With the ongoing depletion of fossil fuels,energy and environmental issues have become increasingly critical,necessitating the search for effective solutions.Catalysis,being one of the hallmarks of modern industry,off...With the ongoing depletion of fossil fuels,energy and environmental issues have become increasingly critical,necessitating the search for effective solutions.Catalysis,being one of the hallmarks of modern industry,offers a promising avenue for researchers.However,the question of how to significantly enhance the performance of catalysts has gradually drawn the attention of scholars.Defect engineering,a commonly employed and effective approach to improve catalyst activity,has become a significant research focus in the catalysis field in recent years.Nonmetal vacancies have received extensive attention due to their simple form.Consequently,exploration of metal vacancies has remained stagnant for a considerable period,resulting in a scarcity of comprehensive reviews on this topic.Therefore,based on the latest research findings,this paper summarizes and consolidates the construction strategies for metal vacancies,characterization techniques,and their roles in typical energy and environmental catalytic reactions.Additionally,it outlines potential challenges in the future,aiming to provide valuable references for researchers interested in investigating metal vacancies.展开更多
The risk of flammability is an unavoidable issue for gel polymer electrolytes(GPEs).Usually,flameretardant solvents are necessary to be used,but most of them would react with anode/cathode easily and cause serious int...The risk of flammability is an unavoidable issue for gel polymer electrolytes(GPEs).Usually,flameretardant solvents are necessary to be used,but most of them would react with anode/cathode easily and cause serious interfacial instability,which is a big challenge for design and application of nonflammable GPEs.Here,a nonflammable GPE(SGPE)is developed by in situ polymerizing trifluoroethyl methacrylate(TFMA)monomers with flame-retardant triethyl phosphate(TEP)solvents and LiTFSI–LiDFOB dual lithium salts.TEP is strongly anchored to PTFMA matrix via polarity interaction between-P=O and-CH_(2)CF_(3).It reduces free TEP molecules,which obviously mitigates interfacial reactions,and enhances flame-retardant performance of TEP surprisingly.Anchored TEP molecules are also inhibited in solvation of Li^(+),leading to anion-dominated solvation sheath,which creates inorganic-rich solid electrolyte interface/cathode electrolyte interface layers.Such coordination structure changes Li^(+)transport from sluggish vehicular to fast structural transport,raising ionic conductivity to 1.03 mS cm^(-1) and transfer number to 0.41 at 30℃.The Li|SGPE|Li cell presents highly reversible Li stripping/plating performance for over 1000 h at 0.1 mA cm^(−2),and 4.2 V LiCoO_(2)|SGPE|Li battery delivers high average specific capacity>120 mAh g^(−1) over 200 cycles.This study paves a new way to make nonflammable GPE that is compatible with Li metal anode.展开更多
Porous organic cages(POCs)with permanent porosity and excellent host–guest property hold great potentials in regulating ion transport behavior,yet their feasibility as solid-state electrolytes has never been testifie...Porous organic cages(POCs)with permanent porosity and excellent host–guest property hold great potentials in regulating ion transport behavior,yet their feasibility as solid-state electrolytes has never been testified in a practical battery.Herein,we design and fabricate a quasi-solid-state electrolyte(QSSE)based on a POC to enable the stable operation of Li-metal batteries(LMBs).Benefiting from the ordered channels and cavity-induced anion-trapping effect of POC,the resulting POC-based QSSE exhibits a high Li+transference number of 0.67 and a high ionic conductivity of 1.25×10^(−4) S cm^(−1) with a low activation energy of 0.17 eV.These allow for homogeneous Li deposition and highly reversible Li plating/stripping for over 2000 h.As a proof of concept,the LMB assembled with POC-based QSSE demonstrates extremely stable cycling performance with 85%capacity retention after 1000 cycles.Therefore,our work demonstrates the practical applicability of POC as SSEs for LMBs and could be extended to other energy-storage systems,such as Na and K batteries.展开更多
Accurately predicting the powder factor during blasting is essential for sustainable production planning in low-grade mines.This research presents a method for predicting powder factor based on the heterogeneity of ro...Accurately predicting the powder factor during blasting is essential for sustainable production planning in low-grade mines.This research presents a method for predicting powder factor based on the heterogeneity of rock mass rating(RMR).Considering a low-grade metal mine as an example,this study exploited geostatistical methods to obtain independent RMR for each block unit.A three-dimensional spatial distribution model for the powder factor was developed on the basis of the relationships between the RMR and the powder factor.Subsequently,models for blasting cost and mining value were built and employed to optimize the open-pit limit.The multi-variable model based on the RMR performed well in predicting the powder factor,achieving a correlation coefficient of 0.88(root mean square error of 4.3)and considerably outperforming the uniaxial compressive strength model.After model optimization,the mean size and standard deviation of the fragments in the blast pile decreased by 8.5%and 35.1%,respectively,whereas the boulder yield and its standard deviation decreased by 33.3%and 58.8%,respectively.Additionally,optimizing the open-pit limit using this method reduced the amount of rock,increased the amount of ore,and lowered blasting costs,thereby enhancing the economic efficiency of the mine.This study provides valuable insights for blasting design and mining decisions,demonstrating the advantages and potential applications of powder factor prediction based on the heterogeneity of rock mass quality.展开更多
Lithium plating/stripping occurs at the a node/electrolyte interface which involves the flow of electrons from the current collector and the migration of lithium ions from the solid-electrolyte interphase(SEI).The dua...Lithium plating/stripping occurs at the a node/electrolyte interface which involves the flow of electrons from the current collector and the migration of lithium ions from the solid-electrolyte interphase(SEI).The dual continuous rapid transport of interfacial electron/ion is required for homogeneous Li deposition.Herein,we propose a strategy to improve the Li metal anode performance by rationally regulating the interfacial electron density and Li ion transport through the SEI film.This key technique involves decreasing the interfacial oxygen density of biomass-derived carbon host by regulating the arrangement of the celluloses precursor fibrils.The higher specific surface area and lower interfacial oxygen density decrease the local current density and ensure the formation of thin and even SEI film,which stabilized Li^(+)transfer through the Li/electrolyte interface.Moreover,the improved graphitization and the interconnected conducting network enhance the surface electronegativity of carbon and enable uninterruptible electron conduction.The result is continuous and rapid coupled interfacial electron/ion transport at the anode/electrolyte reaction interface,which facilitates uniform Li deposition and improves Li anode performance.The Li/C anode shows a high initial Coulombic efficiency of 98%and a long-term lifespan of over 150cycles at a practical low N/P(negative-to-positive)ratio of 1.44 in full cells.展开更多
