Single metal atoms anchored on nitrogen-doped carbon materials(M-N_(4))have been identified as effective active sites for catalyzing the two-electron oxygen reduction reaction(2e-ORR).However,the relationship between ...Single metal atoms anchored on nitrogen-doped carbon materials(M-N_(4))have been identified as effective active sites for catalyzing the two-electron oxygen reduction reaction(2e-ORR).However,the relationship between the local atomic/electronic environments of the M-N_(4) sites(metal atoms coordinated with different types of N species)and their catalytic activity for 2e-ORR has rarely been elaborated clearly,which imposes significant ambiguity for the rational design of catalysts.Herein,guided by the comprehensive density-functional theory calculations and predictions,a series of Zn-N_(4) single-atom catalysts(SACs)are designed with pyrrole/pyridine-N(N_(Po)/N_(Pd))synergistic coordination and prepared by controlling the pyrolysis temperature(600,700,and 800℃),Among them,the dominated Zn-N_(4) configurations with rationally combined N_(Po)/N_(Pd)coordination show~*OOH adsorption strength close to the optimal value,much superior to those with mono N species.Thus,the as-prepared catalyst exhibits a high H_(2)O_(2) selectivity of over 90%both in neutral and alkaline environments,with a superb H_(2)O_(2) yield of up to 33.63 mol g^(-1)h^(-1)in an alkaline with flow cell.More importantly,a new descriptor,dz^(2)+s band center,has been proposed,which is especially feasible for predicting the activity for metal types with fully occupied s and d orbitals.This work thus presents clear guidance for the rational design of highly active SACs toward ORR and provides a complement to the d-band theory for more accurately predicting the catalytic activity of the materials.展开更多
Fluorine owing to its inherently high electronegativity exhibits charge delocalization and ion dissociation capabilities;as a result,there has been an influx of research studies focused on the utilization of fluorides...Fluorine owing to its inherently high electronegativity exhibits charge delocalization and ion dissociation capabilities;as a result,there has been an influx of research studies focused on the utilization of fluorides to optimize solid electrolyte interfaces and provide dynamic protection of electrodes to regulate the reaction and function performance of batteries.Nonetheless,the shuttle effect and the sluggish redox reaction kinetics emphasize the potential bottlenecks of lithium-sulfur batteries.Whether fluorine modulation regulate the reaction process of Li-S chemistry?Here,the TiOF/Ti_(3)C_(2)MXene nanoribbons with a tailored F distribution were constructed via an NH4F fluorinated method.Relying on in situ characterizations and electrochemical analysis,the F activates the catalysis function of Ti metal atoms in the consecutive redox reaction.The positive charge of Ti metal sites is increased due to the formation of O-Ti-F bonds based on the Lewis acid-base mechanism,which contributes to the adsorption of polysulfides,provides more nucleation sites and promotes the cleavage of S-S bonds.This facilitates the deposition of Li_(2)S at lower overpotentials.Additionally,fluorine has the capacity to capture electrons originating from Li_(2)S dissolution due to charge compensation mechanisms.The fluorine modulation strategy holds the promise of guiding the construction of fluorine-based catalysts and facilitating the seamless integration of multiple consecutive heterogeneous catalytic processes.展开更多
Ni-rich layered oxide cathodes have shown promise for high-energy lithium-ion batteries(LIBs)but are usually limited to mild environments because of their rapid performance degradation under extreme temperature condit...Ni-rich layered oxide cathodes have shown promise for high-energy lithium-ion batteries(LIBs)but are usually limited to mild environments because of their rapid performance degradation under extreme temperature conditions(below0°C and above 50 °C).Here,we report the design of F/Mo co-doped LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(FMNCM)cathode for high-performance LIBs from-20 to 60°C.F^(-) doping with high electronegativity into the cathode surface is found to enhance the stability of surface lattice structure and protect the interface from side reactions with the electrolyte by generating a LiF-rich surface layer.Concurrently,the Mo^(6+) doping suppresses phase transition,which blocks Li^(+)/Ni^(2+) mixing,and stabilizes lithium-ion diffusion pathway.Remarkably,the FMNCM cathode demonstrates excellent cycling stability at a high cutoff voltage of 4.4 V,even at 60°C,maintaining 90.6%capacity retention at 3 C after 150 cycles.Additionally,at temperatures as low as-20°C,it retains 77.1%of its room temperature capacity,achieving an impressive 97.5%capacity retention after 500 cycles.Such stable operation under wide temperatures has been further validated in practical Ah-level pouch-cells.This study sheds light on both fundamental mechanisms and practical implications for the design of advanced cathode materials for wide-temperature LIBs,presenting a promising path towards high-energy and long-cycling LIBs with temperatureadaptability.展开更多
Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the ...Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the catalyst design strategies for preparing the Ni supported on ZSM-5 zeolite catalysts to promote ESR.Specifically,two-dimensional ZSM-5 nanosheet and conventional ZSM-5 crystal were used as the catalyst carriers and two synthesis strategies,i.e.,in situ encapsulation and wet impregnation method,were employed to prepare the catalysts.Based on the comparative characterization of the catalysts and comparative catalytic assessments,it was found that the combination of the in situ encapsulation synthesis and the ZSM-5 nanosheet carrier was the effective strategy to develop catalysts for promoting H_(2) production via ESR due to the improved mass transfer(through the 2-D structure of ZSM-5 nanosheet)and formation of confined small Ni nanoparticles(resulted via the in situ encapsulation synthesis).In addition,the resulting ZSM-5 nanosheet supported Ni catalyst also showed high Ni dispersion and high accessibility to Ni sites by the reactants,being able to improve the activity and stability of catalysts and suppress metal sintering and coking during ESR at high reaction temperatures.Thus,the Ni supported on ZSM-5 nanosheet catalyst prepared by encapsulation showed the stable performance with~88% ethanol conversion and~65% H_(2) yield achieved during a 48-h longevity test at 550-C.展开更多
Solar steam generation(SSG)is widely regarded as one of the most sustainable technologies for seawater desalination.However,salt fouling severely compromises the evaporation performance and lifetime of evaporators,lim...Solar steam generation(SSG)is widely regarded as one of the most sustainable technologies for seawater desalination.However,salt fouling severely compromises the evaporation performance and lifetime of evaporators,limiting their practical applications.Herein,we propose a hierarchical salt-rejection(HSR)strategy to prevent salt precipitation during long-term evaporation while maintaining a rapid evaporation rate,even in high-salinity brine.The salt diffusion process is segmented into three steps—insulation,branching diffusion,and arterial transport—that significantly enhance the salt-resistance properties of the evaporator.Moreover,the HSR strategy overcomes the tradeoff between salt resistance and evaporation rate.Consequently,a high evaporation rate of 2.84 kg m^(-2) h^(-1),stable evaporation for 7 days cyclic tests in 20 wt%NaCl solution,and continuous operation for 170 h in natural seawater under 1 sun illumination were achieved.Compared with control evaporators,the HSR evaporator exhibited a>54%enhancement in total water evaporation mass during 24 h continuous evaporation in 20 wt%salt water.Furthermore,a water collection device equipped with the HSR evaporator realized a high water purification rate(1.1 kg m^(-2) h^(-1)),highlighting its potential for agricultural applications.展开更多
