerged as more effective modification strategies.The discussion focuses on the thermodynamic changes induced by nanoscaling and the kinetic enhancements resulting from catalyst doping.Particular emphasis lies in the synergistic improvement strategy of incorporating nanocatalysts with confinement materials,and we revisit typical works on the multi-strategy optimization of MgH2.In conclusion,we conduct an analysis of outstanding challenges and issues,followed by presenting future research and development prospects for MgH2 as hydrogen storage materials.
基金support from the National Natural Science Foundation of China(52201255)the Natural Science Foundation of Jiangsu Province(BK20210884)the Innovation,and Entrepreneurship Program of Jiangsu Province(JSSCBS20211007).
文摘NaBH_(4) was widely regarded as a low-cost hydrogen storage material due to its high-mass hydrogen capacity of approximately 10.8%(mass)and high volumetric hydrogen capacity of around 115 g·L^(–1).However,it exhibits strong stability and requires temperatures above 500℃ for hydrogen release in practical applications.In this study,two polyhydric alcohols,xylitol and erythritol(XE),were prepared as a binary eutectic sugar alcohol through a grinding-melting method.This binary eutectic sugar alcohol was used as a proton-hydrogen carrier to destabilize NaBH_(4).The 19NaBH_(4)-16XE composite material prepared by ball milling could start releasing hydrogen at 57.5℃,and the total hydrogen release can reach over 88.8%(4.45%(mass))of the theoretical capacity.When the 19NaBH_(4)-16XE composite was pressed into solid blocks,the volumetric hydrogen capacity of the block-shaped composite could reach 67.2 g·L^(–1).By controlling the temperature,the hydrogen desorption capacity of the NaBH_(4)-XE composite material was controllable,which has great potential for achieving solid-state hydrogen production from NaBH_(4).
基金supported by the China National Funds for Distinguished Young Scientists(21925503)the National Natural Science Foundation of China(21835004)the Jilin Scientific and Technological Development Program(20220301018GX)。
文摘Cobalt-free,nickel-rich LiNi_(1-x)Al_(x)O_(2)(x≤0.1)is an attractive cathode material because of high energy density and low cost but suffers from severe structural degradation and poor rate performance.In this study,we propose a molten salt-assisted synthesis in combination with a Li-refeeding induced aluminum segregation strategy to prepare Li_(5)AlO_(4)-coated single-crystalline slightly Li-rich Li_(1.04)Ni_(0.92)Al_(0.04)O_(2).The symbiotic formation of Li_(5)AlO_(4)from reaction between molten lithium hydroxide and doped aluminum in the bulk ensures a high lattice matching between the Ni-rich oxide and the homogenous conductive Li_(5)AlO_(4)that permits high Li^(+)conductivity.Benefiting from mitigated undesirable side reactions and phase evolution,the Li_(5)AlO_(4)-coated single-crystalline Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)delivers a high specific capacity of220.2 mA h g^(-1)at 0.1 C and considerable rate capability(182.5 mA h g^(-1)at 10 C).Besides,superior capacity retention of 90.8%is obtained at 1/3 C after 100 cycles in a 498.1 mA h pouch full cell.Furthermore,the particulate morphology of Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)remains intact after cycling at a cutoff voltage of 4.3 V,whereas slightly Li-deficient Li_(0.98)Ni_(0.97)Al_(0.05)O_(2)features intragranular cracks and irreversible lattice distortion.The results highlight the value of molten salt-assisted synthesis and Li-refeeding induced elemental segregation strategy to upgrade Ni-based layered oxide cathode materials for advanced Li-ion batteries.
