In the context of diminishing energy resources and worsening greenhouse effect,thermoelectric materials have great potential for sustainable development due to their green and environmentally friendly characteristics....In the context of diminishing energy resources and worsening greenhouse effect,thermoelectric materials have great potential for sustainable development due to their green and environmentally friendly characteristics.Among inorganic thermoelectric materials,copper sulfide compounds have greater potential than others due to their abundant element reserves on Earth,lower usage costs,non-toxicity,and good biocompatibility.Compared to organic thermoelectric materials,the"phonon liquid-electron crystal"(PLEC)feature of copper sulfide compounds makes them have stronger thermoelectric performance.This review summarizes the latest research progress in the synthesis methods and thermoelectric modification strategies of copper sulfide compounds.It first explains the importance of the solid-phase method in the manufacture of thermoelectric devices,and then focuses on the great potential of nanoscale synthesis technology based on liquid-phase method in the preparation of thermoelectric materials.Finally,it systematically discusses several strategies for regulating the thermoelectric performance of copper sulfide compounds,including adjusting the chemical proportion of Cu_(2-x)S and introducing element doping to regulate the crystal structure,phase composition,chemical composition,band structure,and nanoscale microstructure of copper sulfide compounds,and directly affecting ZT value by adjusting conductivity and thermal conductivity.In addition,it discusses composite engineering based on copper sulfide compounds,including inorganic,organic,and metal compounds,and discusses tri-component compounds derived from sulfide copper.Finally,it discusses the main challenges and prospects of the development of copper sulfide-based thermoelectric materials,hoping that this review will promote the development of copper sulfide-based thermoelectric materials.展开更多
Conversion-alloy-type anodes have attracted considerable attention in potassium-ion batteries due to their high theoretical capacities,but the inferior stability hinders their potential applications.Generally,the fail...Conversion-alloy-type anodes have attracted considerable attention in potassium-ion batteries due to their high theoretical capacities,but the inferior stability hinders their potential applications.Generally,the failure mechanism of conversion-alloy anodes is ascribed to volume expansion or the shuttle effect,which,however,fails to adequately explain their characteristic electrochemical behavior:an initial rapid drop and then a gradual decline in capacity.Herein,by combining electrochemical characterizations with multi-scale microscopies,spectroscopy,and theoretical calculations,we systematically analyze the failure mechanism of Bi_(2)Te_(3),a typical conversion-alloy anode.The failure processes and mechanisms are identified into two stages:(1)the rapid capacity fading dominated by the shuttle effect in the first several cycles and(2)the gradual material deactivation and capacity decline due to solid-electrolyte interphase accumulation in the following cycles.Furthermore,in response to these failure mechanisms,an elaborate design of Bi_(2)Te_(3)-based electrode featuring ultrafine nanoparticles and carbon encapsulation is presented,which exhibits prominent capability in avoiding the above negative effects and substantially enhancing cycling stability.This study reveals the failure mechanism of conversion-alloy anode throughout its entire life cycle,and the gained insight may lead to targeted optimization strategies for stable high-capacity electrodes.展开更多
Anode-free sodium metal batteries hold significant promise for high-energy-density storage but face critical challenges related to sodium deposition dynamics and interfacial instability.Traditional approaches,such as ...Anode-free sodium metal batteries hold significant promise for high-energy-density storage but face critical challenges related to sodium deposition dynamics and interfacial instability.Traditional approaches,such as alloy-based current collectors or fluorinated interfaces,often suffer from irreversible volume expansion or corrosive fabrication processes.This study introduces a solvent co-intercalation-mediated in situ sodiophilic interface engineering strategy to overcome these limitations.A graphitized carbon-modified aluminum current collector dynamically regulates interfacial evolution through solvated sodium-ion co-intercalation during initial cycling,prompting the formation of a C-NaF interface with ultralow Na^(+)adsorption energy.This sodiophilic interface not only facilitates uniform sodium nucleation by providing abundant sodium-philic sites but also encourages the preferential decomposition of anions in the electrolyte,leading to the creation of a robust and NaF-rich solid electrolyte interphase.Consequently,the asymmetric half-cell delivers an ultralow nucleation overpotential(9.7 mV at 0.5 mA cm^(-2))and maintains an average coulombic efficiency of 99.8%over 400 cycles at 1 mA cm^(-2).When combined with a Na_(3)V_(2)(PO_(4))_(2)O_(2)F(NVPOF)cathode,the full cell achieves an energy density of 363 Wh kg^(-1) with 80%capacity retention after 250 cycles at 0.5 C.This work integrates molecular-level dynamic interfacial engineering with macroscopic electrochemical stability,providing a scalable industrial solution for next-generation battery systems.展开更多
Due to their excellent photoelectron chemical properties and suitable energy level alignment with perovskite,perylene diimide(PDI)derivatives are competitive non-fullerene electron transport material(ETM)candidates fo...Due to their excellent photoelectron chemical properties and suitable energy level alignment with perovskite,perylene diimide(PDI)derivatives are competitive non-fullerene electron transport material(ETM)candidates for perovskite solar cells(PSCs).However,the conjugated rigid plane structure of PDI units result in PDI-based ETMs tending to form large aggregates,limiting their application and photovoltaic performance.In this study,to restrict aggregation and further enhance the photovoltaic performance of PDI-type ETMs,two PDI-based ETMs,termed PDO-PDI2(dimer)and PDO-PDI3(trimer),were constructed by introducing a phenothiazine 5,5-dioxide(PDO)core building block.The research manifests that the optoelectronic properties and film formation property of PDO-PDI2 and PDO-PDI3 were deeply affected by the molecular spatial configuration.Applied in PSCs,PDO-PDI3 with threedimensional spiral molecular structure,exhibits superior electron extraction and transport properties,further achieving the best PCE of 18.72%and maintaining 93%of its initial efficiency after a 720-h aging test under ambient conditions.展开更多
The thermal stability of lithium-ion battery separators is a critical determinant of battery safety and performance,especially in the context of rapidly expanding applications in electric vehicles and energy storage s...The thermal stability of lithium-ion battery separators is a critical determinant of battery safety and performance,especially in the context of rapidly expanding applications in electric vehicles and energy storage systems.While traditional polyolefin separators(PP/PE)dominate the market due to their cost-effectiveness and mechanical robustness,their inherent poor thermal stability poses significant safety risks under high-temperature conditions.This review provides a comprehensive analysis of recent advancements in enhancing separator thermal stability through coating materials(metal,ceramic,inorganic)and novel high-temperature-resistant polymers(e.g.,PVDF copolymers,PI,PAN).Notably,we critically evaluate the trade-offs between thermal resilience and electrochemical performance,such as the unintended increase in electronic conductivity from metal coatings(e.g.,Cu,MOFs)and reduced electrolyte wettability in ceramic coatings(e.g.,Al_(2)O_(3)).Innovations in hybrid coatings(e.g.,BN/PAN composites,gradient-structured MOFs)and scalable manufacturing techniques(e.g.,roll-to-roll electrospinning)are highlighted as promising strategies to balance these competing demands.Furthermore,a comparative analysis of next-generation high-temperature-resistant separators underscores their ionic conductivity,mechanical strength,and scalability,offering actionable insights for material selection.The review concludes with forward-looking perspectives on integrating machine learning for material discovery,optimizing interfacial adhesion in ceramic coatings,and advancing semi-/all-solid-state batteries to address both thermal and electrochemical challenges.This work aims to bridge the gap between laboratory innovations and industrial applications,fostering safer and more efficient lithium battery technologies.展开更多