Nanocarbon materials play a critical role in the development of new or improved technologies and devices for sustainable production and use of renewable energy. This perspective paper defines some of the trends and ou...Nanocarbon materials play a critical role in the development of new or improved technologies and devices for sustainable production and use of renewable energy. This perspective paper defines some of the trends and outlooks in this exciting area, with the effort of evidencing some of the possibilities offered from the growing level of knowledge, as testified from the exponentially rising number of publications, and putting bases for a more rational design of these nanomaterials. The basic members of the new carbon family are fullerene, graphene, and carbon nanotube. Derived from them are carbon quantum dots, nanohorn, nanofiber, nano ribbon, nanocapsulate, nanocage and other nanomorphologies. Second generation nanocarbons are those which have been modified by surface functionalization or doping with heteroatoms to create specific tailored properties. The third generation of nanocarbons is the nanoarchitectured supramolecular hybrids or composites of the first and second genera- tion nanocarbons, or with organic or inorganic species. The advantages of the new carbon materials, relating to the field of sustainable energy, are discussed, evidencing the unique properties that they offer for developing next generation solar devices and energy storage solutions.展开更多
CoMn layered double hydroxides(CoMn-LDH)are promising electrode materials for supercapacitors because of their excellent cyclic stability.However,they possess relatively low capacitances.In this work,hybrid CoMn-LDH@M...CoMn layered double hydroxides(CoMn-LDH)are promising electrode materials for supercapacitors because of their excellent cyclic stability.However,they possess relatively low capacitances.In this work,hybrid CoMn-LDH@MnO2 products grown on Ni foams were obtained through a facile hydrothermal method.The as-synthesized samples employed as electrodes deliver a specific capacitance of 2325.01 F g^-1 at 1 A g^-1.An assembled asymmetric supercapacitor using these products as positive electrodes shows a maximum energy density of 59.73 W h kg^-1 at 1000.09 W kg^-1.The prominent electrochemical performance of the as-prepared electrodes could be attributes to hierarchical structures.These findings suggest that hybrid structures might be potential alternatives for future flexible energy storage devices.展开更多
Vanadium pentoxide （V205） exhibits high theoretical capacities when used as a cathode in lithium ion batteries （LIBs）, but its application is limited by its structural instability as well as its low lithium and el...Vanadium pentoxide （V205） exhibits high theoretical capacities when used as a cathode in lithium ion batteries （LIBs）, but its application is limited by its structural instability as well as its low lithium and electronic conductivities. A porous composite of V2Os-SnO2/carbon nanotubes （CNTs） was prepared by a hydrothermal method and followed by thermal treatment. The small particles of V205, their porous structure and the coexistence of SnO2 and CNTs can all facilitate the diffusion rates of the electrons and lithium ions. Electrochemical impedance spectra indicated higher ionic and electric conductivities, as compared to commercial V205. The VzOs-SnOz/CNTs composite gave a reversible discharge capacity of 198 mAh.g- 1 at the voltage range of 2.05-4.0 V, measured at a current rate of 200 mA.g-1, while that of the commercial V205 was only 88 mAh.g-1, demonstrating that the porous V2Os-SnOz/CNTs composite is a promising candidate for high-performance lithium secondary batteries.展开更多
Room temperature sodium–sulfur(RT Na-S)battery with high theoretical energy density and low cost has spurred tremendous interest,which is recognized as an ideal candidate for large-scale energy storage applications.H...Room temperature sodium–sulfur(RT Na-S)battery with high theoretical energy density and low cost has spurred tremendous interest,which is recognized as an ideal candidate for large-scale energy storage applications.However,serious sodium polysulfide shutting and sluggish reaction kinetics lead to rapid capacity decay and poor Coulombic efficiency.Recently,catalytic materials capable of adsorbing and catalyzing the conversion of polysulfides are profiled as a promising method to improve electrochemical performance.In this review,the research progress is summarized that the application of catalytic materials in RT Na-S battery.For the role of catalyst on the conversion of sulfur species,specific attention is focused on the influence factors of reaction rate during different redox processes.Various catalytic materials based on lightweight and high conductive carbon materials,including heteroatom-doped carbon,metals and metal compounds,single-atom and heterostructure,promote the reaction kinetic via lowered energy barrier and accelerated charge transfer.Additionally,the adsorption capacity of the catalytic materials is the key to the catalytic effect.Particular attention to the interaction between polysulfides and sulfur host materials is necessary for the exploration of catalytic mechanism.Lastly,the challenges and outlooks toward the desired design of efficient catalytic materials for RT Na-S battery are discussed.展开更多
With the implementation of new-generation launch vehicles,space stations,lunar and deep space exploration,etc.,the development of spacecraft structures will face new challenges. In order to reduce the spacecraft weigh...With the implementation of new-generation launch vehicles,space stations,lunar and deep space exploration,etc.,the development of spacecraft structures will face new challenges. In order to reduce the spacecraft weight and increase the payload,composite material structures will be widely used. It is difficult to evaluate the strength and life of composite materials due to their complex mechanism and various phenomena in damage and failure.Meanwhile,the structures of composite materials used in spacecrafts will bear complex loads,including the coupling loads of tension,pressure,bending,shear,and torsion. Static loads,thermal loads,and vibration loads may occur at the same time,which asks for verification requirements to ensure the structure safety. Therefore,it is necessary to carry out a systematic multi-level experimental study. In this paper,the building block approach (BBA) is used to investigate the multilevel composite material structures for spacecrafts. The advanced measurement technology is adopted based on digital image correlation (DIC) and piezoelectric and optical fiber sensors to measure the composite material structure deformation. The virtual experiment technology is applied to provide sufficient and reliable data for the evaluation of the composite material structures of spacecrafts.展开更多
The additive manufacturing(AM)of Ni-based superalloys has attracted extensive interest from both academia and industry due to its unique capabilities to fabricate complex and high-performance components for use in hig...The additive manufacturing(AM)of Ni-based superalloys has attracted extensive interest from both academia and industry due to its unique capabilities to fabricate complex and high-performance components for use in high-end industrial systems.However,the intense temperature gradient induced by the rapid heating and cooling processes of AM can generate high levels of residual stress and metastable chemical and structural states,inevitably leading to severe metallurgical defects in Ni-based superalloys.Cracks are the greatest threat to these materials’integrity as they can rapidly propagate and thereby cause sudden and non-predictable failure.Consequently,there is a need for a deeper understanding of residual stress and cracking mechanisms in additively manufactured Ni-based superalloys and ways to potentially prevent cracking,as this knowledge will enable the wider application of these unique materials.To this end,this paper comprehensively reviews the residual stress and the various mechanisms of crack formation in Ni-based superalloys during AM.In addition,several common methods for inhibiting crack formation are presented to assist the research community to develop methods for the fabrication of crack-free additively manufactured components.展开更多
Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity...Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity towards 2e^(-)-ORR due to their unique electronic structures and geometrical configurations.The very low density of single-atom active centers,however,often leads to unsatisfactory H_(2)O_(2)yield rate,significantly inhibiting their practical feasibility.Addressing this,we herein introduce fluorine as a secondary doping element into conventional SACs,which does not directly coordinate with the singleatom metal centers but synergize with them in a remote manner.This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e^(-)-ORR.Consequently,a record-high H_(2)O_(2)yield rate up to 27 mol g^(-1)h^(-1)has been achieved on the Mo–F–C catalyst,with high Faradaic efficiency of 90%.Density functional theory calculations further confirm the very kinetically facile 2e^(-)-ORR over these additional active sites and the superiority of Mo as the single-atom center to others.This strategy thus not only provides a high-performance electrocatalyst for 2e^(-)-ORR but also should shed light on new strategies to significantly increase the active centers number of SACs.展开更多
Piezoelectricity in native bones has been well recognized as the key factor in bone regeneration.Thus,bio-piezoelectric materials have gained substantial attention in repairing damaged bone by mimicking the tissue’s ...Piezoelectricity in native bones has been well recognized as the key factor in bone regeneration.Thus,bio-piezoelectric materials have gained substantial attention in repairing damaged bone by mimicking the tissue’s electrical microenvironment(EM).However,traditional manufacturing strategies still encounter limitations in creating personalized bio-piezoelectric scaffolds,hindering their clinical applications.Three-dimensional(3D)/four-dimensional(4D)printing technology based on the principle of layer-by-layer forming and stacking of discrete materials has demonstrated outstanding advantages in fabricating bio-piezoelectric scaffolds in a more complex-shaped structure.Notably,4D printing functionality-shifting bio-piezoelectric scaffolds can provide a time-dependent programmable tissue EM in response to external stimuli for bone regeneration.In this review,we first summarize the physicochemical properties of commonly used bio-piezoelectric materials(including polymers,ceramics,and their composites)and representative biological findings for bone regeneration.Then,we discuss the latest research advances in the 3D printing of bio-piezoelectric scaffolds in terms of feedstock selection,printing process,induction strategies,and potential applications.Besides,some related challenges such as feedstock scalability,printing resolution,stress-to-polarization conversion efficiency,and non-invasive induction ability after implantation have been put forward.Finally,we highlight the potential of shape/property/functionality-shifting smart 4D bio-piezoelectric scaffolds in bone tissue engineering(BTE).Taken together,this review emphasizes the appealing utility of 3D/4D printed biological piezoelectric scaffolds as next-generation BTE implants.展开更多
The keen interest in fuel cells and metal-air batteries stimulates a great deal of research on the development of a cost-efficient and high-performance catalyst as an alternative to traditional Pt to boost the sluggis...The keen interest in fuel cells and metal-air batteries stimulates a great deal of research on the development of a cost-efficient and high-performance catalyst as an alternative to traditional Pt to boost the sluggish oxygen reduction reaction(ORR)at the cathode.Herein,we report a facile and scalable strategy for the large-scale preparation of a free-standing and flexible porous atomically dispersed Fe-N-doped carbon microtube(FeSAC/PCMT)sponge.Benefiting from its unique structure that greatly facilitates the catalytic kinetics,mass transport,and electron transfer,our FeSAC/PCMT electrode exhibits excellent performance with an ORR potential of 0.942 V at^(-3) mA cm^(-2).When the FeSAC/PCMT sponge was directly used as an oxygen electrode for liquid-state and flexible solid-state zinc-air batteries,high peak power densities of 183.1 and 58.0 mW cm^(-2) were respectively achieved,better than its powdery counterpart and commercial Pt/C catalyst.Experimental and theoretical investigation results demonstrate that such ultrahigh ORR performance can be attributed to atomically dispersed Fe-N_(5) species in FeSAC/PCMT.This study presents a cost-effective and scalable strategy for the fabrication of highly efficient and flexible oxygen electrodes,provides a significant new insight into the catalytic mechanisms,and helps to realize significant advances in energy devices.展开更多
The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for...The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for converting CO_(2)into valuable chemicals and fuels.These conversions have the potential to establish a closed artificial carbon cycle and provide an alternative resource to depleting fossil fuels.Among the various conversion routes,thermochemical CO_(2)reduction stands out as a promising candidate for industrialization.Within the realm of heterogeneous catalysis,single atom catalysts(SACs)have garnered significant attention.The utilization of SACs offers tremendous potential for enhancing catalytic performance.To achieve optimal activity and selectivity of SACs in CO_(2)thermochemical reduction reactions,a comprehensive understanding of key factors such as single atom metal-support interactions,chemical coordination,and accessibility of active sites is crucial.Despite extensive research in this field,the atomic-scale reaction mechanisms in different chemical environments remain largely unexplored.While SACs have been found successful applications in electrochemical and photochemical CO_(2)reduction reactions,their implementation in thermochemical CO_(2)reduction encounters challenges due to the sintering and/or agglomeration effects that occur at elevated temperatures.In this review,we present a unique approach that combines theoretical understanding with experimental strategies to guide researchers in the design of controlled and thermally stable SACs.By elucidating the underlying principles,we aim to enable the creation of SACs that exhibit stable and efficient catalytic activity for thermochemical CO_(2)reduction reactions.Subsequently,we provide a comprehensive overview of recent literature on noble metal-and transition metal-based SACs for thermochemical CO_(2)reduction.The current review is focused on certain CO_(2)-derived products involving one step reduction only for simplicity and for better understanding the SACs enhancement mechanism.We emphasize various synthesis methods employed and highlight the catalytic activity of these SACs.Finally,we delve into the perspectives and challenges associated with SACs in the context of thermochemical CO_(2)reduction reactions,providing valuable insights for future research endeavor.Through this review,we aim to contribute to the advancement of SACs in the field of thermochemical CO_(2)reduction,shedding light on their potential as effective catalysts and addressing the challenges that need to be overcome for their successful implementation as paradigm shift in catalysis.展开更多
Despite the long tradition of fossil carbon(coal,char,and related carbon-based materials)for fueling mankind,the science of transforming them into chemicals is still demandingly progressing in the current energy scena...Despite the long tradition of fossil carbon(coal,char,and related carbon-based materials)for fueling mankind,the science of transforming them into chemicals is still demandingly progressing in the current energy scenario,especially when considering its responsibilities to the global climate change.Traditionally,there are four routes of preparing chemicals directly from fossil carbon,including hydrogasification,gasification,direct liquefaction,and oxidation,in the macroscope of gas-solid reaction(hydrogasification and gasification)and liquid-solid reaction(direct liquefaction and oxidation).When the study goes to microscale,the gas-solid reaction can be considered as the reaction between the severe condensed radicals and gas,while the liquid-solid reaction is the direct reaction between the radical and the activated-molecule.To have a full overview of the area,this review systematically summarizes the main factors in these processes and shows our own perspectives as follows,(ⅰ)stabilizing the free radicals generated from coal and then directly converting them has the highest efficiency in coal utilization;(ⅱ)the research on the self-catalytic process of coal structure will have a profound impact on the direct preparation of chemicals from fossil carbon.Further discussions are also proposed to guide the future study of the area into a more sustainable direction.展开更多
