For dissimilar metal welds(DMWs)involving nickel-based weld metal(WM)and ferritic heat resistant steel base metal(BM)in power plants,there must be an interface between WM and BM,and this interface suffers mechanical a...For dissimilar metal welds(DMWs)involving nickel-based weld metal(WM)and ferritic heat resistant steel base metal(BM)in power plants,there must be an interface between WM and BM,and this interface suffers mechanical and microstructure mismatches and is often the rupture location of premature failure.In this study,a new form of WM/BM interface form,namely double Y-type interface was designed for the DMWs.Creep behaviors and life of DMWs containing double Y-type interface and conventional I-type interface were compared by finite element analysis and creep tests,and creep failure mechanisms were investigated by stress-strain analysis and microstructure characterization.By applying double Y-type interface instead of conventional I-type interface,failure location of DMW could be shifted from the WM/ferritic heat-affected zone(HAZ)interface into the ferritic HAZ or even the ferritic BM,and the failure mode change improved the creep life of DMW.The interface premature failure of I-type interface DMW was related to the coupling effect of microstructure degradation,stress and strain concentrations,and oxide notch on the WM/HAZ interface.The creep failure of double Y-type interface DMW was the result of Type IV fracture due to the creep voids and micro-cracks on fine-grain boundaries in HAZ,which was a result of the matrix softening of HAZ and lack of precipitate pinning at fine-grain boundaries.The double Y-type interface form separated the stress and strain concentrations in DMW from the WM/HAZ interface,preventing the trigger effect of oxide notch on interface failure and inhibiting the interfacial microstructure cracking.It is a novel scheme to prolong creep life and enhance reliability of DMW,by means of optimizing the interface form,decoupling the damage factors from WM/HAZ interface,and then changing the failure mechanism and shifting the failure location.展开更多
Developing sustainable and clean energy sources(e.g.,solar,wind,and tide energy)is essential to achieve the goal of carbon neutrality.Due to the discontinuous and inco nsistent nature of common clean energy sources,hi...Developing sustainable and clean energy sources(e.g.,solar,wind,and tide energy)is essential to achieve the goal of carbon neutrality.Due to the discontinuous and inco nsistent nature of common clean energy sources,high-performance energy storage technologies are a critical part of achieving this target.Aqueous zinc metal batteries(AZMBs)with inherent safety,low cost,and competitive performance are regarded as one of the promising candidates for grid-scale energy storage.However,zinc metal anodes(ZMAs)with irreversible problems of dendrite growth,hydrogen evolution reaction,self-corrosio n,and other side reactions have seriously hindered the development and commercialization of AZMBs.An increasing number of researchers are focusing on the stability of ZMAs,so assessing the effectiveness of existing research strategies is critical to the development of AZMBs.This review aims to provide a comprehensive overview of the fundamentals and challenges of AZMBs.Resea rch strategies for interfacial modification of ZMAs are systematically presented.The features of artificial interfacial coating and in-situ interfacial coating of ZMAs are compared and discussed in detail,as well as the effect of modified interfacial ZMA on the full-battery performance.Finally,perspectives are provided on the problems and challenges of ZMAs.This review is expected to offer a constructive reference for the further development and commercialization of AZMBs.展开更多
Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing...Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing performance.However,previous methods of synthesizing MO_(x)/C composites suffer from problems,including inhomogeneity,aggregation,and challenges in micropatterning.Herein,we introduce a refined method that employs a metal–organic framework(MOF)as a precursor combined with direct laser writing.The inherent structure of MOFs ensures a uniform distribution of metal ions and organic linkers,yielding homogeneous MO_(x)/C structures.The laser processing facilitates precise micropatterning(<2μm,comparable to typical photolithography)of the MO_(x)/C crystals.The optimized MOF-derived MO_(x)/C sensor rapidly detected ethanol gas even at room temperature(105 and 18 s for response and recovery,respectively),with a broad range of sensing performance from 170 to 3,400 ppm and a high response value of up to 3,500%.Additionally,this sensor exhibited enhanced stability and thermal resilience compared to previous MOF-based counterparts.This research opens up promising avenues for practical applications in MOF-derived sensing devices.展开更多
The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clu...The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.展开更多
In this study,the interactions between a Ga-based liquid metal,GaInSn,and several metal materials,including pure metals(Ni and Ti)and alloys(316H stainless steel(SS)and GH3535),at 650℃were investigated.The aim was to...In this study,the interactions between a Ga-based liquid metal,GaInSn,and several metal materials,including pure metals(Ni and Ti)and alloys(316H stainless steel(SS)and GH3535),at 650℃were investigated.The aim was to evaluate the corrosion performance and select a suitable candidate material for use as a molten salt manometer diaphragm in thermal energy storage systems.The results indicated that the alloys(316H SS and GH3535)exhibited less corrosion than pure metals(Ni and Ti)in liquid GaInSn.Ga-rich binary intermetallic compounds were found to form on the surfaces of all the tested metal materials exposed to liquid GaInSn,as a result of the decomposition of liquid GaInSn and its reaction with the constituent elements of the metal materials.The corrosion mechanism for all the tested materials exposed to liquid GaInSn was also investigated and proposed,which may aid in selecting the optimal candidate material when liquid GaInSn is used as the pressure-sensing medium.展开更多
The selective oxidation of hydrocarbons can be used to produce oxygen-containing functional compounds such as alcohols, aldehydes or ketones and its efficient and green conversion lies in the development of efficient ...The selective oxidation of hydrocarbons can be used to produce oxygen-containing functional compounds such as alcohols, aldehydes or ketones and its efficient and green conversion lies in the development of efficient catalysts that activate C-H bonds and O_(2) simultaneously. In this work, the bimetallic organic framework (CoMnBDC) material with morphology of stacked nanosheets was synthesized using terephthalic acid as ligands to coordinate with Co^(2+) and Mn^(2+) cations under solvothermal conditions. As revealed by spectroscopic characterizations, the electron transfer from Mn to Co in the CoMnBDC resulted in the reduction of the Co average oxidation state and increase of the Mn average oxidation state. The CoMnBDC nanosheets were used as catalyst in catalytic oxidation of ethylbenzene, in which the redox effect promotes the effective electron transfer, the activation of O_(2) and benzyl C-H bond. The 96.2% conversion of ethylbenzene and 98.0% selectivity towards acetophenone could be obtained with oxygen as sole oxidant and solvent-free condition. The excellent catalytic performance is related to the structure of CoMnBDC and is also the best when compared with reported results. Various types of aromatic hydrocarbons containing benzyl C-H bonds can be effectively oxidized by CoMnBDC to produce corresponding ketone products. The density functional theory (DFT) calculation revealed that the redox effect leads to the relative enrichment of electrons on Co in CoMnBDC, which is conducive to the activation of O_(2);Mn with higher oxidation state is beneficial for the adsorption of ethylbenzene and activation of C-H bonds. The CoMnBDC has a lower energy barrier for transition state, making it easier for the ethylbenzene oxidation to produce acetophenone.展开更多