This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abun...This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm^(-2)in 1 M KOH,respectively.As both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm^(-2)and exhibited high structural robustness,maintaining stability at 1000 mA cm^(-2)for 300 h.In-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water oxidation.Additionally,ultraviolet photoelectron spectroscopy(UPS)and density functional theory(DFT)analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER activities.This study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.展开更多
A thermodynamically complete multi-phase equation of state(EOS)applicable to both dense and porous metals at wide ranges of temperature and pressure is constructed.A standard three-term decomposition of the Helmholtz ...A thermodynamically complete multi-phase equation of state(EOS)applicable to both dense and porous metals at wide ranges of temperature and pressure is constructed.A standard three-term decomposition of the Helmholtz free energy as a function of specific volume and temperature is presented,where the cold component models both compression and expansion states,the thermal ion component introduces the Debye approximation and melting entropy,and the thermal electron component employs the Thomas-Fermi-Kirzhnits(TFK)model.The porosity of materials is considered by introducing the dynamic porosity coefficientαand the constitutive P-αrelation,connecting the thermodynamic properties between dense and porous systems,allowing for an accurate description of the volume decrease caused by void collapse while maintaining the quasi-static thermodynamic properties of porous systems identical to the dense ones.These models enable the EOS applicable and robust at wide ranges of temperature,pressure and porosity.A systematic evaluation of the new EOS is conducted with aluminum(Al)as an example.300 K isotherm,shock Hugoniot,as well as melting curves of both dense and porous Al are calculated,which shows great agreements with experimental data and validates the effectiveness of the models and the accuracy of parameterizations.Notably,it is for the first time Hugoniot P-σcurves up to 10~6 GPa and shock melting behaviors of porous Al are derived from analytical EOS models,which predict much lower compression limit and shock melting temperatures than those of dense Al.展开更多
Co_(3)O_(4)possesses both direct and indirect oxidation effects and is considered as a promising catalyst for the oxidation of 5-hydroxymethylfurfural(HMF).However,the enrichment and activation effects of Co_(3)O_(4)o...Co_(3)O_(4)possesses both direct and indirect oxidation effects and is considered as a promising catalyst for the oxidation of 5-hydroxymethylfurfural(HMF).However,the enrichment and activation effects of Co_(3)O_(4)on OH-and HMF are weak,which limits its further application.Metal defect engineering can regulate the electronic structure,optimize the adsorption of intermediates,and improve the catalytic activity by breaking the symmetry of the material,which is rarely involved in the upgrading of biomass.In this work,we prepare Co_(3)O_(4)with metal defects and load the precious metal platinum at the defect sites(PtVco).The results of in-situ characterizatio ns,electrochemical measurements,and theoretical calculations indicate that the reduction of Co-Co coordination number and the formation of Pt-Co bond induce the decrease of electron filling in the antibonding orbitals of Co element.The resulting upward shift of the d-band center of Co combined with the characteristic adsorption of Pt species synergically enhances the enrichment and activation of organic molecules and OH species,thus exhibiting excellent HMF oxidation activity(including a lower onset potential(1.14 V)and 19 times higher current density than pure Co_(3)O_(4)at 1.35 V).In summary,this work explores the adsorption enhancement mechanism of metal defect sites modified by precious metal in detail,provides a new option for improving the HMF oxidation activity of cobalt-based materials,broadens the application field of metal defect based materials,and gives an innovative guidance for the functional utilization of metal defect sites in biomass conversion.展开更多
The discovery of phase changings in two-dimensional(2D)materials driven by external stimuli not only helps to understand the various intriguing phases in 2D materials but also provides directions for constructing new ...The discovery of phase changings in two-dimensional(2D)materials driven by external stimuli not only helps to understand the various intriguing phases in 2D materials but also provides directions for constructing new functional devices.Here,by combining angle-resolved photoemission spectroscopy(ARPES)and in-situ alkali-metal deposition,we studied how alkali-metal adatoms affect the electronic structure of T_(d)-WTe_(2)on two different cleaved surfaces.We found that depending on the polarization direction of the cleaved surface,the alkali-metal deposition triggered two successive phase transitions on one surface of WTe_(2),while on the other surface,no phase transition was found.We attributed the observed phase transitions to a Td↑-1T′-Td↓structural transition driven by an alkali-metal induced sliding of WTe2layers.By comparing the band structure obtained in different structural phases of WTe_(2),we found that the evolution of band structure across different phases is characterized by an energy scale that could be related to the degree of orbital hybridization between two adjacent WTe_(2)layers.Our results demonstrate a method that manipulates the surface structure of bulk 2D materials.It also builds a direct correlation between the electronic structure and the degree of interlayer misalignment in this intriguing 2D material.展开更多
Thick electrodes can reduce the ratio of inactive constituents in a holistic energy storage system while improving energy and power densities.Unfortunately,traditional slurry-casting electrodes induce high-tortuous io...Thick electrodes can reduce the ratio of inactive constituents in a holistic energy storage system while improving energy and power densities.Unfortunately,traditional slurry-casting electrodes induce high-tortuous ionic diffusion routes that directly depress the capacitance with a thickening design.To overcome this,a novel 3D low-tortuosity,self-supporting,wood-structured ultrathick electrode(NiMoN@WC,a thickness of~1400 mm)with hierarchical porosity and artificial array-distributed small holes was constructed via anchoring bimetallic nitrides into the monolithic wood carbons.Accompanying the embedded NiMoN nanoclusters with well-designed geometric and electronic structure,the vertically low-tortuous channels,enlarged specific surface area and pore volume,superhydrophilic interface,and excellent charge conductivities,a superior capacitance of NiMoN@WC thick electrodes(~5350 mF cm^(-2)and 184.5 F g^(-1))is achieved without the structural deformation.In especial,monolithic wood carbons with gradient porous network not only function as the high-flux matrices to ameliorate the NiMoN loading via cell wall engineering but also allow fully-exposed electroactive substance and efficient current collection,thereby deliver an acceptable rate capability over 75%retention even at a high sweep rate of 20 mA cm^(-2).Additionally,an asymmetric NiMoN@WC//WC supercapacitor with an available working voltage of 1.0-1.8 V is assembled to demonstrate a maximum energy density of~2.04 mWh cm^(-2)(17.4 Wh kg^(-1))at a power density of 1620 mW cm^(-2),along with a decent long-term lifespan over 10,000 charging-discharging cycles.As a guideline,the rational design of wood ultrathick electrode with nanostructured transition metal nitrides sketch a promising blueprint for alleviating global energy scarcity while expanding carbon-neutral technologies.展开更多
