Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery...Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery damage or fracture is a critical concern.Water-based(aqueous)electrolytes have been receiving attention as an alternative to organic electrolytes.However,a narrow electrochemicalstability window,water decomposition,and the consequent low battery operating voltage and energy density hinder the practical use of aqueous electrolytes.Therefore,developing novel aqueous electrolytes for sustainable,safe,high-performance LIBs remains challenging.This Review first commences by summarizing the roles and requirements of electrolytes–separators and then delineates the progression of aqueous electrolytes for LIBs,encompassing aqueous liquid and gel electrolyte development trends along with detailed principles of the electrolytes.These aqueous electrolytes are progressed based on strategies using superconcentrated salts,concentrated diluents,polymer additives,polymer networks,and artificial passivation layers,which are used for suppressing water decomposition and widening the electrochemical stability window of water of the electrolytes.In addition,this Review discusses potential strategies for the implementation of aqueous Li-metal batteries with improved electrolyte–electrode interfaces.A comprehensive understanding of each strategy in the aqueous system will assist in the design of an aqueous electrolyte and the development of sustainable and safe high-performance batteries.展开更多
Silicon(Si)is a promising anode candidate for next-generation lithium-ion batteries(LIBs),but it suffers from poor electronic conductivity and dramatic volume variation during cycling,which poses a critical challenge ...Silicon(Si)is a promising anode candidate for next-generation lithium-ion batteries(LIBs),but it suffers from poor electronic conductivity and dramatic volume variation during cycling,which poses a critical challenge for stable battery operation.To mitigate these issues simultaneously,we propose a"double carbon synergistic encapsulation"strategy,namely thin carbon shell and nitrogen/phosphorus co-doped two-dimensional(2D)carbon sheet dual encapsulate Si nanoparticles(denoted as 2D NPC/C@Si).This double carbon structure can serve as a conductive medium and buffer matrix to accommodate the volume expansion of Si nanoparticles and enable fast electron/ion transport,which promotes the formation of a stable solid electrolyte interphase film during cycling.Through structural advantages,the resulting 2 D NPC/C@Si electrode demonstrates a high reversible capacity of592 mAh·g^(-1) at 0.2 A·g^(-1) with 90.5%excellent capacity retention after 100 cycles,outstanding rate capability(148 mAh·g^(-1) at 8 A·g^(-1)),and superior long-term cycling stability(326 mAh·g^(-1) at 1 A·g^(-1) for 500 cycles,86%capacity retention).Our findings elucidate the development of high-performance Si@C composite anodes for advanced LTBs.展开更多
By adding 1 wt% damage homogenizer（DH）, i.e. carbon black microparticles, into the electrodes of lithiumion batteries, thermal runaway can be mitigated as the battery cells are subjected to impact loadings. In a dro...By adding 1 wt% damage homogenizer（DH）, i.e. carbon black microparticles, into the electrodes of lithiumion batteries, thermal runaway can be mitigated as the battery cells are subjected to impact loadings. In a drop tower test, the generated heat of the modified cells is reduced by nearly 40%, compared with the reference cells. This phenomenon may be attributed to the weakening effect of the carbon black fillers.The shape of the filler grains does not have a pronounced influence on the temperature profile.展开更多
Nanophotocatalysts have shown great potential for degrading poly-and perfluorinated substances(PFAS).In light of the fact that most of these catalysts were studied in pure water,this study was designed to elucidate ef...Nanophotocatalysts have shown great potential for degrading poly-and perfluorinated substances(PFAS).In light of the fact that most of these catalysts were studied in pure water,this study was designed to elucidate effects from common environmental factors on decomposing and defluorinating perfluorooctanoic acid(PFOA)by In2O3 nanoparticles.Results from this work demonstrated that among the seven parameters,pH,sulfate,chloride,H2O2,In2O3 dose,NOM and O2,the first four had statistically significant negative effects on PFOA degradation.Since PFOA is a strong acid,the best condition leading to the highest PFOA removal was identified for two pH ranges.When pH was between 4 and 8,the optimal condition was:pH=4.2;sulfate=5.00 mg/L;chloride=20.43 mg/L;H2O2=0 mmol/L.Under this condition,PFOA decomposition and defluorination were 55.22 and 23.56%,respectively.When pH was between 2 and 6,the optimal condition was:pH=2;sulfate=5.00 mg/L;chloride=27.31 mg/L;H2O2=0 mmol/L.With this condition,the modeled PFOA decomposition was 97.59%with a defluorination of approximately 100%.These predicted results were all confirmed by experimental data.Thus,In2O3 nanoparticles can be used for degrading PFOA in aqueous solutions.This approach works best when the target contaminated water contains low concentrations of NOM,sulfate and chloride and at a low pH.展开更多
Constructing a reliable and favorable electrode-electrolyte interface is crucial to utilize the exceptional energy storage capability in commercial lithium-ion batteries.Here,we report a facile synthesis approach for ...Constructing a reliable and favorable electrode-electrolyte interface is crucial to utilize the exceptional energy storage capability in commercial lithium-ion batteries.Here,we report a facile synthesis approach for the lithium difluorophosphate(LiPO_(2)F_(2))solution as an effective film-forming additive via direct adding the Li_(2)CO_(3) into LiPF6 solution at 45℃.Benefiting from the significantly reduced interface resistance(RSEI)and charge transfer impedance(Rct)of both the cathode and anode by adding the prepared LiPO_(2)F_(2)solution into a baseline electrolyte,the cycling performance of the graphite||LiNi_(0.5)Mn_(0.3)Co_(0.2)O_(2) pouch cell is remarkably improved under all-climate condition.展开更多
1.Introduction Cemented carbides are composites of WC ceramic phases and metallic Co binders that endow them with superior hardness and excellent toughness.Hard metals are widely used as metal cutting and rock drillin...1.Introduction Cemented carbides are composites of WC ceramic phases and metallic Co binders that endow them with superior hardness and excellent toughness.Hard metals are widely used as metal cutting and rock drilling tools[1,2].Their hardness is believed to be inversely proportional to the sizes of WC grains^([3]).Grain growth inhibitors are widely employed to achieve smaller grain sizes.展开更多