Aqueous Zn metal batteries(AZMBs)with intrinsic safety,high energy density and low cost have been regarded as promising electrochemical energy storage devices.However,the parasitic reaction on metallic Zn anode and th...Aqueous Zn metal batteries(AZMBs)with intrinsic safety,high energy density and low cost have been regarded as promising electrochemical energy storage devices.However,the parasitic reaction on metallic Zn anode and the incompatibility between electrode and electrolytes lead to the deterioration of electrochemical performance of AZMBs during the cycling.The critical point to achieve the stable cycling of AZMBs is to properly regulate the zinc ion solvated structure and transfer behavior between metallic Zn anode and electrolyte.In recent years,numerous achievements have been made to resolve the formation of Zn dendrite and interface incompatible issues faced by AZMBs via optimizing the sheath structure and transport capability of zinc ions at electrode-electrolyte interface.In this review,the challenges for metallic Zn anode and electrode-electrolyte interface in AZMBs including dendrite formation and interface characteristics are presented.Following the influences of different strategies involving designing advanced electrode structu re,artificial solid electrolyte interphase(SEI)on Zn anode and electrolyte engineering to regulate zinc ion solvated sheath structure and transport behavior are summarized and discussed.Finally,the perspectives for the future development of design strategies for dendrite-free Zn metal anode and long lifespan AZMBs are also given.展开更多
The widespread adoption of lithium-ion batteries has been driven by the proliferation of portable electronic devices and electric vehicles,which have increasingly stringent energy density requirements.Lithium metal ba...The widespread adoption of lithium-ion batteries has been driven by the proliferation of portable electronic devices and electric vehicles,which have increasingly stringent energy density requirements.Lithium metal batteries(LMBs),with their ultralow reduction potential and high theoretical capacity,are widely regarded as the most promising technical pathway for achieving high energy density batteries.In this review,we provide a comprehensive overview of fundamental issues related to high reactivity and migrated interfaces in LMBs.Furthermore,we propose improved strategies involving interface engineering,3D current collector design,electrolyte optimization,separator modification,application of alloyed anodes,and external field regulation to address these challenges.The utilization of solid-state electrolytes can significantly enhance the safety of LMBs and represents the only viable approach for advancing them.This review also encompasses the variation in fundamental issues and design strategies for the transition from liquid to solid electrolytes.Particularly noteworthy is that the introduction of SSEs will exacerbate differences in electrochemical and mechanical properties at the interface,leading to increased interface inhomogeneity—a critical factor contributing to failure in all-solidstate lithium metal batteries.Based on recent research works,this perspective highlights the current status of research on developing high-performance LMBs.展开更多
Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and safety.Nonetheless,i...Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and safety.Nonetheless,inherent challenges of deleterious lithium dendrite growth and poor interfacial stability hinder their commercial application.Herein,we report a liquid metal-coated lithium metal(LM@Li)anode strategy to improve the contact between lithium metal and a Li6PS5Cl inorganic electrolyte.The LM@Li symmetric cell shows over 1000 h of stable lithium plating/stripping cycles at 2mA cm^(-2) and a significantly higher critical current density of 9.8 mAcm^(-2) at 25°C.In addition,a full battery assembled with a high-capacity composite LiNbO3@-LiNi_(0.7)Co_(0.2)Mn_(0.1)O_(2)(LNO@NCM721)cathode shows stable cycling performance.Experimental and computational results have demonstrated that dendrite growth tolerance and physical contact in solid-state batteries can be reinforced by using LM interlayers for interfacial modification.展开更多
Engineering transition metal compounds(TMCs)catalysts with excellent adsorption-catalytic ability has been one of the most effec-tive strategies to accelerate the redox kinetics of sulfur cathodes.Herein,this review f...Engineering transition metal compounds(TMCs)catalysts with excellent adsorption-catalytic ability has been one of the most effec-tive strategies to accelerate the redox kinetics of sulfur cathodes.Herein,this review focuses on engineering TMCs catalysts by cation doping/anion doping/dual doping,bimetallic/bi-anionic TMCs,and TMCs-based heterostructure composites.It is obvious that introducing cations/anions to TMCs or constructing heterostructure can boost adsorption-catalytic capacity by regulating the electronic structure including energy band,d/p-band center,electron filling,and valence state.Moreover,the elec-tronic structure of doped/dual-ionic TMCs are adjusted by inducing ions with different electronegativity,electron filling,and ion radius,resulting in electron redistribution,bonds reconstruction,induced vacancies due to the electronic interaction and changed crystal structure such as lat-tice spacing and lattice distortion.Different from the aforementioned two strategies,heterostructures are constructed by two types of TMCs with different Fermi energy levels,which causes built-in electric field and electrons transfer through the interface,and induces electron redistribution and arranged local atoms to regulate the electronic structure.Additionally,the lacking studies of the three strategies to comprehensively regulate electronic structure for improving catalytic performance are pointed out.It is believed that this review can guide the design of advanced TMCs catalysts for boosting redox of lithium sulfur batteries.展开更多
The development of a durable metallic coating on diverse substrates is both intriguing and challenging,particularly in the research of metal-conductive materials for applications such as batteries,soft electronics,and...The development of a durable metallic coating on diverse substrates is both intriguing and challenging,particularly in the research of metal-conductive materials for applications such as batteries,soft electronics,and beyond.Herein,by learning from the pencil-writing process,a facile solid-ink rubbing technology(SIR-tech)is invented to address the above challenge.The solid-ink is exampled by rational combination of liquid metal and graphite particles.By harnessing the synergistic effects between rubbing and adhesion,controllable metallic skin is successfully formed onto metals,woods,ceramics,and plastics without limitation in size and shape.Moreover,outperforming pure liquid-metal coating,the composite metallic skin by SIR-tech is very robust due to the self-lamination of graphite nanoplate exfoliated by liquid-metal rubbing.The critical factors controlling the structures-properties of the composite metallic skin have been systematically investigated as well.For applications,the SIR-tech is demonstrated to fabricate high-performance composite current collectors for next-generation batteries without traditional metal foils.Meanwhile,advanced skin-electrodes are further demonstrated for stable triboelectricity generation even under temperature fluctuation from-196 to 120℃.This facile and highly-flexible SIR-tech may work as a powerful platform for the studies on functional coatings by liquid metals and beyond.展开更多