Organic electrode materials are promising for lithium-ion batteries(LIBs) because of their environmental friendliness and structural diversity.However,they always suffer from limited capacity,poor cycling stability,an...Organic electrode materials are promising for lithium-ion batteries(LIBs) because of their environmental friendliness and structural diversity.However,they always suffer from limited capacity,poor cycling stability,and rate performance.Herein,hexaazatrinaphthalene-based azo-linked hyperbranched polymer(HAHP) is designed and synthesized as a cathode for LIBs.However,the densely stacked morphology lowers the chance of the active sites participating in the redox reaction.To address this issue,the singlewalled carbon nanotube(SWCNT) template is used to induce the growth of nanosized HAHP on the surface of SWCNTs.The HAHP@SWCNT nanocomposites have porous structures and highly accessible active sites.Moreover,the strong π-π interaction between HAHP and highly conductive SWCNTs effectively endows the HAHP@SWCNT nanocomposites with improved cycling stability and fast charge-discharge rates.As a result,the HAHP@SWCNT nanocomposite cathode shows a high specific capacity(320.4 mA h g^(-1)at 100 mA g^(-1)),excellent cycling stability(800 cycles;290 mA h g^(-1)at 100 mA g^(-1),capacity retained 91%) and outstanding rate performance(235 mA h g^(-1)at 2000 mA g^(-1),76% capacity retention versus 50 mA g^(-1)).This work provides a strategy to combine the macromolecular structural design and micromorphology control of electrode materials for obtaining organic polymer cathodes for high-performance LIBs.展开更多
Deformation kink is one of the important strengthening mechanisms of the long-period-stacking-ordered(LPSO)phase containing magnesium(Mg)alloys,while the deformation twin is generally suppressed.To optimize the mechan...Deformation kink is one of the important strengthening mechanisms of the long-period-stacking-ordered(LPSO)phase containing magnesium(Mg)alloys,while the deformation twin is generally suppressed.To optimize the mechanical properties of LPSO containing Mg alloy by simultaneously exciting kink and twin,we successfully prepared the Mg-Zn-Y-Zr alloy featuring intragranular LPSO phase and free grain boundary LPSO phase by homogenization.We unraveled the corresponding strengthening and toughening mechanisms through transmission electron microscopy characterization and theoretical analysis.The high strength and good plasticity of the homogenized alloy benefit from the synergistic deformation mechanism of multiple kinking and twining in the grains.And the activation of kinking and twinning depends on the thicknesses of LPSO lamellae and their relative spacing.These results may shed light on optimizing the design of Mg alloys regulating the microstructure of LPSO phases.展开更多
Passivation by the inorganic-rich solid electrolyte interphase(SEI),especially the LiF-rich SEI,is highly desirable to guarantee the durable lifespan of Li metal batteries(LMBs).Here,we report a diluent with the capab...Passivation by the inorganic-rich solid electrolyte interphase(SEI),especially the LiF-rich SEI,is highly desirable to guarantee the durable lifespan of Li metal batteries(LMBs).Here,we report a diluent with the capability to facilitate the formation of LiF-rich SEI while avoiding the excess consumption of Li salts.Dissimilar to most of reported inert diluents,heptafluoro-l-methoxypropane(HM) is firstly demonstrated to cooperate with the decomposition of anions to generate LiF-rich SEI via releasing Fcontaining species near Li surface.The designed electrolyte consisting of 1.8 M LiFSI in the mixture of1,2-dimethoxyethane(DME)/HM(2:1 by vol.) achieves excellent compatibility with both Li metal anodes(Coulombic efficiency~99.8%) and high-voltage cathodes(4.4 V LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811) and 4.5 V LiCoO_(2)(LCO) vs Li^(+)/Li).The 4.4 V Li(20μm)‖NMC811(2.5 mA h cm^(-2)) and 4.5 V Li(20μm)‖LCO(2.5 mA h cm^(-2)) cells achieve capacity retentions of 80% over 560 cycles and 80% over 505 cycles,respectively.Meanwhile,the anode-free pouch cell delivers an energy density of~293 W h kg^(-1)initially and retains 70% of capacity after 100 deep cycles.This work highlights the critical impact of diluent on the SEI formation,and opens up a new direction for designing desirable interfacial chemistries to enable high-performance LMBs.展开更多
Recently,the family of rare-earth chalcohalides were proposed as candidate compounds to realize the Kitaev spin liquid(KSL)[Chin.Phys.Lett.38047502(2021)].In the present work,we firstly propose an effective spin Hamil...Recently,the family of rare-earth chalcohalides were proposed as candidate compounds to realize the Kitaev spin liquid(KSL)[Chin.Phys.Lett.38047502(2021)].In the present work,we firstly propose an effective spin Hamiltonian consistent with the symmetry group of the crystal structure.Then we apply classical Monte Carlo simulations to preliminarily study the model and establish a phase diagram.When approaching to the low temperature limit,several magnetic long range orders are observed,including the stripe,the zigzag,the antiferromagnetic(AFM),the ferromagnetic(FM),the incommensurate spiral(IS),the multi-Q,and the 120°ones.We further calculate the thermodynamic properties of the system,such as the temperature dependence of the magnetic susceptibility and the heat capacity.The ordering transition temperatures reflected in the two quantities agree with each other.For most interaction regions,the system is magnetically more susceptible in the ab-plane than in the c-direction.The stripe phase is special,where the susceptibility is fairly isotropic in the whole temperature region.These features provide useful information to understand the magnetic properties of related materials.展开更多
基金National Natural Science Foundation of China(No.22379111 and 22179093)。
文摘Single metal atoms anchored on nitrogen-doped carbon materials(M-N_(4))have been identified as effective active sites for catalyzing the two-electron oxygen reduction reaction(2e-ORR).However,the relationship between the local atomic/electronic environments of the M-N_(4) sites(metal atoms coordinated with different types of N species)and their catalytic activity for 2e-ORR has rarely been elaborated clearly,which imposes significant ambiguity for the rational design of catalysts.Herein,guided by the comprehensive density-functional theory calculations and predictions,a series of Zn-N_(4) single-atom catalysts(SACs)are designed with pyrrole/pyridine-N(N_(Po)/N_(Pd))synergistic coordination and prepared by controlling the pyrolysis temperature(600,700,and 800℃),Among them,the dominated Zn-N_(4) configurations with rationally combined N_(Po)/N_(Pd)coordination show~*OOH adsorption strength close to the optimal value,much superior to those with mono N species.Thus,the as-prepared catalyst exhibits a high H_(2)O_(2) selectivity of over 90%both in neutral and alkaline environments,with a superb H_(2)O_(2) yield of up to 33.63 mol g^(-1)h^(-1)in an alkaline with flow cell.More importantly,a new descriptor,dz^(2)+s band center,has been proposed,which is especially feasible for predicting the activity for metal types with fully occupied s and d orbitals.This work thus presents clear guidance for the rational design of highly active SACs toward ORR and provides a complement to the d-band theory for more accurately predicting the catalytic activity of the materials.