Antimony sulfide(Sb_(2)S_(3))is a promising material for photoelectrochemical(PEC)devices that generate green hydrogen from sunlight and water.In this study,we present a synthesis of high-performance Sb_(2)S_(3)photoa...Antimony sulfide(Sb_(2)S_(3))is a promising material for photoelectrochemical(PEC)devices that generate green hydrogen from sunlight and water.In this study,we present a synthesis of high-performance Sb_(2)S_(3)photoanodes via an interface-engineered hydrothermal growth followed by rapid thermal annealing(RTA).A TiO_(2)interfacial layer plays a crucial role in ensuring homogeneous precursor deposition,enhancing light absorption,and forming efficient heterojunctions with Sb_(2)S_(3),thereby significantly improving charge separation and transport.RTA further improves crystallinity and interfacial contact,resulting in dense and uniform Sb_(2)S_(3)films with enlarged grains and fewer defects.The optimized Sb_(2)S_(3)photoanode achieves a photocurrent density of 2.51 mA/cm^(2)at 1.23 V vs.the reversible hydrogen electrode(RHE),one of the highest reported for Sb_(2)S_(3)without additional catalysts or passivation layers.To overcome the limitations of oxygen evolution reaction(OER),we employ the iodide oxidation reaction(IOR)as an alternative,significantly lowering the overpotential and improving charge transfer kinetics.Consequently,it produces a record photocurrent density of 8.9 mA/cm^(2)at 0.54 V vs.RHE.This work highlights the synergy between TiO_(2)interfacial engineering,RTA-induced crystallization,and IOR-driven oxidation,offering a promising pathway for efficient and scalable PEC hydrogen production.展开更多
In this review,we propose a comprehensive overview of additive manufacturing(AM)technologies and design possibilities in manufacturing metamaterials for various applications in the biomedical field,of which many are i...In this review,we propose a comprehensive overview of additive manufacturing(AM)technologies and design possibilities in manufacturing metamaterials for various applications in the biomedical field,of which many are inspired by nature itself.It describes how new AM technologies(e.g.continuous liquid interface production and multiphoton polymerization,etc)and recent developments in more mature AM technologies(e.g.powder bed fusion,stereolithography,and extrusion-based bioprinting(EBB),etc)lead to more precise,efficient,and personalized biomedical components.EBB is a revolutionary topic creating intricate models with remarkable mechanical compatibility of metamaterials,for instance,stress elimination for tissue engineering and regenerative medicine,negative or zero Poisson’s ratio.By exploiting the designs of porous structures(e.g.truss,triply periodic minimal surface,plant/animal-inspired,and functionally graded lattices,etc),AM-made bioactive bone implants,artificial tissues,and organs are made for tissue replacement.The material palette of the AM metamaterials has high diversity nowadays,ranging from alloys and metals(e.g.cobalt-chromium alloys and titanium,etc)to polymers(e.g.biodegradable polycaprolactone and polymethyl methacrylate,etc),which could be even integrated within bioactive ceramics.These advancements are driving the progress of the biomedical field,improving human health and quality of life.展开更多
Phenolic foam(PF)has attracted growing attention in plugging areas due to its lightweight,flame retardancy and high fillability,yet its friable character and high reaction temperature severely weaken its potentials to...Phenolic foam(PF)has attracted growing attention in plugging areas due to its lightweight,flame retardancy and high fillability,yet its friable character and high reaction temperature severely weaken its potentials toward practical coal mining applications.Herein,a novel phenolic composite material filled with modified fly ash(MFA)geopolymer has been proposed to address the above issues.By modifying fly ash(FA)particles with siloxanes,robust interfacial bonding between the organic PF polymer and inorganic geopolymer network has been established,which enables modulation of their micro-morphologies to optimize their macro performances.The foam structure of PF evolves from an open-cell to a closed-cell morphology with the incorporation of MFA,leading to a decreased pulverization ratio(41%)while enhanced mechanical properties(15%).Compared with neat PF,the composite exhibits faster gelation dynamics during curing,with a maximum reaction temperature as low as only 40°C.PF/MFA composite show high reliability against gas leakage during a laboratory designed coal mine plugging test.Furthermore,the formation of a silica hybrid char layer with higher graphitization degree and a multiple continuous closed-cell structure following the combustion of PF/MFA effectively inhibits the release of combustible volatiles and toxic gases.It is provided that this strategy of geopolymer filled polymer cross-linking networks with tunable morphology opens up an avenue for advanced mining phenolic filling materials.展开更多
Development of efficient and stable metal catalysts for the selective aqueous phase hydrodeoxygenation(HDO)of biomass-derived oxygenates to value-added biofuels is highly desired.An innovative surface microenvironment...Development of efficient and stable metal catalysts for the selective aqueous phase hydrodeoxygenation(HDO)of biomass-derived oxygenates to value-added biofuels is highly desired.An innovative surface microenvironment modulation strategy was used to construct the nitrogen-doped hollow carbon sphere encapsulated with Pd(Pd@NHCS-X,X:600–800)nanoreactors for catalytic HDO of biomass-derived vanillin in water.The specific surface microenvironments of Pd@NHCS catalysts including the electronic property of active Pd centers and the surface wettability and porous structure of NHCS supports could be well-controlled by the calcination temperature of catalysts.Intrinsic kinetic evaluations demonstrated that the Pd@NHCS-600 catalyst presented a high turnover frequency of 337.77 h^(–1)and a low apparent activation energy of 18.63 kJ/mol.The excellent catalytic HDO performance was attributed to the unique surface microenvironment of Pd@NHCS catalyst based on structure-performance relationship analysis and DFT calculations.It revealed that pyridinic N species dominated the electronic property regulation of Pd sites through electronic metal-support interaction(EMSI)and produced numerous electron-rich active Pd centers,which not only intensified the dissociation and activation of H2 molecules,but also substantially improved the activation capability of vanillin via the enhanced adsorption of–C=O group.The fine hydrophilicity and abundant porous structure promoted the uniform dispersion of catalyst and ensured the effective access of reactants to catalytic active centers in water.Additionally,the Pd@NHCS-600 catalyst exhibited excellent catalytic stability and broad substrate applicability for the selective aqueous phase HDO of various biomass-derived carbonyl compounds.The proposed surface microenvironment modulation strategy will provide a new consideration for the rational design of high-performance nitrogen-doped carbon-supported metal catalysts for catalytic biomass transformation.展开更多