Fluorinated gases(F-gases)play a vital role in the chemical industry and in the fields of air conditioning,refrigeration,health care,and organic synthesis.However,the direct emission of waste gases containing F-gases ...Fluorinated gases(F-gases)play a vital role in the chemical industry and in the fields of air conditioning,refrigeration,health care,and organic synthesis.However,the direct emission of waste gases containing F-gases into the atmosphere contributes to greenhouse effects and generates toxic substances.Developing porous materials for the energy-efficient capture,separation,and recovery of F-gases is highly desired.Recently,as a highly designable porous adsorbents,metal–organic frameworks(MOFs)exhibit excellent selective sorption performance toward F-gases,especially for the recognition and separation of different F-gases with highly similar properties,showing their great potential in F-gases control and recovery.In this review,we discuss the capture and separation of F-gases and their azeotropic,near-azeotropic,and isomeric mixtures in various application scenarios by MOFs,specifically classify and analyze molecular interaction between F-gases and MOFs,and interpret the mechanisms underlying their high performance regarding both adsorption capacity and selectivity,providing a repertoire for future materials design.Challenges faced in the transformation research roadmap of MOFs adsorbent separation technologies toward F-gases are also discussed,and areas for future research endeavors are highlighted.展开更多
Two-dimensional transition metal dichalcogenides(2D TMDCs)have received considerable attention in local strain engineering due to their extraordinary mechanical flexibility,electonic structure,and optical properties.T...Two-dimensional transition metal dichalcogenides(2D TMDCs)have received considerable attention in local strain engineering due to their extraordinary mechanical flexibility,electonic structure,and optical properties.The strain-induced out-of-plane deformations in 2D TMDCs lead to diverse excitonic behaviors and versatile modulations in optical properties,paving the way for the development of advanced quantum technologies,flexible optoelectronic materials,and straintronic devices.Research on local strain engineering on 2D TMDCs has been delved into fabrication techniques,electronic state variations,and quantum optical applications.This review begins by summarizing the state-of-the-art methods for introducing local strain into 2D TMDCs,followed by an exploration of the impact of local strain engineering on optical properties.The intriguing phenomena resulting from local strain,such as exciton funnelling and anti-funnelling,are also discussed.We then shift the focus to the application of locally strained 2D TMDCs as quantum emitters,with various strategies outlined for modulating the properties of TMDC-based quantum emitters.Finally,we discuss the remaining questions in this field and provide an outlook on the future of local strain engineering on 2D TMDCs.展开更多
Aqueous zinc-ion batteries(AZIBs)present a promising option for next-generation batteries given their high safety,eco-friendliness,and resource sustainability.Nonetheless,the practical application of zinc anodes is hi...Aqueous zinc-ion batteries(AZIBs)present a promising option for next-generation batteries given their high safety,eco-friendliness,and resource sustainability.Nonetheless,the practical application of zinc anodes is hindered by inevitable parasitic reactions and dendrite growth.Here,zinc alloy layers(i.e.,ZnCo and ZnFe alloys)were rationally constructed on the zinc surface by chemical displacement reactions.The alloying process exposes more(002)planes of the ZnCo anode to guide the preferential and dendrite-free zinc deposition.Furthermore,the ZnCo alloy layer not only effectively inhibits water-induced side reactions but also accelerates electrode kinetics,enabling highly reversible zinc plating/stripping.As a result,the ZnCo anode achieves a Coulombic efficiency of 99.2%over 1300 cycles,and the ZnCo symmetric cell exhibits a long cycle life of over 2000 h at 4.4 mA cm^(-2).Importantly,the ZnCo//NH_(4)V_(4)O_(10)full cell retains a high discharge capacity of 218.4 mAh g^(-1)after 800 cycles.Meanwhile,the ZnFe-based symmetric cell also displays excellent cycling stability over 2500 h at 1.77 mA cm^(-2).This strategy provides a facile anode modification approach toward high-performance AZIBs.展开更多
Practical Zn metal batteries have been hindered by several challenges,including Zn dendrite growth,undesirable side reactions,and unstable electrode/electrolyte interface.These issues are particularly more serious in ...Practical Zn metal batteries have been hindered by several challenges,including Zn dendrite growth,undesirable side reactions,and unstable electrode/electrolyte interface.These issues are particularly more serious in low-concentration electrolytes.Herein,we design a Zn salt-mediated electrolyte with in situ ring-opening polymerization of the small molecule organic solvent.The Zn(TFSI)_(2)salt catalyzes the ring-opening polymerization of(1,3-dioxolane(DOL)),generating oxidation-resistant and non-combustible long-chain polymer(poly(1,3-dioxolane)(pDOL)).The pDOL reduces the active H_(2)O molecules in electrolyte and assists in forming stable organic–inorganic gradient solid electrolyte interphase with rich organic constituents,ZnO and ZnF_(2).The introduction of pDOL endows the electrolyte with several advantages:excellent Zn dendrite inhibition,improved corrosion resistance,widened electrochemical window(2.6 V),and enhanced low-temperature performance(freezing point=-34.9°C).Zn plating/stripping in pDOL-enhanced electrolyte lasts for 4200 cycles at 99.02%Coulomb efficiency and maintains a lifetime of 8200 h.Moreover,Zn metal anodes deliver stable cycling for 2500 h with a high Zn utilization of 60%.A Zn//VO_(2)pouch cell assembled with lean electrolyte(electrolyte/capacity(E/C=41 mL(Ah)^(-1))also demonstrates a capacity retention ratio of 92%after 600 cycles.These results highlight the promising application prospects of practical Zn metal batteries enabled by the Zn(TFSI)2-mediated electrolyte engineering.展开更多
Aqueous Zn ion batteries(ZIBs)have received extensive attention due to their intrinsic safety,high abundance,and low cost.However,uncontrolled dendrite growth and water-induced side reactions at electrod e/electrolyte...Aqueous Zn ion batteries(ZIBs)have received extensive attention due to their intrinsic safety,high abundance,and low cost.However,uncontrolled dendrite growth and water-induced side reactions at electrod e/electrolyte interfaces hinder the advancement of ZIBs.Herein,density functional theory(DFT)calculation indicates that Zn heptafluorobutyrate can facilitate uniform Zn^(2+)deposition by leveraging the abundant zincophilic groups(e.g.,-COO^(-)and-CF)and inhibit water-induced side reactions due to the presence of hydrophobic carbon chains.A Zn heptafluorobutyrate protective layer(denoted as ZFA)is constructed on the metallic Zn surface in situ by acid etching process to control Zn^(2+)desolvation and nucleation behaviors,ensuring enhanced reversibility and stability of Zn anodes.Consequently,the Zn@ZFA anode demonstrates stable operation for more than 2200 h at 1 mA cm^(-2)and over 7300cycles at 40 mA cm^(-2),with high Coulombic efficiency of 99.8%over 1900 cycles at 5 mA cm^(-2).Impressively,Zn@ZFA‖VO_(2)full cell achieves exceptional cycle life(204 mA h g^(-1)after 750 cycles at 3 A g^(-1))and remarkable rate performance(236 mA g^(-1)at 10 A g^(-1)).This work provides an insightful guidance for constructing a protection layer of dendrite-free Zn anodes for high-performance ZIBs.展开更多