基金the financial support provided by the National Natural Science Foundation of China(Nos.51932005,22072164)Liaoning Revitalization Talents Program(No.XLYC1807175)the Research Fund of Shenyang National Laboratory for Materials Science,the Natural Science Foundation of Jilin Province(Nos.YDZJ202301ZYTS280,YDZJ202201ZYTS305,YDZJ202401316ZYTS).
文摘Fluorine owing to its inherently high electronegativity exhibits charge delocalization and ion dissociation capabilities;as a result,there has been an influx of research studies focused on the utilization of fluorides to optimize solid electrolyte interfaces and provide dynamic protection of electrodes to regulate the reaction and function performance of batteries.Nonetheless,the shuttle effect and the sluggish redox reaction kinetics emphasize the potential bottlenecks of lithium-sulfur batteries.Whether fluorine modulation regulate the reaction process of Li-S chemistry?Here,the TiOF/Ti_(3)C_(2)MXene nanoribbons with a tailored F distribution were constructed via an NH4F fluorinated method.Relying on in situ characterizations and electrochemical analysis,the F activates the catalysis function of Ti metal atoms in the consecutive redox reaction.The positive charge of Ti metal sites is increased due to the formation of O-Ti-F bonds based on the Lewis acid-base mechanism,which contributes to the adsorption of polysulfides,provides more nucleation sites and promotes the cleavage of S-S bonds.This facilitates the deposition of Li_(2)S at lower overpotentials.Additionally,fluorine has the capacity to capture electrons originating from Li_(2)S dissolution due to charge compensation mechanisms.The fluorine modulation strategy holds the promise of guiding the construction of fluorine-based catalysts and facilitating the seamless integration of multiple consecutive heterogeneous catalytic processes.
基金the financial support from the National Natural Science Foundation of China(51972156,52072378,52102054 and 51927803)the National Key R&D Program of China(2022YFB3803400,2021YFB3800301)+2 种基金the Shenyang Science and Technology Program(22-322-3-19)the Youth Fund of the Education Department of Liaoning Province(LJKQZ20222324)the Outstanding Youth Fund of University of Science and Technology Liaoning(2023YQ11).
文摘Ni-rich layered oxide cathodes have shown promise for high-energy lithium-ion batteries(LIBs)but are usually limited to mild environments because of their rapid performance degradation under extreme temperature conditions(below0°C and above 50 °C).Here,we report the design of F/Mo co-doped LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(FMNCM)cathode for high-performance LIBs from-20 to 60°C.F^(-) doping with high electronegativity into the cathode surface is found to enhance the stability of surface lattice structure and protect the interface from side reactions with the electrolyte by generating a LiF-rich surface layer.Concurrently,the Mo^(6+) doping suppresses phase transition,which blocks Li^(+)/Ni^(2+) mixing,and stabilizes lithium-ion diffusion pathway.Remarkably,the FMNCM cathode demonstrates excellent cycling stability at a high cutoff voltage of 4.4 V,even at 60°C,maintaining 90.6%capacity retention at 3 C after 150 cycles.Additionally,at temperatures as low as-20°C,it retains 77.1%of its room temperature capacity,achieving an impressive 97.5%capacity retention after 500 cycles.Such stable operation under wide temperatures has been further validated in practical Ah-level pouch-cells.This study sheds light on both fundamental mechanisms and practical implications for the design of advanced cathode materials for wide-temperature LIBs,presenting a promising path towards high-energy and long-cycling LIBs with temperatureadaptability.
基金funding from the European Union's Horizon 2020 Research and Innovation Program(872102)P.S.thanks the Science Achievement Scholarship of Thailand(SAST)for her research secondment at The University of Manchester.Y.J.thanks the National Natural Science Foundation of China(22378407)for funding.
文摘Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the catalyst design strategies for preparing the Ni supported on ZSM-5 zeolite catalysts to promote ESR.Specifically,two-dimensional ZSM-5 nanosheet and conventional ZSM-5 crystal were used as the catalyst carriers and two synthesis strategies,i.e.,in situ encapsulation and wet impregnation method,were employed to prepare the catalysts.Based on the comparative characterization of the catalysts and comparative catalytic assessments,it was found that the combination of the in situ encapsulation synthesis and the ZSM-5 nanosheet carrier was the effective strategy to develop catalysts for promoting H_(2) production via ESR due to the improved mass transfer(through the 2-D structure of ZSM-5 nanosheet)and formation of confined small Ni nanoparticles(resulted via the in situ encapsulation synthesis).In addition,the resulting ZSM-5 nanosheet supported Ni catalyst also showed high Ni dispersion and high accessibility to Ni sites by the reactants,being able to improve the activity and stability of catalysts and suppress metal sintering and coking during ESR at high reaction temperatures.Thus,the Ni supported on ZSM-5 nanosheet catalyst prepared by encapsulation showed the stable performance with~88% ethanol conversion and~65% H_(2) yield achieved during a 48-h longevity test at 550-C.
基金support provided by the Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone Shenzhen Park Project(HZQB-KCZYB-2020030)the Research Grants Council of Hong Kong(Project No:AoE/M-402/20.)+1 种基金the Open Project of Yunnan Precious Metals Laboratory Co.,Ltd(YPML-2023050248)the Hong Kong Innovation and Technology Commission via the Hong Kong Branch of National Precious Metals Material Engineering Research Center.
文摘Solar steam generation(SSG)is widely regarded as one of the most sustainable technologies for seawater desalination.However,salt fouling severely compromises the evaporation performance and lifetime of evaporators,limiting their practical applications.Herein,we propose a hierarchical salt-rejection(HSR)strategy to prevent salt precipitation during long-term evaporation while maintaining a rapid evaporation rate,even in high-salinity brine.The salt diffusion process is segmented into three steps—insulation,branching diffusion,and arterial transport—that significantly enhance the salt-resistance properties of the evaporator.Moreover,the HSR strategy overcomes the tradeoff between salt resistance and evaporation rate.Consequently,a high evaporation rate of 2.84 kg m^(-2) h^(-1),stable evaporation for 7 days cyclic tests in 20 wt%NaCl solution,and continuous operation for 170 h in natural seawater under 1 sun illumination were achieved.Compared with control evaporators,the HSR evaporator exhibited a>54%enhancement in total water evaporation mass during 24 h continuous evaporation in 20 wt%salt water.Furthermore,a water collection device equipped with the HSR evaporator realized a high water purification rate(1.1 kg m^(-2) h^(-1)),highlighting its potential for agricultural applications.