The emerging n-type Mg_(3)(Sb,Bi)_(2)-based materials have attracted considerable attention for their excellent thermoelectric performance.Whereas,practical thermoelectric device applications require materials that ex...The emerging n-type Mg_(3)(Sb,Bi)_(2)-based materials have attracted considerable attention for their excellent thermoelectric performance.Whereas,practical thermoelectric device applications require materials that exhibit not only superior thermoelectric performance but also robust mechanical properties.This work systematically investigates the mechanical and thermoelectric properties of Mg_(3.2-x)Ce_(x)SbBi_(0.97)Te_(0.03).The x=0.04 sample exhibits a Vickers hardness of up to 1012 MPa.The compressive and bending stress–strain curves show that minor doping can enhance the strength while maintaining high plasticity.展开更多
Lithium(Li)deposition and nucleation at solid electrolyte interphase(SEI)is the main origin for the capacity decay in Li metal batteries(LMBs).SEI conversion with enhanced electrochemical and mechanical properties is ...Lithium(Li)deposition and nucleation at solid electrolyte interphase(SEI)is the main origin for the capacity decay in Li metal batteries(LMBs).SEI conversion with enhanced electrochemical and mechanical properties is an effective approach to achieve uniform nucleation of Li^(+)and stabilize the lithium metal anode.However,complex interfacial reaction mechanisms and interface compatibility issues hinder the development of SEI conversion strategies for stabilizing lithium metal anodes.Herein,we presented the release of I_(3)^(-)in–NH_(2)-modified metal–organic frameworks for a Li metal surface SEI phase conversion strategy.The–NH_(2)group in MOF pores induced the formation of I_(3)^(-)from I_(2),which was further spontaneously reacted with inactive Li_(2)O transforming into high-performance LiI and LiIO_(3)interphase.Furthermore,theoretical calculation provided deeply insight into the unique reconstructed interfacial formation and electrochemical mechanism of rich LiI and LiIO_(3)SEI.As a result,the Li^(+)deposition and nucleation were improved,facilitating the transport kinetics of Li^(+)and inhibiting the growth of lithium dendrites.The assembled solid-state Li||LiFePO_(4)full cells exhibited superior long-term stability of 800 cycles and high Coulombic efficiency(>99%),Li||LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)pouch cell also displayed superior practical performance over 200 cycles at 2 C,high loading of 5 mg cm^(-2)and safety performance.This innovative SEI design strategy promotes the development of high-performance solid-state Li metal batteries.展开更多
Considering the growing pre-lithiation demand for high-performance Si-based anodes and consequent additional costs caused by the strict pre-lithiation environment,developing effective and environmentally stable pre-li...Considering the growing pre-lithiation demand for high-performance Si-based anodes and consequent additional costs caused by the strict pre-lithiation environment,developing effective and environmentally stable pre-lithiation additives is a challenging research hotspot.Herein,interfacial engineered multifunctional Li_(13)Si_(4)@perfluoropolyether(PFPE)/LiF micro/nanoparticles are proposed as anode pre-lithiation additives,successfully constructed with the hybrid interface on the surface of Li_(13)Si_(4)through PFPE-induced nucleophilic substitution.The synthesized multifunctional Li_(13)Si_(4)@PFPE/LiF realizes the integration of active Li compensation,long-term chemical structural stability in air,and solid electrolyte interface(SEI)optimization.In particular,the Li_(13)Si_(4)@PFPE/LiF with a high pre-lithiation capacity(1102.4 mAh g^(-1))is employed in the pre-lithiation Si-based anode,which exhibits a superior initial Coulombic efficiency of 102.6%.Additionally,in situ X-ray diffraction/Raman,density functional theory calculation,and finite element analysis jointly illustrate that PFPE-predominant hybrid interface with modulated abundant highly electronegative F atoms distribution reduces the water adsorption energy and oxidation kinetics of Li_(13)Si_(4)@PFPE/LiF,which delivers a high pre-lithiation capacity retention of 84.39%after exposure to extremely moist air(60%relative humidity).Intriguingly,a LiF-rich mechanically stable bilayer SEI is constructed on anodes through a pre-lithiation-driven regulation for the behavior of electrolyte decomposition.Benefitting from pre-lithiation via multifunctional Li_(13)Si_(4)@PFPE/LiF,the full cell and pouch cell assembled with pre-lithiated anodes operate with long-time stability of 86.5%capacity retention over 200 cycles and superior energy density of 549.9 Wh kg^(-1),respectively.The universal multifunctional pre-lithiation additives provide enlightenment on promoting large-scale applications of pre-lithiation on commercial high-energy-density and long-cycle-life lithium-ion batteries.展开更多
Pulsed-laser deposition has been developed to prepare large-area In_(2)S_(3)nanofilms and their photoelectric characteristics have been investigated.The In_(2)S_(3)nanofilm grown under 500℃is highly oriented along th...Pulsed-laser deposition has been developed to prepare large-area In_(2)S_(3)nanofilms and their photoelectric characteristics have been investigated.The In_(2)S_(3)nanofilm grown under 500℃is highly oriented along the(103)direction with exceptional crystallinity.The corresponding(103)-oriented In_(2)S_(3)photodetectors exhibit broadband photoresponse from 370.6 nm to 1064 nm.Under 635 nm illumination,the optimized responsivity,external quantum efficiency,and detectivity reach 19.8 A/W,3869%,and 2.59×10^(12)Jones,respectively.In addition,the device exhibits short rise/decay time of 3.9/3.0 ms.Of note,first-principles calculations have unveiled that the effective carrier mass along the(103)lattice plane is much smaller than those along the(100),(110)and(111)lattice planes,which thereby enables high-efficiency transport of photocarriers and thereby the excellent photosensitivity.Profited from the sizable bandgap,the In_(2)S_(3)photodetectors also showcase strong robustness against elevated operating temperature.In the end,proof-of-concept imaging application beyond human vision and under high operating temperature as well as heart rate monitoring have been achieved by using the In_(2)S_(3)device of the sensing component.This study introduces a novel crystal orientation engineering paradigm for the implementation of next-generation advanced optoelectronic systems.展开更多
Device fabrication is increasing with the importance of functional materials for industrial applications.To fulfil increasing demands,rare earth elementbased materials have become important.In particular,lanthanum(La)...Device fabrication is increasing with the importance of functional materials for industrial applications.To fulfil increasing demands,rare earth elementbased materials have become important.In particular,lanthanum(La) and La-based materials have garnered attention in recent years due to their versatile properties and wide range of potential applications.This critical review provides a comprehensive overview of the advancements in the utilization of La and its compounds across various fields.In the realm of sensing and biosensing,La-based materials exhibit better sensitivity and selectivity,indicating their suitability for detecting environmental pollutants and biomolecules.The review also explores their role in supercapacitors,where their unique electrochemical properties contribute to enhanced performance and stability.Furthermore,the catalytic properties of La compounds are highlighted in water-splitting applications,emphasizing their efficiency in oxygen and hydrogen production.The biomedical applications of Labased materials are also examined,focusing on their biocompatibility and potential in drug delivery and medical imaging.This review aims to provide a critical analysis of the current state of research,identify challenges,and suggest future directions for the development and application of La and La-based materials in these diverse fields.展开更多
