This study evaluated the simulation performance of mesoscale convective system(MCS)-induced precipitation,focusing on three selected cases that originated from the Yellow Sea and propagated toward the Korean Peninsula...This study evaluated the simulation performance of mesoscale convective system(MCS)-induced precipitation,focusing on three selected cases that originated from the Yellow Sea and propagated toward the Korean Peninsula.The evaluation was conducted for the European Centre for Medium-Range Weather Forecasts(ECMWF)and National Centers for Environmental Prediction(NCEP)analysis data,as well as the simulation result using them as initial and lateral boundary conditions for the Weather Research and Forecasting model.Particularly,temperature and humidity profiles from 3D dropsonde observations from the National Center for Meteorological Science of the Korea Meteorological Administration served as validation data.Results showed that the ECMWF analysis consistently had smaller errors compared to the NCEP analysis,which exhibited a cold and dry bias in the lower levels below 850 hPa.The model,in terms of the precipitation simulations,particularly for high-intensity precipitation over the Yellow Sea,demonstrated higher accuracy when applying ECMWF analysis data as the initial condition.This advantage also positively influenced the simulation of rainfall events on the Korean Peninsula by reasonably inducing convective-favorable thermodynamic features(i.e.,warm and humid lower-level atmosphere)over the Yellow Sea.In conclusion,this study provides specific information about two global analysis datasets and their impacts on MCS-induced heavy rainfall simulation by employing dropsonde observation data.Furthermore,it suggests the need to enhance the initial field for MCS-induced heavy rainfall simulation and the applicability of assimilating dropsonde data for this purpose in the future.展开更多
Growing energy demand drives the rapid development of clean and reliable energy sources.In the past years,the exploration of novel materials with considerable efficiency and durability has drawn attention in the area ...Growing energy demand drives the rapid development of clean and reliable energy sources.In the past years,the exploration of novel materials with considerable efficiency and durability has drawn attention in the area of electrochemical energy conversion.Transition metal macrocyclic metallophthalocyanines(MPcs)-based catalysts with a peculiar 2D constitution have emerged with a promising future account of their highly structural tailorability and molecular functionality which greatly extend their functionalities as electrocatalytic materials for energy conversion.This review summarizes the systematic engineering of synthesis of MPcs and their analogs in detail,and mostly pays attention to the frontier research of MPc-based high-performance catalysts toward different electrocatalytic processes concerning hydrogen,oxygen,water,carbon dioxide,and nitrogen,with a particular focus on discussing the interrelationship between the electrocatalytic activity and component/structure,as well as functional applications of MPcs.Finally,we give the gaps that need to be addressed after much thought.展开更多
Molybdenum disulfide(MoS_(2))has garnered significant attention in the field of catalysis due to the high density of active sites in its unique two-dimensional(2D)structure,which could be developed into numerous high-...Molybdenum disulfide(MoS_(2))has garnered significant attention in the field of catalysis due to the high density of active sites in its unique two-dimensional(2D)structure,which could be developed into numerous high-performance catalysts.The synthesis of ultra-small MoS2 particles(<10 nm)is highly desired in various experimental studies.The ultra-small structure could often lead to a distinct S-Mo coordination state and nonstoichiometric composition in MoSx,minimizing in-plane active sites of the 2D structure and making it probable to regulate the atomic and electronic structure of its intrinsic active sites on a large extent,especially in MoSx clusters.This article summarizes the recent progress of catalysis over ultra-small undoped MoS_(2) particles for renewable fuel production.Through a systematic review of their synthesis,structural,and spectral characteristics,as well as the relationship between their catalytic performance and inherent defects,we aim to provide insights into catalysis over this matrix that may potentially enable advancement in the development of high-performance MoS_(2)-based catalysts for sustainable energy generation in the future.展开更多
The development of superconducting joining technology for reacted magnesium diboride(MgB_(2))conductors remains a critical challenge for the advancement of cryogen-free MgB_(2)-based magnets for magnetic resonance ima...The development of superconducting joining technology for reacted magnesium diboride(MgB_(2))conductors remains a critical challenge for the advancement of cryogen-free MgB_(2)-based magnets for magnetic resonance imaging(MRI).Herein,the fabrication of superconducting joints using reacted carbon-doped multifilament MgB_(2)wires for MRI magnets is reported.To achieve successful superconducting joints,the powder-in-mold method was employed,which involved tuning the filament protection mechanism,the powder compaction pressure,and the heat treatment condition.The fabricated joints demonstrated clear superconducting-to-normal transitions in self-field,with effective magnetic field screening up to 0.5 T at 20 K.To evaluate the interface between one of the MgB_(2)filaments and the MgB_(2)bulk within the joint,serial sectioning was conducted for the first time in this type of superconducting joint.The serial sectioning revealed space formation at the interface,potentially caused by the volume shrinkage associated with the MgB_(2)formation or the combined effect of the volume shrinkage and the different thermal expansion coefficients of the MgB_(2)bulk,the filament,the mold,and the sealing material.These findings are expected to be pivotal in developing MgB_(2)superconducting joining technology for MRI magnet applications through interface engineering.展开更多
Magnesium-ion batteries(MIBs)are promising candidates for lithium-ion batteries because of their abundance,non-toxicity,and favorable electrochemical properties.This review explores the reaction mechanisms and electro...Magnesium-ion batteries(MIBs)are promising candidates for lithium-ion batteries because of their abundance,non-toxicity,and favorable electrochemical properties.This review explores the reaction mechanisms and electrochemical characteristics of Mg-alloy anode materials.While Mg metal anodes provide high volumetric capacity and dendrite-free electrodeposition,their practical application is hindered by challenges such as sluggish Mg^(2+)ion diffusion and electrolyte compatibility.Alloy-type anodes that incorporate groups XIII,XIV,and XV elements have the potential to overcome these limitations.We review various Mg alloys,emphasizing their alloying/dealloying reaction mechanisms,their theoretical capacities,and the practical aspects of MIBs.Furthermore,we discuss the influence of the electrolyte composition on the reversibility and efficiency of these alloy anodes.Emphasis is placed on overcoming current limitations through innovative materials and structural engineering.This review concludes with perspectives on future research directions aimed at enhancing the performance and commercial viability of Mg alloy anodes and contributing to the development of high-capacity,safe,and cost-effective energy storage systems.展开更多