The glass-forming ability(GFA)of metallic glasses is a key scientific challenge in their development and application,with compositional dependence playing a crucial role.Experimental studies have demonstrated that the...The glass-forming ability(GFA)of metallic glasses is a key scientific challenge in their development and application,with compositional dependence playing a crucial role.Experimental studies have demonstrated that the addition of specific minor elements can greatly enhance the GFA of parent alloys,yet the underlying mechanism remains unclear.In this study,we use the ZrCuAl system as a model to explore how the addition of minor Al influences the crystallization rate by modulating the properties of the crystal-liquid interface,thereby affecting the GFA.The results reveal that the minor addition of Al significantly reduces the crystal growth rate,a phenomenon not governed by particle density fluctuations at the interface.The impact of minor element additions extends beyond a modest increase in crystal-unfavorable motifs in the bulk supercooled liquid.More importantly,it leads to a significant enrichment of these motifs at the crystal-supercooled liquid interface,forming a dense topological network of crystal-unfavorable structures that effectively prevent the growth of the crystalline interface and enhance GFA.Our results provide valuable insights for the design and development of high-performance metallic glasses.展开更多
Micron-sized silicon(μSi)is a promising anode material for next-generation lithium-ion batteries due to its high specific capacity,low cost,and abundant reserves.However,the volume expansion that occurs during cyclin...Micron-sized silicon(μSi)is a promising anode material for next-generation lithium-ion batteries due to its high specific capacity,low cost,and abundant reserves.However,the volume expansion that occurs during cycling leads to the accumulation of undesirable stresses,resulting in pulverization of silicon microparticles and shortened lifespan of the batteries.Herein,a composite film of Cu-PET-Cu is proposed as the current collector(CC)forμSi anodes to replace the conventional Cu CC.Cu-PET-Cu CC is prepared by depositing Cu on both sides of a polyethylene terephthalate(PET)film.The PET layer promises good ductility of the film,permitting the Cu-PET-Cu CC to accommodate the volumetric changes of silicon microparticles and facilitates the stress release through ductile deformation.As a result,theμSi electrode with Cu-PET-Cu CC retains a high specific capacity of 2181 mA h g^(-1),whereas theμSi electrode with Cu CC(μSi/Cu)exhibits a specific capacity of 1285 mA h g^(-1)after 80 cycles.The stress relieving effect of CuPET-Cu was demonstrated by in-situ fiber optic stress monitoring and multi-physics simulations.This work proposes an effective stress relief strategy at the electrode level for the practical implementation ofμSi anodes.展开更多
Lithium metal batteries(LMBs)with high energy density are impeded by the instability of solid electrolyte interface(SEI)and the uncontrolled growth of lithium(Li)dendrite.To mitigate these challenges,optimizing the SE...Lithium metal batteries(LMBs)with high energy density are impeded by the instability of solid electrolyte interface(SEI)and the uncontrolled growth of lithium(Li)dendrite.To mitigate these challenges,optimizing the SEI structure and Li deposition behavior is the key to stable LMBs.This study novelty proposes a facile synthesis of MgF_(2)/carbon(C)nanocomposite through the mechanochemical reaction between metallic Mg and polytetrafluoroethylene(PTFE)powders,and its modified polypropylene(PP)separator enhances LMB performance.The in-situ formed highly conductive fluorine-doped C species play a crucial role in facilitating ion/electron transport,thereby accelerating electrochemical kinetics and altering Li deposition direction.During cycling,the in-situ reaction between MgF_(2)and Li leads to the formation of LiMg alloy,along with a LiF-rich SEI layer,which reduces the nucleation overpotential and reinforces the interphase strength,leading to homogeneous Li deposition with dendrite-free feature.Benefiting from these merits,the Li metal is densely and uniformly deposited on the MgF_(2)/C@PP separator side rather than on the current collector side.Furthermore,the symmetric cell with MgF_(2)/C@PP exhibits superb Li plating/stripping performance over 2800 h at 1 mA cm^(-2)and 2 mA h cm^(-2).More importantly,the assembled Li@MgF_(2)/C@PPILiFePO4full cell with a low negative/positive ratio of 3.6delivers an impressive cyclability with 82.7%capacity retention over 1400 cycles at 1 C.展开更多
Scrap metals are typically covered with surface contaminants,such as paint,dust,and rust,which can significantly affect the emission spectrum during laser-induced breakdown spectroscopy(LIBS)based sorting.In this stud...Scrap metals are typically covered with surface contaminants,such as paint,dust,and rust,which can significantly affect the emission spectrum during laser-induced breakdown spectroscopy(LIBS)based sorting.In this study,the effects of paint layers on metal surfaces during LIBS classification were investigated.LIBS spectra were collected from metal surfaces painted with black and white paints by ablation with a nanosecond pulsed laser(wavelength=1064 nm,pulse width=7 ns).For the black-painted samples,the LIBS spectra showed a broad background emission,emission lines unrelated to the target metals,large shot-to-shot variation,and a relatively low signal intensity of the target metal,causing poor classification accuracy even at high shot numbers.Cleaning the black paint layer by ablating over a wide area prior to LIBS analysis resulted in high classification accuracy with fewer shot numbers.A method to determine the number of cleaning shots necessary to obtain high classification accuracy and high throughput is proposed on the basis of the change in LIBS signal intensity during cleaning shots.For the white-painted samples,the paint peeled off the metal surface after the first shot,and strong LIBS signals were measured after the following shot,which were attributed to the nanoparticles generated by the ablation of the paint,allowing an accurate classification after only two shots.The results demonstrate that different approaches must be employed depending on the paint color to achieve high classification accuracy with fewer shot numbers.展开更多
Solar-driven interfacial evaporation is one of the most attractive approaches to addressing the global freshwater shortage.However,achieving an integrated high evaporation rate,salt harvesting,and multifunctionality i...Solar-driven interfacial evaporation is one of the most attractive approaches to addressing the global freshwater shortage.However,achieving an integrated high evaporation rate,salt harvesting,and multifunctionality in evaporator is still a crucial challenge.Here,a novel composite membrane with biomimetic micronanostructured superhydrophobic surface is designed via ultrafast laser etching technology.Attractively,the double-transition-metal(V_(1/2)Mo_(1/2))_(2)CT_(x)MXene nanomaterials as a photothermal layer,exhibiting the enhanced photothermal conversion performance due to elevated joint densities of states,which enables high populations of photoexcited carrier relaxation and heat release,provides a new insight into the photothermal conversion mechanism for multiple principal element MXene.Hence,the(V_(1/2)Mo_(1/2))_(2)CT_(x)MXene-200 composite membrane can achieve a high evaporation rate of 2.23 kg m^(−2)h^(−1)under one sun,owing to the enhanced“light trap”effect,photothermal conversion,and high-throughput water transfer.Synergetically,the membrane can induce the directed precipitation of salt at the membrane edge,thus enabling salt harvesting for recycling and zero-emission of brine water.Moreover,the composite membrane is endowed with excellent multifunctionality of anti-/de-icing,anti-fouling,and antibacterial,overcoming the disadvantage that versatility is difficult to be compatible.Therefore,the evaporator and the promising strategy hold great potential for the practical application of solar evaporation.展开更多
基金financially supported by National Key R&D Program of China(2021YFB3500702)National Natural Science Foundation of China(Nos.21677010 and 51808037)Special fund of Beijing Key Laboratory of Indoor Air Quality Evaluation and Control(No.BZ0344KF21-04).