基金the financial support by MOST (2011CBA00504)NSFC (21133010, 50921004, 212111074) of China
文摘Nanocarbon materials play a critical role in the development of new or improved technologies and devices for sustainable production and use of renewable energy. This perspective paper defines some of the trends and outlooks in this exciting area, with the effort of evidencing some of the possibilities offered from the growing level of knowledge, as testified from the exponentially rising number of publications, and putting bases for a more rational design of these nanomaterials. The basic members of the new carbon family are fullerene, graphene, and carbon nanotube. Derived from them are carbon quantum dots, nanohorn, nanofiber, nano ribbon, nanocapsulate, nanocage and other nanomorphologies. Second generation nanocarbons are those which have been modified by surface functionalization or doping with heteroatoms to create specific tailored properties. The third generation of nanocarbons is the nanoarchitectured supramolecular hybrids or composites of the first and second genera- tion nanocarbons, or with organic or inorganic species. The advantages of the new carbon materials, relating to the field of sustainable energy, are discussed, evidencing the unique properties that they offer for developing next generation solar devices and energy storage solutions.
基金supported by the Fundamental Research Funds for the Central Universities (No 30919011410)。
文摘CoMn layered double hydroxides(CoMn-LDH)are promising electrode materials for supercapacitors because of their excellent cyclic stability.However,they possess relatively low capacitances.In this work,hybrid CoMn-LDH@MnO2 products grown on Ni foams were obtained through a facile hydrothermal method.The as-synthesized samples employed as electrodes deliver a specific capacitance of 2325.01 F g^-1 at 1 A g^-1.An assembled asymmetric supercapacitor using these products as positive electrodes shows a maximum energy density of 59.73 W h kg^-1 at 1000.09 W kg^-1.The prominent electrochemical performance of the as-prepared electrodes could be attributes to hierarchical structures.These findings suggest that hybrid structures might be potential alternatives for future flexible energy storage devices.
基金supported by the National Natural Science Foundation of China (No. 51001098)the Institute of Metal Research of CAS (No. 09NBA211A1)
文摘Vanadium pentoxide （V205） exhibits high theoretical capacities when used as a cathode in lithium ion batteries （LIBs）, but its application is limited by its structural instability as well as its low lithium and electronic conductivities. A porous composite of V2Os-SnO2/carbon nanotubes （CNTs） was prepared by a hydrothermal method and followed by thermal treatment. The small particles of V205, their porous structure and the coexistence of SnO2 and CNTs can all facilitate the diffusion rates of the electrons and lithium ions. Electrochemical impedance spectra indicated higher ionic and electric conductivities, as compared to commercial V205. The VzOs-SnOz/CNTs composite gave a reversible discharge capacity of 198 mAh.g- 1 at the voltage range of 2.05-4.0 V, measured at a current rate of 200 mA.g-1, while that of the commercial V205 was only 88 mAh.g-1, demonstrating that the porous V2Os-SnOz/CNTs composite is a promising candidate for high-performance lithium secondary batteries.
基金financial support from National Natural Science Foundation of China(Nos.52020105010,51972313,51927803,52072378,51902316 and 51525206)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA22010602)+2 种基金LiaoNing Revitalization Talents Program(No.XLYC1908015)Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.Y201942)the Special Projects of the Central Government in Guidance of Local Science and Technology Development(No.2020JH6/10500024)。
文摘Room temperature sodium–sulfur(RT Na-S)battery with high theoretical energy density and low cost has spurred tremendous interest,which is recognized as an ideal candidate for large-scale energy storage applications.However,serious sodium polysulfide shutting and sluggish reaction kinetics lead to rapid capacity decay and poor Coulombic efficiency.Recently,catalytic materials capable of adsorbing and catalyzing the conversion of polysulfides are profiled as a promising method to improve electrochemical performance.In this review,the research progress is summarized that the application of catalytic materials in RT Na-S battery.For the role of catalyst on the conversion of sulfur species,specific attention is focused on the influence factors of reaction rate during different redox processes.Various catalytic materials based on lightweight and high conductive carbon materials,including heteroatom-doped carbon,metals and metal compounds,single-atom and heterostructure,promote the reaction kinetic via lowered energy barrier and accelerated charge transfer.Additionally,the adsorption capacity of the catalytic materials is the key to the catalytic effect.Particular attention to the interaction between polysulfides and sulfur host materials is necessary for the exploration of catalytic mechanism.Lastly,the challenges and outlooks toward the desired design of efficient catalytic materials for RT Na-S battery are discussed.
文摘With the implementation of new-generation launch vehicles,space stations,lunar and deep space exploration,etc.,the development of spacecraft structures will face new challenges. In order to reduce the spacecraft weight and increase the payload,composite material structures will be widely used. It is difficult to evaluate the strength and life of composite materials due to their complex mechanism and various phenomena in damage and failure.Meanwhile,the structures of composite materials used in spacecrafts will bear complex loads,including the coupling loads of tension,pressure,bending,shear,and torsion. Static loads,thermal loads,and vibration loads may occur at the same time,which asks for verification requirements to ensure the structure safety. Therefore,it is necessary to carry out a systematic multi-level experimental study. In this paper,the building block approach (BBA) is used to investigate the multilevel composite material structures for spacecrafts. The advanced measurement technology is adopted based on digital image correlation (DIC) and piezoelectric and optical fiber sensors to measure the composite material structure deformation. The virtual experiment technology is applied to provide sufficient and reliable data for the evaluation of the composite material structures of spacecrafts.
基金This work was supported by Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone Shenzhen Park Project:HZQB-KCZYB-2020030the National Natural Science Foundation of China(No.91860131and No.52074157)+2 种基金Guangdong Provincial Department of Science and Technology,Key-Area Research and Development Program of Guangdong Province(No.2020B090923002)the National Key Research and Development Program of China(No.2017YFB0702901)the Shenzhen Science and Technology Innovation Commission(No.JCYJ20170817111811303,No.KQTD20170328154443162and No.ZDSYS201703031748354).
文摘The additive manufacturing(AM)of Ni-based superalloys has attracted extensive interest from both academia and industry due to its unique capabilities to fabricate complex and high-performance components for use in high-end industrial systems.However,the intense temperature gradient induced by the rapid heating and cooling processes of AM can generate high levels of residual stress and metastable chemical and structural states,inevitably leading to severe metallurgical defects in Ni-based superalloys.Cracks are the greatest threat to these materials’integrity as they can rapidly propagate and thereby cause sudden and non-predictable failure.Consequently,there is a need for a deeper understanding of residual stress and cracking mechanisms in additively manufactured Ni-based superalloys and ways to potentially prevent cracking,as this knowledge will enable the wider application of these unique materials.To this end,this paper comprehensively reviews the residual stress and the various mechanisms of crack formation in Ni-based superalloys during AM.In addition,several common methods for inhibiting crack formation are presented to assist the research community to develop methods for the fabrication of crack-free additively manufactured components.