A dye-sensitized photocatalyst combining Pt-loaded TiO_(2) and Ru(Ⅱ)tris-diimine sensitizer(RuP)was constructed and its activity for photochemical hydrogen evolution was compared with that of Pt-intercalated HCa_(2)N...A dye-sensitized photocatalyst combining Pt-loaded TiO_(2) and Ru(Ⅱ)tris-diimine sensitizer(RuP)was constructed and its activity for photochemical hydrogen evolution was compared with that of Pt-intercalated HCa_(2)Nb_(3)O_(10) nanosheets.When the sacrificial donor ethylenediaminetetraacetic acid(EDTA)disodium salt dihydrate was used,RuP/Pt/TiO_(2) showed higher activity than RuP/Pt/HCa_(2)Nb_(3)O_(10).In contrast,when NaI(a reversible electron donor)was used,RuP/Pt/TiO_(2) showed little activity due to back electron transfer to the electron acceptor(I_(3)-),which was gener-ated as the oxidation product of I-.By modification with anionic polymers(sodium poly(styrenesulfonate)or sodium polymethacrylate)that could inhibit the scavenging of conduction band electrons by I_(3)-,the H_(2) production activity from aqueous NaI was improved,but it did not exceed that of RuP/Pt/HCa_(2)Nb_(3)O_(10).Transient absorption measurements showed that the rate of semiconductor-to-dye back electron transfer was slower in the case of TiO_(2) than HCa_(2)Nb_(3)O_(10),but the electron transfer reaction to I3-was much faster.These results indicate that Pt/TiO_(2) is useful for reactions with sacrificial reductants(e.g.,EDTA),where the back electron transfer reaction to the more reducible product can be neglected.However,more careful design of the catalyst will be nec-essary when a reversible electron donor is employed.展开更多
The current global warming,coupled with the growing demand for energy in our daily lives,necessitates the development of more efficient and reliable energy storage devices.Lithium batteries(LBs)are at the forefront of...The current global warming,coupled with the growing demand for energy in our daily lives,necessitates the development of more efficient and reliable energy storage devices.Lithium batteries(LBs)are at the forefront of emerging power sources addressing these challenges.Recent studies have shown that integrating hexagonal boron nitride(h-BN)nanomaterials into LBs enhances the safety,longevity,and electrochemical performance of all LB components,including electrodes,electrolytes,and separators,thereby suggesting their potential value in advancing eco-friendly energy solutions.This review provides an overview of the most recent applications of h-BN nanomaterials in LBs.It begins with an informative introduction to h-BN nanomaterials and their relevant properties in the context of LB applications.Subsequently,it addresses the challenges posed by h-BN and discusses existing strategies to overcome these limitations,offering valuable insights into the potential of BN nanomaterials.The review then proceeds to outline the functions of h-BN in LB components,emphasizing the molecular-level mechanisms responsible for performance improvements.Finally,the review concludes by presenting the current challenges and prospects of integrating h-BN nanomaterials into battery research.展开更多
The high cost of using the niobium(Nb)barrier for manufacturing magnesium diboride(MgB2)mono-and multi-filamentary wires for large-scale applications has become one of the barriers to replacing current commercial niob...The high cost of using the niobium(Nb)barrier for manufacturing magnesium diboride(MgB2)mono-and multi-filamentary wires for large-scale applications has become one of the barriers to replacing current commercial niobium-titanium superconductors.The potential of replacing the Nb barrier with a low-cost iron(Fe)barrier for multifilament MgB2 superconducting wires is investigated in this manuscript.Therefore,MgB2 wires with Fe barrier sintered with different temperatures are studied(from 650°C to 900°C for 1 h)to investigate the non-superconducting reaction phase of Fe-B.Their superconducting performance including engineering critical current density(Je)and n-value are tested at 4.2 K in various external magnetic fields.The best sample sintered at 650°C for 1 h has achieved a Je value of 3.64×10^(4) A cm^(−2) and an n-value of 61 in 2 T magnetic field due to the reduced formation of Fe2B,better grain connectivity and homogenous microstructure.For microstructural analysis,the focused ion beam(FIB)is utilised for the first time to acquire three-dimensional microstructures and elemental mappings of the interface between the Fe barrier and MgB2 core of different wires.The results have shown that if the sintering temperature can be controlled properly,the Je and n-value of the wire are still acceptable for magnet applications.The formation of Fe2B is identified along the edge of MgB2,as the temperature increases,the content of Fe2B also increases which causes the degradation in the performance of wires.展开更多
Due to the push for carbon neutrality in various human activities,the development of methods for producing electricity without relying on chemical reaction processes or heat sources has become highly significant.Also,...Due to the push for carbon neutrality in various human activities,the development of methods for producing electricity without relying on chemical reaction processes or heat sources has become highly significant.Also,the challenge lies in achieving microwatt-scale outputs due to the inherent conductivity of the materials and diverting electric currents.To address this challenge,our research has concentrated on utilizing nonconductive mediums for water-based low-cost microfibrous ceramic wools in conjunction with a NaCl aqueous solution for power generation.The main source of electricity originates from the directed movement of water molecules and surface ions through densely packed microfibrous ceramic wools due to the effect of dynamic electric double layer.This occurrence bears resemblance to the natural water transpiration in plants,thereby presenting a fresh and straightforward approach for producing electricity in an ecofriendly manner.The generator module demonstrated in this study,measuring 12×6 cm^(2),exhibited a noteworthy open-circuit voltage of 0.35 V,coupled with a short-circuit current of 0.51 mA.Such low-cost ceramic wools are suitable for ubiquitous,permanent energy sources and hold potential for use as self-powered sensors and systems,eliminating the requirement for external energy sources such as sunlight or heat.展开更多