文摘With the ongoing depletion of fossil fuels,energy and environmental issues have become increasingly critical,necessitating the search for effective solutions.Catalysis,being one of the hallmarks of modern industry,offers a promising avenue for researchers.However,the question of how to significantly enhance the performance of catalysts has gradually drawn the attention of scholars.Defect engineering,a commonly employed and effective approach to improve catalyst activity,has become a significant research focus in the catalysis field in recent years.Nonmetal vacancies have received extensive attention due to their simple form.Consequently,exploration of metal vacancies has remained stagnant for a considerable period,resulting in a scarcity of comprehensive reviews on this topic.Therefore,based on the latest research findings,this paper summarizes and consolidates the construction strategies for metal vacancies,characterization techniques,and their roles in typical energy and environmental catalytic reactions.Additionally,it outlines potential challenges in the future,aiming to provide valuable references for researchers interested in investigating metal vacancies.
基金supported by the National Natural Science Foundation of China(Nos.52172214,52272221,52171182)the Postdoctoral Innovation Project of Shandong Province(No.202102003)+2 种基金The Key Research and Development Program of Shandong Province(2021ZLGX01)the Qilu Young Scholar ProgramHPC Cloud Platform of Shandong University are also thanked.
文摘The risk of flammability is an unavoidable issue for gel polymer electrolytes(GPEs).Usually,flameretardant solvents are necessary to be used,but most of them would react with anode/cathode easily and cause serious interfacial instability,which is a big challenge for design and application of nonflammable GPEs.Here,a nonflammable GPE(SGPE)is developed by in situ polymerizing trifluoroethyl methacrylate(TFMA)monomers with flame-retardant triethyl phosphate(TEP)solvents and LiTFSI–LiDFOB dual lithium salts.TEP is strongly anchored to PTFMA matrix via polarity interaction between-P=O and-CH_(2)CF_(3).It reduces free TEP molecules,which obviously mitigates interfacial reactions,and enhances flame-retardant performance of TEP surprisingly.Anchored TEP molecules are also inhibited in solvation of Li^(+),leading to anion-dominated solvation sheath,which creates inorganic-rich solid electrolyte interface/cathode electrolyte interface layers.Such coordination structure changes Li^(+)transport from sluggish vehicular to fast structural transport,raising ionic conductivity to 1.03 mS cm^(-1) and transfer number to 0.41 at 30℃.The Li|SGPE|Li cell presents highly reversible Li stripping/plating performance for over 1000 h at 0.1 mA cm^(−2),and 4.2 V LiCoO_(2)|SGPE|Li battery delivers high average specific capacity>120 mAh g^(−1) over 200 cycles.This study paves a new way to make nonflammable GPE that is compatible with Li metal anode.
基金supported by the National Natural Science Foundation of China(No.92372123)Guangdong Basic and Applied Basic Research Foundation(No.2022A1515012057,2022B1515020005,2023B1515130004)Guangzhou Basic and Applied Basic Research Foundation(No.202201011342).
文摘Porous organic cages(POCs)with permanent porosity and excellent host–guest property hold great potentials in regulating ion transport behavior,yet their feasibility as solid-state electrolytes has never been testified in a practical battery.Herein,we design and fabricate a quasi-solid-state electrolyte(QSSE)based on a POC to enable the stable operation of Li-metal batteries(LMBs).Benefiting from the ordered channels and cavity-induced anion-trapping effect of POC,the resulting POC-based QSSE exhibits a high Li+transference number of 0.67 and a high ionic conductivity of 1.25×10^(−4) S cm^(−1) with a low activation energy of 0.17 eV.These allow for homogeneous Li deposition and highly reversible Li plating/stripping for over 2000 h.As a proof of concept,the LMB assembled with POC-based QSSE demonstrates extremely stable cycling performance with 85%capacity retention after 1000 cycles.Therefore,our work demonstrates the practical applicability of POC as SSEs for LMBs and could be extended to other energy-storage systems,such as Na and K batteries.
基金supported by the National Key Research and Development Program of China(No.2022YFC2903902)the National Natural Science Foundation of China(Nos.52204080and 52174070)the Fundamental Research Funds for the Central Universities of China(No.2023GFYD17)。
文摘Accurately predicting the powder factor during blasting is essential for sustainable production planning in low-grade mines.This research presents a method for predicting powder factor based on the heterogeneity of rock mass rating(RMR).Considering a low-grade metal mine as an example,this study exploited geostatistical methods to obtain independent RMR for each block unit.A three-dimensional spatial distribution model for the powder factor was developed on the basis of the relationships between the RMR and the powder factor.Subsequently,models for blasting cost and mining value were built and employed to optimize the open-pit limit.The multi-variable model based on the RMR performed well in predicting the powder factor,achieving a correlation coefficient of 0.88(root mean square error of 4.3)and considerably outperforming the uniaxial compressive strength model.After model optimization,the mean size and standard deviation of the fragments in the blast pile decreased by 8.5%and 35.1%,respectively,whereas the boulder yield and its standard deviation decreased by 33.3%and 58.8%,respectively.Additionally,optimizing the open-pit limit using this method reduced the amount of rock,increased the amount of ore,and lowered blasting costs,thereby enhancing the economic efficiency of the mine.This study provides valuable insights for blasting design and mining decisions,demonstrating the advantages and potential applications of powder factor prediction based on the heterogeneity of rock mass quality.
基金supported by the National Natural Science Foundation of China(21975091,22122902,and 52272208)the Fundamental Research Fund for the Central Universities of China(2662023LXPY001 and 2662021JC004).