基金financially supported by the Natural Science Foundation of Shandong Province(ZR2021QB055,ZR2023MB017,ZR2022JQ10)the National Natural Science Foundation of China(21901146,220781792,22274083)。
文摘Constructing heterostructure is considered as an effective strategy to address the sluggish electronic and ionic kinetics of anode materials for sodium ion batteries(SIBs).However,realizing the orientated growth and uniform distribution of the heterostructure is still a great challenge.Herein,the regulated novel CoSe_(2)/NiSe_(2)heterostructure confined in N-doped carbon nanofibers(CoSe_(2)/NiSe_(2)@N-C)are prepared by using Co/Ni-ZIF template,in which,the CoSe_(2)/NiSe_(2)heterostructures realize uniform distribution on a micro level.Benefiting from the unique heterostructure and N-doped carbon nanofibers,the CoSe_(2)/NiSe_(2)@N-C deliveries superior rate capability and durable cycle lifespan with a reversible capacity of 400.5 mA h g^(-1)after 5000 cycles at 2 A g^(-1).The Na-ion full battery with CoSe_(2)/NiSe_(2)@N-C anode and layered oxide cathode displays a remarkable energy density of 563 W h kg^(-1)with 241.1 W kg^(-1)at 0.1 A g^(-1).The theoretical calculations disclose that the periodic and directional built-in electric-field along with the heterointerfaces of CoSe_(2)/NiSe_(2)@N-C can accelerate electrochemical reaction kinetics.The in(ex)situ experimental measurements reveal the reversible conversion reaction and stable structure of CoSe_(2)/NiSe_(2)@N-C during Na+insertion/extraction.The study highlights the potential ability of precisely controlled heterostructure to stimulate the electrochemical performances of advanced anode for SIBs.
基金supported by the National Natural Science Foundation of China(No.22075115)Natural Science Foundation of Jiangsu Province(No.BK20211352)+2 种基金Joint Funds of the National Natural Science Foundation of China(No.U2141201)Natural Science Foundation(No.22KJA430005)of Jiangsu Education Committee of ChinaPostgraduate Research and Practice Innovation Program of Jiangsu Normal University(No.2021XKT0296).
文摘Zinc ion batteries are considered as potential energy storage devices due to their advantages of low-cost,high-safety,and high theoretical capacity.However,dendrite growth and chemical corrosion occurring on Zn anode limit their commercialization.These problems can be tackled through the optimization of the electrolyte.However,the screening of electrolyte additives using normal electrochemical methods is time-consuming and labor-intensive.Herein,a fast and simple method based on the digital holography is developed.It can realize the in situ monitoring of electrode/electrolyte interface and provide direct information concerning ion concentration evolution of the diffusion layer.It is effective and time-saving in estimating the homogeneity of the deposition layer and predicting the tendency of dendrite growth,thus able to value the applicability of electrolyte additives.The feasibility of this method is further validated by the forecast and evaluation of thioacetamide additive.Based on systematic characterization,it is proved that the introduction of thioacetamide can not only regulate the interficial ion flux to induce dendrite-free Zn deposition,but also construct adsorption molecule layers to inhibit side reactions of Zn anode.Being easy to operate,capable of in situ observation,and able to endure harsh conditions,digital holography method will be a promising approach for the interfacial investigation of other battery systems.
基金supported by the National Research Foundation of Korea(NRF-2021R1A2C1008272)supported by the Institute of Information&communications Technology Planning&Evaluation(IITP)grant funded by the Korean government(MSIT)(No.2021-0-00259,Development of a Fast Wireless Charging System for Portable Terminals with improved heat dissipation and shielding performance)supported by the Applied Basic Research Program of Changzhou City(CJ20220030).
文摘Lithium-sulfur(Li-S)batteries are one of the most promising modern-day energy supply systems because of their high theoretical energy density and low cost.However,the development of high-energy density Li-S batteries with high loading of flammable sulfur faces the challenges of electrochemical performance degradation owing to the shuttle effect and safety issues related to fire or explosion accidents.In this work,we report a three-dimensional(3D)conductive nitrogen-doped carbon foam supported electrostatic self-assembled MXene-ammonium polyphosphate(NCF-MXene-APP)layer as a heat-resistant,thermally-insulated,flame-retardant,and freestanding host for Li-S batteries with a facile and costeffective synthesis method.Consequently,through the use of NCF-MXene-APP hosts that strongly anchor polysulfides,the Li-S batteries demonstrate outstanding electrochemical properties,including a high initial discharge capacity of 1191.6 mA h g^(-1),excellent rate capacity of 755.0 mA h g^(-1)at 1 C,and long-term cycling stability with an extremely low-capacity decay rate of 0.12%per cycle at 2 C.More importantly,these batteries can continue to operate reliably under high temperature or flame attack conditions.Thus,this study provides valuable insights into the design of safe high-performance Li-S batteries.