High-throughput computational materials design provides one efficient solution to accelerate the discovery and development of functional materials. Its core concept is to build a large quantum materials repository and...High-throughput computational materials design provides one efficient solution to accelerate the discovery and development of functional materials. Its core concept is to build a large quantum materials repository and to search for target materials with desired properties via appropriate materials descriptors in a high-throughput fashion, which shares the same idea with the materials genome approach. This article reviews recent progress of discovering and developing new functional materials using high-throughput computational materials design approach. Emphasis is placed on the rational design of high-throughput screening procedure and the development of appropriate materials descriptors, concentrating on the electronic and magnetic properties of functional materials for various types of industrial applications in nanoelectronics.展开更多
Conversion-type reaction anode materials with high specific capacity are attractive candidates to improve lithium ion batteries(LIBs), yet the rapid capacity fading and poor rate capability caused by drastic volume ch...Conversion-type reaction anode materials with high specific capacity are attractive candidates to improve lithium ion batteries(LIBs), yet the rapid capacity fading and poor rate capability caused by drastic volume change and low electronic conductivity greatly hinder their practical applications. To circumvent these issues, the successful design of yolk@shell Fe2 O3@C hybrid composed of a columnar-like Fe2O3 core within a hollow cavity completely surrounded by a thin, self-supported carbon(C) shell is presented as an anode for high-performance LIBs. This yolk@shell structure allows each Fe2O3 core to swell upon lithiation without deforming the carbon shell. This preserves the structural and electrical integrity against pulverization, as revealed by in situ transmission electron microscopy(TEM) measurement. Benefiting from these structural advantages, the resulting electrode exhibits a high reversible capacity(1013 m Ah g-1 after80 cycles at 0.2 A g-1), outstanding rate capability(710 m Ah g-1 at 8 A g-1) and superior cycling stability(800 m Ah g-1 after 300 cycles at 4 A g-1). A Li-ion full cell using prelithiated yolk@shell Fe2 O3@C hybrid as the anode and commercial Li CoO2(LCO) as the cathode demonstrates impressive cycling stability with a capacity retention of 84.5% after 100 cycles at 1 C rate, holding great promise for future practical applications.展开更多
Li-rich layered oxide cathodes have received considerable attention because of the high operating potential and specific capacity. However, the structural instability and parasitic reactions at high potential cause se...Li-rich layered oxide cathodes have received considerable attention because of the high operating potential and specific capacity. However, the structural instability and parasitic reactions at high potential cause severe degradation of the electrochemical performance. In our studies, the cycling stability of Li_(1.14)Ni_(0.133)Co_(0.133)Mn_(0.544)O_(2) cathode is improved with LiPO_(2)F_(2) electrolyte additive. After 500 cycles, the capacity retention is increased from 53.6% to 85% at 3 C by LiPO_(2)F_(2) modification. This performance is mainly attributed to the enhanced interfacial stability of the Li-rich cathode. Based on systematic characterization, LiPO_(2)F_(2) additive was found to promote a stable interface film on the cathode surface during the cycling and mitigates the interfacial side reactions. This study provides new insights for improving high-potential Li-rich layered oxide batteries.展开更多
Staphylococcus aureus(S.aureus)is a leading human pathogen capable of producing severe invasive infections such as bacteremia,sepsis,and endocarditis with high morbidity and mortality,exacerbated by the increasingly w...Staphylococcus aureus(S.aureus)is a leading human pathogen capable of producing severe invasive infections such as bacteremia,sepsis,and endocarditis with high morbidity and mortality,exacerbated by the increasingly widespread antibiotic resistance exemplified by methicillin-resistant strains(MRSA).S.aureus pathogenesis is fueled by the secretion of toxins—such as the membrane-damaging pore-forming atoxin,which have diverse cellular targets including the epithelium,endothelium,leukocytes,and platelets.Here,we examine the use of human platelet membrane-coated nanoparticles(PNPs)as a biomimetic decoy strategy to neutralize S.aureus toxins and preserve host cell defense functions.The PNPs blocked platelet damage induced by S.aureus secreted toxins,thereby supporting platelet activation and bactericidal activity.Likewise,the PNPs blocked macrophage damage induced by S.aureus secreted toxins,thus supporting macrophage oxidative burst,nitric oxide production,and bactericidal activity,and diminishing MRSA-induced neutrophil extracellular trap release.In a mouse model of MRSA systemic infection,PNP administration reduced bacterial counts in the blood and protected against mortality.Taken together,the results from the present work provide a proof of principle of the therapeutic benefit of PNPs in toxin neutralization,cytoprotection,and increased host resistance to invasive S.aureus infection.展开更多
As promising anode candidates for potassium-ion batteries(PIBs),antimony sulfide(Sb_(2)S_(3))possesses high specific capacity but suffers from massive volume expansion and sluggish kinetics due to the large K^(+)inser...As promising anode candidates for potassium-ion batteries(PIBs),antimony sulfide(Sb_(2)S_(3))possesses high specific capacity but suffers from massive volume expansion and sluggish kinetics due to the large K^(+)insertion,resulting in inferior cycling and rate performance.To address these challenges,a yolk-shell structured Sb_(2)S_(3)confined in N,S co-doped hollow carbon nanorod(YS-Sb_(2)S_(3)@NSC)working as a viable anode for PIBs is proposed.As directly verified by in situ transmission electron microscopy(TEM),the buffer space between the Sb_(2)S_(3)core and thin carbon shell can effectively accommodate the large expansion stress of Sb_(2)S_(3)without cracking the shell and the carbon shell can accelerate electron transport and K^(+)diffusion,which plays a significant role in reinforcing the structural stability and facilitating charge transfer.As a result,the YS-Sb_(2)S_(3)@NSC electrode delivers a high reversible K^(+)storage capacity of 594.58 m A h g^(-1)at 0.1 A g^(-1)and a long cycle life with a slight capacity degradation(0.01%per cycle)for 2000 cycles at 1 A g^(-1)while maintaining outstanding rate capability.Importantly,utilizing in in situ/ex situ microscopic and spectroscopic characterizations,the origins of performance enhancement and K^(+)storage mechanism of Sb_(2)S_(3)were clearly elucidated.This work provides valuable insights into the rational design of high-performance and durable transition metal sulfides-based anodes for PIBs.展开更多