基金supported by the National Natural Science Foundation of China(Nos.22179093 and 21905202)。
文摘Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity towards 2e^(-)-ORR due to their unique electronic structures and geometrical configurations.The very low density of single-atom active centers,however,often leads to unsatisfactory H_(2)O_(2)yield rate,significantly inhibiting their practical feasibility.Addressing this,we herein introduce fluorine as a secondary doping element into conventional SACs,which does not directly coordinate with the singleatom metal centers but synergize with them in a remote manner.This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e^(-)-ORR.Consequently,a record-high H_(2)O_(2)yield rate up to 27 mol g^(-1)h^(-1)has been achieved on the Mo–F–C catalyst,with high Faradaic efficiency of 90%.Density functional theory calculations further confirm the very kinetically facile 2e^(-)-ORR over these additional active sites and the superiority of Mo as the single-atom center to others.This strategy thus not only provides a high-performance electrocatalyst for 2e^(-)-ORR but also should shed light on new strategies to significantly increase the active centers number of SACs.
基金supported by grants from the National Natural Science Foundation of China(52205363)Fundamental Research Funds for the Central Universities(2019kfyRCPY044 and 2021GCRC002)+3 种基金Program for HUST Academic Frontier Youth Team(2018QYTD04)Program for Innovative Research Team of the Ministry of Education(IRT1244)Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone Shenzhen Park Project:HZQB-KCZYB-2020030the Guangdong Provincial Department of Science and Technology(Key-Area Research and Development Program of Guangdong Province)under the Grant 2020B090923002。
文摘Piezoelectricity in native bones has been well recognized as the key factor in bone regeneration.Thus,bio-piezoelectric materials have gained substantial attention in repairing damaged bone by mimicking the tissue’s electrical microenvironment(EM).However,traditional manufacturing strategies still encounter limitations in creating personalized bio-piezoelectric scaffolds,hindering their clinical applications.Three-dimensional(3D)/four-dimensional(4D)printing technology based on the principle of layer-by-layer forming and stacking of discrete materials has demonstrated outstanding advantages in fabricating bio-piezoelectric scaffolds in a more complex-shaped structure.Notably,4D printing functionality-shifting bio-piezoelectric scaffolds can provide a time-dependent programmable tissue EM in response to external stimuli for bone regeneration.In this review,we first summarize the physicochemical properties of commonly used bio-piezoelectric materials(including polymers,ceramics,and their composites)and representative biological findings for bone regeneration.Then,we discuss the latest research advances in the 3D printing of bio-piezoelectric scaffolds in terms of feedstock selection,printing process,induction strategies,and potential applications.Besides,some related challenges such as feedstock scalability,printing resolution,stress-to-polarization conversion efficiency,and non-invasive induction ability after implantation have been put forward.Finally,we highlight the potential of shape/property/functionality-shifting smart 4D bio-piezoelectric scaffolds in bone tissue engineering(BTE).Taken together,this review emphasizes the appealing utility of 3D/4D printed biological piezoelectric scaffolds as next-generation BTE implants.
基金supported by the start-up fund from Kunming University of Science and Technology,the National Natural Science Foundation of China (Grants 52102046,51872293,52130209,52072375)Liaoning Revitalization Talents Program (XLYC2002037)Basic Research Project of Natural Science Foundation of Shandong Province,China (ZR2019ZD49).
文摘The keen interest in fuel cells and metal-air batteries stimulates a great deal of research on the development of a cost-efficient and high-performance catalyst as an alternative to traditional Pt to boost the sluggish oxygen reduction reaction(ORR)at the cathode.Herein,we report a facile and scalable strategy for the large-scale preparation of a free-standing and flexible porous atomically dispersed Fe-N-doped carbon microtube(FeSAC/PCMT)sponge.Benefiting from its unique structure that greatly facilitates the catalytic kinetics,mass transport,and electron transfer,our FeSAC/PCMT electrode exhibits excellent performance with an ORR potential of 0.942 V at^(-3) mA cm^(-2).When the FeSAC/PCMT sponge was directly used as an oxygen electrode for liquid-state and flexible solid-state zinc-air batteries,high peak power densities of 183.1 and 58.0 mW cm^(-2) were respectively achieved,better than its powdery counterpart and commercial Pt/C catalyst.Experimental and theoretical investigation results demonstrate that such ultrahigh ORR performance can be attributed to atomically dispersed Fe-N_(5) species in FeSAC/PCMT.This study presents a cost-effective and scalable strategy for the fabrication of highly efficient and flexible oxygen electrodes,provides a significant new insight into the catalytic mechanisms,and helps to realize significant advances in energy devices.
基金support by Khalifa University through CIRA-2020-077 and RC2-2018-024 grants。
文摘The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for converting CO_(2)into valuable chemicals and fuels.These conversions have the potential to establish a closed artificial carbon cycle and provide an alternative resource to depleting fossil fuels.Among the various conversion routes,thermochemical CO_(2)reduction stands out as a promising candidate for industrialization.Within the realm of heterogeneous catalysis,single atom catalysts(SACs)have garnered significant attention.The utilization of SACs offers tremendous potential for enhancing catalytic performance.To achieve optimal activity and selectivity of SACs in CO_(2)thermochemical reduction reactions,a comprehensive understanding of key factors such as single atom metal-support interactions,chemical coordination,and accessibility of active sites is crucial.Despite extensive research in this field,the atomic-scale reaction mechanisms in different chemical environments remain largely unexplored.While SACs have been found successful applications in electrochemical and photochemical CO_(2)reduction reactions,their implementation in thermochemical CO_(2)reduction encounters challenges due to the sintering and/or agglomeration effects that occur at elevated temperatures.In this review,we present a unique approach that combines theoretical understanding with experimental strategies to guide researchers in the design of controlled and thermally stable SACs.By elucidating the underlying principles,we aim to enable the creation of SACs that exhibit stable and efficient catalytic activity for thermochemical CO_(2)reduction reactions.Subsequently,we provide a comprehensive overview of recent literature on noble metal-and transition metal-based SACs for thermochemical CO_(2)reduction.The current review is focused on certain CO_(2)-derived products involving one step reduction only for simplicity and for better understanding the SACs enhancement mechanism.We emphasize various synthesis methods employed and highlight the catalytic activity of these SACs.Finally,we delve into the perspectives and challenges associated with SACs in the context of thermochemical CO_(2)reduction reactions,providing valuable insights for future research endeavor.Through this review,we aim to contribute to the advancement of SACs in the field of thermochemical CO_(2)reduction,shedding light on their potential as effective catalysts and addressing the challenges that need to be overcome for their successful implementation as paradigm shift in catalysis.