Lithium metal batteries(LMBs) promise energy density over 400 Wh kg^(-1).However,they suffer severe electrochemical performance deterioration at sub-zero temperatures.Such failure behavior highly correlates to inferio...Lithium metal batteries(LMBs) promise energy density over 400 Wh kg^(-1).However,they suffer severe electrochemical performance deterioration at sub-zero temperatures.Such failure behavior highly correlates to inferior lithium metal anode(LMA) compatibility and sluggish Li^(+) desolvation.Here,we demonstrate that cyclopentylmethyl ether(CPME) based diluted high-concentration electrolyte(DHCE)enables-60℃ LMBs operation.By leveraging the loose coordination between Li^(+) and CPME,such developed electrolyte boosts the formation of ion clusters to derive anion-dominant interfacial chemistry for enhancing LMA compatibility and greatly accelerates Li^(+) desolvation kinetics.The resulting electrolyte demonstrates high Coulombic efficiencies(CE),providing over 99.5%,99.1%,98.5% and 95% at 25,-20,-40,and-60℃respectively.The assembled Li-S battery exhibits remarkable cyclic stability in-20,and-40℃ at 0.2 C charging and 0.5 C discharging.Even at-60℃,Li-S cell with this designed electrolyte retains> 70% of the initial capacity over 170 cycles.Besides,lithium metal coin cell and pouch cell with10 mg cm^(-2) high S cathode loading exhibit cycling stability at-20℃.This work offers an opportunity for rational designing electrolytes toward low temperature LMBs.展开更多
The control of oxygen is paramount in achieving high-performance titanium(Ti)parts by powder metallurgy such as metal in-jection molding(MIM).In this study,we purposely selected the Ti and Ti-6Al-4V powders as the ref...The control of oxygen is paramount in achieving high-performance titanium(Ti)parts by powder metallurgy such as metal in-jection molding(MIM).In this study,we purposely selected the Ti and Ti-6Al-4V powders as the reference materials since these two are the most representative Ti materials in the industry.Herein,hydride-dehydride(HDH)Ti powders were pre-oxidized to examine the ef-fect of oxygen variation on the characteristics of oxide layer on the particle surface and its resultant color feature.The results indicate that the thickness and Ti oxide level(Ti^(0)→Ti^(4+))of the oxide layer on the HDH Ti powders increased as the oxygen content increased,lead-ing to the transition of color appearance from grey,brown to blue.This work aids in the powder feedstock selection at the initial stage in powder metallurgy.In addition,the development of oxygen content was comprehensively studied during the MIM process using the gas-atomized(GA)Ti-6Al-4V powders.Particularly,the oxygen variation in the form of oxide layer,the change of oxygen content in the powders,and the relevant parts were investigated during the processes of kneading,injection,debinding,and sintering.The oxygen vari-ation was mainly concentrated in the sintering stage,and the content increased with the increase of sintering temperature.The variation of oxygen content during the MIM process demonstrates the crucial role of powder feedstock and sintering stage in controlling oxygen con-tent.This work provides a piece of valuable information on oxygen detecting,control,and manipulation for the powder and processing in the industry of Ti and its alloys by powder metallurgy.展开更多
The electrochemical oxidation of 5-hydroxymethylfurfural(HMF) represents a significant avenue for sustainable chemical synthesis, owing to its potential to generate high-value derivatives from biomass feedstocks. Tran...The electrochemical oxidation of 5-hydroxymethylfurfural(HMF) represents a significant avenue for sustainable chemical synthesis, owing to its potential to generate high-value derivatives from biomass feedstocks. Transition metal catalysts offer a cost-effective alternative to precious metals for catalyzing HMF oxidation, with transition bimetallic catalysts emerging as particularly promising candidates. In this review, we delve into the intricate reaction pathways and electrochemical mechanisms underlying HMF oxidation, emphasizing the pivotal role of transition bimetallic catalysts in enhancing catalytic efficiency. Subsequently, various types of transition bimetallic catalysts are explored, detailing their synthesis methods and structural modulation strategies. By elucidating the mechanisms behind catalyst modification and performance enhancement, this review sets the stage for upcoming advancements in the field, ultimately advancing the electrochemical HMF conversion and facilitating the transition towards sustainable chemical production.展开更多
The application of Li metal anodes in rechargeable batteries is impeded by safety issues arising from the severe volume changes and formation of dendritic Li deposits.Three‐dimensional hollow carbon is receiving incr...The application of Li metal anodes in rechargeable batteries is impeded by safety issues arising from the severe volume changes and formation of dendritic Li deposits.Three‐dimensional hollow carbon is receiving increasing attention as a host material capable of accommodating Li metal inside its cavity;however,uncontrollable and nonuniform deposition of Li remains a challenge.In this study,we synthesize metal–organic framework‐derived carbon microcapsules with heteroatom clusters(Zn and Ag)on the capsule walls and it is demonstrated that Ag‐assisted nucleation of Li metal alters the outward‐to‐inward growth in the microcapsule host.Zn‐incorporated microcapsules are prepared via chemical etching of zeolitic imidazole framework‐8 polyhedra and are subsequently decorated with Ag by a galvanic displacement reaction between Ag^(+) and metallic Zn.Galvanically introduced Ag significantly reduces the energy barrier and increases the reaction rate for Li nucleation in the microcapsule host upon Li plating.Through combined electrochemical,microstructural,and computational studies,we verify the beneficial role of Ag‐assisted Li nucleation in facilitating inward growth inside the cavity of the microcapsule host and,in turn,enhancing electrochemical performance.This study provides new insights into the design of reversible host materials for practical Li metal batteries.展开更多
Copper possesses very strong chacophile properties,but under the conditions found in meteorites,its behavior is like that of siderophile elements.The Suizhou meteorite is a highly shocked L6 chondrite.Troilite and tae...Copper possesses very strong chacophile properties,but under the conditions found in meteorites,its behavior is like that of siderophile elements.The Suizhou meteorite is a highly shocked L6 chondrite.Troilite and taenite are considered the main primary carrier of copper in this meteorite,and the post-shock thermal episode is considered the main reason that elemental Cu migrates from its original host phase and forms metallic grains.The Suizhou meteorite contains a few very thin shock melt veins.The occurrence and behavior of metallic copper in this meteorite were studied by optical microscopic examination,electron microprobe analyses,and high-resolution X-ray elemental intensity mapping.Our results show that metallic copper is abundant in the Suizhou chondritic rock.Metallic copper grains adjacent to small troilite grains inside FeNi metal are the most common occurrence,and those at the FeNi metal–troilite interface are the second most common case.The metallic copper grains occurring at the interface of FeNi metal/troililte and silicate are rather rare.Metallic copper grains are not observed within the Suizhou shock veins,Instead,Cu in elemental form is transferred through shock metamorphism into FeNi metal+troilite intergrowths.Four diff erent occurrence types of Cu in the FeNi metal+troilite intergrowths have been identifi ed:the concentrations of Cu in the FeNi+FeS intergrowths for four occurrence types are rather close,we estimate it might be lower than 1 wt%.展开更多