Multi-functional nanoshuttles for remotely targeted and on-demand delivery of therapeutic molecules and imaging to defined tissues and organs hold great potentials in personalized medicine, including precise early dia...Multi-functional nanoshuttles for remotely targeted and on-demand delivery of therapeutic molecules and imaging to defined tissues and organs hold great potentials in personalized medicine, including precise early diagnosis, efficient prevention and therapy without toxicity. Yet, in spite of 25 years of research, there are still no such shuttles available. To this end, we have designed magnetic and gold nanoparticles （NP）-embedded silica nanoshuttles （MGNSs） with nanopores on their surface. Fluorescently labeled Doxombicin （DOX）, a cancer drug, was loaded in the MGNSs as a payload. DOX loaded MGNSs were encapsulated in heat and pH sensitive polymer P（NIPAM-co- MAA） to enable controlled release of the payload. Magnetically-guided transport of MGNSs was examined in： （a） a glass capillary tube to simulate their delivery via blood vessels; and （b） porous hydrogels to simulate their transport in composite human tissues, including bone, cartilage, tendon, muscles and blood-brain barrier {BBB）. The viscoelastic properties of hydrogels were examined by atomic force microscopy （AFM）. Cellular uptake of DOX- loaded MGNSs and the subsequent pH and temperature-mediated release were demonstrated in differentiated human neurons derived from induced pluripotent stem cells （iPSCs） as well as epithelial HeLa cells. The presence of embedded iron and gold NPs in silica shells and polymer-coating are supported by SEM and TEM. Fluorescence spectroscopy and microscopy documented DOX loading in the MGNSs. Time-dependent transport of MGNSs guided by an external magnetic field was observed in both glass capillary tubes and in the porous hydrogel. AFM results affirmed that the stiffness of the hydrogels model the rigidity range from soft tissues to bone. pH and temperature-dependent drug release analysis showed stimuli responsive and gradual drug release. Cells＇ viability MTT assays showed that MGNSs are non-toxic. The cell death from on-demand DOX release was observed in both neurons and epithelial cells even though the drug release efficiency was higher in neurons. Therefore, development of smart nanoshuttles have significant translational potential for controlled delivery of theranostics＇ payloads and precisely guided transport in specified tissues and organs （for example, bone, cartilage, tendon, bone marrow, heart, lung, liver, kidney, and brain） for highly efficient personalized medicine applications.展开更多
The interest in using therapeutic nanoparticles to bind with harmful molecules or pathogens and subsequently neutralize their bioactivity has grown tremendously.Among various nanomedicine platforms,cell membrane-coate...The interest in using therapeutic nanoparticles to bind with harmful molecules or pathogens and subsequently neutralize their bioactivity has grown tremendously.Among various nanomedicine platforms,cell membrane-coated nanoparticles,namely,“cellular nanosponges,”stand out for their broadspectrum neutralization capability challenging to achieve in traditional countermeasure technologies.Such ability is attributable to their cellular function-based rather than target structure-based working principle.Integrating cellular nanosponges with various synthetic substrates further makes their applications exceptionally versatile and adaptive.This review discusses the latest cellular nanosponge technology focusing on how the structure–function relationship in different designs has led to versatile and potent medical countermeasures.Four design strategies are discussed,including harnessing native cell membrane functions for biological neutralization,functionalizing cell membrane coatings to enhance neutralization capabilities,combining cell membranes and functional cores for multimodal neutralization,and integrating cellular nanosponges with hydrogels for localized applications.Examples in each design strategy are selected,and the discussion is to highlight their structure–function relationships in complex disease settings.The review may inspire additional design strategies for cellular nanosponges and fulfill even broader medical applications.展开更多
Autonomously self-propelled nanoswimmers represent the nextgeneration nano-devices for bio-and environmental technology.However,current nanoswimmers generate limited energy output and can only move in short distances ...Autonomously self-propelled nanoswimmers represent the nextgeneration nano-devices for bio-and environmental technology.However,current nanoswimmers generate limited energy output and can only move in short distances and duration,thus are struggling to be applied in practical challenges,such as living cell transportation.Here,we describe the construction of biodegradable metal-organic framework based nanobots with chemically driven buoyancy to achieve highly efficient,long-distance,directional vertical motion to“find-and-fetch”target cells.Nanobots surface-functionalized with antibodies against the cell surface marker carcinoembryonic antigen are exploited to impart the nanobots with specific cell targeting capacity to recognize and separate cancer cells.We demonstrate that the self-propelled motility of the nanobots can sufficiently transport the recognized cells autonomously,and the separated cells can be easily collected with a customized glass column,and finally regain their full metabolic potential after the separation.The utilization of nanobots with easy synthetic pathway shows considerable promise in cell recognition,separation,and enrichment.展开更多
Machine learning interatomic potentials(MLIPs)enable accurate simulations of materials at scales beyond that accessible by ab initio methods and play an increasingly important role in the study and design of materials...Machine learning interatomic potentials(MLIPs)enable accurate simulations of materials at scales beyond that accessible by ab initio methods and play an increasingly important role in the study and design of materials.However,MLIPs are only as accurate and robust as the data on which they are trained.Here,we present DImensionality-Reduced Encoded Clusters with sTratified(DIRECT)sampling as an approach to select a robust training set of structures from a large and complex configuration space.By applying DIRECT sampling on the Materials Project relaxation trajectories dataset with over one million structures and 89 elements,we develop an improved materials 3-body graph network(M3GNet)universal potential that extrapolates more reliably to unseen structures.We further show that molecular dynamics(MD)simulations with the M3GNet universal potential can be used instead of expensive ab initioMDto rapidly create a large configuration space for target systems.We combined this scheme with DIRECT sampling to develop a reliable moment tensor potential for titanium hydrides without the need for iterative augmentation of training structures.This work paves the way for robust high-throughput development of MLIPs across any compositional complexity.展开更多