文摘Lithium plating/stripping occurs at the a node/electrolyte interface which involves the flow of electrons from the current collector and the migration of lithium ions from the solid-electrolyte interphase(SEI).The dual continuous rapid transport of interfacial electron/ion is required for homogeneous Li deposition.Herein,we propose a strategy to improve the Li metal anode performance by rationally regulating the interfacial electron density and Li ion transport through the SEI film.This key technique involves decreasing the interfacial oxygen density of biomass-derived carbon host by regulating the arrangement of the celluloses precursor fibrils.The higher specific surface area and lower interfacial oxygen density decrease the local current density and ensure the formation of thin and even SEI film,which stabilized Li^(+)transfer through the Li/electrolyte interface.Moreover,the improved graphitization and the interconnected conducting network enhance the surface electronegativity of carbon and enable uninterruptible electron conduction.The result is continuous and rapid coupled interfacial electron/ion transport at the anode/electrolyte reaction interface,which facilitates uniform Li deposition and improves Li anode performance.The Li/C anode shows a high initial Coulombic efficiency of 98%and a long-term lifespan of over 150cycles at a practical low N/P(negative-to-positive)ratio of 1.44 in full cells.
基金National Programs for NanoKey Project(2022YFA1504002)National Natural Science Foundation of China(22078233)。
文摘This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm^(-2)in 1 M KOH,respectively.As both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm^(-2)and exhibited high structural robustness,maintaining stability at 1000 mA cm^(-2)for 300 h.In-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water oxidation.Additionally,ultraviolet photoelectron spectroscopy(UPS)and density functional theory(DFT)analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER activities.This study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12205023,U2230401,12374056,U23A20537,11904027)。
文摘A thermodynamically complete multi-phase equation of state(EOS)applicable to both dense and porous metals at wide ranges of temperature and pressure is constructed.A standard three-term decomposition of the Helmholtz free energy as a function of specific volume and temperature is presented,where the cold component models both compression and expansion states,the thermal ion component introduces the Debye approximation and melting entropy,and the thermal electron component employs the Thomas-Fermi-Kirzhnits(TFK)model.The porosity of materials is considered by introducing the dynamic porosity coefficientαand the constitutive P-αrelation,connecting the thermodynamic properties between dense and porous systems,allowing for an accurate description of the volume decrease caused by void collapse while maintaining the quasi-static thermodynamic properties of porous systems identical to the dense ones.These models enable the EOS applicable and robust at wide ranges of temperature,pressure and porosity.A systematic evaluation of the new EOS is conducted with aluminum(Al)as an example.300 K isotherm,shock Hugoniot,as well as melting curves of both dense and porous Al are calculated,which shows great agreements with experimental data and validates the effectiveness of the models and the accuracy of parameterizations.Notably,it is for the first time Hugoniot P-σcurves up to 10~6 GPa and shock melting behaviors of porous Al are derived from analytical EOS models,which predict much lower compression limit and shock melting temperatures than those of dense Al.
基金financially supported by the Natural Science Foundation of Shandong Province(ZR2023QB235,ZR202111240183,ZR2021QF120)the Postdoctoral Science Foundation of China(2022M711956)the Taishan Scholar Program of Shandong Province(tsqnz20231216).
文摘Co_(3)O_(4)possesses both direct and indirect oxidation effects and is considered as a promising catalyst for the oxidation of 5-hydroxymethylfurfural(HMF).However,the enrichment and activation effects of Co_(3)O_(4)on OH-and HMF are weak,which limits its further application.Metal defect engineering can regulate the electronic structure,optimize the adsorption of intermediates,and improve the catalytic activity by breaking the symmetry of the material,which is rarely involved in the upgrading of biomass.In this work,we prepare Co_(3)O_(4)with metal defects and load the precious metal platinum at the defect sites(PtVco).The results of in-situ characterizatio ns,electrochemical measurements,and theoretical calculations indicate that the reduction of Co-Co coordination number and the formation of Pt-Co bond induce the decrease of electron filling in the antibonding orbitals of Co element.The resulting upward shift of the d-band center of Co combined with the characteristic adsorption of Pt species synergically enhances the enrichment and activation of organic molecules and OH species,thus exhibiting excellent HMF oxidation activity(including a lower onset potential(1.14 V)and 19 times higher current density than pure Co_(3)O_(4)at 1.35 V).In summary,this work explores the adsorption enhancement mechanism of metal defect sites modified by precious metal in detail,provides a new option for improving the HMF oxidation activity of cobalt-based materials,broadens the application field of metal defect based materials,and gives an innovative guidance for the functional utilization of metal defect sites in biomass conversion.
基金Project supported by the National Key Research and Development Program of China(Grant No.2022YFA1403502)the National Natural Science Foundation of China(Grant No.11888101)。
文摘The discovery of phase changings in two-dimensional(2D)materials driven by external stimuli not only helps to understand the various intriguing phases in 2D materials but also provides directions for constructing new functional devices.Here,by combining angle-resolved photoemission spectroscopy(ARPES)and in-situ alkali-metal deposition,we studied how alkali-metal adatoms affect the electronic structure of T_(d)-WTe_(2)on two different cleaved surfaces.We found that depending on the polarization direction of the cleaved surface,the alkali-metal deposition triggered two successive phase transitions on one surface of WTe_(2),while on the other surface,no phase transition was found.We attributed the observed phase transitions to a Td↑-1T′-Td↓structural transition driven by an alkali-metal induced sliding of WTe2layers.By comparing the band structure obtained in different structural phases of WTe_(2),we found that the evolution of band structure across different phases is characterized by an energy scale that could be related to the degree of orbital hybridization between two adjacent WTe_(2)layers.Our results demonstrate a method that manipulates the surface structure of bulk 2D materials.It also builds a direct correlation between the electronic structure and the degree of interlayer misalignment in this intriguing 2D material.
基金support from the National Natural Science Foundation of China(32171728)Wuhan Knowledge Innovation Project(2022020801020312).
文摘Thick electrodes can reduce the ratio of inactive constituents in a holistic energy storage system while improving energy and power densities.Unfortunately,traditional slurry-casting electrodes induce high-tortuous ionic diffusion routes that directly depress the capacitance with a thickening design.To overcome this,a novel 3D low-tortuosity,self-supporting,wood-structured ultrathick electrode(NiMoN@WC,a thickness of~1400 mm)with hierarchical porosity and artificial array-distributed small holes was constructed via anchoring bimetallic nitrides into the monolithic wood carbons.Accompanying the embedded NiMoN nanoclusters with well-designed geometric and electronic structure,the vertically low-tortuous channels,enlarged specific surface area and pore volume,superhydrophilic interface,and excellent charge conductivities,a superior capacitance of NiMoN@WC thick electrodes(~5350 mF cm^(-2)and 184.5 F g^(-1))is achieved without the structural deformation.In especial,monolithic wood carbons with gradient porous network not only function as the high-flux matrices to ameliorate the NiMoN loading via cell wall engineering but also allow fully-exposed electroactive substance and efficient current collection,thereby deliver an acceptable rate capability over 75%retention even at a high sweep rate of 20 mA cm^(-2).Additionally,an asymmetric NiMoN@WC//WC supercapacitor with an available working voltage of 1.0-1.8 V is assembled to demonstrate a maximum energy density of~2.04 mWh cm^(-2)(17.4 Wh kg^(-1))at a power density of 1620 mW cm^(-2),along with a decent long-term lifespan over 10,000 charging-discharging cycles.As a guideline,the rational design of wood ultrathick electrode with nanostructured transition metal nitrides sketch a promising blueprint for alleviating global energy scarcity while expanding carbon-neutral technologies.