Solid-state polymer electrolytes(SPEs)are candidate schemes for meeting the safety and energy density needs of advanced lithium-based battery because of their improved mechanical and electrochemical stability compared...Solid-state polymer electrolytes(SPEs)are candidate schemes for meeting the safety and energy density needs of advanced lithium-based battery because of their improved mechanical and electrochemical stability compared to traditional liquid electrolytes.However,low ionic conductivity and side reactions occurring in traditional high-voltage lithium metal batteries(LMBs)hinder their practical applications.Here,amino-modified metal-organic frameworks(UiO-66-NH_(2))with abundant defects as multifunctional fillers in the polyurethane based SPEs achieve the collaborative promotion of the mechanical strength and room temperature ionic conductivity.The surface modified amino groups serve as anchoring points for oxygen atoms of polymer chains,forming a firmly hydrogen-bond interface with polycarbonate-based polyurethane frameworks.The rich interfaces between UiO-66-NH_(2) and polymers dramatically decrease the crystallization of polymer chains and reduce ion transport impedance,which markedly boosted the ionic conductivity to 2.1×10^(−4) S·cm^(−1) with a high Li+transference numbers of 0.71.As a result,LiFePO4∣SPEs∣Li cells exhibit prominent cyclability for 700 cycles under 0.5 C with 96.5%capacity retention.The LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)∣SPEs∣Li cells deliver excellent long-term lifespan for 260 cycles with a high capacity retention of 91.9%and high average Coulombic efficiency(98.5%)under ambient conditions.This simple and effective hybrid SPE design strategy sheds a milestone significance light for high-voltage Li-metal batteries.展开更多
Dry reforming of methane (DRM) can simultaneously convert two critical greenhouse gases CH4 and CO_(2) into high-value syngas. However, the catalyst deactivation caused by sintering and carbon deposition of Ni-based c...Dry reforming of methane (DRM) can simultaneously convert two critical greenhouse gases CH4 and CO_(2) into high-value syngas. However, the catalyst deactivation caused by sintering and carbon deposition of Ni-based catalysts at high temperature is a significant problem to be solved for DRM industrialization. Herein, we represent a hierarchical Ni-La@S-1 catalyst for DRM reaction, showing high anti-sintering/coke capacity to improve DRM stability. The La and Ni nitrates were first grinded into the pores of SBA-15 followed by N2-treatment;the sample was then recrystallized by a unique template assisted-uniformly dispersed strategy to obtain the hierarchical Ni-La@S-1 catalyst. This strategy achieves uniform encapsulation of stabilized Ni-La bimetallic nanoparticles in S-1 with high loading, exhibiting high DRM activity and stability at 700 °C and 36,000 mL·g^(−1)·h^(−1). Moreover, La addition promoted CO_(2) to form bidentate carbonate, a critical intermediate in DRM, which greatly ameliorated carbon deposition in Ni catalysts. This work offers promising clue for tailoring the industrial DRM catalysts.展开更多
Owning various crystal structures and high theoretical capacity,metal tellurides are emerging as promising electrode materials for high-performance metal-ion batteries(MBs).Since metal telluride-based MBs are quite ne...Owning various crystal structures and high theoretical capacity,metal tellurides are emerging as promising electrode materials for high-performance metal-ion batteries(MBs).Since metal telluride-based MBs are quite new,fundamental issues raise regarding the energy storage mechanism and other aspects affecting electrochemical performance.Severe volume expansion,low intrinsic conductivity and slow ion diffusion kinetics jeopardize the performance of metal tellurides,so that rational design and engineering are crucial to circumvent these disadvantages.Herein,this review provides an in-depth discussion of recent investigations and progresses of metal tellurides,beginning with a critical discussion on the energy storage mechanisms of metal tellurides in various MBs.In the following,recent design and engineering strategies of metal tellurides,including morphology engineering,compositing,defect engineering and heterostructure construction,for high-performance MBs are summarized.The primary focus is to present a comprehensive understanding of the structural evolution based on the mechanism and corresponding effects of dimension control,composition,electron configuration and structural complexity on the electrochemical performance.In closing,outlooks and prospects for future development of metal tellurides are proposed.This work also highlights the promising directions of design and engineering strategies of metal tellurides with high performance and low cost.展开更多
The realization of 100%polarized topologicalWeyl fermions in half-metallic ferromagnets is of particular importance for fundamental research and spintronic applications.Here,we theoretically investigate the electronic...The realization of 100%polarized topologicalWeyl fermions in half-metallic ferromagnets is of particular importance for fundamental research and spintronic applications.Here,we theoretically investigate the electronic and topological properties of the zinc-blende compound VAs,which was deemed as a half-metallic ferromagnet related to dynamic correlations.Based on the combination of density functional theory and dynamical mean field theory,we uncover that the half-metallic ferromagnet VAs exhibits attractive Weyl semimetallic behaviors which are very close to the Fermi level in the DFT+U regime with effect U values ranging from 1.5 eV to 2.5 eV.Meanwhile,we also investigate the magnetization-dependent topological properties;the results show that the change of magnetization directions only slightly affects the positions of Weyl points,which is attributed to the weak spin–orbital coupling effects.The topological surface states of VAs projected on semi-infinite(001)and(111)surfaces are investigated.The Fermi arcs of all Weyl points are clearly visible on the projected Fermi surfaces.Our findings suggest that VAs is a fully spin-polarized Weyl semimetal with many-body correlated effects in the effective U values range from 1.5 eV to 2.5 eV.展开更多
基金Supported by Youth Elite Project of CNNC and Modular HTGR Super-critical Power Generation Technology Collaborative Project between CNNC and Tsinghua University Project of China(Grant No.ZHJTIZYFGWD20201).
文摘For dissimilar metal welds(DMWs)involving nickel-based weld metal(WM)and ferritic heat resistant steel base metal(BM)in power plants,there must be an interface between WM and BM,and this interface suffers mechanical and microstructure mismatches and is often the rupture location of premature failure.In this study,a new form of WM/BM interface form,namely double Y-type interface was designed for the DMWs.Creep behaviors and life of DMWs containing double Y-type interface and conventional I-type interface were compared by finite element analysis and creep tests,and creep failure mechanisms were investigated by stress-strain analysis and microstructure characterization.By applying double Y-type interface instead of conventional I-type interface,failure location of DMW could be shifted from the WM/ferritic heat-affected zone(HAZ)interface into the ferritic HAZ or even the ferritic BM,and the failure mode change improved the creep life of DMW.The interface premature failure of I-type interface DMW was related to the coupling effect of microstructure degradation,stress and strain concentrations,and oxide notch on the WM/HAZ interface.The creep failure of double Y-type interface DMW was the result of Type IV fracture due to the creep voids and micro-cracks on fine-grain boundaries in HAZ,which was a result of the matrix softening of HAZ and lack of precipitate pinning at fine-grain boundaries.The double Y-type interface form separated the stress and strain concentrations in DMW from the WM/HAZ interface,preventing the trigger effect of oxide notch on interface failure and inhibiting the interfacial microstructure cracking.It is a novel scheme to prolong creep life and enhance reliability of DMW,by means of optimizing the interface form,decoupling the damage factors from WM/HAZ interface,and then changing the failure mechanism and shifting the failure location.