基金supported by National Natural Science Foundation of China(52161145403 and 22072164)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(Grant.YLU-DNL Fund 2022002)。
文摘Despite the long tradition of fossil carbon(coal,char,and related carbon-based materials)for fueling mankind,the science of transforming them into chemicals is still demandingly progressing in the current energy scenario,especially when considering its responsibilities to the global climate change.Traditionally,there are four routes of preparing chemicals directly from fossil carbon,including hydrogasification,gasification,direct liquefaction,and oxidation,in the macroscope of gas-solid reaction(hydrogasification and gasification)and liquid-solid reaction(direct liquefaction and oxidation).When the study goes to microscale,the gas-solid reaction can be considered as the reaction between the severe condensed radicals and gas,while the liquid-solid reaction is the direct reaction between the radical and the activated-molecule.To have a full overview of the area,this review systematically summarizes the main factors in these processes and shows our own perspectives as follows,(ⅰ)stabilizing the free radicals generated from coal and then directly converting them has the highest efficiency in coal utilization;(ⅱ)the research on the self-catalytic process of coal structure will have a profound impact on the direct preparation of chemicals from fossil carbon.Further discussions are also proposed to guide the future study of the area into a more sustainable direction.
基金supported by the National Natural Science Foundation of China(Grant No.51903100)the Science and Technology Development Plan of Jilin Province,China(Grant No.20210402060GH)。
文摘Organic electrode materials are promising for lithium-ion batteries(LIBs) because of their environmental friendliness and structural diversity.However,they always suffer from limited capacity,poor cycling stability,and rate performance.Herein,hexaazatrinaphthalene-based azo-linked hyperbranched polymer(HAHP) is designed and synthesized as a cathode for LIBs.However,the densely stacked morphology lowers the chance of the active sites participating in the redox reaction.To address this issue,the singlewalled carbon nanotube(SWCNT) template is used to induce the growth of nanosized HAHP on the surface of SWCNTs.The HAHP@SWCNT nanocomposites have porous structures and highly accessible active sites.Moreover,the strong π-π interaction between HAHP and highly conductive SWCNTs effectively endows the HAHP@SWCNT nanocomposites with improved cycling stability and fast charge-discharge rates.As a result,the HAHP@SWCNT nanocomposite cathode shows a high specific capacity(320.4 mA h g^(-1)at 100 mA g^(-1)),excellent cycling stability(800 cycles;290 mA h g^(-1)at 100 mA g^(-1),capacity retained 91%) and outstanding rate performance(235 mA h g^(-1)at 2000 mA g^(-1),76% capacity retention versus 50 mA g^(-1)).This work provides a strategy to combine the macromolecular structural design and micromorphology control of electrode materials for obtaining organic polymer cathodes for high-performance LIBs.
基金This work was supported by the National Natural Science Foundation of China(Grant No.52101015,52171021,and 51871222)Natural Science Foundation of Hebei Province(Grant No.E2020208083)Science and Technology Research Project of Colleges and Universities in Hebei Province(Grant No.BJK2022020).
文摘Deformation kink is one of the important strengthening mechanisms of the long-period-stacking-ordered(LPSO)phase containing magnesium(Mg)alloys,while the deformation twin is generally suppressed.To optimize the mechanical properties of LPSO containing Mg alloy by simultaneously exciting kink and twin,we successfully prepared the Mg-Zn-Y-Zr alloy featuring intragranular LPSO phase and free grain boundary LPSO phase by homogenization.We unraveled the corresponding strengthening and toughening mechanisms through transmission electron microscopy characterization and theoretical analysis.The high strength and good plasticity of the homogenized alloy benefit from the synergistic deformation mechanism of multiple kinking and twining in the grains.And the activation of kinking and twinning depends on the thicknesses of LPSO lamellae and their relative spacing.These results may shed light on optimizing the design of Mg alloys regulating the microstructure of LPSO phases.
基金supported by the National Natural Science Foundation of China(22072134,22161142017,and U21A2081)the Natural Science Foundation of Zhejiang Province(LZ21B030002)+2 种基金the Fundamental Research Funds for the Zhejiang Provincial Universities(2021XZZX010)the Fundamental Research Funds for the Central Universities(2021FZZX001-09)“Hundred Talents Program” of Zhejiang University。
文摘Passivation by the inorganic-rich solid electrolyte interphase(SEI),especially the LiF-rich SEI,is highly desirable to guarantee the durable lifespan of Li metal batteries(LMBs).Here,we report a diluent with the capability to facilitate the formation of LiF-rich SEI while avoiding the excess consumption of Li salts.Dissimilar to most of reported inert diluents,heptafluoro-l-methoxypropane(HM) is firstly demonstrated to cooperate with the decomposition of anions to generate LiF-rich SEI via releasing Fcontaining species near Li surface.The designed electrolyte consisting of 1.8 M LiFSI in the mixture of1,2-dimethoxyethane(DME)/HM(2:1 by vol.) achieves excellent compatibility with both Li metal anodes(Coulombic efficiency~99.8%) and high-voltage cathodes(4.4 V LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811) and 4.5 V LiCoO_(2)(LCO) vs Li^(+)/Li).The 4.4 V Li(20μm)‖NMC811(2.5 mA h cm^(-2)) and 4.5 V Li(20μm)‖LCO(2.5 mA h cm^(-2)) cells achieve capacity retentions of 80% over 560 cycles and 80% over 505 cycles,respectively.Meanwhile,the anode-free pouch cell delivers an energy density of~293 W h kg^(-1)initially and retains 70% of capacity after 100 deep cycles.This work highlights the critical impact of diluent on the SEI formation,and opens up a new direction for designing desirable interfacial chemistries to enable high-performance LMBs.
基金Project supported by the National Key Research and Development Program of China (Grant Nos. 2017YFA0302904 and 2016YFA0300504)the National Natural Science Foundation of China (Grant Nos. U1932215, 11774419, 11574392, and 11974421)+4 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDB33010100)the Fundamental Research Funds for the Central Universities,Chinathe Research Funds of Renmin University of China (Grant No. 19XNLG11)the support from Users with Excellence Program of Hefei Science CenterHigh Magnetic Field Facility,CAS
文摘Recently,the family of rare-earth chalcohalides were proposed as candidate compounds to realize the Kitaev spin liquid(KSL)[Chin.Phys.Lett.38047502(2021)].In the present work,we firstly propose an effective spin Hamiltonian consistent with the symmetry group of the crystal structure.Then we apply classical Monte Carlo simulations to preliminarily study the model and establish a phase diagram.When approaching to the low temperature limit,several magnetic long range orders are observed,including the stripe,the zigzag,the antiferromagnetic(AFM),the ferromagnetic(FM),the incommensurate spiral(IS),the multi-Q,and the 120°ones.We further calculate the thermodynamic properties of the system,such as the temperature dependence of the magnetic susceptibility and the heat capacity.The ordering transition temperatures reflected in the two quantities agree with each other.For most interaction regions,the system is magnetically more susceptible in the ab-plane than in the c-direction.The stripe phase is special,where the susceptibility is fairly isotropic in the whole temperature region.These features provide useful information to understand the magnetic properties of related materials.
