Locked segments are high-strength structural elements in fault zones that release significantseismic energy during earthquakes.In fracture mechanics,they act as high-stress concentration patches(asperities)where ruptu...Locked segments are high-strength structural elements in fault zones that release significantseismic energy during earthquakes.In fracture mechanics,they act as high-stress concentration patches(asperities)where rupture initiates.The progressive failure of locked segments along faults plays a crucial role in the energy partition of earthquakes.The impact of locked segments on the near-fielddeformation and nucleation of faults,however,remains poorly understood.In this study,rock-like materials with pre-manufactured strike-slip faults containing various locked segments lengths under uniaxial stress.The mechanical properties,local deformation fields,and slip displacement rates during the uniaxial loading of the models were quantified.Results indicate that the uniaxial compressive strength and elastic modulus of the system peak once the ratio of locked segment to fault length is approximately 0.6.Meanwhile,the resistance of the models to deformation increased,and the failure mode transformed from shear failure to tensile failure.Under loading,compression and dilatation quadrants were formed on both sides of the fault.Large-scale fractures dominate the dilatation quadrants,and the degree of deformation disturbance in this region was significantly higher than that in the compression quadrants.With increasing locked segment length,the amplitude of deformation perturbations decreased after the peak strength.Shorter locked segments were more susceptible to deformation and failure.In the fracture evolution process,a relationship between the stress deflectionangle and the displacement rate was found,which is empirically described by an exponential function.These findings clarify geological structures failure mechanisms and support seismic hazard assessment for strike-slip earthquake regions.展开更多
Although manganese Prussian blue analogues(Mn-PBAs)offer advantages as cost-effective,high-energy-density cathode materials for sodium-ion batteries,their practical application is severely constrained by substantial c...Although manganese Prussian blue analogues(Mn-PBAs)offer advantages as cost-effective,high-energy-density cathode materials for sodium-ion batteries,their practical application is severely constrained by substantial capacity degradation during long-term cycling.This performance deterioration is closely associated with the structural instability of the material during the cycling process,which is mainly attributed to the gradual dissolution of the active material into the electrolyte and severe lattice distortion during Na+intercalation/deintercalation.Fortunately,the aforementioned challenges can be effectively addressed by fabricating an in situ engineered nickel cage(ISE-NC)on Mn-PBAs(denoted as Mn-PBAs-NC).Experimental characterization combined with theoretical calculations reveals that this spontaneously formed nickel cage not only suppresses the diffusion of Mn-PBAs into the electrolyte but also acts as a structural stabilizer,significantly alleviating lattice distortion during cycling.This dual stabilization mechanism ensures remarkable cycling stability,with Mn-PBAs-NC delivering a retained capacity of 96.4 mA h g−1(80%capacity retention)over 2,300 cycles at 2 C,elevating the cycle life of Mn-PBAs to unprecedented levels.展开更多
The adduct 5-carboxylcytosine(5caC),one of the products involved in demethylation pathway,has the potential to serve as a target for specifically deciphering proteins that regulate gene expression and chromatin organi...The adduct 5-carboxylcytosine(5caC),one of the products involved in demethylation pathway,has the potential to serve as a target for specifically deciphering proteins that regulate gene expression and chromatin organization.The fluorescence detection with its ultra-high sensitivity can break through the limitations of traditional detection methods and achieve single molecule detection of 5caC.In this work,the guanine analogue Gr3with largeπ-conjugation and large Stokes shift(89.25 nm)is selected as the fluorescence probe to specifically recognize and monitor 5caC.Because of its bright fluorescence when paired with C and a complete fluorescence quenching when paired with 5caC,this on-off switching feature of Gr3stems from excited-state intermolecular charge transfer.Furthermore,it is found that after linking with deoxyribose,this discriminative function remains unchanged.This strategy could contribute to detecting the presence of 5caC in the genetic material,and thus prevent diseases associated with this epigenetic modification.展开更多
High-moisture meat analogues(HMMAs)offer sustainable protein alternatives to conventional meat and become a research hotspot in recent years.This study systematically investigated the impact of nori powder(NP)incorpor...High-moisture meat analogues(HMMAs)offer sustainable protein alternatives to conventional meat and become a research hotspot in recent years.This study systematically investigated the impact of nori powder(NP)incorporation(0.5%–2.0%)on the physicochemical and structural properties of HMMAs.Rheological analysis revealed that NP reduced the viscosity(consistency coefficient K decreased from 65.67 Pa⋅s to 16.66–19.99 Pa⋅s)and enhanced the fluidity(flow behavior index n increased from 0.25 to 0.33–0.38)of raw material.NP addition progressively decreased the redness values(a*),except for 0.5%NP level.At 1.0%NP level,HMMAs exhibited a denser microstructure with reduced water mobility,resulting in the lowest water holding capacity(2.07 g/g).Conversely,2.0%NP promoted highly oriented fibrous structures,achieving a maximal texturization degree of 1.51.Secondary structure analysis indicated NP facilitated a shift fromα-helix toβ-sheet conformations(β-sheet content increased from 26.06%to 29.92%at 2.0%NP),resulting in stabilized protein networks.These modifications were attributed to NP-induced hydrophobic interactions and polysaccharide-protein crosslinking.The study demonstrates NP's role in modulating HMMA texture and nutrition,providing critical insights for developing fiber-enhanced,nutrient-fortified HMMAs.展开更多
In this paper,we study an acoustic black hole in Hayward spacetime within the framework of relativistic Gross-Pitaevskii theory.By examining the critical null geodesics,we sketch the shadow of the acoustic horizon.The...In this paper,we study an acoustic black hole in Hayward spacetime within the framework of relativistic Gross-Pitaevskii theory.By examining the critical null geodesics,we sketch the shadow of the acoustic horizon.The quasinormal mode(QNM)frequencies of the acoustic Hayward black hole are then computed numerically using the WKB method.The results show that these modes are more stable than those of the Hayward black hole,and that variations in the QNM frequencies are correlated with the behavior of the effective potential.We also verify the relationship between QNMs and the acoustic sphere(and the acoustic shadow)in the eikonal limit.Moreover,the WKB method is employed to calculate the grey-body factor and energy emission rate of the analogue Hawking radiation.It is shown that,as the tuning parameter increases,both the grey-body factor and the energy emission rate are enhanced,which can likewise be attributed to changes in the effective potential.In addition,the acoustic shadow radius also increases with the tuning parameter.Our work extends the acoustic black hole model to regular black hole spacetime,and the findings provide a potential application for distinguishing regular black holes from black holes with singularities in astrophysical environments via acoustic black hole effects.展开更多