基金funded by the National Key Research and Development Program of China(2022YFE0110500)National Natural Science Foundation of China(22376161,52373154,52103181)+1 种基金the Fundamental Research Funds for the Central Universities of Chinathe Interdisciplinary Project in Environmental Science and Engineering of Tongji University(2023-3-YB-02)。
文摘Fluorinated gases(F-gases)play a vital role in the chemical industry and in the fields of air conditioning,refrigeration,health care,and organic synthesis.However,the direct emission of waste gases containing F-gases into the atmosphere contributes to greenhouse effects and generates toxic substances.Developing porous materials for the energy-efficient capture,separation,and recovery of F-gases is highly desired.Recently,as a highly designable porous adsorbents,metal–organic frameworks(MOFs)exhibit excellent selective sorption performance toward F-gases,especially for the recognition and separation of different F-gases with highly similar properties,showing their great potential in F-gases control and recovery.In this review,we discuss the capture and separation of F-gases and their azeotropic,near-azeotropic,and isomeric mixtures in various application scenarios by MOFs,specifically classify and analyze molecular interaction between F-gases and MOFs,and interpret the mechanisms underlying their high performance regarding both adsorption capacity and selectivity,providing a repertoire for future materials design.Challenges faced in the transformation research roadmap of MOFs adsorbent separation technologies toward F-gases are also discussed,and areas for future research endeavors are highlighted.
基金support from National Natural Science Foundation of China(Grant Nos.62205223)Natural Science Foundation of Guangdong Province(Grant Nos.2023A1515011455)+6 种基金Science and Technology Innovation Commission of Shenzhen(Grant Nos.20231121120748002)support from Guangdong Introducing Innovative and Entrepreneurial Teams(Grant Nos.2019ZT08L101)Natural Science Foundation of Guangdong Province(Grant Nos.2023A1515110091)Science and Technology Innovation Commission of Shenzhen(Grant Nos.JSGGKQTD20221101115701006)support from National Key R&D Program of China(Grant Nos.2021YFA1401100)National Natural Science Foundation of China(Grant Nos.12104317)Scientific Instrument Developing Project of Shenzhen University(Grant Nos.2023YQ003)。
文摘Two-dimensional transition metal dichalcogenides(2D TMDCs)have received considerable attention in local strain engineering due to their extraordinary mechanical flexibility,electonic structure,and optical properties.The strain-induced out-of-plane deformations in 2D TMDCs lead to diverse excitonic behaviors and versatile modulations in optical properties,paving the way for the development of advanced quantum technologies,flexible optoelectronic materials,and straintronic devices.Research on local strain engineering on 2D TMDCs has been delved into fabrication techniques,electronic state variations,and quantum optical applications.This review begins by summarizing the state-of-the-art methods for introducing local strain into 2D TMDCs,followed by an exploration of the impact of local strain engineering on optical properties.The intriguing phenomena resulting from local strain,such as exciton funnelling and anti-funnelling,are also discussed.We then shift the focus to the application of locally strained 2D TMDCs as quantum emitters,with various strategies outlined for modulating the properties of TMDC-based quantum emitters.Finally,we discuss the remaining questions in this field and provide an outlook on the future of local strain engineering on 2D TMDCs.
基金supported by the Prospective Basic Research Projects of CNPC(Grant Nos.2022DJ5406,2022DJ5407,2022DJ5408,2022DJ4507,TGRI-2021-1,2022DQ03-03).
文摘Aqueous zinc-ion batteries(AZIBs)present a promising option for next-generation batteries given their high safety,eco-friendliness,and resource sustainability.Nonetheless,the practical application of zinc anodes is hindered by inevitable parasitic reactions and dendrite growth.Here,zinc alloy layers(i.e.,ZnCo and ZnFe alloys)were rationally constructed on the zinc surface by chemical displacement reactions.The alloying process exposes more(002)planes of the ZnCo anode to guide the preferential and dendrite-free zinc deposition.Furthermore,the ZnCo alloy layer not only effectively inhibits water-induced side reactions but also accelerates electrode kinetics,enabling highly reversible zinc plating/stripping.As a result,the ZnCo anode achieves a Coulombic efficiency of 99.2%over 1300 cycles,and the ZnCo symmetric cell exhibits a long cycle life of over 2000 h at 4.4 mA cm^(-2).Importantly,the ZnCo//NH_(4)V_(4)O_(10)full cell retains a high discharge capacity of 218.4 mAh g^(-1)after 800 cycles.Meanwhile,the ZnFe-based symmetric cell also displays excellent cycling stability over 2500 h at 1.77 mA cm^(-2).This strategy provides a facile anode modification approach toward high-performance AZIBs.
基金financially supported by the National Natural Science Foundation of China(52162036 and 22378342)Key Project of Nature Science Foundation of Xinjiang(2021D01D08)+2 种基金Major Projects of Xinjiang(2022A01005-4 and 2021A01001-1)Key Research and Development Project of Xinjiang(2023B01025-1)the support from the Doctoral Student Special Program of the Young Talents Support Project of the China Association for Science and Technology in 2024。
文摘Practical Zn metal batteries have been hindered by several challenges,including Zn dendrite growth,undesirable side reactions,and unstable electrode/electrolyte interface.These issues are particularly more serious in low-concentration electrolytes.Herein,we design a Zn salt-mediated electrolyte with in situ ring-opening polymerization of the small molecule organic solvent.The Zn(TFSI)_(2)salt catalyzes the ring-opening polymerization of(1,3-dioxolane(DOL)),generating oxidation-resistant and non-combustible long-chain polymer(poly(1,3-dioxolane)(pDOL)).The pDOL reduces the active H_(2)O molecules in electrolyte and assists in forming stable organic–inorganic gradient solid electrolyte interphase with rich organic constituents,ZnO and ZnF_(2).The introduction of pDOL endows the electrolyte with several advantages:excellent Zn dendrite inhibition,improved corrosion resistance,widened electrochemical window(2.6 V),and enhanced low-temperature performance(freezing point=-34.9°C).Zn plating/stripping in pDOL-enhanced electrolyte lasts for 4200 cycles at 99.02%Coulomb efficiency and maintains a lifetime of 8200 h.Moreover,Zn metal anodes deliver stable cycling for 2500 h with a high Zn utilization of 60%.A Zn//VO_(2)pouch cell assembled with lean electrolyte(electrolyte/capacity(E/C=41 mL(Ah)^(-1))also demonstrates a capacity retention ratio of 92%after 600 cycles.These results highlight the promising application prospects of practical Zn metal batteries enabled by the Zn(TFSI)2-mediated electrolyte engineering.