Polygalacturonase inhibiting proteins(PGIPs)are plant proteins involved in the inhibition of polygalacturonases(PGs),cell-wall degrading enzymes often secreted by phytopathogenic fungi.Previously,we confirmed that PGI...Polygalacturonase inhibiting proteins(PGIPs)are plant proteins involved in the inhibition of polygalacturonases(PGs),cell-wall degrading enzymes often secreted by phytopathogenic fungi.Previously,we confirmed that PGIP2 from Phaseolus vulgaris(PvPGIP2)can inhibit the growth of Aspergillus niger and Botrytis cinerea on agar plate.In this study,we further validated the feasibility of using PGIP as an environmental and ecological friendly agent to prevent fungal infection post-harvest.We found that application of either purified PGIP(full length PvPGIP2 or truncated tPvPGIP2_5-8),or PGIP-secreting Saccharomyces cerevisiae strains can effectively inhibit fungal growth and necrotic lesions on tobacco leaf.We also examined the effective amount and thermostability of PGIP when applied on plants.A concentration of 0.75 mg/mL or higher can significantly reduce the area of B.cinerea lesions.The activity of full-length PvPGIPs is not affected after incubation at various temperatures ranging from20 to 42◦C for 24 h,while truncated tPvPGIP2_5-8 lost some efficacy after incubation at 42◦C.Furthermore,we have also examined the efficacy of PGIP on tomato fruit.When the purified PvPGIP2 proteins were applied to tomato fruit inoculated with B.cinerea at a concentration of roughly 1.0 mg/mL,disease inci-dence and area of disease had reduced by more than half compared to the controls without PGIP treatment.This study explores the potential of PGIPs as exogenously applied,eco-friendly fungal control agents on fruit and vegetables post-harvest.展开更多
Photothermal CO_(2) hydrogenation is a promising route to produce methanol as a sustainable liquid solar fuel.However,most existing catalysts require a combination of solar irradiation and additional heat input to ach...Photothermal CO_(2) hydrogenation is a promising route to produce methanol as a sustainable liquid solar fuel.However,most existing catalysts require a combination of solar irradiation and additional heat input to achieve a satisfactory reaction rate.For the few that can be driven solely by light,their reaction rates are one order of magnitude lower.We develop a photothermal catalyst with multilevel interfaces that achieves improvedmethanol production from photothermal CO_(2) hydrogenation without external heat.The catalyst features a layered structure comprising Cu/ZnO/Al_(2)O_(3)(CZA)covered by oxidized carbon black(oCB),where the oCB/CZA interface promotes efficient heat generation and transfer,and the Cu/oxide interface contributes to high catalytic activity.Under a mild pressure of 8 bar,our oCB/CZA catalyst shows a methanol selectivity of 64.7%with a superior production rate of 4.91 mmol-geza-1-h-1,at least one order of magnitude higher than other photothermal catalysts solely driven by light.This work demonstrates a photothermal catalyst design strategy for liquid solar fuel production.展开更多
A new class of high-entropy M3B4 borides of the Ta_(3)B_(4)-prototyped orthorhombic structure has been synthesized in the bulk form for the first time.Specimens with compositions of(V0.2Cr0.2Nb0.2Mo0.2Ta0.2)3B4 and(V0...A new class of high-entropy M3B4 borides of the Ta_(3)B_(4)-prototyped orthorhombic structure has been synthesized in the bulk form for the first time.Specimens with compositions of(V0.2Cr0.2Nb0.2Mo0.2Ta0.2)3B4 and(V0.2Cr0.2Nb0.2Ta0.2W0.2)_(3)B_(4) were fabricated via reactive spark plasma sintering of high-energy-ball-milled elemental boron and metal precursors.The sintered specimens were〜98.7%in relative densities with virtually no oxide contamination,albeit the presence of minor(4-5 vol%)secondary high-entropy M5B6 phases.Despite that Mo_(3)B_(4) or W_(3)B_(4) are not stable phase,20%of M03B4 and W3B4 can be stabilized into the high-entropy M3B4 borides.Vickers hardness was measured to be 18.6 and 19.8 GPa at a standard load of 9.8 N.This work has further expanded the family of different structures of high-entropy ceramics reported to date.展开更多
Although high-entropy materials are attracting considerable interest due to a combination of useful properties and promising applications,predicting their formation remains a hindrance for rational discovery of new sy...Although high-entropy materials are attracting considerable interest due to a combination of useful properties and promising applications,predicting their formation remains a hindrance for rational discovery of new systems.Experimental approaches are based on physical intuition and/or expensive trial and error strategies.Most computational methods rely on the availability of sufficient experimental data and computational power.Machine learning(ML)applied to materials science can accelerate development and reduce costs.In this study,we propose an ML method,leveraging thermodynamic and compositional attributes of a given material for predicting the synthesizability(i.e.,entropy-forming ability)of disordered metal carbides.展开更多
Deviation between thermodynamic and experimental voltages is one of the key issues in Li-ion conversion-type electrode materials; the factor that affects this phenomenon has not been understood well in spite of its im...Deviation between thermodynamic and experimental voltages is one of the key issues in Li-ion conversion-type electrode materials; the factor that affects this phenomenon has not been understood well in spite of its importance. In this work, we combine first principles calculations and electrochemical experiments with characterization tools to probe the conversion reaction voltage of transition metal difluorides MF2（M = Fe, Ni, and Cu）. We find that the conversion reaction voltage is heavily dependent on the size of the metal nanoparticles generated. The surface energy of metal nanoparticles appears to penalize the reaction energy, which results in a lower voltage compared to the thermodynamic voltage of a bulk-phase reaction. Furthermore, we develop a reversible CuF2 electrode coated with NiO. Electron energy loss spectroscopy （EELS） elemental maps demonstrate that the lithiation process mostly occurs in the area of high NiO content. This suggests that NiO can be considered a suitable artificial solid electrolyte interphase that prevents direct contact between Cu nanoparticles and the electrolyte. Thus, it alleviates Cu dissolution into the electrolyte and improves the reversibility of CuF2.展开更多
基金the National Research Foundation(NRF)of Korea(No.2022R1A2B5B02002097),funded by the Korea government(MSIT).