Lithium-ion batteries(LIBs)have dominated the portable electronic and electrochemical energy markets since their commercialisation,whose high cost and lithium scarcity have prompted the development of other alkali-ion...Lithium-ion batteries(LIBs)have dominated the portable electronic and electrochemical energy markets since their commercialisation,whose high cost and lithium scarcity have prompted the development of other alkali-ion batteries(AIBs)including sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs).Owing to larger ion sizes of Na+and K+compared with Li+,nanocomposites with excellent crystallinity orientation and well-developed porosity show unprecedented potential for advanced lithium/sodium/potassium storage.With enticing open rigid framework structures,Prussian blue analogues(PBAs)remain promising self-sacrificial templates for the preparation of various nanocomposites,whose appeal originates from the well-retained porous structures and exceptional electrochemical activities after thermal decomposition.This review focuses on the recent progress of PBA-derived nanocomposites from their fabrication,lithium/sodium/potassium storage mechanism,and applications in AIBs(LIBs,SIBs,and PIBs).To distinguish various PBA derivatives,the working mechanism and applications of PBA-templated metal oxides,metal chalcogenides,metal phosphides,and other nanocomposites are systematically evaluated,facilitating the establishment of a structure–activity correlation for these materials.Based on the fruitful achievements of PBA-derived nanocomposites,perspectives for their future development are envisioned,aiming to narrow down the gap between laboratory study and industrial reality.展开更多
Aqueous zinc-ion batteries(AZIBs)show great potential in the field of electrochemical energy storage with the advantages of high safety,low cost and environmental friendliness.Prussian blue analogues(PBAs)are consider...Aqueous zinc-ion batteries(AZIBs)show great potential in the field of electrochemical energy storage with the advantages of high safety,low cost and environmental friendliness.Prussian blue analogues(PBAs)are considered as the highly promising cathode materials for AZIBs because of their low cost and high voltage potential.Its excellent electrochemical performance and sustainable energy storage capability provide a new direction and opportunity for the development of AZIBs technology.The practical application of PBAs in AZIBs,however,is restrained by its unstable cycle life deriving from PBAs’inherent structure deficiencies and its dissolution in aqueous electrolyte.Based on the summary of series of literature,we will comprehensively introduce the PBAs as cathodes for AZIBs in this review.Firstly,some basic knowledge of PBAs is introduced,including structural characteristics,advantages and issues.Secondly,several commonly used modification methods to improve the properties of PBAs,as well as electrolytes to stabilize PBAs,are presented.Finally,the future research directions and commercial prospects of PBAs in AZIBs are proposed to encourage further exploration and promote technological innovation.展开更多
Prussian blue/Prussian blue analogues(PB/PBAs)are widely used in electrochemistry and materials science fields,such as electrochemical energy storage,catalysis,water purification,and electromagnetic wave absorption,ow...Prussian blue/Prussian blue analogues(PB/PBAs)are widely used in electrochemistry and materials science fields,such as electrochemical energy storage,catalysis,water purification,and electromagnetic wave absorption,owing to their 3D open-framework structure,tunable composition,and large specific surface area.However,the co-precipitation method,which is most suitable for large-scale production of PB/PBAs,often leads to the formation of numerous crystal defects and severe lattice distortion,which significantly affects the structural stability of PB/PBAs.To obtain high-crystallinity PB/PBAs with targeted properties,precise synthesis considering various detailed conditions is especially needed.Herein,this review comprehensively summarizes the fundamental structure composition,key factors in synthesis,and applications in the electrochemistry of PB/PBAs.Unlike previous reports,this review elucidates the relationship between the physicochemical properties of PB/PBAs and their structural composition,with a particular focus on revealing the mechanisms and significance of specific preparation methods during the synthesis process,including reactant concentration,chelating agent,aging,atmosphere,temperature,and drying conditions,for achieving the precise fabrication of PB/PBAs nanomaterials.As PB/PBAs gradually become materials for multidimensional applications,we urge greater attention to the unique properties of PB/PBAs that are sustained by high crystallinity and stable crystal structures.This will effectively ensure the maximization of their advantages in practical applications.展开更多
CoFe-Prussian blue analog(CoFe-PBA)template derived porous nanocages comprising hollow(Co,Fe)O nanoparticles are introduced as a highly efficient anode for lithium-ion batteries(LIBs)by integrat-ing the co-precipitati...CoFe-Prussian blue analog(CoFe-PBA)template derived porous nanocages comprising hollow(Co,Fe)O nanoparticles are introduced as a highly efficient anode for lithium-ion batteries(LIBs)by integrat-ing the co-precipitation and nanoscale Kirkendall diffusion processes.This strategic approach employs a solution-based facile polydopamine(PDA)-derived carbon coating process to control the oxidation rate of nanoparticles during subsequent heat treatment to achieve the hollow structure by the nanoscale Kirk-endall diffusion effect.The application of different concentrations of PDA to the nanocages resulted in the formation of porous nanocages of three types,such as(Co,Fe)O@PDA-C-20,(Co,Fe)O@PDA-C-100,and(Co,Fe)O@PDA-C-200.Notably,(Co,Fe)O@PDA-C-100 porous nanocages exhibit remarkable cycling stability by the hollow structured(Co,Fe)O nanoparticles.Additionally,the hollow and porous structures facilitate rapid charge species diffusion,efficient electrolyte infiltration,and effective management of volumetric changes.When used as anodes for LIBs,the hollow(Co,Fe)O@PDA-C-100 anodes demonstrate impressive structural robustness and high-rate performance.They exhibit remarkable structural integrity,demon-strating stable cycling performance for up to 300 cycles at 0.5 and 1.0 A g-1(capacity retentions of 99.3%and 97.2%,respectively).In terms of rate capability,the hollow(Co,Fe)O@PDA-C-100 porous nanocages exhibit a high discharge capacity of 284 mA h g-1 at 10 A g-1.Moreover,the practical application po-tential of the prepared hollow(Co,Fe)O@PDA-C-100 anode is demonstrated by a full-cell test paired with and Li(Ni0.8Co0.1Mn0.1)O2 cathode under the condition of practical application.This clearly highlights the structural advantages of the prepared hollow(Co,Fe)O@PDA-C-100 porous nanocages.展开更多
To explore high-performance cathode materials for aqueous ammonium ion batteries(AAIBs),vanadium-based Prussian blue analogue composites(VFe-PBAs)were prepared by hydrothermal coprecipitation method to enhance the rev...To explore high-performance cathode materials for aqueous ammonium ion batteries(AAIBs),vanadium-based Prussian blue analogue composites(VFe-PBAs)were prepared by hydrothermal coprecipitation method to enhance the reversible storage of NH4+.Benefiting from the stable three-dimensional structure and spacious gap position,VFe-PBAs-2 cathode displays excellent electrochemical activity and rate performance,achieving a high specific capacity of 84.3 mA·h/g at a current density of 1000 mA/g.In addition,VFe-PBAs-2 cathode also shows impressive long-term cycle durability with 85.2% capacity retention after 3×104 cycles at 5000 mA/g.The synthesized cathode materials combined with the high electrochemical activity of vanadium ions significantly promote the rapid transfer of NH4+.Furthermore,NH4+embedding/extraction mechanism of VFe-PBAs-2 cathode was revealed by electrochemical kinetics tests and advanced ex-situ characterizations.The experimental results demonstrate that vanadium-modified VFe-PBAs-2 as a cathode material can remarkably improve the capacity,electrochemical activity and cycling stability of AAIBs to achieve high performance NH4+storage.展开更多