Polyurea(PUA)is widely valued in protective coatings and structural reinforcement because of its impressive mechanical strength and resistance to corrosion.Its high flammability,together with the poor dispersion that ...Polyurea(PUA)is widely valued in protective coatings and structural reinforcement because of its impressive mechanical strength and resistance to corrosion.Its high flammability,together with the poor dispersion that often comes with simply blending in flame retardants,continues to limit its use in demanding environments.To overcome these issues,this study introduces a different approach.We grafted 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide(DOPO)onto the surface of a metal-organic framework(MOF)and then partially amino-functionalized the DOPO layer,ultimately creating an amino-modified DOPO-MOF hybrid.The introduced amino groups can directly react with the isocyanate(-NCO)groups in the PUA matrix,allowing the flame-retardant component to be integrated via reactive integration rather than physical blending.This approach helps avoid the interfacial defects and the mechanical weakening typically observed in conventional blending.With 5 wt% ZIF-67@DOPO-NH2 added to the PUA system,the composite successfully reached a UL-94 V-0 classification and showed a notable increase in limiting oxygen index(LOI),from19.2% to 23.8%.The peak heat release rate and total heat release dropped by 36.3% and 38.7%,respectively.Meanwhile,the tensile strength decreased from 25.74 to 22.52 MPa,while the elongation at break remained above 300%,indicating that the material maintained excellent toughness.展开更多
Ammonium-ion hybrid supercapacitors(A-HSCs)have emerged as promising candidates for next-generation energy storage owing to their inherent safety and environmental sustainability.Hexagonal tungsten oxide(h-WO_(3)),wit...Ammonium-ion hybrid supercapacitors(A-HSCs)have emerged as promising candidates for next-generation energy storage owing to their inherent safety and environmental sustainability.Hexagonal tungsten oxide(h-WO_(3)),with its well-defined tunnel structure,holds great promise as a negative electrode material for NH^(4+)storage.However,its practical application is hindered by structural instability and poor intrinsic electrical conductivity.To address these challenges,a dual-regulation strategy is proposed,integrating molybdenum(Mo)doping and NH^(4+)pre-intercalation to concurrently optimize the tunnel structure and electronic environment of h-WO_(3)(Mo-NWO).Comprehensive experimental and theoretical analyses reveal that Mo doping narrows the bandgap of WO_(3)and reduces the diffusion energy barrier,thereby accelerating NH^(4+)adsorption and diffusion.Simultaneously,NH^(4+)pre-intercalation stabilizes the tunnel framework via hydrogen bonding,ensuring structural reversibility.As expected,the Mo-NWO/AC electrode achieves a high areal capacitance of 13.6 F cm^(−2)at 5 mA cm^(−2)and retains 80.14%of its capacitance after 5000 cycles,demonstrating exceptional rate capability and cycling stability.Moreover,the assembled Mn_(3)O_(4)//Mo-NWO/AC device delivers a high energy density of 3.41 mWh cm^(−2)and outstanding long-term stability(85.75%retention after 12,000 cycles).This work provides a viable strategy for designing high-performance NH^(4+)storage materials and advances the development of sustainable energy storage systems.展开更多
Photocatalysis is one of the most promising technologies for solving environmental and energy problems,but current photocatalysts still suffer from low visible light utilization and insufficient photogenerated charge ...Photocatalysis is one of the most promising technologies for solving environmental and energy problems,but current photocatalysts still suffer from low visible light utilization and insufficient photogenerated charge separation efficiency.Therefore,in this work,D-A tubular materials with tubular carbon nitride(TCN)as electron donor(D)and 2-mercaptobenzothiazole(BZ)as electron acceptor(A)were constructed by molecular doping and modulation of the carbon nitride geometry.It was shown that the introduction of BZ could modulate the electronic structure of the catalyst,promote electron migration from TCN to BZ,and inhibit the recombination of photogenerated electrons and holes.Meanwhile,the ultra-thin tubular structure could expose more active sites.In addition,the adsorption of protons by BZ-TCN was further improved due to the modulation of the charge distribution between the components by the introduction of small molecules.Among them,the photocatalytic hydrogen production rate of BZ_(0.1)-TCN was twice that of TCN.The in-depth discussion of the components through theoretical calculations and characterization tests contributes to the understanding of the mechanism of photocatalytic hydrogen production.展开更多
Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully syn...Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.展开更多
Thermocells are attracting growing interest as a promising thermoelectric technology for low-grade heat harvesting.However,the scarcity of high-performance redox couples featuring intrinsically high thermopower(Se)and...Thermocells are attracting growing interest as a promising thermoelectric technology for low-grade heat harvesting.However,the scarcity of high-performance redox couples featuring intrinsically high thermopower(Se)and fast redox kinetics hinders the rapid development of thermocells.Identifying potential intrinsically high-performance redox couples remains a significant challenge.This work introduces a novel n-type copper(I/II)chloride(CuCl/CuCl2)redox couple with intrinsically high performance.Through tailored electrolyte design,long-term stability was significantly improved by reducing proton concentration to suppress cuprous ion photo-oxidation,while ammonium chloride solvation enhanced cuprous ion solubility.The resulting system achieves a Se value closely aligned with theoretical predictions and exhibits rapid redox kinetics.Consequently,the optimized CuCl/CuCl_(2) intrinsic system demonstrated a high S_(e) of 1.52 mV K^(−1) and a record-high normalized power density Pmax(ΔT)^(−2) of 0.399 mW m^(−2) K^(−2),surpassing previously reported intrinsic n-type thermocells and rivaling the performance of p-type pristine 0.4 M ferri/ferrocyanide systems.A prototype module comprising 30 p-n units successfully powered a line of light-emitting diodes or a thermohygrometer.This work introduces a valuable redox couple for further advancing high-performance thermocells and demonstrates a viable strategy for developing novel redox systems.展开更多
The thermal conductivity of nanofluids is an important property that influences the heat transfer capabilities of nanofluids.Researchers rely on experimental investigations to explore nanofluid properties,as it is a n...The thermal conductivity of nanofluids is an important property that influences the heat transfer capabilities of nanofluids.Researchers rely on experimental investigations to explore nanofluid properties,as it is a necessary step before their practical application.As these investigations are time and resource-consuming undertakings,an effective prediction model can significantly improve the efficiency of research operations.In this work,an Artificial Neural Network(ANN)model is developed to predict the thermal conductivity of metal oxide water-based nanofluid.For this,a comprehensive set of 691 data points was collected from the literature.This dataset is split into training(70%),validation(15%),and testing(15%)and used to train the ANN model.The developed model is a backpropagation artificial neural network with a 4–12–1 architecture.The performance of the developed model shows high accuracy with R values above 0.90 and rapid convergence.It shows that the developed ANN model accurately predicts the thermal conductivity of nanofluids.展开更多