基金the financial support from the Australian Research Council,Centre for Materials Science,Queensland University of Technologythe Supported by the Fundamental Research Funds for the Central Universities。
文摘Developing sustainable and clean energy sources(e.g.,solar,wind,and tide energy)is essential to achieve the goal of carbon neutrality.Due to the discontinuous and inco nsistent nature of common clean energy sources,high-performance energy storage technologies are a critical part of achieving this target.Aqueous zinc metal batteries(AZMBs)with inherent safety,low cost,and competitive performance are regarded as one of the promising candidates for grid-scale energy storage.However,zinc metal anodes(ZMAs)with irreversible problems of dendrite growth,hydrogen evolution reaction,self-corrosio n,and other side reactions have seriously hindered the development and commercialization of AZMBs.An increasing number of researchers are focusing on the stability of ZMAs,so assessing the effectiveness of existing research strategies is critical to the development of AZMBs.This review aims to provide a comprehensive overview of the fundamentals and challenges of AZMBs.Resea rch strategies for interfacial modification of ZMAs are systematically presented.The features of artificial interfacial coating and in-situ interfacial coating of ZMAs are compared and discussed in detail,as well as the effect of modified interfacial ZMA on the full-battery performance.Finally,perspectives are provided on the problems and challenges of ZMAs.This review is expected to offer a constructive reference for the further development and commercialization of AZMBs.
基金supported by the National Research Foundation of Korea(NRF)grants funded by the Ministry of Science and ICT(MSIT)(RS-2023-00251283,and 2022M3D1A2083618)by the Ministry of Education(2020R1A6A1A03040516).
文摘Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing performance.However,previous methods of synthesizing MO_(x)/C composites suffer from problems,including inhomogeneity,aggregation,and challenges in micropatterning.Herein,we introduce a refined method that employs a metal–organic framework(MOF)as a precursor combined with direct laser writing.The inherent structure of MOFs ensures a uniform distribution of metal ions and organic linkers,yielding homogeneous MO_(x)/C structures.The laser processing facilitates precise micropatterning(<2μm,comparable to typical photolithography)of the MO_(x)/C crystals.The optimized MOF-derived MO_(x)/C sensor rapidly detected ethanol gas even at room temperature(105 and 18 s for response and recovery,respectively),with a broad range of sensing performance from 170 to 3,400 ppm and a high response value of up to 3,500%.Additionally,this sensor exhibited enhanced stability and thermal resilience compared to previous MOF-based counterparts.This research opens up promising avenues for practical applications in MOF-derived sensing devices.
基金supported by the National Natural Science Foundation of China(22205209,52202373 and U21A200972)China Postdoctoral Science Foundation(2022M722867)Key Research Project of Higher Education Institutions in Henan Province(23A530001)。
文摘The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.
基金supported by the National Natural Science Foundation of China(Nos.12005289 and 52071331)the National Key R&D Program of China(No.2019YFA0210000)the State Key Laboratory of Nuclear Detection and Electronics,University of Science and Technology of China(No.SKLPDE-KF-202316)。
文摘In this study,the interactions between a Ga-based liquid metal,GaInSn,and several metal materials,including pure metals(Ni and Ti)and alloys(316H stainless steel(SS)and GH3535),at 650℃were investigated.The aim was to evaluate the corrosion performance and select a suitable candidate material for use as a molten salt manometer diaphragm in thermal energy storage systems.The results indicated that the alloys(316H SS and GH3535)exhibited less corrosion than pure metals(Ni and Ti)in liquid GaInSn.Ga-rich binary intermetallic compounds were found to form on the surfaces of all the tested metal materials exposed to liquid GaInSn,as a result of the decomposition of liquid GaInSn and its reaction with the constituent elements of the metal materials.The corrosion mechanism for all the tested materials exposed to liquid GaInSn was also investigated and proposed,which may aid in selecting the optimal candidate material when liquid GaInSn is used as the pressure-sensing medium.
基金supported by the Key Research and Development Project of Anhui Province(No.2022a05020048)the Open Project of Anhui Provincial Key Laboratory for Degradation and Monitoring of Pollution of the Environment(No.FSKFKT007D)+2 种基金the State Key Laboratory of Heavy Oil Processing(No.SKLHOP202202007)the Excellent Youth Research Project in Universities of Anhui Province(No.2023AH030050)the University Collaborative Innovation Project of Anhui Province(No.GXXT-2023-034).
文摘The selective oxidation of hydrocarbons can be used to produce oxygen-containing functional compounds such as alcohols, aldehydes or ketones and its efficient and green conversion lies in the development of efficient catalysts that activate C-H bonds and O_(2) simultaneously. In this work, the bimetallic organic framework (CoMnBDC) material with morphology of stacked nanosheets was synthesized using terephthalic acid as ligands to coordinate with Co^(2+) and Mn^(2+) cations under solvothermal conditions. As revealed by spectroscopic characterizations, the electron transfer from Mn to Co in the CoMnBDC resulted in the reduction of the Co average oxidation state and increase of the Mn average oxidation state. The CoMnBDC nanosheets were used as catalyst in catalytic oxidation of ethylbenzene, in which the redox effect promotes the effective electron transfer, the activation of O_(2) and benzyl C-H bond. The 96.2% conversion of ethylbenzene and 98.0% selectivity towards acetophenone could be obtained with oxygen as sole oxidant and solvent-free condition. The excellent catalytic performance is related to the structure of CoMnBDC and is also the best when compared with reported results. Various types of aromatic hydrocarbons containing benzyl C-H bonds can be effectively oxidized by CoMnBDC to produce corresponding ketone products. The density functional theory (DFT) calculation revealed that the redox effect leads to the relative enrichment of electrons on Co in CoMnBDC, which is conducive to the activation of O_(2);Mn with higher oxidation state is beneficial for the adsorption of ethylbenzene and activation of C-H bonds. The CoMnBDC has a lower energy barrier for transition state, making it easier for the ethylbenzene oxidation to produce acetophenone.