Transition metal oxides(TMOs)have received extensive attention for their unique physical and chemical properties.It is worth noting that Fe-based materials stand out because of their rich natural resources,low toxicit...Transition metal oxides(TMOs)have received extensive attention for their unique physical and chemical properties.It is worth noting that Fe-based materials stand out because of their rich natural resources,low toxicity,low price and other advantages,but at the same time confront with critical challenges such as capacity attenuation and volume expansion.Here,a universal synthesis method of MO/MFe2O4(M=Ni,Cu,Zn)nanomaterials derived from Prussian blue analogues(PBAs)is proposed based on the self-sacrificing template strategy of metal-organic frameworks(MOFs).The calcined products retain the porous structure and small particle size of PBAs,which shorten the ion transport path,provide abundant electroactive sites and void space,effectively alleviate the effect of volume expansion,and improve the reaction kinetics.These MO/MFe2O4anode materials exhibit excellent cyclic reversibility and stability during repeated charge/discharge process,among which,NiO/NiFe2O4 shows the best electrochemical performance,retaining a superior specific capacity of 1301.7 mAh g-1 following 230 cycles at 0.1 A g-1.In addition,the lithium adsorption capacity of the materials was further explored through the calculation of density functional theory(DFT).The research perspectives and strategies reported in this paper have strong universality and offer innovative insights for the synthesis of alternative advanced materials.展开更多
Prussian blue analogues(PBAs)have emerged as highly promising cathode materials for sodium-ion batteries(SIBs)due to their simple synthesis,low cost,structural tunability,and high theoretical capacity.However,despite ...Prussian blue analogues(PBAs)have emerged as highly promising cathode materials for sodium-ion batteries(SIBs)due to their simple synthesis,low cost,structural tunability,and high theoretical capacity.However,despite their significant potential,practical applications of PBAs still face multiple performance limitations.This review provides a comprehensive examination of PBAs structures and their electrochemical reaction mechanisms,and systematically summarizes current synthesis methods and modification strategies,while offering forward-looking insights.Furthermore,from the perspective of industrialization,this review systematically analyzes the synthesis,modification,and core challenges of PBAs by comparatively evaluating the feasibility of different technological pathways based on multiple dimensions,including cost-effectiveness,process scalability,environmental impact,and supply chain security,with the aim of providing forward-looking guidance for bridging the critical gap from lab to market.展开更多
Diphenylalanine and its analogs cause many concerns owing to their perfect self-assembly properties in the fields of biology,medicine,and nanotechnology.Experimental research has shown that diphenylalanine-based analo...Diphenylalanine and its analogs cause many concerns owing to their perfect self-assembly properties in the fields of biology,medicine,and nanotechnology.Experimental research has shown that diphenylalanine-based analogs with ethylenediamine linkers(PA,P=phenylalanine,and A=analog)can self-assemble into spherical assemblies,which can serve as novel anticancer drug carriers.In this work,to understand the assembly pathways,drug loading behavior,and formation mechanism of PA aggregates at the molecular level,we carried out dissipative particle dynamics(DPD)simulations of PA molecule systems.Our simulation results demonstrate that PA molecules spontaneously assemble into nanospheres and can self-assemble into drug-loaded nanospheres upon addition of the cancer chemotherapeutic agent doxorubicin(DOX).We also found that the hydrophobic side chain beads of PA molecules exhibited a unique onion-like distribution inside the nanospheres,which was not observed in the experiment.The onion-like nanospheres were verified by calculating the radial distribution function(RDF)of the DPD beads.Furthermore,based on the analysis of the percentages of different interaction components in the total nonbonded energies,main chain-side chain interactions between PA molecules may be important in the formation of onion-like nanospheres,and the synergistic effects of main chain-side chain,main chain-drug,side chain-drug,and main chain-solvent interactions are significant in the formation of drug-loaded nanospheres.These findings provide new insights into the structure and self-assembly pathway of PA assemblies,which may be helpful for the design of efficient and effective drug delivery systems.展开更多
ⅢThe superior adaptability of Prussian blue analogues(PBAs)in interacting with potassium ions has shifted research focus toward their potential application as cathodes of potassium-ion batteries(PIBs).The large inter...ⅢThe superior adaptability of Prussian blue analogues(PBAs)in interacting with potassium ions has shifted research focus toward their potential application as cathodes of potassium-ion batteries(PIBs).The large interstitial space formed between metal ions and–C≡N–in PBAs can accommodate large-radius K+.However,the rapid nucleation in the co-precipitation synthesis process of PBAs induces many lattice defects of[M(CN)6]4-vacancies(V[M–C≡N]),interstitial and coordinated H2O molecules,which will directly lead to performance degradation.Moreover,originating from various transition metal elements in low/high-spin electron configuration states,PBAs exhibit diverse electrochemical behaviors,such as low reaction kinetics of low-spin iron(Ⅱ),Jahn-Teller distortion and dissolution of manganese(Ⅲ),and electrochemical inertness of nickel(Ⅱ)and copper(Ⅱ).Here,we summarize recently reported structures and properties of PBAs,classifying them based on the types of transition metals(iron,cobalt,manganese,copper,nickel)employed.Advanced synthesis strategies,including control engineering of crystallinity based on H2O molecules and V[M–C≡N],were discussed.Also,the approaches for enhancing the electrochemical performance of PBAs were highlighted.Finally,the challenges and prospects towards the future development of PBAs are put forward.The review is expected to provide technical and theoretical support for the design of high-performance PBAs.展开更多
Volatile aromatic aldehydes,including benzaldehyde(BzH),4-fluorobenzaldehyde(4-F-BzH),4-isobutylbenzaldehyde(4-iBu-BzH),3-trifluoromethylbenzaldehyde(3-CF3-BzH),p-methoxybenzaldehyde(4-MeO-BzH),and o-trifluoromethy...Volatile aromatic aldehydes,including benzaldehyde(BzH),4-fluorobenzaldehyde(4-F-BzH),4-isobutylbenzaldehyde(4-iBu-BzH),3-trifluoromethylbenzaldehyde(3-CF3-BzH),p-methoxybenzaldehyde(4-MeO-BzH),and o-trifluoromethylbenzaldehyde(2-CF3-BzH),are crucial raw materials for the synthesis of various pesticides and pharmaceuticals[1].展开更多
Nickel-zinc aqueous batteries have great potential for application in the field of advanced energy storage and conversion due to their environmental-friendliness,high safety,and ideal output voltage(~1.75 V).Herein,Fe...Nickel-zinc aqueous batteries have great potential for application in the field of advanced energy storage and conversion due to their environmental-friendliness,high safety,and ideal output voltage(~1.75 V).Herein,FePBA,NiFe-PBA,and NiCoFe-PBA are synthesized by a facile coprecipitation strategy,and the structure of NiCoFePBA is optimized by modulating the doping ratios of Ni2+and Co2+.展开更多