基金National Natural Science Foundation of China,Grant/Award Number:22179006Natural Science Foundation of Zhejiang Province,Grant/Award Number:LQ23E020002+4 种基金National Natural Science Foundation of China,Grant/Award Numbers:52202284,52072036Cooperation between Industry and Education Project of Ministry of Education,Grant/Award Number:220601318235513WenZhou Natural Science Foundation,Grant/Award Numbers:G20220019,G20220021State Key Laboratory of Electrical Insulation and Power Equipment,Xi'an Jiaotong University,Grant/Award Number:EIPE22208Key Research and Development Program of Henan province,China,Grant/Award Number:231111242500。
文摘The commercialization of silicon-based anodes is affected by their low initial Coulombic efficiency(ICE)and capacity decay,which are attributed to the formation of an unstable solid electrolyte interface(SEI)layer.Herein,a feasible and cost-effective prelithiation method under a localized highconcentration electrolyte system(LHCE)for the silicon-silica/graphite(Si-SiO_(2)/C@G)anode is designed for stabilizing the SEI layer and enhancing the ICE.The thin SiO_(2)/C layers with-NH_(2) groups covered on nano-Si surfaces are demonstrated to be beneficial to the prelithiation process by density functional theory calculations and electrochemical performance.The SEI formed under LHCE is proven to be rich in ionic conductivity,inorganic substances,and flexible organic products.Thus,faster Li+transportation across the SEI further enhances the prelithiation effect and the rate performance of Si-SiO_(2)/C@G anodes.LHCE also leads to uniform decomposition and high stability of the SEI with abundant organic components.As a result,the prepared anode shows a high reversible specific capacity of 937.5 mAh g^(-1)after 400 cycles at a current density of 1 C.NCM 811‖Li-SSGLHCE full cell achieves a high-capacity retention of 126.15 mAh g^(-1)at 1 C over 750 cycles with 84.82%ICE,indicating the great value of this strategy for Si-based anodes in large-scale applications.
基金supported by the National Natural Science Foundation of China(22279063,52001170)Tianjin Natural Science Foundation(22JCYBJC00590)the Fundamental Research Funds for the Central Universities.We thank the Haihe Laboratoryof Sustainable Chemical Transformations for financial support.
文摘The unstable zinc(Zn)/electrolyte interfaces formed by undesired dendrites and parasitic side reactions greatly hinder the development of aqueous zinc ion batteries.Herein,the hydroxy-rich sorbitol was used as an additive to reshape the solvation structure and modulate the interface chemistry.The strong interactions among sorbitol and both water molecules and Zn electrode can reduce the free water activity,optimize the solvation shell of water and Zn^(2+)ions,and regulate the formation of local water(H_(2)O)-poor environment on the surface of Zn electrode,which effectively inhibit the decomposition of water molecules,and thus,achieve the thermodynamically stable and highly reversible Zn electrochemistry.As a result,the assembled Zn/Zn symmetric cells with the sorbitol additive realized an excellent cycling life of 2000 h at 1 mA·cm^(-2)and 1 mAh·cm^(-2),and over 250 h at 5 mA.cm^(-2)and 5 mAh.cm^(-2).Moreover,the Zn/Cu asymmetric cells with the sorbitol additive achieved a high Coulombic efficiency of 99.6%,obtaining a better performance than that with a pure 2 mol-L^(-1)ZnSO_(4)electrolyte.And the constructed Zn/poly1,5-naphthalenediamine(PNDA)batteries could be stably discharged for 2300 cycles at 1 A g^(-1)with an excellent capacity retention rate.This result indicates that the addition of 1 mol-L^(-1)non-toxic sorbitol into a conventional ZnSO_(4)electrolyte can successfully protect the Zn anode interface by improving the electrochemical properties of Zn reversible deposition/decomposition,which greatly promotes its cycle performance,providing a new approach in future development of high performance aqueous Zn ion batteries.