文摘In the context of diminishing energy resources and worsening greenhouse effect,thermoelectric materials have great potential for sustainable development due to their green and environmentally friendly characteristics.Among inorganic thermoelectric materials,copper sulfide compounds have greater potential than others due to their abundant element reserves on Earth,lower usage costs,non-toxicity,and good biocompatibility.Compared to organic thermoelectric materials,the"phonon liquid-electron crystal"(PLEC)feature of copper sulfide compounds makes them have stronger thermoelectric performance.This review summarizes the latest research progress in the synthesis methods and thermoelectric modification strategies of copper sulfide compounds.It first explains the importance of the solid-phase method in the manufacture of thermoelectric devices,and then focuses on the great potential of nanoscale synthesis technology based on liquid-phase method in the preparation of thermoelectric materials.Finally,it systematically discusses several strategies for regulating the thermoelectric performance of copper sulfide compounds,including adjusting the chemical proportion of Cu_(2-x)S and introducing element doping to regulate the crystal structure,phase composition,chemical composition,band structure,and nanoscale microstructure of copper sulfide compounds,and directly affecting ZT value by adjusting conductivity and thermal conductivity.In addition,it discusses composite engineering based on copper sulfide compounds,including inorganic,organic,and metal compounds,and discusses tri-component compounds derived from sulfide copper.Finally,it discusses the main challenges and prospects of the development of copper sulfide-based thermoelectric materials,hoping that this review will promote the development of copper sulfide-based thermoelectric materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.52172240)the Natural Science Foundation of Jiangsu Province of China(BK20240591)the General Project of Education Department of Jiangsu Province(24KJB480008)。
文摘Conversion-alloy-type anodes have attracted considerable attention in potassium-ion batteries due to their high theoretical capacities,but the inferior stability hinders their potential applications.Generally,the failure mechanism of conversion-alloy anodes is ascribed to volume expansion or the shuttle effect,which,however,fails to adequately explain their characteristic electrochemical behavior:an initial rapid drop and then a gradual decline in capacity.Herein,by combining electrochemical characterizations with multi-scale microscopies,spectroscopy,and theoretical calculations,we systematically analyze the failure mechanism of Bi_(2)Te_(3),a typical conversion-alloy anode.The failure processes and mechanisms are identified into two stages:(1)the rapid capacity fading dominated by the shuttle effect in the first several cycles and(2)the gradual material deactivation and capacity decline due to solid-electrolyte interphase accumulation in the following cycles.Furthermore,in response to these failure mechanisms,an elaborate design of Bi_(2)Te_(3)-based electrode featuring ultrafine nanoparticles and carbon encapsulation is presented,which exhibits prominent capability in avoiding the above negative effects and substantially enhancing cycling stability.This study reveals the failure mechanism of conversion-alloy anode throughout its entire life cycle,and the gained insight may lead to targeted optimization strategies for stable high-capacity electrodes.
基金supported by the Natural Science Foundation Project of CQ(cstb2023nscq-msX0046).
文摘Anode-free sodium metal batteries hold significant promise for high-energy-density storage but face critical challenges related to sodium deposition dynamics and interfacial instability.Traditional approaches,such as alloy-based current collectors or fluorinated interfaces,often suffer from irreversible volume expansion or corrosive fabrication processes.This study introduces a solvent co-intercalation-mediated in situ sodiophilic interface engineering strategy to overcome these limitations.A graphitized carbon-modified aluminum current collector dynamically regulates interfacial evolution through solvated sodium-ion co-intercalation during initial cycling,prompting the formation of a C-NaF interface with ultralow Na^(+)adsorption energy.This sodiophilic interface not only facilitates uniform sodium nucleation by providing abundant sodium-philic sites but also encourages the preferential decomposition of anions in the electrolyte,leading to the creation of a robust and NaF-rich solid electrolyte interphase.Consequently,the asymmetric half-cell delivers an ultralow nucleation overpotential(9.7 mV at 0.5 mA cm^(-2))and maintains an average coulombic efficiency of 99.8%over 400 cycles at 1 mA cm^(-2).When combined with a Na_(3)V_(2)(PO_(4))_(2)O_(2)F(NVPOF)cathode,the full cell achieves an energy density of 363 Wh kg^(-1) with 80%capacity retention after 250 cycles at 0.5 C.This work integrates molecular-level dynamic interfacial engineering with macroscopic electrochemical stability,providing a scalable industrial solution for next-generation battery systems.
基金financially supported by the National Natural Science Foundation of China(Grants 21805114,21905119)Key Research and Development program of Jiangsu Province(BE2019009-2)+4 种基金Natural Science Foundation of Jiangsu province(BK20180869,BK20180867)China Postdoctoral Science Foundation(2019M651741),Top talents in Jiangsu province(XNY066)the Jiangsu University Foundation(17JDG032,17JDG031)Hightech Research Key laboratory of Zhenjiang(SS2018002)the State Key Laboratory of Fine Chemicals(KF1902)。
文摘Due to their excellent photoelectron chemical properties and suitable energy level alignment with perovskite,perylene diimide(PDI)derivatives are competitive non-fullerene electron transport material(ETM)candidates for perovskite solar cells(PSCs).However,the conjugated rigid plane structure of PDI units result in PDI-based ETMs tending to form large aggregates,limiting their application and photovoltaic performance.In this study,to restrict aggregation and further enhance the photovoltaic performance of PDI-type ETMs,two PDI-based ETMs,termed PDO-PDI2(dimer)and PDO-PDI3(trimer),were constructed by introducing a phenothiazine 5,5-dioxide(PDO)core building block.The research manifests that the optoelectronic properties and film formation property of PDO-PDI2 and PDO-PDI3 were deeply affected by the molecular spatial configuration.Applied in PSCs,PDO-PDI3 with threedimensional spiral molecular structure,exhibits superior electron extraction and transport properties,further achieving the best PCE of 18.72%and maintaining 93%of its initial efficiency after a 720-h aging test under ambient conditions.
基金supported by Beijing Institute of Technology Student Innovation Training Program(BIT2024LH013).
文摘The thermal stability of lithium-ion battery separators is a critical determinant of battery safety and performance,especially in the context of rapidly expanding applications in electric vehicles and energy storage systems.While traditional polyolefin separators(PP/PE)dominate the market due to their cost-effectiveness and mechanical robustness,their inherent poor thermal stability poses significant safety risks under high-temperature conditions.This review provides a comprehensive analysis of recent advancements in enhancing separator thermal stability through coating materials(metal,ceramic,inorganic)and novel high-temperature-resistant polymers(e.g.,PVDF copolymers,PI,PAN).Notably,we critically evaluate the trade-offs between thermal resilience and electrochemical performance,such as the unintended increase in electronic conductivity from metal coatings(e.g.,Cu,MOFs)and reduced electrolyte wettability in ceramic coatings(e.g.,Al_(2)O_(3)).Innovations in hybrid coatings(e.g.,BN/PAN composites,gradient-structured MOFs)and scalable manufacturing techniques(e.g.,roll-to-roll electrospinning)are highlighted as promising strategies to balance these competing demands.Furthermore,a comparative analysis of next-generation high-temperature-resistant separators underscores their ionic conductivity,mechanical strength,and scalability,offering actionable insights for material selection.The review concludes with forward-looking perspectives on integrating machine learning for material discovery,optimizing interfacial adhesion in ceramic coatings,and advancing semi-/all-solid-state batteries to address both thermal and electrochemical challenges.This work aims to bridge the gap between laboratory innovations and industrial applications,fostering safer and more efficient lithium battery technologies.