基金supported by the National Key Research and Development Programs(2021YFB2400400)Major Science and Technology Innovation Project of Hunan Province(2020GK10102020GK1014-4)+7 种基金National Natural Science Foundation of China(32201162)the 70th general grant of China Postdoctoral Science Foundation(2021M702947)Natural Science Foundation of Henan(232300420404)Key Scientific and Technological Project of Henan Province(232102320290,232102311156)Key Research Project Plan for Higher Education Institutions in Henan Province(24A150009,23B430011)Doctor Foundation of Henan University of Engineering(D2022002)the Science and Technology Innovation Program of Hunan Province(2023RC3154)the scientific research projects of Education Department of Hunan Province(23A0188)。
文摘Aqueous Zn metal batteries(AZMBs)with intrinsic safety,high energy density and low cost have been regarded as promising electrochemical energy storage devices.However,the parasitic reaction on metallic Zn anode and the incompatibility between electrode and electrolytes lead to the deterioration of electrochemical performance of AZMBs during the cycling.The critical point to achieve the stable cycling of AZMBs is to properly regulate the zinc ion solvated structure and transfer behavior between metallic Zn anode and electrolyte.In recent years,numerous achievements have been made to resolve the formation of Zn dendrite and interface incompatible issues faced by AZMBs via optimizing the sheath structure and transport capability of zinc ions at electrode-electrolyte interface.In this review,the challenges for metallic Zn anode and electrode-electrolyte interface in AZMBs including dendrite formation and interface characteristics are presented.Following the influences of different strategies involving designing advanced electrode structu re,artificial solid electrolyte interphase(SEI)on Zn anode and electrolyte engineering to regulate zinc ion solvated sheath structure and transport behavior are summarized and discussed.Finally,the perspectives for the future development of design strategies for dendrite-free Zn metal anode and long lifespan AZMBs are also given.
基金This work is supported by the Technologies R&D Program of Huzhou City(No.2022JB01)the Key Research and Development Program of Zhejiang Province(No.2023C01127)the Highstar Corporation HSD20210118.
文摘The widespread adoption of lithium-ion batteries has been driven by the proliferation of portable electronic devices and electric vehicles,which have increasingly stringent energy density requirements.Lithium metal batteries(LMBs),with their ultralow reduction potential and high theoretical capacity,are widely regarded as the most promising technical pathway for achieving high energy density batteries.In this review,we provide a comprehensive overview of fundamental issues related to high reactivity and migrated interfaces in LMBs.Furthermore,we propose improved strategies involving interface engineering,3D current collector design,electrolyte optimization,separator modification,application of alloyed anodes,and external field regulation to address these challenges.The utilization of solid-state electrolytes can significantly enhance the safety of LMBs and represents the only viable approach for advancing them.This review also encompasses the variation in fundamental issues and design strategies for the transition from liquid to solid electrolytes.Particularly noteworthy is that the introduction of SSEs will exacerbate differences in electrochemical and mechanical properties at the interface,leading to increased interface inhomogeneity—a critical factor contributing to failure in all-solidstate lithium metal batteries.Based on recent research works,this perspective highlights the current status of research on developing high-performance LMBs.
基金financially supported by the Shenzhen Science and Technology Program (Grant No.KQTD20200820113045083,ZDSYS20190902093220279,and JCYJ20220818102403007)the National Natural Science Foundation of China (52201257)the Shenzhen Research Fund for Returned Scholars (DD11409017).
文摘Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and safety.Nonetheless,inherent challenges of deleterious lithium dendrite growth and poor interfacial stability hinder their commercial application.Herein,we report a liquid metal-coated lithium metal(LM@Li)anode strategy to improve the contact between lithium metal and a Li6PS5Cl inorganic electrolyte.The LM@Li symmetric cell shows over 1000 h of stable lithium plating/stripping cycles at 2mA cm^(-2) and a significantly higher critical current density of 9.8 mAcm^(-2) at 25°C.In addition,a full battery assembled with a high-capacity composite LiNbO3@-LiNi_(0.7)Co_(0.2)Mn_(0.1)O_(2)(LNO@NCM721)cathode shows stable cycling performance.Experimental and computational results have demonstrated that dendrite growth tolerance and physical contact in solid-state batteries can be reinforced by using LM interlayers for interfacial modification.
基金The authors acknowledge funding from National Natural Science Foundation of China(52302307)Shaanxi Province(2023-ZDLGY-24,2023-JC-QN-0473)+2 种基金project funded by China Postdoctoral Science Foundation(2023MD734210)the Open Foundation of State Key Laboratory for Advanced Metals and Materials(2022-Z01)Shaanxi Provincial Department of Education industrialization project(21JC018).
文摘Engineering transition metal compounds(TMCs)catalysts with excellent adsorption-catalytic ability has been one of the most effec-tive strategies to accelerate the redox kinetics of sulfur cathodes.Herein,this review focuses on engineering TMCs catalysts by cation doping/anion doping/dual doping,bimetallic/bi-anionic TMCs,and TMCs-based heterostructure composites.It is obvious that introducing cations/anions to TMCs or constructing heterostructure can boost adsorption-catalytic capacity by regulating the electronic structure including energy band,d/p-band center,electron filling,and valence state.Moreover,the elec-tronic structure of doped/dual-ionic TMCs are adjusted by inducing ions with different electronegativity,electron filling,and ion radius,resulting in electron redistribution,bonds reconstruction,induced vacancies due to the electronic interaction and changed crystal structure such as lat-tice spacing and lattice distortion.Different from the aforementioned two strategies,heterostructures are constructed by two types of TMCs with different Fermi energy levels,which causes built-in electric field and electrons transfer through the interface,and induces electron redistribution and arranged local atoms to regulate the electronic structure.Additionally,the lacking studies of the three strategies to comprehensively regulate electronic structure for improving catalytic performance are pointed out.It is believed that this review can guide the design of advanced TMCs catalysts for boosting redox of lithium sulfur batteries.
基金the financial support from the National Natural Science Foundation of China (52125301 and 52203123)the Fundamental Research Funds for the Central Universitiespartially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘The development of a durable metallic coating on diverse substrates is both intriguing and challenging,particularly in the research of metal-conductive materials for applications such as batteries,soft electronics,and beyond.Herein,by learning from the pencil-writing process,a facile solid-ink rubbing technology(SIR-tech)is invented to address the above challenge.The solid-ink is exampled by rational combination of liquid metal and graphite particles.By harnessing the synergistic effects between rubbing and adhesion,controllable metallic skin is successfully formed onto metals,woods,ceramics,and plastics without limitation in size and shape.Moreover,outperforming pure liquid-metal coating,the composite metallic skin by SIR-tech is very robust due to the self-lamination of graphite nanoplate exfoliated by liquid-metal rubbing.The critical factors controlling the structures-properties of the composite metallic skin have been systematically investigated as well.For applications,the SIR-tech is demonstrated to fabricate high-performance composite current collectors for next-generation batteries without traditional metal foils.Meanwhile,advanced skin-electrodes are further demonstrated for stable triboelectricity generation even under temperature fluctuation from-196 to 120℃.This facile and highly-flexible SIR-tech may work as a powerful platform for the studies on functional coatings by liquid metals and beyond.