基金supported by the National Natural Science Foundation of China(22205209,52202373 and U21A200972)China Postdoctoral Science Foundation(2022M722867)Key Research Project of Higher Education Institutions in Henan Province(23A530001)。
文摘The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.
基金The authors acknowledge the support of the Shenyang University of Technology(QNPY202209-4)the National Natural Science Foundation of China(21571132)+1 种基金Jiangsu University Advanced Talent Fund(5501710002)the Education Department of Liaoning Province(JYTQN2023285).
文摘Anode materials are an essential part of lithium-ion batteries(LIBs),which determine the performance and safety of LIBs.Currently,graphite,as the anode material of commercial LIBs,is limited by its low theoretical capacity of 372 mA·h·g^(−1),thus hindering further development toward high-capacity and large-scale applications.Alkaline earth metal iron-based oxides are considered a promising candidate to replace graphite because of their low preparation cost,good thermal stability,superior stability,and high electrochemical performance.Nonetheless,many issues and challenges remain to be addressed.Herein,we systematically summarize the research progress of alkaline earth metal iron-based oxides as LIB anodes.Meanwhile,the material and structural properties,synthesis methods,electrochemical reaction mechanisms,and improvement strategies are introduced.Finally,existing challenges and future research directions are discussed to accelerate their practical application in commercial LIBs.
基金financially supported by Tianjin Natural Science Foundation (No. 18JCZDJC31100)MOST(2017YFA0206700 and 2016YFA0202503)+1 种基金MOE(B12015)the Fundamental Research Funds for the Central Universities
文摘Rechargeable aqueous zinc-ion batteries are recently gaining incremental attention because of low cost and material abundance, but their development is plagued by limited choice of cathode materials with satisfactory cycling performance. Here, we report a porous V2O5 nanofibers cathode with high Znstorage performance in an aqueous Zn(CF3SO3)2 electrolyte. We propose a reaction mechanism based on phase transition from orthorhombic V2O5 to zinc pyrovanadate on first discharging and reversible Zn^2+ (de)intercalation in the open-structured hosts during subsequent cycling. This open and stable architecture enables a high reversible capacity of 319 mAh g^-1 at 20 mAg^-1 and a capacity retention of 81% over 500 cycles. The remarkable electrochemical performance makes V2O5 a promising cathode for aqueous zinc-ion batteries.
基金supported by the Programs of National 973(2011CB935900)NSFC(21231005)+1 种基金MOE(B12015 and 113016A)the Fundamental Research Funds for the Central Universities
文摘In this paper,we report on the preparation of Li2FeSiO4,sintered Li2FeSiO4,and Li2FeSiO4-C composite with spindle-like morphologies and their application as cathode materials of lithium-ion batteries.Spindle-like Li2FeSi04 was synthesized by a facile hydrothermal method with(NH4)2Fe(SO4)2 as the iron source.The spindle-like Li2FeSiO4 was sintered at 600 ℃ for 6 h in Ar atmosphere.Li2FeSiO4-C composite was obtained by the hydrothermal treatment of spindle-like Li2FeSiO4 in glucose solution at 190 ℃ for 3 h.Electrochemical measurements show that after carbon coating,the electrode performances such as discharge capacity and high-rate capability are greatly enhanced.In particular.Li2FeSiO4-C with carbon content of 7.21 wt%delivers the discharge capacities of 160.9 mAh·g-1 at room temperature and 213 mAh·g-1 at45℃(0.1 C),revealing the potential application in lithium-ion batteries.