Controlling Li ion transport in glasses at atomic and molecular levels is key to realizing all-solid-state batteries,a promising technology for electric vehicles.In this context,Li_(3)PS_(4)glass,a promising solid ele...Controlling Li ion transport in glasses at atomic and molecular levels is key to realizing all-solid-state batteries,a promising technology for electric vehicles.In this context,Li_(3)PS_(4)glass,a promising solid electrolyte candidate,exhibits dynamic coupling between the Li^(+)cation mobility and the PS_(4)^(3-)anion libration,which is commonly referred to as the paddlewheel effect.In addition,it exhibits a concerted cation diffusion effect(i.e.,a cation-cation interaction),which is regarded as the essence of high Li ion transport.However,the correlation between the Li^(+)ions within the glass structure can only be vaguely determined,due to the limited experimental information that can be obtained.Here,this study reports that the Li ions present in glasses can be classified by evaluating their valence oscillations via Bader analysis to topologically analyze the chemical bonds.It is found that three types of Li ions are present in Li_(3)PS_(4)glass,and that the more mobile Li ions(i.e.,the Li3-type ions)exhibit a characteristic correlation at relatively long distances of 4.0-5.0A.Furthermore,reverse Monte Carlo simulations combined with deep learning potentials that reproduce X-ray,neutron,and electron diffraction pair distribution functions showed an increase in the number of Li3-type ions for partially crystallized glass structures with improved Li ion transport properties.Our results show order within the disorder of the Li ion distribution in the glass by a topological analysis of their valences.Thus,considering the molecular vibrations in the glass during the evaluation of the Li ion valences is expected to lead to the development of new solid electrolytes.展开更多
As a new generation of materials/structures,heterostructure is characterized by heterogeneous zones with dramatically different mechanical,physical or chemical properties.This endows heterostructure with unique interf...As a new generation of materials/structures,heterostructure is characterized by heterogeneous zones with dramatically different mechanical,physical or chemical properties.This endows heterostructure with unique interfaces,robust architectures,and synergistic effects,making it a promising option as advanced biomaterials for the highly variable anatomy and complex functionalities of individual patients.However,the main challenges of developing heterostructure lie in the control of crystal/phase evolution and the distribution/fraction of components and structures.In recent years,additive manufacturing techniques have attracted increasing attention in developing heterostructure due to the unique flexibility in tailored structures and synthetic multimaterials.This review focuses on the additive manufacturing of heterostructure for biomedical applications.The structural features and functional mechanisms of heterostructure are summarized.The typical material systems of heterostructure,mainly including metals,polymers,ceramics,and their composites,are presented.And the resulting synergistic effects on multiple properties are also systematically discussed in terms of mechanical,biocompatible,biodegradable,antibacterial,biosensitive and magnetostrictive properties.Next,this work outlines the research progress of additive manufacturing employed in developing heterostructure from the aspects of advantages,processes,properties,and applications.This review also highlights the prospective utilization of heterostructure in biomedical fields,with particular attention to bioscaffolds,vasculatures,biosensors and biodetections.Finally,future research directions and breakthroughs of heterostructure are prospected with focus on their more prospective applications in infection prevention and drug delivery.展开更多
The development of clean and sustainable energy sources has received widespread interest in the past few decades due to the rolling energy demands while extenuating the rising tiers of greenhouse gases and environment...The development of clean and sustainable energy sources has received widespread interest in the past few decades due to the rolling energy demands while extenuating the rising tiers of greenhouse gases and environmental pollution.Due to their intermittent nature,these green and sustainable sources require appropriate energy storage systems.Amongst different energy storage technologies,electrochemical energy storage devices,particularly supercapacitors(SCs),have fascinated global attention for their utilization in electric vehicles,power supports,portable electronics,and many others application requiring electric energy devices for their operation.Thus,the growth of SCs in the commercial market has squeezed requirements,and further developments are obligatory for their effective industrialization.In the meantime,SCs also face technical complications and contests for their introduction in industrial settings because of their low energy density and high Levelized cost.The present study combines core strengths,weaknesses,opportunities,and threats(SWOT)analysis of SCs with new perspectives and recent ideas.The challenges and the future progressive prospects of SCs are also presented in detail.This review will afford consistent direction and new superhighways for the further development of SCs as standalone and complementary energy storage systems.展开更多
The d-band state of materials is an important descriptor for activity of oxygen evolution reaction(OER).For NiO materials,there is rarely concern about tuning their d-band states to tailor the OER behaviors.Herein,NiO...The d-band state of materials is an important descriptor for activity of oxygen evolution reaction(OER).For NiO materials,there is rarely concern about tuning their d-band states to tailor the OER behaviors.Herein,NiO nanocrystals with doping small amount of La^(3+)were used to regulate d-band states for promoting OER activity.Density of states calculations based on density functional theory revealed that La^(3+)doping produced upper shift of d-band center,which would induce stronger electronic interaction between surface Ni atoms and species of oxygen evolution reaction intermediates.Further density functional theory calculation illustrated that La^(3+)doped NiO possessed reduced Gibbs free energy in adsorbing species of OER intermediate.Predicted by theoretical calculations,trace La^(3+)was introduced into crystal lattice of NiO nanoparticles.The La^(3+)doped NiO nanocrystal showed much promoted OER activity than corresponding pristine NiO product.Further electrochemical analysis revealed that La^(3+)doping into NiO increased the intrinsic activity such as improved active sites and reduced charge transfer resistance.The in-situ Raman spectra suggested that NiO phase in La^(3+)doped NiO could be better maintained than pristine NiO during the OER.This work provides an effective strategy to tune the d-band center of NiO for efficient electrocatalytic OER.展开更多