基金supported by the National Natural Science Foundation of China(Nos.21975087,22008082)。
文摘Lithium metal batteries(LMBs) promise energy density over 400 Wh kg^(-1).However,they suffer severe electrochemical performance deterioration at sub-zero temperatures.Such failure behavior highly correlates to inferior lithium metal anode(LMA) compatibility and sluggish Li^(+) desolvation.Here,we demonstrate that cyclopentylmethyl ether(CPME) based diluted high-concentration electrolyte(DHCE)enables-60℃ LMBs operation.By leveraging the loose coordination between Li^(+) and CPME,such developed electrolyte boosts the formation of ion clusters to derive anion-dominant interfacial chemistry for enhancing LMA compatibility and greatly accelerates Li^(+) desolvation kinetics.The resulting electrolyte demonstrates high Coulombic efficiencies(CE),providing over 99.5%,99.1%,98.5% and 95% at 25,-20,-40,and-60℃respectively.The assembled Li-S battery exhibits remarkable cyclic stability in-20,and-40℃ at 0.2 C charging and 0.5 C discharging.Even at-60℃,Li-S cell with this designed electrolyte retains> 70% of the initial capacity over 170 cycles.Besides,lithium metal coin cell and pouch cell with10 mg cm^(-2) high S cathode loading exhibit cycling stability at-20℃.This work offers an opportunity for rational designing electrolytes toward low temperature LMBs.
基金financially supported by the National Key Research and Development Program of China(No.2021 YFB3701900)the National Natural Science Foundation Program of China(No.51971036)the Open Research Fund of State Key Laboratory of Mesoscience and Engineering(No.MESO-23-D07).
文摘The control of oxygen is paramount in achieving high-performance titanium(Ti)parts by powder metallurgy such as metal in-jection molding(MIM).In this study,we purposely selected the Ti and Ti-6Al-4V powders as the reference materials since these two are the most representative Ti materials in the industry.Herein,hydride-dehydride(HDH)Ti powders were pre-oxidized to examine the ef-fect of oxygen variation on the characteristics of oxide layer on the particle surface and its resultant color feature.The results indicate that the thickness and Ti oxide level(Ti^(0)→Ti^(4+))of the oxide layer on the HDH Ti powders increased as the oxygen content increased,lead-ing to the transition of color appearance from grey,brown to blue.This work aids in the powder feedstock selection at the initial stage in powder metallurgy.In addition,the development of oxygen content was comprehensively studied during the MIM process using the gas-atomized(GA)Ti-6Al-4V powders.Particularly,the oxygen variation in the form of oxide layer,the change of oxygen content in the powders,and the relevant parts were investigated during the processes of kneading,injection,debinding,and sintering.The oxygen vari-ation was mainly concentrated in the sintering stage,and the content increased with the increase of sintering temperature.The variation of oxygen content during the MIM process demonstrates the crucial role of powder feedstock and sintering stage in controlling oxygen con-tent.This work provides a piece of valuable information on oxygen detecting,control,and manipulation for the powder and processing in the industry of Ti and its alloys by powder metallurgy.
基金Hubei Provincial Natural Science Foundation of China (2023AFB0049)Scientific Research Fund Project of Wuhan Institute of Technology (K202232 and K2023028)Graduate Education Innovation Fund of Wuhan Institute of Technology (CX2023091)。
文摘The electrochemical oxidation of 5-hydroxymethylfurfural(HMF) represents a significant avenue for sustainable chemical synthesis, owing to its potential to generate high-value derivatives from biomass feedstocks. Transition metal catalysts offer a cost-effective alternative to precious metals for catalyzing HMF oxidation, with transition bimetallic catalysts emerging as particularly promising candidates. In this review, we delve into the intricate reaction pathways and electrochemical mechanisms underlying HMF oxidation, emphasizing the pivotal role of transition bimetallic catalysts in enhancing catalytic efficiency. Subsequently, various types of transition bimetallic catalysts are explored, detailing their synthesis methods and structural modulation strategies. By elucidating the mechanisms behind catalyst modification and performance enhancement, this review sets the stage for upcoming advancements in the field, ultimately advancing the electrochemical HMF conversion and facilitating the transition towards sustainable chemical production.
基金National Research Foundation,Grant/Award Numbers:NRF‐2018R1A5A1025594,NRF‐2022M3J1A1062644。
文摘The application of Li metal anodes in rechargeable batteries is impeded by safety issues arising from the severe volume changes and formation of dendritic Li deposits.Three‐dimensional hollow carbon is receiving increasing attention as a host material capable of accommodating Li metal inside its cavity;however,uncontrollable and nonuniform deposition of Li remains a challenge.In this study,we synthesize metal–organic framework‐derived carbon microcapsules with heteroatom clusters(Zn and Ag)on the capsule walls and it is demonstrated that Ag‐assisted nucleation of Li metal alters the outward‐to‐inward growth in the microcapsule host.Zn‐incorporated microcapsules are prepared via chemical etching of zeolitic imidazole framework‐8 polyhedra and are subsequently decorated with Ag by a galvanic displacement reaction between Ag^(+) and metallic Zn.Galvanically introduced Ag significantly reduces the energy barrier and increases the reaction rate for Li nucleation in the microcapsule host upon Li plating.Through combined electrochemical,microstructural,and computational studies,we verify the beneficial role of Ag‐assisted Li nucleation in facilitating inward growth inside the cavity of the microcapsule host and,in turn,enhancing electrochemical performance.This study provides new insights into the design of reversible host materials for practical Li metal batteries.
基金supported by Science and Technology Planning Project of Guangdong Province,2023B1212060048.