Temperate woodland vegetation is initially determined by spatiotemporal and historical factors,mediated by complex biotic interactions.However,catastrophic events such as disease outbreaks(e.g.,sweet chestnut blight,a...Temperate woodland vegetation is initially determined by spatiotemporal and historical factors,mediated by complex biotic interactions.However,catastrophic events such as disease outbreaks(e.g.,sweet chestnut blight,ash dieback),infestations of insect pests,and human-accelerated climate change can create canopy gaps due to systematic decline in,or loss of,tree species that was once an important part of the canopy.Resultant cascade effects have the potential to alter the composition of woodland ecosystems quickly and radically,but inherent lag times make primary research into these effects challenging.Here,we explore change in woodland vegetation at 10 sites in response to canopy opening using the Elm Decline,a rapid loss of Ulmus in woodlands across northwestern Europe~5800 years ago that coexisted alongside other stressors such as increasing human activity,as a palaeoecological analogue.For arboreal taxa,community evenness significantly decreased,within-site turnover significantly increased,and richness remained unchanged.Changes in arboreal taxa were highly site-specific but there was a substantial decline in woody climbing taxa,especially Hedera(ivy),across the majority of sites.For shrub taxa,richness significantly increased but evenness and turnover remained consistent.Interestingly,however,there was a significant increase in abundance of shrubs at 70%of sites,including Calluna(heather),Ilex(holly)and Corylus(hazel),suggesting structural change.Surprisingly,there was no change in richness,evenness or turnover for herb taxa,possibly because change was highly variable spatially.However,there was a marked uptick in the disturbance indicator Plantago(plantain).Overall,these findings suggest that woodlands with sustained reduction in,or loss of,a tree species that once formed an important part of the canopy has profound,but often spatially idiosyncratic,impacts on vegetation diversity(richness),composition(evenness),stability(turnover),and on abundance of specific taxa,especially within the shrub layer.Use of this palaeoecological analogue,which was itself complicated by cooccurring changes in human activity,provides a valuable empirical insight into possible cascade effects of similar change in canopy opening in contemporary settings,including Ash Dieback.展开更多
In this paper, an analogue correction method of errors (ACE) based on a complicated atmospheric model is further developed and applied to numerical weather prediction (NWP). The analysis shows that the ACE can eff...In this paper, an analogue correction method of errors (ACE) based on a complicated atmospheric model is further developed and applied to numerical weather prediction (NWP). The analysis shows that the ACE can effectively reduce model errors by combining the statistical analogue method with the dynamical model together in order that the information of plenty of historical data is utilized in the current complicated NWP model, Furthermore, in the ACE, the differences of the similarities between different historical analogues and the current initial state are considered as the weights for estimating model errors. The results of daily, decad and monthly prediction experiments on a complicated T63 atmospheric model show that the performance of the ACE by correcting model errors based on the estimation of the errors of 4 historical analogue predictions is not only better than that of the scheme of only introducing the correction of the errors of every single analogue prediction, but is also better than that of the T63 model.展开更多
In the applications of large-scale energy storage,aqueous batteries are considered as rivals for organic batteries due to their environmentally friendly and low-cost nature.However,carrier ions always exhibit huge hyd...In the applications of large-scale energy storage,aqueous batteries are considered as rivals for organic batteries due to their environmentally friendly and low-cost nature.However,carrier ions always exhibit huge hydrated radius in aqueous electrolyte,which brings difficulty to find suitable host materials that can achieve highly reversible insertion and extraction of cations.Owing to open threedimensional rigid framework and facile synthesis,Prussian blue analogues(PBAs)receive the most extensive attention among various host candidates in aqueous system.Herein,a comprehensive review on recent progresses of PBAs in aqueous batteries is presented.Based on the application in different aqueous systems,the relationship between electrochemical behaviors(redox potential,capacity,cycling stability and rate performance)and structural characteristics(preparation method,structure type,particle size,morphology,crystallinity,defect,metal atom in highspin state and chemical composition)is analyzed and summarized thoroughly.It can be concluded that the required type of PBAs is different for various carrier ions.In particular,the desalination batteries worked with the same mechanism as aqueous batteries are also discussed in detail to introduce the application of PBAs in aqueous systems comprehensively.This report can help the readers to understand the relationship between physical/chemical characteristics and electrochemical properties for PBAs and find a way to fabricate high-performance PBAs in aqueous batteries and desalination batteries.展开更多
Prussian blue analogue Na2Ni[Fe(CN)6](Ni-PB)has been widely studied as a cathode material for sodium-ion battery due to its excellent cycling performance.However,Ni-PB has a low theoretical capacity of 85 mAh g−1 b...Prussian blue analogue Na2Ni[Fe(CN)6](Ni-PB)has been widely studied as a cathode material for sodium-ion battery due to its excellent cycling performance.However,Ni-PB has a low theoretical capacity of 85 mAh g−1 because of the electrochemical inertness of Ni.Herein,ternary Ni-PB is successfully synthesized by double doping with Co and Fe at Ni-site,and the effect of doping with Co and Fe on the electrochemical performance of Ni-PB is systematically investigated through theoretical calculations and electrochemical tests.The first principles calculations confirm that double doping with Co and Fe can significantly reduce the energy barrier and bandgap of Ni-PB.X-ray diffraction and composition analysis results indicate that ternary NiCoFe-PB composite not only has good crystallinity and high Na content but also has low defects and crystal water.Electrochemical tests reveal that,besides the capacity contribution of high-spin Co/Fe and low-spin Fe,Co-doping enhances the electrochemical activity of low-spin Fe and Fe-doping improves the activity of high-spin Co;moreover,double doping can decrease the diffusion resistance of Na+ions through solid electrolyte interface film,accelerate the kinetics for both ion diffusion process and Faradic reaction,and increase active sites.Under the synergistic effect of Co and Fe,this ternary NiCoFe-PB exhibits outstanding electrochemical performance with a high initial discharge capacity of 120.4 mAh g−1 at 20mA g−1 and an extremely low capacity fading rate of 0.0044%per cycle at a high current density of 2 A g−1 even after 10,000 cycles,showing great application potential of ternary NiCoFe-PB in the field of large-scale energy storage.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.42372322)Science and Technology Innovation Program for Postgraduate students in IDP subsidized by Fundamental Research Funds for the Central Universities(Grant No.ZY20240314)the research project of Spark Plan for Earthquake Science and Technology(Grant No.XH24060A).