文摘Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery damage or fracture is a critical concern.Water-based(aqueous)electrolytes have been receiving attention as an alternative to organic electrolytes.However,a narrow electrochemicalstability window,water decomposition,and the consequent low battery operating voltage and energy density hinder the practical use of aqueous electrolytes.Therefore,developing novel aqueous electrolytes for sustainable,safe,high-performance LIBs remains challenging.This Review first commences by summarizing the roles and requirements of electrolytes–separators and then delineates the progression of aqueous electrolytes for LIBs,encompassing aqueous liquid and gel electrolyte development trends along with detailed principles of the electrolytes.These aqueous electrolytes are progressed based on strategies using superconcentrated salts,concentrated diluents,polymer additives,polymer networks,and artificial passivation layers,which are used for suppressing water decomposition and widening the electrochemical stability window of water of the electrolytes.In addition,this Review discusses potential strategies for the implementation of aqueous Li-metal batteries with improved electrolyte–electrode interfaces.A comprehensive understanding of each strategy in the aqueous system will assist in the design of an aqueous electrolyte and the development of sustainable and safe high-performance batteries.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.52072323,21805278 and 51872098)the Leading Project Foundation of Science Department of Fujian Province(No.2018H0034)+2 种基金the“Double-First Class”Foundation of Materials and Intelligent Manufacturing Discipline of Xiamen Universitythe Opening Project of National Joint Engineering Research Center for Abrasion Control and Molding of Metal MaterialsHenan Key Laboratory of High-temperature Structural and Functional Materials,Henan University of Science and Technology(No.HKDNM2019013)。
文摘Silicon(Si)is a promising anode candidate for next-generation lithium-ion batteries(LIBs),but it suffers from poor electronic conductivity and dramatic volume variation during cycling,which poses a critical challenge for stable battery operation.To mitigate these issues simultaneously,we propose a"double carbon synergistic encapsulation"strategy,namely thin carbon shell and nitrogen/phosphorus co-doped two-dimensional(2D)carbon sheet dual encapsulate Si nanoparticles(denoted as 2D NPC/C@Si).This double carbon structure can serve as a conductive medium and buffer matrix to accommodate the volume expansion of Si nanoparticles and enable fast electron/ion transport,which promotes the formation of a stable solid electrolyte interphase film during cycling.Through structural advantages,the resulting 2 D NPC/C@Si electrode demonstrates a high reversible capacity of592 mAh·g^(-1) at 0.2 A·g^(-1) with 90.5%excellent capacity retention after 100 cycles,outstanding rate capability(148 mAh·g^(-1) at 8 A·g^(-1)),and superior long-term cycling stability(326 mAh·g^(-1) at 1 A·g^(-1) for 500 cycles,86%capacity retention).Our findings elucidate the development of high-performance Si@C composite anodes for advanced LTBs.
基金supported by the Advanced Research Projects Agency-Energy(ARPA-E)(No.DE-AR0000396)
文摘By adding 1 wt% damage homogenizer（DH）, i.e. carbon black microparticles, into the electrodes of lithiumion batteries, thermal runaway can be mitigated as the battery cells are subjected to impact loadings. In a drop tower test, the generated heat of the modified cells is reduced by nearly 40%, compared with the reference cells. This phenomenon may be attributed to the weakening effect of the carbon black fillers.The shape of the filler grains does not have a pronounced influence on the temperature profile.
基金funding provided by University at Albany,State University of New York。
文摘Nanophotocatalysts have shown great potential for degrading poly-and perfluorinated substances(PFAS).In light of the fact that most of these catalysts were studied in pure water,this study was designed to elucidate effects from common environmental factors on decomposing and defluorinating perfluorooctanoic acid(PFOA)by In2O3 nanoparticles.Results from this work demonstrated that among the seven parameters,pH,sulfate,chloride,H2O2,In2O3 dose,NOM and O2,the first four had statistically significant negative effects on PFOA degradation.Since PFOA is a strong acid,the best condition leading to the highest PFOA removal was identified for two pH ranges.When pH was between 4 and 8,the optimal condition was:pH=4.2;sulfate=5.00 mg/L;chloride=20.43 mg/L;H2O2=0 mmol/L.Under this condition,PFOA decomposition and defluorination were 55.22 and 23.56%,respectively.When pH was between 2 and 6,the optimal condition was:pH=2;sulfate=5.00 mg/L;chloride=27.31 mg/L;H2O2=0 mmol/L.With this condition,the modeled PFOA decomposition was 97.59%with a defluorination of approximately 100%.These predicted results were all confirmed by experimental data.Thus,In2O3 nanoparticles can be used for degrading PFOA in aqueous solutions.This approach works best when the target contaminated water contains low concentrations of NOM,sulfate and chloride and at a low pH.
基金National Natural Science Foundation of China(Nos.21935009,21761132030 and 21621091)National Key Research and Development Program of China(No.2018YFB0905400)the Doctoral Research Foundation of Binzhou University(No.2016Y06)。
文摘Constructing a reliable and favorable electrode-electrolyte interface is crucial to utilize the exceptional energy storage capability in commercial lithium-ion batteries.Here,we report a facile synthesis approach for the lithium difluorophosphate(LiPO_(2)F_(2))solution as an effective film-forming additive via direct adding the Li_(2)CO_(3) into LiPF6 solution at 45℃.Benefiting from the significantly reduced interface resistance(RSEI)and charge transfer impedance(Rct)of both the cathode and anode by adding the prepared LiPO_(2)F_(2)solution into a baseline electrolyte,the cycling performance of the graphite||LiNi_(0.5)Mn_(0.3)Co_(0.2)O_(2) pouch cell is remarkably improved under all-climate condition.
基金the support from the National Natural Science Foundation of China(Nos.51871058 and 51701170)Financial support from the Project of Science and Technology Plan of Fujian Province(No.2018J01520)the Talented Youth Scientist Support Program of the Eyas Program of Fujian Province。
文摘1.Introduction Cemented carbides are composites of WC ceramic phases and metallic Co binders that endow them with superior hardness and excellent toughness.Hard metals are widely used as metal cutting and rock drilling tools[1,2].Their hardness is believed to be inversely proportional to the sizes of WC grains^([3]).Grain growth inhibitors are widely employed to achieve smaller grain sizes.
基金support by National Science Foundation under award number ACI-1550404American Chemical Society Petroleum Research Fund under the award number 55481-DNI6+1 种基金Global Research Outreach(GRO)Program of Samsung Advanced Institute of Technology under the award number 20164974the Vannevar Bush Faculty Fellowship program sponsored by the Basic Research Office of the Assistant Secretary of Defense for Research and Engineering under the Office of Naval Research grant N00014-16-1-2569
文摘High-throughput computational materials design provides one efficient solution to accelerate the discovery and development of functional materials. Its core concept is to build a large quantum materials repository and to search for target materials with desired properties via appropriate materials descriptors in a high-throughput fashion, which shares the same idea with the materials genome approach. This article reviews recent progress of discovering and developing new functional materials using high-throughput computational materials design approach. Emphasis is placed on the rational design of high-throughput screening procedure and the development of appropriate materials descriptors, concentrating on the electronic and magnetic properties of functional materials for various types of industrial applications in nanoelectronics.