基金supported financially by the National Natural Foundation of China(Grant No.51672234)the Research Foundation for Hunan Youth Outstanding People from Hunan Provincial Science and Technology Department(2015RS4030)+1 种基金Hunan 2011 Collaborative Innovation Center of Chemical Engineering&Technology with Environmental Benignity and Effective Resource UtilizationProgram for Innovative Research Cultivation Team in University of Ministry of Education of China(1337304)
文摘Hierarchical Sb_2S_3 hollow microspheres assembled by nanowires have been successfully synthesized by a simple and practical hydrothermal reaction. The possible formation process of this architecture was investigated by X-ray diffraction, focused-ion beam-scanning electron microscopy dual-beam system, and transmission electron microscopy. When used as the anode material for lithium-ion batteries, Sb_2S_3 hollow microspheres manifest excellent rate property and enhanced lithium-storage capability and can deliver a discharge capacity of 674 m Ah g^(-1) at a current density of 200 m A g^(-1) after 50 cycles. Even at a high currentdensity of 5000 m A g^(-1), a discharge capacity of541 m Ah g^(-1) is achieved. Sb_2S_3 hollow microspheres also display a prominent sodium-storage capacity and maintain a reversible discharge capacity of 384 m Ah g^(-1) at a current density of 200 m A g^(-1) after 50 cycles. The remarkable lithium/sodium-storage property may be attributed to the synergetic effect of its nanometer size and three-dimensional hierarchical architecture, and the outstanding stability property is attributed to the sufficient interior void space,which can buffer the volume expansion.
基金the financial support of the National Natural Science Foundation of China(Nos.21875206,21403187)the Natural Science Foundation of Hebei Province(No.B2019203487)the open project in Key Lab Adv.Energy Mat.Chem.(Nankai University)。
文摘The development of novel organic electrode materials is of great significance for improving the reversible capacity and cycle stability of rechargeable batteries.Before practical application,it is essential to characterize the electrode materials to study their structures,redox mechanisms and electrochemical performances.In this review,the common characterization methods that have been adopted so far are summarized from two aspects:experimental characterization and theoretical calculation.The experimental characterization is introduced in detail from structural characterization,electrochemical characterization and electrode reaction chara cterization.The experimental purposes and working principles of various experimental characterization methods are briefly illustrated.As the auxilia ry means,theoretical calculation provides the theoretical basis for characterizing the electrochemical reaction mechanism of organic electrode materials.Through these characterizations,we will have a deep understanding about the material structures,electrochemical redox mechanisms,electrochemical properties and the relationships of structure-property.It is hoped that this review would help researchers to select the suitable characterization methods to analyze the structures and performances of organic electrode materials quickly and effectively.
基金Project(51672234)supported by the National Natural Science Foundation of ChinaProject(1337304)supported by the Program for Innovative Research Cultivation Team in University,Ministry of Education,China
文摘Na0.44MnO2 nanorods have been prepared by a hydrothermal method.The experimental parameters have been systematically investigated and optimized.The results show that Na0.44MnO2 nanorods obtained via the hydrothermal treatment at 200℃for 16 h show the best electrochemical properties,which deliver the high initial discharge capacity of 110.7 mA·h/g at 50 mA/g in potential window 2.0-4.0 V.To further improve their electrochemical properties,a ball milling process with graphene has been carried out to obtain Na0.44MnO2/graphene composite.The initial discharge capacity of Na0.44MnO2/graphene composite is 106.9 mA·h/g at a current density of 50 mA/g.After 100 cycles,the residual discharge capacity is 91.8 mA·h/g and the capacity retention rate is 85.9%,which is much higher than that of pristine Na0.44MnO2 nanorods(74.7%)at the same condition.What is more,when the current density reaches 500 and 1000 mA/g,the corresponding discharge capacities of Na0.44MnO2/graphene composite are about 89 and 78 mA·h/g,respectively,indicating outstanding rate capability.