Taking copper doped ZnS(ZnS:Cu)nanocrystals as the main body of photocatalyst,the influence of different base transition metal ions(M^(2+)=Ni^(2+),Co^(2+),Fe^(2+)and Cd^(2+))on photocatalytic CO_(2)reduction in inorga...Taking copper doped ZnS(ZnS:Cu)nanocrystals as the main body of photocatalyst,the influence of different base transition metal ions(M^(2+)=Ni^(2+),Co^(2+),Fe^(2+)and Cd^(2+))on photocatalytic CO_(2)reduction in inorganic reaction system is investigated.Confined single-atom Ni^(2+),Co^(2+),and Cd^(2+)sites were created via cation-exchange process and enhanced CO_(2)reduction,while Fe^(2+)suppressed the photocatalytic activity for both water and CO_(2)reduction.The modified ZnS:Cu photocatalysts(M/ZnS:Cu)demonstrated tunable product selectivity,with Ni^(2+)and Co^(2+)showing high selectivity for syngas production and Cd^(2+)displaying remarkable formate selectivity.DFT calculations indicated favorable H adsorption free energy on Ni^(2+)and Co^(2+)sites,promoting the hydrogen evolution reaction.The selectivity of CO_(2)reduction products was found to be sensitive to the initial intermediate adsorption states.*COOH formed on Ni^(2+)and Co^(2+)while*OCHO formed on Cd^(2+),favoring the production of CO and HCOOH as the main products,respectively.This work provides valuable insights for developing efficient solar-to-fuel platforms with controlled CO_(2)reduction selectivity.展开更多
The d-band states of catalytic materials participate in adsorbing reactive intermediate species and determine the catalytic behaviors in CO_(2)reduction reactions.However,surface d-band states relating to the photocat...The d-band states of catalytic materials participate in adsorbing reactive intermediate species and determine the catalytic behaviors in CO_(2)reduction reactions.However,surface d-band states relating to the photocatalytic CO_(2)reduction reactions behaviors are rarely concerned.Herein,a slightly amount of Cd^(2+)is decorated on the surface of(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material(Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4))to tune the surface d-band states for improved CO_(2)+2reduction reactions.The Cd/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)is fabricated via the facile ions-exchange method to make that slightly Zn2+is substituted by Cd^(2+).The Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)exhibits much enhanced photocatalytic activity in CO_(2)reduction reactions to produce CO and water splitting to produce H_(2).Physical characterizations show that the energy band structure is not changed obviously.Density functional theory reveals that Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)possesses a closer shift of d-band center to Fermi level than(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4),suggesting easier adsorption of CO_(2)reduction reactive intermediates after Cd^(2+)decoration.Further calculations confirm that a relatively reduced adsorption Gibbs energy of reactive intermediates in CO_(2)reduction reaction is required on Zn atoms in Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material,benefiting the photocatalytic CO_(2)reduction reactions.This work engineers surface d-band states by surface Cd^(2+)decoration,which gives an effective strategy to design highly efficient photocatalysts for syngas production.展开更多
Electrocatalytic conversion of carbon dioxide to high value-added chemicals is a promising method for solving the energy crisis and global warming.Electrochemical active metal-containing conjugated polymers have been ...Electrocatalytic conversion of carbon dioxide to high value-added chemicals is a promising method for solving the energy crisis and global warming.Electrochemical active metal-containing conjugated polymers have been widely studied for heterogeneous carbon dioxide reduction.In the present contribution,we designed and synthesized a stable cobalt phthalocyanine-based conjugated polymer,named CoPPc-TFPPy-CP,and also explored its electro-catalytic application in carbon dioxide reduction to liquid products in an aqueous solution.In the catalyst,cobalt phthalocyanine acts as building blocks connected with 1,3,6,8-tetrakis(4-formyl phenyl)pyrenes via imine-linkages,leading to mesoporous formation polymers with the pore size centered at 4.1nm.And the central co-balt atoms shifted to a higher oxidation state after condensation.With these chemical and structural natures,the catalyst displayed a remarkable electrocatalytic CO_(2) reduction performance with an ethanol Faradaic efficiency of 43.25%at-1.0V vs RHE.While at the same time,the electrochemical reduction process catalyzed by cobalt phthalocyanine produced only carbon monoxide and hydrogen.To the best of our knowledge,CoPPc-TFPPy-CP is the first example among organic polymers and metal-organic frameworks that produces ethanol from CO_(2) with a remarkable selectivity.展开更多
基金supported by the Korea Meteorological Administration Research and Development Program “Developing Application Technology for Atmospheric Research Aircraft” (Grant No. KMA2018-00222)
文摘This study evaluated the simulation performance of mesoscale convective system(MCS)-induced precipitation,focusing on three selected cases that originated from the Yellow Sea and propagated toward the Korean Peninsula.The evaluation was conducted for the European Centre for Medium-Range Weather Forecasts(ECMWF)and National Centers for Environmental Prediction(NCEP)analysis data,as well as the simulation result using them as initial and lateral boundary conditions for the Weather Research and Forecasting model.Particularly,temperature and humidity profiles from 3D dropsonde observations from the National Center for Meteorological Science of the Korea Meteorological Administration served as validation data.Results showed that the ECMWF analysis consistently had smaller errors compared to the NCEP analysis,which exhibited a cold and dry bias in the lower levels below 850 hPa.The model,in terms of the precipitation simulations,particularly for high-intensity precipitation over the Yellow Sea,demonstrated higher accuracy when applying ECMWF analysis data as the initial condition.This advantage also positively influenced the simulation of rainfall events on the Korean Peninsula by reasonably inducing convective-favorable thermodynamic features(i.e.,warm and humid lower-level atmosphere)over the Yellow Sea.In conclusion,this study provides specific information about two global analysis datasets and their impacts on MCS-induced heavy rainfall simulation by employing dropsonde observation data.Furthermore,it suggests the need to enhance the initial field for MCS-induced heavy rainfall simulation and the applicability of assimilating dropsonde data for this purpose in the future.