基金supported by the National Research Foundation of Korea(NRF)grant fu nded by the Korean government(MSIT)(No.RS-2024-00335976)。
文摘Antimony sulfide(Sb_(2)S_(3))is a promising material for photoelectrochemical(PEC)devices that generate green hydrogen from sunlight and water.In this study,we present a synthesis of high-performance Sb_(2)S_(3)photoanodes via an interface-engineered hydrothermal growth followed by rapid thermal annealing(RTA).A TiO_(2)interfacial layer plays a crucial role in ensuring homogeneous precursor deposition,enhancing light absorption,and forming efficient heterojunctions with Sb_(2)S_(3),thereby significantly improving charge separation and transport.RTA further improves crystallinity and interfacial contact,resulting in dense and uniform Sb_(2)S_(3)films with enlarged grains and fewer defects.The optimized Sb_(2)S_(3)photoanode achieves a photocurrent density of 2.51 mA/cm^(2)at 1.23 V vs.the reversible hydrogen electrode(RHE),one of the highest reported for Sb_(2)S_(3)without additional catalysts or passivation layers.To overcome the limitations of oxygen evolution reaction(OER),we employ the iodide oxidation reaction(IOR)as an alternative,significantly lowering the overpotential and improving charge transfer kinetics.Consequently,it produces a record photocurrent density of 8.9 mA/cm^(2)at 0.54 V vs.RHE.This work highlights the synergy between TiO_(2)interfacial engineering,RTA-induced crystallization,and IOR-driven oxidation,offering a promising pathway for efficient and scalable PEC hydrogen production.
基金sponsored by the Science and Technology Program of Hubei Province,China(2022EHB020,2023BBB096)support provided by Centre of the Excellence in Production Research(XPRES)at KTH。
文摘In this review,we propose a comprehensive overview of additive manufacturing(AM)technologies and design possibilities in manufacturing metamaterials for various applications in the biomedical field,of which many are inspired by nature itself.It describes how new AM technologies(e.g.continuous liquid interface production and multiphoton polymerization,etc)and recent developments in more mature AM technologies(e.g.powder bed fusion,stereolithography,and extrusion-based bioprinting(EBB),etc)lead to more precise,efficient,and personalized biomedical components.EBB is a revolutionary topic creating intricate models with remarkable mechanical compatibility of metamaterials,for instance,stress elimination for tissue engineering and regenerative medicine,negative or zero Poisson’s ratio.By exploiting the designs of porous structures(e.g.truss,triply periodic minimal surface,plant/animal-inspired,and functionally graded lattices,etc),AM-made bioactive bone implants,artificial tissues,and organs are made for tissue replacement.The material palette of the AM metamaterials has high diversity nowadays,ranging from alloys and metals(e.g.cobalt-chromium alloys and titanium,etc)to polymers(e.g.biodegradable polycaprolactone and polymethyl methacrylate,etc),which could be even integrated within bioactive ceramics.These advancements are driving the progress of the biomedical field,improving human health and quality of life.
基金supported by the National Natural Science Foundation of China(No.U22A20151)Taiyuan Major Science and Technology Project in 2021.
文摘Phenolic foam(PF)has attracted growing attention in plugging areas due to its lightweight,flame retardancy and high fillability,yet its friable character and high reaction temperature severely weaken its potentials toward practical coal mining applications.Herein,a novel phenolic composite material filled with modified fly ash(MFA)geopolymer has been proposed to address the above issues.By modifying fly ash(FA)particles with siloxanes,robust interfacial bonding between the organic PF polymer and inorganic geopolymer network has been established,which enables modulation of their micro-morphologies to optimize their macro performances.The foam structure of PF evolves from an open-cell to a closed-cell morphology with the incorporation of MFA,leading to a decreased pulverization ratio(41%)while enhanced mechanical properties(15%).Compared with neat PF,the composite exhibits faster gelation dynamics during curing,with a maximum reaction temperature as low as only 40°C.PF/MFA composite show high reliability against gas leakage during a laboratory designed coal mine plugging test.Furthermore,the formation of a silica hybrid char layer with higher graphitization degree and a multiple continuous closed-cell structure following the combustion of PF/MFA effectively inhibits the release of combustible volatiles and toxic gases.It is provided that this strategy of geopolymer filled polymer cross-linking networks with tunable morphology opens up an avenue for advanced mining phenolic filling materials.
文摘Development of efficient and stable metal catalysts for the selective aqueous phase hydrodeoxygenation(HDO)of biomass-derived oxygenates to value-added biofuels is highly desired.An innovative surface microenvironment modulation strategy was used to construct the nitrogen-doped hollow carbon sphere encapsulated with Pd(Pd@NHCS-X,X:600–800)nanoreactors for catalytic HDO of biomass-derived vanillin in water.The specific surface microenvironments of Pd@NHCS catalysts including the electronic property of active Pd centers and the surface wettability and porous structure of NHCS supports could be well-controlled by the calcination temperature of catalysts.Intrinsic kinetic evaluations demonstrated that the Pd@NHCS-600 catalyst presented a high turnover frequency of 337.77 h^(–1)and a low apparent activation energy of 18.63 kJ/mol.The excellent catalytic HDO performance was attributed to the unique surface microenvironment of Pd@NHCS catalyst based on structure-performance relationship analysis and DFT calculations.It revealed that pyridinic N species dominated the electronic property regulation of Pd sites through electronic metal-support interaction(EMSI)and produced numerous electron-rich active Pd centers,which not only intensified the dissociation and activation of H2 molecules,but also substantially improved the activation capability of vanillin via the enhanced adsorption of–C=O group.The fine hydrophilicity and abundant porous structure promoted the uniform dispersion of catalyst and ensured the effective access of reactants to catalytic active centers in water.Additionally,the Pd@NHCS-600 catalyst exhibited excellent catalytic stability and broad substrate applicability for the selective aqueous phase HDO of various biomass-derived carbonyl compounds.The proposed surface microenvironment modulation strategy will provide a new consideration for the rational design of high-performance nitrogen-doped carbon-supported metal catalysts for catalytic biomass transformation.
基金supported by the National Natural Science Foundation of China(Nos.12174297,and 12204342)the Fundamental Research Program of Shanxi Province(Nos.202203021212323,and 202203021212304)+2 种基金the Taiyuan University of Science and Technology Scientific Research Initial Funding(No.20222015,and 20232094)Funding for Outstanding Doctoral Research in Jin(Nos.20222039,and 20222040)the Research Practice and Innovation Program for Graduate Student of Shanxi Province(Nos.2024KY631,and 2024SJ301).
文摘The emerging n-type Mg_(3)(Sb,Bi)_(2)-based materials have attracted considerable attention for their excellent thermoelectric performance.Whereas,practical thermoelectric device applications require materials that exhibit not only superior thermoelectric performance but also robust mechanical properties.This work systematically investigates the mechanical and thermoelectric properties of Mg_(3.2-x)Ce_(x)SbBi_(0.97)Te_(0.03).The x=0.04 sample exhibits a Vickers hardness of up to 1012 MPa.The compressive and bending stress–strain curves show that minor doping can enhance the strength while maintaining high plasticity.