文摘Copper possesses very strong chacophile properties,but under the conditions found in meteorites,its behavior is like that of siderophile elements.The Suizhou meteorite is a highly shocked L6 chondrite.Troilite and taenite are considered the main primary carrier of copper in this meteorite,and the post-shock thermal episode is considered the main reason that elemental Cu migrates from its original host phase and forms metallic grains.The Suizhou meteorite contains a few very thin shock melt veins.The occurrence and behavior of metallic copper in this meteorite were studied by optical microscopic examination,electron microprobe analyses,and high-resolution X-ray elemental intensity mapping.Our results show that metallic copper is abundant in the Suizhou chondritic rock.Metallic copper grains adjacent to small troilite grains inside FeNi metal are the most common occurrence,and those at the FeNi metal–troilite interface are the second most common case.The metallic copper grains occurring at the interface of FeNi metal/troililte and silicate are rather rare.Metallic copper grains are not observed within the Suizhou shock veins,Instead,Cu in elemental form is transferred through shock metamorphism into FeNi metal+troilite intergrowths.Four diff erent occurrence types of Cu in the FeNi metal+troilite intergrowths have been identifi ed:the concentrations of Cu in the FeNi+FeS intergrowths for four occurrence types are rather close,we estimate it might be lower than 1 wt%.
基金financially supported by the National Natural Science Foundation of China(Nos.52202236 and 5202780089)China Postdoctoral Science Foundation(Nos.2024T170300 and 2022M711232).
文摘Solid-state polymer electrolytes(SPEs)are candidate schemes for meeting the safety and energy density needs of advanced lithium-based battery because of their improved mechanical and electrochemical stability compared to traditional liquid electrolytes.However,low ionic conductivity and side reactions occurring in traditional high-voltage lithium metal batteries(LMBs)hinder their practical applications.Here,amino-modified metal-organic frameworks(UiO-66-NH_(2))with abundant defects as multifunctional fillers in the polyurethane based SPEs achieve the collaborative promotion of the mechanical strength and room temperature ionic conductivity.The surface modified amino groups serve as anchoring points for oxygen atoms of polymer chains,forming a firmly hydrogen-bond interface with polycarbonate-based polyurethane frameworks.The rich interfaces between UiO-66-NH_(2) and polymers dramatically decrease the crystallization of polymer chains and reduce ion transport impedance,which markedly boosted the ionic conductivity to 2.1×10^(−4) S·cm^(−1) with a high Li+transference numbers of 0.71.As a result,LiFePO4∣SPEs∣Li cells exhibit prominent cyclability for 700 cycles under 0.5 C with 96.5%capacity retention.The LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)∣SPEs∣Li cells deliver excellent long-term lifespan for 260 cycles with a high capacity retention of 91.9%and high average Coulombic efficiency(98.5%)under ambient conditions.This simple and effective hybrid SPE design strategy sheds a milestone significance light for high-voltage Li-metal batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.21776311,22102215,and 22372197)the Natural Science Foundation of Shandong Province,China(No.ZR2023MB101)+4 种基金the Fundamental Research Funds for the Central Universities(Nos.22CX03001A and 21CX06013A)the Taishan Scholar Foundation of Shandong Province(Nos.tspd20210308 and tsqnz20221119)the “111” Program of National College Disciplinary Innovation(No.B13031)the Special Program for Basic Researc of CNPC(No.2023ZZ36)the College Students’ Innovative Entrepreneurial Training Plan Program(No.202403018CX).
文摘Dry reforming of methane (DRM) can simultaneously convert two critical greenhouse gases CH4 and CO_(2) into high-value syngas. However, the catalyst deactivation caused by sintering and carbon deposition of Ni-based catalysts at high temperature is a significant problem to be solved for DRM industrialization. Herein, we represent a hierarchical Ni-La@S-1 catalyst for DRM reaction, showing high anti-sintering/coke capacity to improve DRM stability. The La and Ni nitrates were first grinded into the pores of SBA-15 followed by N2-treatment;the sample was then recrystallized by a unique template assisted-uniformly dispersed strategy to obtain the hierarchical Ni-La@S-1 catalyst. This strategy achieves uniform encapsulation of stabilized Ni-La bimetallic nanoparticles in S-1 with high loading, exhibiting high DRM activity and stability at 700 °C and 36,000 mL·g^(−1)·h^(−1). Moreover, La addition promoted CO_(2) to form bidentate carbonate, a critical intermediate in DRM, which greatly ameliorated carbon deposition in Ni catalysts. This work offers promising clue for tailoring the industrial DRM catalysts.
基金supported by the International Collaboration Program of Jilin Provincial Department of Science and Technology,China(20230402051GH)the National Natural Science Foundation of China(51932003,51902050)+2 种基金the Open Project Program of Key Laboratory of Preparation and Application of Environmental friendly Materials(Jilin Normal University)of Ministry of China(2021006)the Fundamental Research Funds for the Central Universities JLU“Double-First Class”Discipline for Materials Science&Engineering。
文摘Owning various crystal structures and high theoretical capacity,metal tellurides are emerging as promising electrode materials for high-performance metal-ion batteries(MBs).Since metal telluride-based MBs are quite new,fundamental issues raise regarding the energy storage mechanism and other aspects affecting electrochemical performance.Severe volume expansion,low intrinsic conductivity and slow ion diffusion kinetics jeopardize the performance of metal tellurides,so that rational design and engineering are crucial to circumvent these disadvantages.Herein,this review provides an in-depth discussion of recent investigations and progresses of metal tellurides,beginning with a critical discussion on the energy storage mechanisms of metal tellurides in various MBs.In the following,recent design and engineering strategies of metal tellurides,including morphology engineering,compositing,defect engineering and heterostructure construction,for high-performance MBs are summarized.The primary focus is to present a comprehensive understanding of the structural evolution based on the mechanism and corresponding effects of dimension control,composition,electron configuration and structural complexity on the electrochemical performance.In closing,outlooks and prospects for future development of metal tellurides are proposed.This work also highlights the promising directions of design and engineering strategies of metal tellurides with high performance and low cost.
基金the National Natural Science Foun-dation of China(Grant Nos.12204074,12222402,92365101,and 12347101)the Natural Science Foundation of Chong-ging(Grant No.CSTB2023NSCQ-JQX0024).
文摘The realization of 100%polarized topologicalWeyl fermions in half-metallic ferromagnets is of particular importance for fundamental research and spintronic applications.Here,we theoretically investigate the electronic and topological properties of the zinc-blende compound VAs,which was deemed as a half-metallic ferromagnet related to dynamic correlations.Based on the combination of density functional theory and dynamical mean field theory,we uncover that the half-metallic ferromagnet VAs exhibits attractive Weyl semimetallic behaviors which are very close to the Fermi level in the DFT+U regime with effect U values ranging from 1.5 eV to 2.5 eV.Meanwhile,we also investigate the magnetization-dependent topological properties;the results show that the change of magnetization directions only slightly affects the positions of Weyl points,which is attributed to the weak spin–orbital coupling effects.The topological surface states of VAs projected on semi-infinite(001)and(111)surfaces are investigated.The Fermi arcs of all Weyl points are clearly visible on the projected Fermi surfaces.Our findings suggest that VAs is a fully spin-polarized Weyl semimetal with many-body correlated effects in the effective U values range from 1.5 eV to 2.5 eV.