基金financially supported by the National Natural Science Foundation of China(51702291)the China Postdoctoral Science Foundation(2020M682352)+2 种基金the State Key Laboratory of Powder Metallurgy,Central South University,Changsha,Chinasupport from the Project of Zhongyuan Critical Metals Laboratory(GJJSGFYQ202336)the Youth Talent Program of Zhengzhou University(32340398)
文摘Growing energy demand drives the rapid development of clean and reliable energy sources.In the past years,the exploration of novel materials with considerable efficiency and durability has drawn attention in the area of electrochemical energy conversion.Transition metal macrocyclic metallophthalocyanines(MPcs)-based catalysts with a peculiar 2D constitution have emerged with a promising future account of their highly structural tailorability and molecular functionality which greatly extend their functionalities as electrocatalytic materials for energy conversion.This review summarizes the systematic engineering of synthesis of MPcs and their analogs in detail,and mostly pays attention to the frontier research of MPc-based high-performance catalysts toward different electrocatalytic processes concerning hydrogen,oxygen,water,carbon dioxide,and nitrogen,with a particular focus on discussing the interrelationship between the electrocatalytic activity and component/structure,as well as functional applications of MPcs.Finally,we give the gaps that need to be addressed after much thought.
基金support from the Tangshan Talent Funding Project(A202202007)the National Natural Science Foundation of China(21703065)+1 种基金the Natural Science Foundation of Hebei Province(B2018209267,E2022209039)the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China(51888103).
文摘Molybdenum disulfide(MoS_(2))has garnered significant attention in the field of catalysis due to the high density of active sites in its unique two-dimensional(2D)structure,which could be developed into numerous high-performance catalysts.The synthesis of ultra-small MoS2 particles(<10 nm)is highly desired in various experimental studies.The ultra-small structure could often lead to a distinct S-Mo coordination state and nonstoichiometric composition in MoSx,minimizing in-plane active sites of the 2D structure and making it probable to regulate the atomic and electronic structure of its intrinsic active sites on a large extent,especially in MoSx clusters.This article summarizes the recent progress of catalysis over ultra-small undoped MoS_(2) particles for renewable fuel production.Through a systematic review of their synthesis,structural,and spectral characteristics,as well as the relationship between their catalytic performance and inherent defects,we aim to provide insights into catalysis over this matrix that may potentially enable advancement in the development of high-performance MoS_(2)-based catalysts for sustainable energy generation in the future.
基金the Japan Society for the Promotion of Science(JSPS)KAKENHI Grant Number JP18F18714Cryogenic Station,Research Network and Facility Services Division,National Institute for Materials Science(NIMS),Japansupported by the ARC Linkage Project(LP200200689)。
文摘The development of superconducting joining technology for reacted magnesium diboride(MgB_(2))conductors remains a critical challenge for the advancement of cryogen-free MgB_(2)-based magnets for magnetic resonance imaging(MRI).Herein,the fabrication of superconducting joints using reacted carbon-doped multifilament MgB_(2)wires for MRI magnets is reported.To achieve successful superconducting joints,the powder-in-mold method was employed,which involved tuning the filament protection mechanism,the powder compaction pressure,and the heat treatment condition.The fabricated joints demonstrated clear superconducting-to-normal transitions in self-field,with effective magnetic field screening up to 0.5 T at 20 K.To evaluate the interface between one of the MgB_(2)filaments and the MgB_(2)bulk within the joint,serial sectioning was conducted for the first time in this type of superconducting joint.The serial sectioning revealed space formation at the interface,potentially caused by the volume shrinkage associated with the MgB_(2)formation or the combined effect of the volume shrinkage and the different thermal expansion coefficients of the MgB_(2)bulk,the filament,the mold,and the sealing material.These findings are expected to be pivotal in developing MgB_(2)superconducting joining technology for MRI magnet applications through interface engineering.
基金supported by the Global Joint Research Program funded by the Pukyong National University(202411790001).