基金financial support from National Natural Science Foundation of China(22271178,U2032131,21972103)International Cooperation Key Project of Science and Technology Department of Shaanxi,China(2022KWZ-06)+3 种基金the Youth Talent Promotion Project of Science and Technology Association of Universities of Shaanxi Province(20210602)Research Project of Xi’an Science and Technology Bureau(2022GXFW0011)Science and Technology New Star in Shaanxi Province(2023KJXX-045)Shaanxi Provincial Department of Education Service Local Special Project,Industrialization Cultivation Project(23JC007)。
文摘Lithium(Li)deposition and nucleation at solid electrolyte interphase(SEI)is the main origin for the capacity decay in Li metal batteries(LMBs).SEI conversion with enhanced electrochemical and mechanical properties is an effective approach to achieve uniform nucleation of Li^(+)and stabilize the lithium metal anode.However,complex interfacial reaction mechanisms and interface compatibility issues hinder the development of SEI conversion strategies for stabilizing lithium metal anodes.Herein,we presented the release of I_(3)^(-)in–NH_(2)-modified metal–organic frameworks for a Li metal surface SEI phase conversion strategy.The–NH_(2)group in MOF pores induced the formation of I_(3)^(-)from I_(2),which was further spontaneously reacted with inactive Li_(2)O transforming into high-performance LiI and LiIO_(3)interphase.Furthermore,theoretical calculation provided deeply insight into the unique reconstructed interfacial formation and electrochemical mechanism of rich LiI and LiIO_(3)SEI.As a result,the Li^(+)deposition and nucleation were improved,facilitating the transport kinetics of Li^(+)and inhibiting the growth of lithium dendrites.The assembled solid-state Li||LiFePO_(4)full cells exhibited superior long-term stability of 800 cycles and high Coulombic efficiency(>99%),Li||LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)pouch cell also displayed superior practical performance over 200 cycles at 2 C,high loading of 5 mg cm^(-2)and safety performance.This innovative SEI design strategy promotes the development of high-performance solid-state Li metal batteries.
基金Huaiyu Shao acknowledges the Shenzhen-Hong Kong-Macao Science and Technology Plan Project(Category C)(Grant No.SGDX20220530111004028)the Macao Science and Technology Development Fund(FDCT)for funding(FDCT No.0013/2024/RIB1,FDCT-MOST joint project No.0026/2022/AMJ and No.006/2022/ALC of the Macao Centre for Research and Development in Advanced Materials[2022–2024])+2 种基金the Multi-Year Research Grant(MYRG)from University of Macao(project No.MYRG-GRG2023-00140-IAPME-UMDF and No.MYRG-GRG2024-00206-IAPME)Natural Science Foundation of Guangdong Province(Grant No.2023A1515010765)Science and Technology Program of Guangdong Province of China(Grant No.2023A0505030001)。
文摘Considering the growing pre-lithiation demand for high-performance Si-based anodes and consequent additional costs caused by the strict pre-lithiation environment,developing effective and environmentally stable pre-lithiation additives is a challenging research hotspot.Herein,interfacial engineered multifunctional Li_(13)Si_(4)@perfluoropolyether(PFPE)/LiF micro/nanoparticles are proposed as anode pre-lithiation additives,successfully constructed with the hybrid interface on the surface of Li_(13)Si_(4)through PFPE-induced nucleophilic substitution.The synthesized multifunctional Li_(13)Si_(4)@PFPE/LiF realizes the integration of active Li compensation,long-term chemical structural stability in air,and solid electrolyte interface(SEI)optimization.In particular,the Li_(13)Si_(4)@PFPE/LiF with a high pre-lithiation capacity(1102.4 mAh g^(-1))is employed in the pre-lithiation Si-based anode,which exhibits a superior initial Coulombic efficiency of 102.6%.Additionally,in situ X-ray diffraction/Raman,density functional theory calculation,and finite element analysis jointly illustrate that PFPE-predominant hybrid interface with modulated abundant highly electronegative F atoms distribution reduces the water adsorption energy and oxidation kinetics of Li_(13)Si_(4)@PFPE/LiF,which delivers a high pre-lithiation capacity retention of 84.39%after exposure to extremely moist air(60%relative humidity).Intriguingly,a LiF-rich mechanically stable bilayer SEI is constructed on anodes through a pre-lithiation-driven regulation for the behavior of electrolyte decomposition.Benefitting from pre-lithiation via multifunctional Li_(13)Si_(4)@PFPE/LiF,the full cell and pouch cell assembled with pre-lithiated anodes operate with long-time stability of 86.5%capacity retention over 200 cycles and superior energy density of 549.9 Wh kg^(-1),respectively.The universal multifunctional pre-lithiation additives provide enlightenment on promoting large-scale applications of pre-lithiation on commercial high-energy-density and long-cycle-life lithium-ion batteries.
基金supported by the National Natural Science Foundation of China(Nos.52272175,U2001215 and 12474226)the Guangzhou Science and Technology Programme(No.2025A04J2596)+2 种基金the Natural Science Foundation of Guangdong Province(Nos.2024A1515012688,2022A1515011487,2021A1515110403 and 2023A1515010652)the Young Top Talents Program(No.2021QN02C068)State Key Laboratory of Optoelectronic Materials and Technologies of Sun Yat-sen University.
文摘Pulsed-laser deposition has been developed to prepare large-area In_(2)S_(3)nanofilms and their photoelectric characteristics have been investigated.The In_(2)S_(3)nanofilm grown under 500℃is highly oriented along the(103)direction with exceptional crystallinity.The corresponding(103)-oriented In_(2)S_(3)photodetectors exhibit broadband photoresponse from 370.6 nm to 1064 nm.Under 635 nm illumination,the optimized responsivity,external quantum efficiency,and detectivity reach 19.8 A/W,3869%,and 2.59×10^(12)Jones,respectively.In addition,the device exhibits short rise/decay time of 3.9/3.0 ms.Of note,first-principles calculations have unveiled that the effective carrier mass along the(103)lattice plane is much smaller than those along the(100),(110)and(111)lattice planes,which thereby enables high-efficiency transport of photocarriers and thereby the excellent photosensitivity.Profited from the sizable bandgap,the In_(2)S_(3)photodetectors also showcase strong robustness against elevated operating temperature.In the end,proof-of-concept imaging application beyond human vision and under high operating temperature as well as heart rate monitoring have been achieved by using the In_(2)S_(3)device of the sensing component.This study introduces a novel crystal orientation engineering paradigm for the implementation of next-generation advanced optoelectronic systems.
基金financially supported by the Nanomaterial Technology Development Program(Nos.RS-202300234581)the Basic Science Research Program(Nos.2020-NR049321,RS-2019-NR040077)through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT,&Future Planning and the Ministry of Education
文摘Device fabrication is increasing with the importance of functional materials for industrial applications.To fulfil increasing demands,rare earth elementbased materials have become important.In particular,lanthanum(La) and La-based materials have garnered attention in recent years due to their versatile properties and wide range of potential applications.This critical review provides a comprehensive overview of the advancements in the utilization of La and its compounds across various fields.In the realm of sensing and biosensing,La-based materials exhibit better sensitivity and selectivity,indicating their suitability for detecting environmental pollutants and biomolecules.The review also explores their role in supercapacitors,where their unique electrochemical properties contribute to enhanced performance and stability.Furthermore,the catalytic properties of La compounds are highlighted in water-splitting applications,emphasizing their efficiency in oxygen and hydrogen production.The biomedical applications of Labased materials are also examined,focusing on their biocompatibility and potential in drug delivery and medical imaging.This review aims to provide a critical analysis of the current state of research,identify challenges,and suggest future directions for the development and application of La and La-based materials in these diverse fields.