基金supported by the National Natural Science Foundation of China(Grants No.21703185)the leading Project Foundation of Science Department of Fujian Province(Grants No.2018H0034)+1 种基金Fundamental Research Funds for the Central Universities(Xiamen University:20720170042)the“Double-First Class”Foundation of Materials and Intelligent Manufacturing Discipline of Xiamen University。
文摘Conversion-type reaction anode materials with high specific capacity are attractive candidates to improve lithium ion batteries(LIBs), yet the rapid capacity fading and poor rate capability caused by drastic volume change and low electronic conductivity greatly hinder their practical applications. To circumvent these issues, the successful design of yolk@shell Fe2 O3@C hybrid composed of a columnar-like Fe2O3 core within a hollow cavity completely surrounded by a thin, self-supported carbon(C) shell is presented as an anode for high-performance LIBs. This yolk@shell structure allows each Fe2O3 core to swell upon lithiation without deforming the carbon shell. This preserves the structural and electrical integrity against pulverization, as revealed by in situ transmission electron microscopy(TEM) measurement. Benefiting from these structural advantages, the resulting electrode exhibits a high reversible capacity(1013 m Ah g-1 after80 cycles at 0.2 A g-1), outstanding rate capability(710 m Ah g-1 at 8 A g-1) and superior cycling stability(800 m Ah g-1 after 300 cycles at 4 A g-1). A Li-ion full cell using prelithiated yolk@shell Fe2 O3@C hybrid as the anode and commercial Li CoO2(LCO) as the cathode demonstrates impressive cycling stability with a capacity retention of 84.5% after 100 cycles at 1 C rate, holding great promise for future practical applications.
基金supported partially by the Natural Science Foundation of Beijing Municipality (L172036)the Joint Funds of the Equipment Pre-Research and Ministry of Education (6141A020225)+2 种基金the National Natural Science Foundation of China (Grants Nos. 52072323 and 51872098)the Science and Technology Beijing 100 Leading Talent Training Projectthe NCEPU ‘‘Double First-Class” Program. We thank Dr. Rui Liu for suggestions on the crystal structure analysis。
文摘Li-rich layered oxide cathodes have received considerable attention because of the high operating potential and specific capacity. However, the structural instability and parasitic reactions at high potential cause severe degradation of the electrochemical performance. In our studies, the cycling stability of Li_(1.14)Ni_(0.133)Co_(0.133)Mn_(0.544)O_(2) cathode is improved with LiPO_(2)F_(2) electrolyte additive. After 500 cycles, the capacity retention is increased from 53.6% to 85% at 3 C by LiPO_(2)F_(2) modification. This performance is mainly attributed to the enhanced interfacial stability of the Li-rich cathode. Based on systematic characterization, LiPO_(2)F_(2) additive was found to promote a stable interface film on the cathode surface during the cycling and mitigates the interfacial side reactions. This study provides new insights for improving high-potential Li-rich layered oxide batteries.
基金This work was supported by National Institutes of Health grants HL125352 and U01AI124316(VN).
文摘Staphylococcus aureus(S.aureus)is a leading human pathogen capable of producing severe invasive infections such as bacteremia,sepsis,and endocarditis with high morbidity and mortality,exacerbated by the increasingly widespread antibiotic resistance exemplified by methicillin-resistant strains(MRSA).S.aureus pathogenesis is fueled by the secretion of toxins—such as the membrane-damaging pore-forming atoxin,which have diverse cellular targets including the epithelium,endothelium,leukocytes,and platelets.Here,we examine the use of human platelet membrane-coated nanoparticles(PNPs)as a biomimetic decoy strategy to neutralize S.aureus toxins and preserve host cell defense functions.The PNPs blocked platelet damage induced by S.aureus secreted toxins,thereby supporting platelet activation and bactericidal activity.Likewise,the PNPs blocked macrophage damage induced by S.aureus secreted toxins,thus supporting macrophage oxidative burst,nitric oxide production,and bactericidal activity,and diminishing MRSA-induced neutrophil extracellular trap release.In a mouse model of MRSA systemic infection,PNP administration reduced bacterial counts in the blood and protected against mortality.Taken together,the results from the present work provide a proof of principle of the therapeutic benefit of PNPs in toxin neutralization,cytoprotection,and increased host resistance to invasive S.aureus infection.
基金supported by the National Natural Science Foundation of China(Grants Nos.52072323 and 52122211)the"Double-First Class"Foundation of Materials and Intelligent Manufacturing Discipline of Xiamen Universitythe State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources(Grant No.LAPS22005)。
文摘As promising anode candidates for potassium-ion batteries(PIBs),antimony sulfide(Sb_(2)S_(3))possesses high specific capacity but suffers from massive volume expansion and sluggish kinetics due to the large K^(+)insertion,resulting in inferior cycling and rate performance.To address these challenges,a yolk-shell structured Sb_(2)S_(3)confined in N,S co-doped hollow carbon nanorod(YS-Sb_(2)S_(3)@NSC)working as a viable anode for PIBs is proposed.As directly verified by in situ transmission electron microscopy(TEM),the buffer space between the Sb_(2)S_(3)core and thin carbon shell can effectively accommodate the large expansion stress of Sb_(2)S_(3)without cracking the shell and the carbon shell can accelerate electron transport and K^(+)diffusion,which plays a significant role in reinforcing the structural stability and facilitating charge transfer.As a result,the YS-Sb_(2)S_(3)@NSC electrode delivers a high reversible K^(+)storage capacity of 594.58 m A h g^(-1)at 0.1 A g^(-1)and a long cycle life with a slight capacity degradation(0.01%per cycle)for 2000 cycles at 1 A g^(-1)while maintaining outstanding rate capability.Importantly,utilizing in in situ/ex situ microscopic and spectroscopic characterizations,the origins of performance enhancement and K^(+)storage mechanism of Sb_(2)S_(3)were clearly elucidated.This work provides valuable insights into the rational design of high-performance and durable transition metal sulfides-based anodes for PIBs.