摘要Locked segments are high-strength structural elements in fault zones that release significantseismic energy during earthquakes.In fracture mechanics,they act as high-stress concentration patches(asperities)where rupture initiates.The progressive failure of locked segments along faults plays a crucial role in the energy partition of earthquakes.The impact of locked segments on the near-fielddeformation and nucleation of faults,however,remains poorly understood.In this study,rock-like materials with pre-manufactured strike-slip faults containing various locked segments lengths under uniaxial stress.The mechanical properties,local deformation fields,and slip displacement rates during the uniaxial loading of the models were quantified.Results indicate that the uniaxial compressive strength and elastic modulus of the system peak once the ratio of locked segment to fault length is approximately 0.6.Meanwhile,the resistance of the models to deformation increased,and the failure mode transformed from shear failure to tensile failure.Under loading,compression and dilatation quadrants were formed on both sides of the fault.Large-scale fractures dominate the dilatation quadrants,and the degree of deformation disturbance in this region was significantly higher than that in the compression quadrants.With increasing locked segment length,the amplitude of deformation perturbations decreased after the peak strength.Shorter locked segments were more susceptible to deformation and failure.In the fracture evolution process,a relationship between the stress deflectionangle and the displacement rate was found,which is empirically described by an exponential function.These findings clarify geological structures failure mechanisms and support seismic hazard assessment for strike-slip earthquake regions.
基金financially supported by the Ten-thousand Talents Programthe K. C. Wong Pioneer Talent Program+3 种基金China Three Gorges Corporation (WWKY-2021–0027)Inner Mongolia Science and Technology Plan (2021ZD0033)the National Natural Science Foundation of China (52202121)funded by China Petroleum&Chemical Corporation (123091)
摘要Although manganese Prussian blue analogues(Mn-PBAs)offer advantages as cost-effective,high-energy-density cathode materials for sodium-ion batteries,their practical application is severely constrained by substantial capacity degradation during long-term cycling.This performance deterioration is closely associated with the structural instability of the material during the cycling process,which is mainly attributed to the gradual dissolution of the active material into the electrolyte and severe lattice distortion during Na+intercalation/deintercalation.Fortunately,the aforementioned challenges can be effectively addressed by fabricating an in situ engineered nickel cage(ISE-NC)on Mn-PBAs(denoted as Mn-PBAs-NC).Experimental characterization combined with theoretical calculations reveals that this spontaneously formed nickel cage not only suppresses the diffusion of Mn-PBAs into the electrolyte but also acts as a structural stabilizer,significantly alleviating lattice distortion during cycling.This dual stabilization mechanism ensures remarkable cycling stability,with Mn-PBAs-NC delivering a retained capacity of 96.4 mA h g−1(80%capacity retention)over 2,300 cycles at 2 C,elevating the cycle life of Mn-PBAs to unprecedented levels.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12274265 and 11804195)Partial support by the Natural Science Foundation of Shandong Province,China(Grant No.ZR2022MA006)。
摘要The adduct 5-carboxylcytosine(5caC),one of the products involved in demethylation pathway,has the potential to serve as a target for specifically deciphering proteins that regulate gene expression and chromatin organization.The fluorescence detection with its ultra-high sensitivity can break through the limitations of traditional detection methods and achieve single molecule detection of 5caC.In this work,the guanine analogue Gr3with largeπ-conjugation and large Stokes shift(89.25 nm)is selected as the fluorescence probe to specifically recognize and monitor 5caC.Because of its bright fluorescence when paired with C and a complete fluorescence quenching when paired with 5caC,this on-off switching feature of Gr3stems from excited-state intermolecular charge transfer.Furthermore,it is found that after linking with deoxyribose,this discriminative function remains unchanged.This strategy could contribute to detecting the presence of 5caC in the genetic material,and thus prevent diseases associated with this epigenetic modification.
基金funded by The Science Foundation of Henan University of Technology(2021BS038)The Open Project Program of National Engineering Re-search Center of Wheat and Corn Further Processing(NL2022014)Henan Province Science and Technology R&D Program Joint Fund(Application Research and De-velopment Category)(242103810082).
摘要High-moisture meat analogues(HMMAs)offer sustainable protein alternatives to conventional meat and become a research hotspot in recent years.This study systematically investigated the impact of nori powder(NP)incorporation(0.5%–2.0%)on the physicochemical and structural properties of HMMAs.Rheological analysis revealed that NP reduced the viscosity(consistency coefficient K decreased from 65.67 Pa⋅s to 16.66–19.99 Pa⋅s)and enhanced the fluidity(flow behavior index n increased from 0.25 to 0.33–0.38)of raw material.NP addition progressively decreased the redness values(a*),except for 0.5%NP level.At 1.0%NP level,HMMAs exhibited a denser microstructure with reduced water mobility,resulting in the lowest water holding capacity(2.07 g/g).Conversely,2.0%NP promoted highly oriented fibrous structures,achieving a maximal texturization degree of 1.51.Secondary structure analysis indicated NP facilitated a shift fromα-helix toβ-sheet conformations(β-sheet content increased from 26.06%to 29.92%at 2.0%NP),resulting in stabilized protein networks.These modifications were attributed to NP-induced hydrophobic interactions and polysaccharide-protein crosslinking.The study demonstrates NP's role in modulating HMMA texture and nutrition,providing critical insights for developing fiber-enhanced,nutrient-fortified HMMAs.
基金Supported by the National Natural Science Foundation of China(12475069)the Guangdong Basic and Applied Basic Research Foundation(2025A1515011321)。
摘要In this paper,we study an acoustic black hole in Hayward spacetime within the framework of relativistic Gross-Pitaevskii theory.By examining the critical null geodesics,we sketch the shadow of the acoustic horizon.The quasinormal mode(QNM)frequencies of the acoustic Hayward black hole are then computed numerically using the WKB method.The results show that these modes are more stable than those of the Hayward black hole,and that variations in the QNM frequencies are correlated with the behavior of the effective potential.We also verify the relationship between QNMs and the acoustic sphere(and the acoustic shadow)in the eikonal limit.Moreover,the WKB method is employed to calculate the grey-body factor and energy emission rate of the analogue Hawking radiation.It is shown that,as the tuning parameter increases,both the grey-body factor and the energy emission rate are enhanced,which can likewise be attributed to changes in the effective potential.In addition,the acoustic shadow radius also increases with the tuning parameter.Our work extends the acoustic black hole model to regular black hole spacetime,and the findings provide a potential application for distinguishing regular black holes from black holes with singularities in astrophysical environments via acoustic black hole effects.