文摘Magnesium-ion batteries(MIBs)are promising candidates for lithium-ion batteries because of their abundance,non-toxicity,and favorable electrochemical properties.This review explores the reaction mechanisms and electrochemical characteristics of Mg-alloy anode materials.While Mg metal anodes provide high volumetric capacity and dendrite-free electrodeposition,their practical application is hindered by challenges such as sluggish Mg^(2+)ion diffusion and electrolyte compatibility.Alloy-type anodes that incorporate groups XIII,XIV,and XV elements have the potential to overcome these limitations.We review various Mg alloys,emphasizing their alloying/dealloying reaction mechanisms,their theoretical capacities,and the practical aspects of MIBs.Furthermore,we discuss the influence of the electrolyte composition on the reversibility and efficiency of these alloy anodes.Emphasis is placed on overcoming current limitations through innovative materials and structural engineering.This review concludes with perspectives on future research directions aimed at enhancing the performance and commercial viability of Mg alloy anodes and contributing to the development of high-capacity,safe,and cost-effective energy storage systems.
文摘A dye-sensitized photocatalyst combining Pt-loaded TiO_(2) and Ru(Ⅱ)tris-diimine sensitizer(RuP)was constructed and its activity for photochemical hydrogen evolution was compared with that of Pt-intercalated HCa_(2)Nb_(3)O_(10) nanosheets.When the sacrificial donor ethylenediaminetetraacetic acid(EDTA)disodium salt dihydrate was used,RuP/Pt/TiO_(2) showed higher activity than RuP/Pt/HCa_(2)Nb_(3)O_(10).In contrast,when NaI(a reversible electron donor)was used,RuP/Pt/TiO_(2) showed little activity due to back electron transfer to the electron acceptor(I_(3)-),which was gener-ated as the oxidation product of I-.By modification with anionic polymers(sodium poly(styrenesulfonate)or sodium polymethacrylate)that could inhibit the scavenging of conduction band electrons by I_(3)-,the H_(2) production activity from aqueous NaI was improved,but it did not exceed that of RuP/Pt/HCa_(2)Nb_(3)O_(10).Transient absorption measurements showed that the rate of semiconductor-to-dye back electron transfer was slower in the case of TiO_(2) than HCa_(2)Nb_(3)O_(10),but the electron transfer reaction to I3-was much faster.These results indicate that Pt/TiO_(2) is useful for reactions with sacrificial reductants(e.g.,EDTA),where the back electron transfer reaction to the more reducible product can be neglected.However,more careful design of the catalyst will be nec-essary when a reversible electron donor is employed.
基金AP is grateful for the financial support of Science Foundation Ireland(SFI)under grant number 18/SIRG/5621 and Enterprise Ireland under grant number CS20212089DG is grateful to the Australian Research Council(ARC)for a support in the frame of an ARC Laureate project No FL160100089.Open access funding provided by IReL.
文摘The current global warming,coupled with the growing demand for energy in our daily lives,necessitates the development of more efficient and reliable energy storage devices.Lithium batteries(LBs)are at the forefront of emerging power sources addressing these challenges.Recent studies have shown that integrating hexagonal boron nitride(h-BN)nanomaterials into LBs enhances the safety,longevity,and electrochemical performance of all LB components,including electrodes,electrolytes,and separators,thereby suggesting their potential value in advancing eco-friendly energy solutions.This review provides an overview of the most recent applications of h-BN nanomaterials in LBs.It begins with an informative introduction to h-BN nanomaterials and their relevant properties in the context of LB applications.Subsequently,it addresses the challenges posed by h-BN and discusses existing strategies to overcome these limitations,offering valuable insights into the potential of BN nanomaterials.The review then proceeds to outline the functions of h-BN in LB components,emphasizing the molecular-level mechanisms responsible for performance improvements.Finally,the review concludes by presenting the current challenges and prospects of integrating h-BN nanomaterials into battery research.
基金support from the Australian Research Council(ARC)Linkage Project(LP200200689).
文摘The high cost of using the niobium(Nb)barrier for manufacturing magnesium diboride(MgB2)mono-and multi-filamentary wires for large-scale applications has become one of the barriers to replacing current commercial niobium-titanium superconductors.The potential of replacing the Nb barrier with a low-cost iron(Fe)barrier for multifilament MgB2 superconducting wires is investigated in this manuscript.Therefore,MgB2 wires with Fe barrier sintered with different temperatures are studied(from 650°C to 900°C for 1 h)to investigate the non-superconducting reaction phase of Fe-B.Their superconducting performance including engineering critical current density(Je)and n-value are tested at 4.2 K in various external magnetic fields.The best sample sintered at 650°C for 1 h has achieved a Je value of 3.64×10^(4) A cm^(−2) and an n-value of 61 in 2 T magnetic field due to the reduced formation of Fe2B,better grain connectivity and homogenous microstructure.For microstructural analysis,the focused ion beam(FIB)is utilised for the first time to acquire three-dimensional microstructures and elemental mappings of the interface between the Fe barrier and MgB2 core of different wires.The results have shown that if the sintering temperature can be controlled properly,the Je and n-value of the wire are still acceptable for magnet applications.The formation of Fe2B is identified along the edge of MgB2,as the temperature increases,the content of Fe2B also increases which causes the degradation in the performance of wires.
基金supported by JSPS Kakenhi program(program number 16H06364)and JST CRESTThe authors extend their appreciation to the Deputyship for Research and Innovation,“Ministry of Education”in Saudi Arabia for funding this research(IFKSUOR3-615-5)O.M.also thank the support of Tomsk State University Development Programme(priority-2030)for this work.