基金supported in part by the National Institute on Aging of National Institutes of Health(Grant AG028709)the FUMEC and AMC for funds to support the 2016 summer research yield at the University of California in San Diego
文摘Multi-functional nanoshuttles for remotely targeted and on-demand delivery of therapeutic molecules and imaging to defined tissues and organs hold great potentials in personalized medicine, including precise early diagnosis, efficient prevention and therapy without toxicity. Yet, in spite of 25 years of research, there are still no such shuttles available. To this end, we have designed magnetic and gold nanoparticles （NP）-embedded silica nanoshuttles （MGNSs） with nanopores on their surface. Fluorescently labeled Doxombicin （DOX）, a cancer drug, was loaded in the MGNSs as a payload. DOX loaded MGNSs were encapsulated in heat and pH sensitive polymer P（NIPAM-co- MAA） to enable controlled release of the payload. Magnetically-guided transport of MGNSs was examined in： （a） a glass capillary tube to simulate their delivery via blood vessels; and （b） porous hydrogels to simulate their transport in composite human tissues, including bone, cartilage, tendon, muscles and blood-brain barrier {BBB）. The viscoelastic properties of hydrogels were examined by atomic force microscopy （AFM）. Cellular uptake of DOX- loaded MGNSs and the subsequent pH and temperature-mediated release were demonstrated in differentiated human neurons derived from induced pluripotent stem cells （iPSCs） as well as epithelial HeLa cells. The presence of embedded iron and gold NPs in silica shells and polymer-coating are supported by SEM and TEM. Fluorescence spectroscopy and microscopy documented DOX loading in the MGNSs. Time-dependent transport of MGNSs guided by an external magnetic field was observed in both glass capillary tubes and in the porous hydrogel. AFM results affirmed that the stiffness of the hydrogels model the rigidity range from soft tissues to bone. pH and temperature-dependent drug release analysis showed stimuli responsive and gradual drug release. Cells＇ viability MTT assays showed that MGNSs are non-toxic. The cell death from on-demand DOX release was observed in both neurons and epithelial cells even though the drug release efficiency was higher in neurons. Therefore, development of smart nanoshuttles have significant translational potential for controlled delivery of theranostics＇ payloads and precisely guided transport in specified tissues and organs （for example, bone, cartilage, tendon, bone marrow, heart, lung, liver, kidney, and brain） for highly efficient personalized medicine applications.
基金This work is supported by the Defense Threat Reduction Agency Joint Science and Technology Office for Chemical and Biological Defense under Award Numbers HDTRA1-21-1-0010 and HDTRA1-21-C-0019.
文摘The interest in using therapeutic nanoparticles to bind with harmful molecules or pathogens and subsequently neutralize their bioactivity has grown tremendously.Among various nanomedicine platforms,cell membrane-coated nanoparticles,namely,“cellular nanosponges,”stand out for their broadspectrum neutralization capability challenging to achieve in traditional countermeasure technologies.Such ability is attributable to their cellular function-based rather than target structure-based working principle.Integrating cellular nanosponges with various synthetic substrates further makes their applications exceptionally versatile and adaptive.This review discusses the latest cellular nanosponge technology focusing on how the structure–function relationship in different designs has led to versatile and potent medical countermeasures.Four design strategies are discussed,including harnessing native cell membrane functions for biological neutralization,functionalizing cell membrane coatings to enhance neutralization capabilities,combining cell membranes and functional cores for multimodal neutralization,and integrating cellular nanosponges with hydrogels for localized applications.Examples in each design strategy are selected,and the discussion is to highlight their structure–function relationships in complex disease settings.The review may inspire additional design strategies for cellular nanosponges and fulfill even broader medical applications.
基金supported by the Australian Research Council (ARC, DP210100422)the National Breast Cancer Foundation, Australia (IIRS-22-104)the financial support by the Australian Government Research Training Program Scholarship
文摘Autonomously self-propelled nanoswimmers represent the nextgeneration nano-devices for bio-and environmental technology.However,current nanoswimmers generate limited energy output and can only move in short distances and duration,thus are struggling to be applied in practical challenges,such as living cell transportation.Here,we describe the construction of biodegradable metal-organic framework based nanobots with chemically driven buoyancy to achieve highly efficient,long-distance,directional vertical motion to“find-and-fetch”target cells.Nanobots surface-functionalized with antibodies against the cell surface marker carcinoembryonic antigen are exploited to impart the nanobots with specific cell targeting capacity to recognize and separate cancer cells.We demonstrate that the self-propelled motility of the nanobots can sufficiently transport the recognized cells autonomously,and the separated cells can be easily collected with a customized glass column,and finally regain their full metabolic potential after the separation.The utilization of nanobots with easy synthetic pathway shows considerable promise in cell recognition,separation,and enrichment.
基金The authors acknowledge support from Shell International Exploration and Production Inc.(Contract No.CW649697)The authors also acknowledge data and software infrastructure supported by the Materials Project,funded by the US Department of Energy,Office of Science,Office of Basic Energy Sciences,Materials Sciences and Engineering Division.Part of this work was carried out under the auspices of the US Department of Energy by Lawrence Livermore National Laboratory(LLNL)under contract Nos.DE-AC52-07NA27344+1 种基金B.C.W.and T.A.P.acknowledge support from LLNL Laboratory Directed Research and Development(LDRD)Program Grant Nos.20-SI-004 and 22-ERD-014Computational work was performed using the Expanse at the San Diego Supercomputer Center(SDSC)from the Advanced Cyberinfrastructure Coordination Ecosystem:Services and Support(ACCESS)program supported by National Science Foundation grants Nos.2138259,2138286,2138307,2137603,and 2138296,in addition to the Triton Super Computer Center(TSCC)at the University of California,San Diego and the National Energy Research Scientific Computing Center(NERSC).