基金financial support from the Special Funds for the Cultivation of Guangdong College Students’Scientific and Technological Innovation(“Climbing Program”Special Funds,pdjh2023b0145)the Scientific Research Innovation Project of Graduate School of South China Normal University(2024KYLX047)financial support from the Australian Research Council,Centre for Materials Science,Queensland University of Technology.
摘要Lithium-ion batteries(LIBs)have dominated the portable electronic and electrochemical energy markets since their commercialisation,whose high cost and lithium scarcity have prompted the development of other alkali-ion batteries(AIBs)including sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs).Owing to larger ion sizes of Na+and K+compared with Li+,nanocomposites with excellent crystallinity orientation and well-developed porosity show unprecedented potential for advanced lithium/sodium/potassium storage.With enticing open rigid framework structures,Prussian blue analogues(PBAs)remain promising self-sacrificial templates for the preparation of various nanocomposites,whose appeal originates from the well-retained porous structures and exceptional electrochemical activities after thermal decomposition.This review focuses on the recent progress of PBA-derived nanocomposites from their fabrication,lithium/sodium/potassium storage mechanism,and applications in AIBs(LIBs,SIBs,and PIBs).To distinguish various PBA derivatives,the working mechanism and applications of PBA-templated metal oxides,metal chalcogenides,metal phosphides,and other nanocomposites are systematically evaluated,facilitating the establishment of a structure–activity correlation for these materials.Based on the fruitful achievements of PBA-derived nanocomposites,perspectives for their future development are envisioned,aiming to narrow down the gap between laboratory study and industrial reality.
基金financially supported by the National Natural Science Foundation of China(Youth Program,Nos.52204378 and No.22309209)the Natural Science Foundation of Hunan Province in China(No.2023JJ40709).
摘要Aqueous zinc-ion batteries(AZIBs)show great potential in the field of electrochemical energy storage with the advantages of high safety,low cost and environmental friendliness.Prussian blue analogues(PBAs)are considered as the highly promising cathode materials for AZIBs because of their low cost and high voltage potential.Its excellent electrochemical performance and sustainable energy storage capability provide a new direction and opportunity for the development of AZIBs technology.The practical application of PBAs in AZIBs,however,is restrained by its unstable cycle life deriving from PBAs’inherent structure deficiencies and its dissolution in aqueous electrolyte.Based on the summary of series of literature,we will comprehensively introduce the PBAs as cathodes for AZIBs in this review.Firstly,some basic knowledge of PBAs is introduced,including structural characteristics,advantages and issues.Secondly,several commonly used modification methods to improve the properties of PBAs,as well as electrolytes to stabilize PBAs,are presented.Finally,the future research directions and commercial prospects of PBAs in AZIBs are proposed to encourage further exploration and promote technological innovation.
基金financial support from the National Natural Science Foundation of China(NSFC,Grant No.52202253,52372193,and 22293041)Natural Science Foundation of Jiangsu Province(Grant No.BK20220914)Large Instrument and Equipment Sharing Fund of Nanjing University of Aeronautics and Astronautics。
摘要Prussian blue/Prussian blue analogues(PB/PBAs)are widely used in electrochemistry and materials science fields,such as electrochemical energy storage,catalysis,water purification,and electromagnetic wave absorption,owing to their 3D open-framework structure,tunable composition,and large specific surface area.However,the co-precipitation method,which is most suitable for large-scale production of PB/PBAs,often leads to the formation of numerous crystal defects and severe lattice distortion,which significantly affects the structural stability of PB/PBAs.To obtain high-crystallinity PB/PBAs with targeted properties,precise synthesis considering various detailed conditions is especially needed.Herein,this review comprehensively summarizes the fundamental structure composition,key factors in synthesis,and applications in the electrochemistry of PB/PBAs.Unlike previous reports,this review elucidates the relationship between the physicochemical properties of PB/PBAs and their structural composition,with a particular focus on revealing the mechanisms and significance of specific preparation methods during the synthesis process,including reactant concentration,chelating agent,aging,atmosphere,temperature,and drying conditions,for achieving the precise fabrication of PB/PBAs nanomaterials.As PB/PBAs gradually become materials for multidimensional applications,we urge greater attention to the unique properties of PB/PBAs that are sustained by high crystallinity and stable crystal structures.This will effectively ensure the maximization of their advantages in practical applications.
基金supported by the National Research Foundation of Korea(NRF)and the Commercialization Promotion Agency for R&D Outcomes(COMPA)funded by the Ministry of Science and ICT(Nos.RS-2023-00217581 and RS-2023-00304768).
摘要CoFe-Prussian blue analog(CoFe-PBA)template derived porous nanocages comprising hollow(Co,Fe)O nanoparticles are introduced as a highly efficient anode for lithium-ion batteries(LIBs)by integrat-ing the co-precipitation and nanoscale Kirkendall diffusion processes.This strategic approach employs a solution-based facile polydopamine(PDA)-derived carbon coating process to control the oxidation rate of nanoparticles during subsequent heat treatment to achieve the hollow structure by the nanoscale Kirk-endall diffusion effect.The application of different concentrations of PDA to the nanocages resulted in the formation of porous nanocages of three types,such as(Co,Fe)O@PDA-C-20,(Co,Fe)O@PDA-C-100,and(Co,Fe)O@PDA-C-200.Notably,(Co,Fe)O@PDA-C-100 porous nanocages exhibit remarkable cycling stability by the hollow structured(Co,Fe)O nanoparticles.Additionally,the hollow and porous structures facilitate rapid charge species diffusion,efficient electrolyte infiltration,and effective management of volumetric changes.When used as anodes for LIBs,the hollow(Co,Fe)O@PDA-C-100 anodes demonstrate impressive structural robustness and high-rate performance.They exhibit remarkable structural integrity,demon-strating stable cycling performance for up to 300 cycles at 0.5 and 1.0 A g-1(capacity retentions of 99.3%and 97.2%,respectively).In terms of rate capability,the hollow(Co,Fe)O@PDA-C-100 porous nanocages exhibit a high discharge capacity of 284 mA h g-1 at 10 A g-1.Moreover,the practical application po-tential of the prepared hollow(Co,Fe)O@PDA-C-100 anode is demonstrated by a full-cell test paired with and Li(Ni0.8Co0.1Mn0.1)O2 cathode under the condition of practical application.This clearly highlights the structural advantages of the prepared hollow(Co,Fe)O@PDA-C-100 porous nanocages.
基金supported by the National Natural Science Foundation of China(No.52374301)the Hebei Provincial Natural Science Foundation,China(No.E2024501010)+2 种基金the Shijiazhuang Basic Research Project,China(No.241790667A)the Fundamental Research Funds for the Central Universities,China(No.N2423054)the Performance Subsidy Fund for Key Laboratory of Dielectric and Electrolyte Functional Material of Hebei Province,China(No.22567627H).