文摘Due to the push for carbon neutrality in various human activities,the development of methods for producing electricity without relying on chemical reaction processes or heat sources has become highly significant.Also,the challenge lies in achieving microwatt-scale outputs due to the inherent conductivity of the materials and diverting electric currents.To address this challenge,our research has concentrated on utilizing nonconductive mediums for water-based low-cost microfibrous ceramic wools in conjunction with a NaCl aqueous solution for power generation.The main source of electricity originates from the directed movement of water molecules and surface ions through densely packed microfibrous ceramic wools due to the effect of dynamic electric double layer.This occurrence bears resemblance to the natural water transpiration in plants,thereby presenting a fresh and straightforward approach for producing electricity in an ecofriendly manner.The generator module demonstrated in this study,measuring 12×6 cm^(2),exhibited a noteworthy open-circuit voltage of 0.35 V,coupled with a short-circuit current of 0.51 mA.Such low-cost ceramic wools are suitable for ubiquitous,permanent energy sources and hold potential for use as self-powered sensors and systems,eliminating the requirement for external energy sources such as sunlight or heat.
基金partially supported by JSPS KAKENHI(Grant Numbers 19 K05025,19H05814,19H05815,19H05816,20H02430,21H02038,and 21H05549)
文摘Controlling Li ion transport in glasses at atomic and molecular levels is key to realizing all-solid-state batteries,a promising technology for electric vehicles.In this context,Li_(3)PS_(4)glass,a promising solid electrolyte candidate,exhibits dynamic coupling between the Li^(+)cation mobility and the PS_(4)^(3-)anion libration,which is commonly referred to as the paddlewheel effect.In addition,it exhibits a concerted cation diffusion effect(i.e.,a cation-cation interaction),which is regarded as the essence of high Li ion transport.However,the correlation between the Li^(+)ions within the glass structure can only be vaguely determined,due to the limited experimental information that can be obtained.Here,this study reports that the Li ions present in glasses can be classified by evaluating their valence oscillations via Bader analysis to topologically analyze the chemical bonds.It is found that three types of Li ions are present in Li_(3)PS_(4)glass,and that the more mobile Li ions(i.e.,the Li3-type ions)exhibit a characteristic correlation at relatively long distances of 4.0-5.0A.Furthermore,reverse Monte Carlo simulations combined with deep learning potentials that reproduce X-ray,neutron,and electron diffraction pair distribution functions showed an increase in the number of Li3-type ions for partially crystallized glass structures with improved Li ion transport properties.Our results show order within the disorder of the Li ion distribution in the glass by a topological analysis of their valences.Thus,considering the molecular vibrations in the glass during the evaluation of the Li ion valences is expected to lead to the development of new solid electrolytes.
基金The Natural Science Foundation of China(51935014,52275395,82072084)Hunan Provincial Natural Science Foundation of China(2020JJ3047)+4 种基金Central South University Innovation-Driven Research Programme(2023CXQD023)JiangXi Provincial Natural Science Foundation of China(20224ACB204013)Technology Innovation Platform Project of Shenzhen Institute of Information Technology 2020(PT2020E002)Guangdong Province Precision Manufacturing and Intelligent Production Education Integration Innovation Platform(2022CJPT019)The Project of State Key Laboratory of Precision Manufacturing for Extreme Service Performance。
文摘As a new generation of materials/structures,heterostructure is characterized by heterogeneous zones with dramatically different mechanical,physical or chemical properties.This endows heterostructure with unique interfaces,robust architectures,and synergistic effects,making it a promising option as advanced biomaterials for the highly variable anatomy and complex functionalities of individual patients.However,the main challenges of developing heterostructure lie in the control of crystal/phase evolution and the distribution/fraction of components and structures.In recent years,additive manufacturing techniques have attracted increasing attention in developing heterostructure due to the unique flexibility in tailored structures and synthetic multimaterials.This review focuses on the additive manufacturing of heterostructure for biomedical applications.The structural features and functional mechanisms of heterostructure are summarized.The typical material systems of heterostructure,mainly including metals,polymers,ceramics,and their composites,are presented.And the resulting synergistic effects on multiple properties are also systematically discussed in terms of mechanical,biocompatible,biodegradable,antibacterial,biosensitive and magnetostrictive properties.Next,this work outlines the research progress of additive manufacturing employed in developing heterostructure from the aspects of advantages,processes,properties,and applications.This review also highlights the prospective utilization of heterostructure in biomedical fields,with particular attention to bioscaffolds,vasculatures,biosensors and biodetections.Finally,future research directions and breakthroughs of heterostructure are prospected with focus on their more prospective applications in infection prevention and drug delivery.
基金supported by the Japan Society for the Promotion of Science(JSPS)KAKENHI Grant Number JP22F22368。
文摘The development of clean and sustainable energy sources has received widespread interest in the past few decades due to the rolling energy demands while extenuating the rising tiers of greenhouse gases and environmental pollution.Due to their intermittent nature,these green and sustainable sources require appropriate energy storage systems.Amongst different energy storage technologies,electrochemical energy storage devices,particularly supercapacitors(SCs),have fascinated global attention for their utilization in electric vehicles,power supports,portable electronics,and many others application requiring electric energy devices for their operation.Thus,the growth of SCs in the commercial market has squeezed requirements,and further developments are obligatory for their effective industrialization.In the meantime,SCs also face technical complications and contests for their introduction in industrial settings because of their low energy density and high Levelized cost.The present study combines core strengths,weaknesses,opportunities,and threats(SWOT)analysis of SCs with new perspectives and recent ideas.The challenges and the future progressive prospects of SCs are also presented in detail.This review will afford consistent direction and new superhighways for the further development of SCs as standalone and complementary energy storage systems.