文摘Machine learning interatomic potentials(MLIPs)enable accurate simulations of materials at scales beyond that accessible by ab initio methods and play an increasingly important role in the study and design of materials.However,MLIPs are only as accurate and robust as the data on which they are trained.Here,we present DImensionality-Reduced Encoded Clusters with sTratified(DIRECT)sampling as an approach to select a robust training set of structures from a large and complex configuration space.By applying DIRECT sampling on the Materials Project relaxation trajectories dataset with over one million structures and 89 elements,we develop an improved materials 3-body graph network(M3GNet)universal potential that extrapolates more reliably to unseen structures.We further show that molecular dynamics(MD)simulations with the M3GNet universal potential can be used instead of expensive ab initioMDto rapidly create a large configuration space for target systems.We combined this scheme with DIRECT sampling to develop a reliable moment tensor potential for titanium hydrides without the need for iterative augmentation of training structures.This work paves the way for robust high-throughput development of MLIPs across any compositional complexity.
文摘Polygalacturonase inhibiting proteins(PGIPs)are plant proteins involved in the inhibition of polygalacturonases(PGs),cell-wall degrading enzymes often secreted by phytopathogenic fungi.Previously,we confirmed that PGIP2 from Phaseolus vulgaris(PvPGIP2)can inhibit the growth of Aspergillus niger and Botrytis cinerea on agar plate.In this study,we further validated the feasibility of using PGIP as an environmental and ecological friendly agent to prevent fungal infection post-harvest.We found that application of either purified PGIP(full length PvPGIP2 or truncated tPvPGIP2_5-8),or PGIP-secreting Saccharomyces cerevisiae strains can effectively inhibit fungal growth and necrotic lesions on tobacco leaf.We also examined the effective amount and thermostability of PGIP when applied on plants.A concentration of 0.75 mg/mL or higher can significantly reduce the area of B.cinerea lesions.The activity of full-length PvPGIPs is not affected after incubation at various temperatures ranging from20 to 42◦C for 24 h,while truncated tPvPGIP2_5-8 lost some efficacy after incubation at 42◦C.Furthermore,we have also examined the efficacy of PGIP on tomato fruit.When the purified PvPGIP2 proteins were applied to tomato fruit inoculated with B.cinerea at a concentration of roughly 1.0 mg/mL,disease inci-dence and area of disease had reduced by more than half compared to the controls without PGIP treatment.This study explores the potential of PGIPs as exogenously applied,eco-friendly fungal control agents on fruit and vegetables post-harvest.
文摘Photothermal CO_(2) hydrogenation is a promising route to produce methanol as a sustainable liquid solar fuel.However,most existing catalysts require a combination of solar irradiation and additional heat input to achieve a satisfactory reaction rate.For the few that can be driven solely by light,their reaction rates are one order of magnitude lower.We develop a photothermal catalyst with multilevel interfaces that achieves improvedmethanol production from photothermal CO_(2) hydrogenation without external heat.The catalyst features a layered structure comprising Cu/ZnO/Al_(2)O_(3)(CZA)covered by oxidized carbon black(oCB),where the oCB/CZA interface promotes efficient heat generation and transfer,and the Cu/oxide interface contributes to high catalytic activity.Under a mild pressure of 8 bar,our oCB/CZA catalyst shows a methanol selectivity of 64.7%with a superior production rate of 4.91 mmol-geza-1-h-1,at least one order of magnitude higher than other photothermal catalysts solely driven by light.This work demonstrates a photothermal catalyst design strategy for liquid solar fuel production.
基金an office of Naval Research MURI Program(Grant No.N00014-15-1-2863)Qizhang YAN and Jian LUO also acknowledge partial support from the Air Force Office of Scientific Research(Grant No.FA9550-19-1-01327)for the microscopy work.
文摘A new class of high-entropy M3B4 borides of the Ta_(3)B_(4)-prototyped orthorhombic structure has been synthesized in the bulk form for the first time.Specimens with compositions of(V0.2Cr0.2Nb0.2Mo0.2Ta0.2)3B4 and(V0.2Cr0.2Nb0.2Ta0.2W0.2)_(3)B_(4) were fabricated via reactive spark plasma sintering of high-energy-ball-milled elemental boron and metal precursors.The sintered specimens were〜98.7%in relative densities with virtually no oxide contamination,albeit the presence of minor(4-5 vol%)secondary high-entropy M5B6 phases.Despite that Mo_(3)B_(4) or W_(3)B_(4) are not stable phase,20%of M03B4 and W3B4 can be stabilized into the high-entropy M3B4 borides.Vickers hardness was measured to be 18.6 and 19.8 GPa at a standard load of 9.8 N.This work has further expanded the family of different structures of high-entropy ceramics reported to date.
基金We acknowledge support through the Office of Naval Research ONR-MURI(grant number N00014-15-1-2863)K.K.acknowledges support by the Department of Defense(DoD)through the National Defense Science and Engineering Graduate Fellowship(NDSEG)Program+1 种基金K.K.also acknowledges the financial support of the ARCS Foundation,San Diego ChapterK.S.V.acknowledges the financial generosity of the Oerlikon Group in support of his research group.
文摘Although high-entropy materials are attracting considerable interest due to a combination of useful properties and promising applications,predicting their formation remains a hindrance for rational discovery of new systems.Experimental approaches are based on physical intuition and/or expensive trial and error strategies.Most computational methods rely on the availability of sufficient experimental data and computational power.Machine learning(ML)applied to materials science can accelerate development and reduce costs.In this study,we propose an ML method,leveraging thermodynamic and compositional attributes of a given material for predicting the synthesizability(i.e.,entropy-forming ability)of disordered metal carbides.
文摘Deviation between thermodynamic and experimental voltages is one of the key issues in Li-ion conversion-type electrode materials; the factor that affects this phenomenon has not been understood well in spite of its importance. In this work, we combine first principles calculations and electrochemical experiments with characterization tools to probe the conversion reaction voltage of transition metal difluorides MF2（M = Fe, Ni, and Cu）. We find that the conversion reaction voltage is heavily dependent on the size of the metal nanoparticles generated. The surface energy of metal nanoparticles appears to penalize the reaction energy, which results in a lower voltage compared to the thermodynamic voltage of a bulk-phase reaction. Furthermore, we develop a reversible CuF2 electrode coated with NiO. Electron energy loss spectroscopy （EELS） elemental maps demonstrate that the lithiation process mostly occurs in the area of high NiO content. This suggests that NiO can be considered a suitable artificial solid electrolyte interphase that prevents direct contact between Cu nanoparticles and the electrolyte. Thus, it alleviates Cu dissolution into the electrolyte and improves the reversibility of CuF2.