摘要To explore high-performance cathode materials for aqueous ammonium ion batteries(AAIBs),vanadium-based Prussian blue analogue composites(VFe-PBAs)were prepared by hydrothermal coprecipitation method to enhance the reversible storage of NH4+.Benefiting from the stable three-dimensional structure and spacious gap position,VFe-PBAs-2 cathode displays excellent electrochemical activity and rate performance,achieving a high specific capacity of 84.3 mA·h/g at a current density of 1000 mA/g.In addition,VFe-PBAs-2 cathode also shows impressive long-term cycle durability with 85.2% capacity retention after 3×104 cycles at 5000 mA/g.The synthesized cathode materials combined with the high electrochemical activity of vanadium ions significantly promote the rapid transfer of NH4+.Furthermore,NH4+embedding/extraction mechanism of VFe-PBAs-2 cathode was revealed by electrochemical kinetics tests and advanced ex-situ characterizations.The experimental results demonstrate that vanadium-modified VFe-PBAs-2 as a cathode material can remarkably improve the capacity,electrochemical activity and cycling stability of AAIBs to achieve high performance NH4+storage.
摘要Transition metal oxides(TMOs)have received extensive attention for their unique physical and chemical properties.It is worth noting that Fe-based materials stand out because of their rich natural resources,low toxicity,low price and other advantages,but at the same time confront with critical challenges such as capacity attenuation and volume expansion.Here,a universal synthesis method of MO/MFe2O4(M=Ni,Cu,Zn)nanomaterials derived from Prussian blue analogues(PBAs)is proposed based on the self-sacrificing template strategy of metal-organic frameworks(MOFs).The calcined products retain the porous structure and small particle size of PBAs,which shorten the ion transport path,provide abundant electroactive sites and void space,effectively alleviate the effect of volume expansion,and improve the reaction kinetics.These MO/MFe2O4anode materials exhibit excellent cyclic reversibility and stability during repeated charge/discharge process,among which,NiO/NiFe2O4 shows the best electrochemical performance,retaining a superior specific capacity of 1301.7 mAh g-1 following 230 cycles at 0.1 A g-1.In addition,the lithium adsorption capacity of the materials was further explored through the calculation of density functional theory(DFT).The research perspectives and strategies reported in this paper have strong universality and offer innovative insights for the synthesis of alternative advanced materials.
基金supported by the National Natural Science Foundation of China(NSFC)(No.52301257,62475003)the Beijing Natural Science Foundation(No.2252031)。
摘要Prussian blue analogues(PBAs)have emerged as highly promising cathode materials for sodium-ion batteries(SIBs)due to their simple synthesis,low cost,structural tunability,and high theoretical capacity.However,despite their significant potential,practical applications of PBAs still face multiple performance limitations.This review provides a comprehensive examination of PBAs structures and their electrochemical reaction mechanisms,and systematically summarizes current synthesis methods and modification strategies,while offering forward-looking insights.Furthermore,from the perspective of industrialization,this review systematically analyzes the synthesis,modification,and core challenges of PBAs by comparatively evaluating the feasibility of different technological pathways based on multiple dimensions,including cost-effectiveness,process scalability,environmental impact,and supply chain security,with the aim of providing forward-looking guidance for bridging the critical gap from lab to market.
基金financially supported by the National Natural Science Foundation of China(Nos.20904047 and 12074151)the Natural Science Foundation of Zhejiang Province(Nos.LY17A040001 and LY19F03004)。
摘要Diphenylalanine and its analogs cause many concerns owing to their perfect self-assembly properties in the fields of biology,medicine,and nanotechnology.Experimental research has shown that diphenylalanine-based analogs with ethylenediamine linkers(PA,P=phenylalanine,and A=analog)can self-assemble into spherical assemblies,which can serve as novel anticancer drug carriers.In this work,to understand the assembly pathways,drug loading behavior,and formation mechanism of PA aggregates at the molecular level,we carried out dissipative particle dynamics(DPD)simulations of PA molecule systems.Our simulation results demonstrate that PA molecules spontaneously assemble into nanospheres and can self-assemble into drug-loaded nanospheres upon addition of the cancer chemotherapeutic agent doxorubicin(DOX).We also found that the hydrophobic side chain beads of PA molecules exhibited a unique onion-like distribution inside the nanospheres,which was not observed in the experiment.The onion-like nanospheres were verified by calculating the radial distribution function(RDF)of the DPD beads.Furthermore,based on the analysis of the percentages of different interaction components in the total nonbonded energies,main chain-side chain interactions between PA molecules may be important in the formation of onion-like nanospheres,and the synergistic effects of main chain-side chain,main chain-drug,side chain-drug,and main chain-solvent interactions are significant in the formation of drug-loaded nanospheres.These findings provide new insights into the structure and self-assembly pathway of PA assemblies,which may be helpful for the design of efficient and effective drug delivery systems.
基金financially supported by research grants from Innovative Research Group Project of National Natural Science Foundation of China(No.52021004)National Key Research and Development Program of China(2022YFB3803300)+2 种基金National Natural Science Foundation of China(62474026 and 62074022)Natural Science Foundation of Chongqing(CSTB2024NSCQ-MSX1215,cstc2021jcyj-jqX0015 and CSTB2022NSCQ-MSX1183)the Youth Talent Support Program of Chongqing(CQYC2021059206).
摘要ⅢThe superior adaptability of Prussian blue analogues(PBAs)in interacting with potassium ions has shifted research focus toward their potential application as cathodes of potassium-ion batteries(PIBs).The large interstitial space formed between metal ions and–C≡N–in PBAs can accommodate large-radius K+.However,the rapid nucleation in the co-precipitation synthesis process of PBAs induces many lattice defects of[M(CN)6]4-vacancies(V[M–C≡N]),interstitial and coordinated H2O molecules,which will directly lead to performance degradation.Moreover,originating from various transition metal elements in low/high-spin electron configuration states,PBAs exhibit diverse electrochemical behaviors,such as low reaction kinetics of low-spin iron(Ⅱ),Jahn-Teller distortion and dissolution of manganese(Ⅲ),and electrochemical inertness of nickel(Ⅱ)and copper(Ⅱ).Here,we summarize recently reported structures and properties of PBAs,classifying them based on the types of transition metals(iron,cobalt,manganese,copper,nickel)employed.Advanced synthesis strategies,including control engineering of crystallinity based on H2O molecules and V[M–C≡N],were discussed.Also,the approaches for enhancing the electrochemical performance of PBAs were highlighted.Finally,the challenges and prospects towards the future development of PBAs are put forward.The review is expected to provide technical and theoretical support for the design of high-performance PBAs.
基金supported by National Natural Science Foundation of China(22361031,22308260).