基金financial support from the National Natural Science Foundation of China(No.22072183)the Natural Science Foundation of Hunan Province,China(No.2022JJ30690)。
文摘The d-band state of materials is an important descriptor for activity of oxygen evolution reaction(OER).For NiO materials,there is rarely concern about tuning their d-band states to tailor the OER behaviors.Herein,NiO nanocrystals with doping small amount of La^(3+)were used to regulate d-band states for promoting OER activity.Density of states calculations based on density functional theory revealed that La^(3+)doping produced upper shift of d-band center,which would induce stronger electronic interaction between surface Ni atoms and species of oxygen evolution reaction intermediates.Further density functional theory calculation illustrated that La^(3+)doped NiO possessed reduced Gibbs free energy in adsorbing species of OER intermediate.Predicted by theoretical calculations,trace La^(3+)was introduced into crystal lattice of NiO nanoparticles.The La^(3+)doped NiO nanocrystal showed much promoted OER activity than corresponding pristine NiO product.Further electrochemical analysis revealed that La^(3+)doping into NiO increased the intrinsic activity such as improved active sites and reduced charge transfer resistance.The in-situ Raman spectra suggested that NiO phase in La^(3+)doped NiO could be better maintained than pristine NiO during the OER.This work provides an effective strategy to tune the d-band center of NiO for efficient electrocatalytic OER.
基金financial support from the Tangshan Talent Funding Project(A202202007)the National Natural Science Foundation of China(21703065)+3 种基金the Natural Science Foundation of Hebei Province(B2018209267)the World Premier International Research Center Initiative(WPI Initiative)on Materials Nanoarchitectonics(MANA),the MEXT(Japan)the Photoexcitonix Project in Hokkaido Universitythe JSPS KAKENHI(Grant Number JP18H02065)。
文摘Taking copper doped ZnS(ZnS:Cu)nanocrystals as the main body of photocatalyst,the influence of different base transition metal ions(M^(2+)=Ni^(2+),Co^(2+),Fe^(2+)and Cd^(2+))on photocatalytic CO_(2)reduction in inorganic reaction system is investigated.Confined single-atom Ni^(2+),Co^(2+),and Cd^(2+)sites were created via cation-exchange process and enhanced CO_(2)reduction,while Fe^(2+)suppressed the photocatalytic activity for both water and CO_(2)reduction.The modified ZnS:Cu photocatalysts(M/ZnS:Cu)demonstrated tunable product selectivity,with Ni^(2+)and Co^(2+)showing high selectivity for syngas production and Cd^(2+)displaying remarkable formate selectivity.DFT calculations indicated favorable H adsorption free energy on Ni^(2+)and Co^(2+)sites,promoting the hydrogen evolution reaction.The selectivity of CO_(2)reduction products was found to be sensitive to the initial intermediate adsorption states.*COOH formed on Ni^(2+)and Co^(2+)while*OCHO formed on Cd^(2+),favoring the production of CO and HCOOH as the main products,respectively.This work provides valuable insights for developing efficient solar-to-fuel platforms with controlled CO_(2)reduction selectivity.
基金the financial support from the National Natural Science Foundation of China(22072183)the Natural Science Foundation of Hunan Province,China(2022JJ30690)supported in part by the High Performance Computing Center of Central South University。
文摘The d-band states of catalytic materials participate in adsorbing reactive intermediate species and determine the catalytic behaviors in CO_(2)reduction reactions.However,surface d-band states relating to the photocatalytic CO_(2)reduction reactions behaviors are rarely concerned.Herein,a slightly amount of Cd^(2+)is decorated on the surface of(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material(Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4))to tune the surface d-band states for improved CO_(2)+2reduction reactions.The Cd/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)is fabricated via the facile ions-exchange method to make that slightly Zn2+is substituted by Cd^(2+).The Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)exhibits much enhanced photocatalytic activity in CO_(2)reduction reactions to produce CO and water splitting to produce H_(2).Physical characterizations show that the energy band structure is not changed obviously.Density functional theory reveals that Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)possesses a closer shift of d-band center to Fermi level than(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4),suggesting easier adsorption of CO_(2)reduction reactive intermediates after Cd^(2+)decoration.Further calculations confirm that a relatively reduced adsorption Gibbs energy of reactive intermediates in CO_(2)reduction reaction is required on Zn atoms in Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material,benefiting the photocatalytic CO_(2)reduction reactions.This work engineers surface d-band states by surface Cd^(2+)decoration,which gives an effective strategy to design highly efficient photocatalysts for syngas production.
基金the financial support from the National Natural Science Foundation of China(22005099)。
文摘Electrocatalytic conversion of carbon dioxide to high value-added chemicals is a promising method for solving the energy crisis and global warming.Electrochemical active metal-containing conjugated polymers have been widely studied for heterogeneous carbon dioxide reduction.In the present contribution,we designed and synthesized a stable cobalt phthalocyanine-based conjugated polymer,named CoPPc-TFPPy-CP,and also explored its electro-catalytic application in carbon dioxide reduction to liquid products in an aqueous solution.In the catalyst,cobalt phthalocyanine acts as building blocks connected with 1,3,6,8-tetrakis(4-formyl phenyl)pyrenes via imine-linkages,leading to mesoporous formation polymers with the pore size centered at 4.1nm.And the central co-balt atoms shifted to a higher oxidation state after condensation.With these chemical and structural natures,the catalyst displayed a remarkable electrocatalytic CO_(2) reduction performance with an ethanol Faradaic efficiency of 43.25%at-1.0V vs RHE.While at the same time,the electrochemical reduction process catalyzed by cobalt phthalocyanine produced only carbon monoxide and hydrogen.To the best of our knowledge,CoPPc-TFPPy-CP is the first example among organic polymers and metal-organic frameworks that produces ethanol from CO_(2) with a remarkable selectivity.