基金supported financially by the National Natural Science Foundation of China (Grant No.51672234)Hunan 2011 Collaborative Innovation Center of Chemical Engineering and Technology with Environmental Benignity and Effective Resource Utilization, Program for Innovative Research Cultivation Team in University of Ministry of Education of China (1337304)the 111 Project (B12015)
文摘Nitrogen-doped TiO_2–C composite nanofibers(TiO_2/N–C NFs) were manufactured by a convenient and green electrospinning technique in which urea acted as both the nitrogen source and a pore-forming agent. The TiO_2/N–C NFs exhibit a large specific surface area(213.04 m^2 g^(-1)) and a suitable nitrogen content(5.37 wt%). The large specific surface area can increase the contribution of the extrinsic pseudocapacitance, which greatly enhances the rate capability. Further, the diffusion coefficient of sodium ions(DNa_+) could be greatly improved by the incorporation of nitrogen atoms. Thus, the TiO_2/N–C NFs display excellent electrochemical properties in Na-ion batteries. A TiO_2/N–C NF anode delivers a high reversible discharge capacity of 265.8 mAh g^(-1) at 0.05 A g^(-1) and an outstanding long cycling performance even at a high current density(118.1 m Ah g^(-1)) with almost no capacity decay at 5 A g^(-1) over 2000 cycles. Therefore, this work sheds light on the application of TiO_2-based materials in sodium-ion batteries.
文摘Exploring the production and application of clean energy has always been the core of sustainable development.As a clean and sustainable technology,electrocatalysis has been receiving widespread attention.It is crucial to achieve efficient,stable and cheap electrocatalysts.However,the traditional“trial and error”method is time-consuming,laborious and costly.In recent years,with the significant increase in computing power,computations have played an important role in electrocatalyst design.Nevertheless,it is still difficult to search for advanced electrocatalysts in the vast chemical space through traditional density functional theory(DFT)computations.Fortunately,the development of machine learning and interdisciplinary integration will inject new impetus into targeted design of electrocatalysts.Machine learning is able to predict electrochemical performances with an accuracy close to DFT.Here we provide an overview of the application of machine learning in electrocatalyst design,including the prediction of structure,thermodynamic properties and kinetic barriers.We also discuss the potential of explicit solvent model combined with machine learning molecular dynamics in this field.Finally,the favorable circumstances and challenges are outlined for the future development of machine learning in electrocatalysis.The studies on electrochemical processes by machine learning will further realize targeted design of high-efficiency electrocatalysts.
基金supported by National Natural Science Foundation of China(Nos.51772272 and 51728204)Fundamental Research Funds for the Central Universities(No.2018QNA4011)+3 种基金Science and Technology Program of Guangdong Province of China(No.2016A010104020)Pearl River S&T Nova Program of Guangzhou(No.201610010116)Qianjiang Talents Plan D(QJD1602029)Startup Foundation for Hundred-Talent Program of Zhejiang University.
文摘Rational design of hybrid carbon host with high electrical conductivity and strong adsorption toward soluble lithium polysulfides is the main challenge for achieving high-performance lithium-sulfur batteries(LSBs).Herein,novel binder-free Ni@N-doped carbon nanospheres(N-CNSs)films as sulfur host are firstly synthesized via a facile combined hydrothermal-atomic layer deposition method.The cross-linked multilayer N-CNSs films can effectively enhance the electrical conductivity of electrode and provide physical blocking“dams”toward the soluble long-chain polysulfides.Moreover,the doped N heteroatoms and superficial NiO layer on Ni layer can work synergistically to suppress the shuttle of lithium polysulfides by effective chemical interaction/adsorption.In virtue of the unique composite architecture and reinforced dual physical and chemical adsorption to the soluble polysulfides,the obtained Ni@N-CNSs/S electrode is demonstrated with enhanced rate performance(816 mAh g?1 at 2 C)and excellent long cycling life(87%after 200 cycles at 0.1 C),much better than N-CNSs/S electrode and other carbon/S counterparts.Our proposed design strategy offers a promising prospect for construction of advanced sulfur cathodes for applications in LSBs and other energy storage systems.