基金financially supported by Natural Science Foundation of Shandong Province(Grant No.ZR2021ME019).
文摘Polyurea(PUA)is widely valued in protective coatings and structural reinforcement because of its impressive mechanical strength and resistance to corrosion.Its high flammability,together with the poor dispersion that often comes with simply blending in flame retardants,continues to limit its use in demanding environments.To overcome these issues,this study introduces a different approach.We grafted 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide(DOPO)onto the surface of a metal-organic framework(MOF)and then partially amino-functionalized the DOPO layer,ultimately creating an amino-modified DOPO-MOF hybrid.The introduced amino groups can directly react with the isocyanate(-NCO)groups in the PUA matrix,allowing the flame-retardant component to be integrated via reactive integration rather than physical blending.This approach helps avoid the interfacial defects and the mechanical weakening typically observed in conventional blending.With 5 wt% ZIF-67@DOPO-NH2 added to the PUA system,the composite successfully reached a UL-94 V-0 classification and showed a notable increase in limiting oxygen index(LOI),from19.2% to 23.8%.The peak heat release rate and total heat release dropped by 36.3% and 38.7%,respectively.Meanwhile,the tensile strength decreased from 25.74 to 22.52 MPa,while the elongation at break remained above 300%,indicating that the material maintained excellent toughness.
基金supported by the National Natural Science Foundation of Guangxi Province(2024GXNSFBA010033)the Special Fund for Science and Technology Development of Guangxi(Grant No.AD25069078).
文摘Ammonium-ion hybrid supercapacitors(A-HSCs)have emerged as promising candidates for next-generation energy storage owing to their inherent safety and environmental sustainability.Hexagonal tungsten oxide(h-WO_(3)),with its well-defined tunnel structure,holds great promise as a negative electrode material for NH^(4+)storage.However,its practical application is hindered by structural instability and poor intrinsic electrical conductivity.To address these challenges,a dual-regulation strategy is proposed,integrating molybdenum(Mo)doping and NH^(4+)pre-intercalation to concurrently optimize the tunnel structure and electronic environment of h-WO_(3)(Mo-NWO).Comprehensive experimental and theoretical analyses reveal that Mo doping narrows the bandgap of WO_(3)and reduces the diffusion energy barrier,thereby accelerating NH^(4+)adsorption and diffusion.Simultaneously,NH^(4+)pre-intercalation stabilizes the tunnel framework via hydrogen bonding,ensuring structural reversibility.As expected,the Mo-NWO/AC electrode achieves a high areal capacitance of 13.6 F cm^(−2)at 5 mA cm^(−2)and retains 80.14%of its capacitance after 5000 cycles,demonstrating exceptional rate capability and cycling stability.Moreover,the assembled Mn_(3)O_(4)//Mo-NWO/AC device delivers a high energy density of 3.41 mWh cm^(−2)and outstanding long-term stability(85.75%retention after 12,000 cycles).This work provides a viable strategy for designing high-performance NH^(4+)storage materials and advances the development of sustainable energy storage systems.
基金financially supported by the National Natural Science Foundation of China(No.22208129)2023 Jiangsu Province Large Scientific Instrument Open Sharing Autonomous Research Project(No.TC2023A033)。
文摘Photocatalysis is one of the most promising technologies for solving environmental and energy problems,but current photocatalysts still suffer from low visible light utilization and insufficient photogenerated charge separation efficiency.Therefore,in this work,D-A tubular materials with tubular carbon nitride(TCN)as electron donor(D)and 2-mercaptobenzothiazole(BZ)as electron acceptor(A)were constructed by molecular doping and modulation of the carbon nitride geometry.It was shown that the introduction of BZ could modulate the electronic structure of the catalyst,promote electron migration from TCN to BZ,and inhibit the recombination of photogenerated electrons and holes.Meanwhile,the ultra-thin tubular structure could expose more active sites.In addition,the adsorption of protons by BZ-TCN was further improved due to the modulation of the charge distribution between the components by the introduction of small molecules.Among them,the photocatalytic hydrogen production rate of BZ_(0.1)-TCN was twice that of TCN.The in-depth discussion of the components through theoretical calculations and characterization tests contributes to the understanding of the mechanism of photocatalytic hydrogen production.
基金financially supported by the National Natural Science Foundation of China (52272209)
文摘Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.
基金supported by research grants from Innovative Research Group Project of National Natural Science Foundation of China(52021004)the National Key Research and Development Program of China(2022YFB3803300)+1 种基金the National Natural Science Foundation of China(62474026,62205140,and 12204071)the China Postdoctoral Science Foundation(2022M710532).
文摘Thermocells are attracting growing interest as a promising thermoelectric technology for low-grade heat harvesting.However,the scarcity of high-performance redox couples featuring intrinsically high thermopower(Se)and fast redox kinetics hinders the rapid development of thermocells.Identifying potential intrinsically high-performance redox couples remains a significant challenge.This work introduces a novel n-type copper(I/II)chloride(CuCl/CuCl2)redox couple with intrinsically high performance.Through tailored electrolyte design,long-term stability was significantly improved by reducing proton concentration to suppress cuprous ion photo-oxidation,while ammonium chloride solvation enhanced cuprous ion solubility.The resulting system achieves a Se value closely aligned with theoretical predictions and exhibits rapid redox kinetics.Consequently,the optimized CuCl/CuCl_(2) intrinsic system demonstrated a high S_(e) of 1.52 mV K^(−1) and a record-high normalized power density Pmax(ΔT)^(−2) of 0.399 mW m^(−2) K^(−2),surpassing previously reported intrinsic n-type thermocells and rivaling the performance of p-type pristine 0.4 M ferri/ferrocyanide systems.A prototype module comprising 30 p-n units successfully powered a line of light-emitting diodes or a thermohygrometer.This work introduces a valuable redox couple for further advancing high-performance thermocells and demonstrates a viable strategy for developing novel redox systems.
基金supported by Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(2021R1A6A1A10044950).
文摘The thermal conductivity of nanofluids is an important property that influences the heat transfer capabilities of nanofluids.Researchers rely on experimental investigations to explore nanofluid properties,as it is a necessary step before their practical application.As these investigations are time and resource-consuming undertakings,an effective prediction model can significantly improve the efficiency of research operations.In this work,an Artificial Neural Network(ANN)model is developed to predict the thermal conductivity of metal oxide water-based nanofluid.For this,a comprehensive set of 691 data points was collected from the literature.This dataset is split into training(70%),validation(15%),and testing(15%)and used to train the ANN model.The developed model is a backpropagation artificial neural network with a 4–12–1 architecture.The performance of the developed model shows high accuracy with R values above 0.90 and rapid convergence.It shows that the developed ANN model accurately predicts the thermal conductivity of nanofluids.