摘要Volatile aromatic aldehydes,including benzaldehyde(BzH),4-fluorobenzaldehyde(4-F-BzH),4-isobutylbenzaldehyde(4-iBu-BzH),3-trifluoromethylbenzaldehyde(3-CF3-BzH),p-methoxybenzaldehyde(4-MeO-BzH),and o-trifluoromethylbenzaldehyde(2-CF3-BzH),are crucial raw materials for the synthesis of various pesticides and pharmaceuticals[1].
基金financially supported by the National Natural Science Foundation of China(No.52371240)
摘要Nickel-zinc aqueous batteries have great potential for application in the field of advanced energy storage and conversion due to their environmental-friendliness,high safety,and ideal output voltage(~1.75 V).Herein,FePBA,NiFe-PBA,and NiCoFe-PBA are synthesized by a facile coprecipitation strategy,and the structure of NiCoFePBA is optimized by modulating the doping ratios of Ni2+and Co2+.
摘要Temperate woodland vegetation is initially determined by spatiotemporal and historical factors,mediated by complex biotic interactions.However,catastrophic events such as disease outbreaks(e.g.,sweet chestnut blight,ash dieback),infestations of insect pests,and human-accelerated climate change can create canopy gaps due to systematic decline in,or loss of,tree species that was once an important part of the canopy.Resultant cascade effects have the potential to alter the composition of woodland ecosystems quickly and radically,but inherent lag times make primary research into these effects challenging.Here,we explore change in woodland vegetation at 10 sites in response to canopy opening using the Elm Decline,a rapid loss of Ulmus in woodlands across northwestern Europe~5800 years ago that coexisted alongside other stressors such as increasing human activity,as a palaeoecological analogue.For arboreal taxa,community evenness significantly decreased,within-site turnover significantly increased,and richness remained unchanged.Changes in arboreal taxa were highly site-specific but there was a substantial decline in woody climbing taxa,especially Hedera(ivy),across the majority of sites.For shrub taxa,richness significantly increased but evenness and turnover remained consistent.Interestingly,however,there was a significant increase in abundance of shrubs at 70%of sites,including Calluna(heather),Ilex(holly)and Corylus(hazel),suggesting structural change.Surprisingly,there was no change in richness,evenness or turnover for herb taxa,possibly because change was highly variable spatially.However,there was a marked uptick in the disturbance indicator Plantago(plantain).Overall,these findings suggest that woodlands with sustained reduction in,or loss of,a tree species that once formed an important part of the canopy has profound,but often spatially idiosyncratic,impacts on vegetation diversity(richness),composition(evenness),stability(turnover),and on abundance of specific taxa,especially within the shrub layer.Use of this palaeoecological analogue,which was itself complicated by cooccurring changes in human activity,provides a valuable empirical insight into possible cascade effects of similar change in canopy opening in contemporary settings,including Ash Dieback.
基金Project supported by the National Natural Science Foundation of China (Grant Nos 40575036 and 40325015).Acknowledgement The authors thank Drs Zhang Pei-Qun and Bao Ming very much for their valuable comments on the present paper.
摘要In this paper, an analogue correction method of errors (ACE) based on a complicated atmospheric model is further developed and applied to numerical weather prediction (NWP). The analysis shows that the ACE can effectively reduce model errors by combining the statistical analogue method with the dynamical model together in order that the information of plenty of historical data is utilized in the current complicated NWP model, Furthermore, in the ACE, the differences of the similarities between different historical analogues and the current initial state are considered as the weights for estimating model errors. The results of daily, decad and monthly prediction experiments on a complicated T63 atmospheric model show that the performance of the ACE by correcting model errors based on the estimation of the errors of 4 historical analogue predictions is not only better than that of the scheme of only introducing the correction of the errors of every single analogue prediction, but is also better than that of the T63 model.
基金This work was sponsored by NSAF Joint Fund(U1830106)Science and Technology Innovation 2025 Major Program of Ningbo(2018B10061)K.C.Wong Magna Fund in Ningbo University.
摘要In the applications of large-scale energy storage,aqueous batteries are considered as rivals for organic batteries due to their environmentally friendly and low-cost nature.However,carrier ions always exhibit huge hydrated radius in aqueous electrolyte,which brings difficulty to find suitable host materials that can achieve highly reversible insertion and extraction of cations.Owing to open threedimensional rigid framework and facile synthesis,Prussian blue analogues(PBAs)receive the most extensive attention among various host candidates in aqueous system.Herein,a comprehensive review on recent progresses of PBAs in aqueous batteries is presented.Based on the application in different aqueous systems,the relationship between electrochemical behaviors(redox potential,capacity,cycling stability and rate performance)and structural characteristics(preparation method,structure type,particle size,morphology,crystallinity,defect,metal atom in highspin state and chemical composition)is analyzed and summarized thoroughly.It can be concluded that the required type of PBAs is different for various carrier ions.In particular,the desalination batteries worked with the same mechanism as aqueous batteries are also discussed in detail to introduce the application of PBAs in aqueous systems comprehensively.This report can help the readers to understand the relationship between physical/chemical characteristics and electrochemical properties for PBAs and find a way to fabricate high-performance PBAs in aqueous batteries and desalination batteries.
基金National Natural Science Foundation of China,Grant/Award Number:52072217,51802261,51772169National Key R&D Program of China,Grant/Award Number:2018YFB0905400Major Technological Innovation Project of Hubei Science and Technology Department,Grant/Award Number:2019AAA164。
摘要Prussian blue analogue Na2Ni[Fe(CN)6](Ni-PB)has been widely studied as a cathode material for sodium-ion battery due to its excellent cycling performance.However,Ni-PB has a low theoretical capacity of 85 mAh g−1 because of the electrochemical inertness of Ni.Herein,ternary Ni-PB is successfully synthesized by double doping with Co and Fe at Ni-site,and the effect of doping with Co and Fe on the electrochemical performance of Ni-PB is systematically investigated through theoretical calculations and electrochemical tests.The first principles calculations confirm that double doping with Co and Fe can significantly reduce the energy barrier and bandgap of Ni-PB.X-ray diffraction and composition analysis results indicate that ternary NiCoFe-PB composite not only has good crystallinity and high Na content but also has low defects and crystal water.Electrochemical tests reveal that,besides the capacity contribution of high-spin Co/Fe and low-spin Fe,Co-doping enhances the electrochemical activity of low-spin Fe and Fe-doping improves the activity of high-spin Co;moreover,double doping can decrease the diffusion resistance of Na+ions through solid electrolyte interface film,accelerate the kinetics for both ion diffusion process and Faradic reaction,and increase active sites.Under the synergistic effect of Co and Fe,this ternary NiCoFe-PB exhibits outstanding electrochemical performance with a high initial discharge capacity of 120.4 mAh g−1 at 20mA g−1 and an extremely low capacity fading rate of 0.0044%per cycle at a high current density of 2 A g−1 even after 10,000 cycles,showing great application potential of ternary NiCoFe-PB in the field of large-scale energy storage.