基金supported by the National Natural Science Foundation of China(52372164,52302085,and 52172174)the Anhui Provincial Natural Science Foundation(2308085Y05 and 2308085QE143)+1 种基金the Key Natural Science Research Project of Anhui Provincial Education Department(2023AH050094)the startup grants from Anhui University(S020318031/001).
文摘Aqueous Zn ion batteries(ZIBs)have received extensive attention due to their intrinsic safety,high abundance,and low cost.However,uncontrolled dendrite growth and water-induced side reactions at electrod e/electrolyte interfaces hinder the advancement of ZIBs.Herein,density functional theory(DFT)calculation indicates that Zn heptafluorobutyrate can facilitate uniform Zn^(2+)deposition by leveraging the abundant zincophilic groups(e.g.,-COO^(-)and-CF)and inhibit water-induced side reactions due to the presence of hydrophobic carbon chains.A Zn heptafluorobutyrate protective layer(denoted as ZFA)is constructed on the metallic Zn surface in situ by acid etching process to control Zn^(2+)desolvation and nucleation behaviors,ensuring enhanced reversibility and stability of Zn anodes.Consequently,the Zn@ZFA anode demonstrates stable operation for more than 2200 h at 1 mA cm^(-2)and over 7300cycles at 40 mA cm^(-2),with high Coulombic efficiency of 99.8%over 1900 cycles at 5 mA cm^(-2).Impressively,Zn@ZFA‖VO_(2)full cell achieves exceptional cycle life(204 mA h g^(-1)after 750 cycles at 3 A g^(-1))and remarkable rate performance(236 mA g^(-1)at 10 A g^(-1)).This work provides an insightful guidance for constructing a protection layer of dendrite-free Zn anodes for high-performance ZIBs.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.T2325004 and 52161160330)the support from the Hong Kong Institute of Advanced Studies through the materials cluster project。
文摘The glass-forming ability(GFA)of metallic glasses is a key scientific challenge in their development and application,with compositional dependence playing a crucial role.Experimental studies have demonstrated that the addition of specific minor elements can greatly enhance the GFA of parent alloys,yet the underlying mechanism remains unclear.In this study,we use the ZrCuAl system as a model to explore how the addition of minor Al influences the crystallization rate by modulating the properties of the crystal-liquid interface,thereby affecting the GFA.The results reveal that the minor addition of Al significantly reduces the crystal growth rate,a phenomenon not governed by particle density fluctuations at the interface.The impact of minor element additions extends beyond a modest increase in crystal-unfavorable motifs in the bulk supercooled liquid.More importantly,it leads to a significant enrichment of these motifs at the crystal-supercooled liquid interface,forming a dense topological network of crystal-unfavorable structures that effectively prevent the growth of the crystalline interface and enhance GFA.Our results provide valuable insights for the design and development of high-performance metallic glasses.
基金supported by the the National Key R&D Program of China(2022YFB3803500)the Natural Science Foundation of Hubei Province(2021CFA066).
文摘Micron-sized silicon(μSi)is a promising anode material for next-generation lithium-ion batteries due to its high specific capacity,low cost,and abundant reserves.However,the volume expansion that occurs during cycling leads to the accumulation of undesirable stresses,resulting in pulverization of silicon microparticles and shortened lifespan of the batteries.Herein,a composite film of Cu-PET-Cu is proposed as the current collector(CC)forμSi anodes to replace the conventional Cu CC.Cu-PET-Cu CC is prepared by depositing Cu on both sides of a polyethylene terephthalate(PET)film.The PET layer promises good ductility of the film,permitting the Cu-PET-Cu CC to accommodate the volumetric changes of silicon microparticles and facilitates the stress release through ductile deformation.As a result,theμSi electrode with Cu-PET-Cu CC retains a high specific capacity of 2181 mA h g^(-1),whereas theμSi electrode with Cu CC(μSi/Cu)exhibits a specific capacity of 1285 mA h g^(-1)after 80 cycles.The stress relieving effect of CuPET-Cu was demonstrated by in-situ fiber optic stress monitoring and multi-physics simulations.This work proposes an effective stress relief strategy at the electrode level for the practical implementation ofμSi anodes.
基金financially supported by the Natural Science Foundation of China(52277218)the Hubei Provincial Natural Science Foundation of China(2024AFA094)+1 种基金the Excellent Discipline Cultivation Project by JHUN(2023XKZ009)the Graduate Student Innovation Fund of JHUN(KYCXJJ202422).
文摘Lithium metal batteries(LMBs)with high energy density are impeded by the instability of solid electrolyte interface(SEI)and the uncontrolled growth of lithium(Li)dendrite.To mitigate these challenges,optimizing the SEI structure and Li deposition behavior is the key to stable LMBs.This study novelty proposes a facile synthesis of MgF_(2)/carbon(C)nanocomposite through the mechanochemical reaction between metallic Mg and polytetrafluoroethylene(PTFE)powders,and its modified polypropylene(PP)separator enhances LMB performance.The in-situ formed highly conductive fluorine-doped C species play a crucial role in facilitating ion/electron transport,thereby accelerating electrochemical kinetics and altering Li deposition direction.During cycling,the in-situ reaction between MgF_(2)and Li leads to the formation of LiMg alloy,along with a LiF-rich SEI layer,which reduces the nucleation overpotential and reinforces the interphase strength,leading to homogeneous Li deposition with dendrite-free feature.Benefiting from these merits,the Li metal is densely and uniformly deposited on the MgF_(2)/C@PP separator side rather than on the current collector side.Furthermore,the symmetric cell with MgF_(2)/C@PP exhibits superb Li plating/stripping performance over 2800 h at 1 mA cm^(-2)and 2 mA h cm^(-2).More importantly,the assembled Li@MgF_(2)/C@PPILiFePO4full cell with a low negative/positive ratio of 3.6delivers an impressive cyclability with 82.7%capacity retention over 1400 cycles at 1 C.
基金supported by the R&D Center for Valuable Recycling (Global-Top R&D Program)of the Ministry of Environment (No.2016002250003)。
文摘Scrap metals are typically covered with surface contaminants,such as paint,dust,and rust,which can significantly affect the emission spectrum during laser-induced breakdown spectroscopy(LIBS)based sorting.In this study,the effects of paint layers on metal surfaces during LIBS classification were investigated.LIBS spectra were collected from metal surfaces painted with black and white paints by ablation with a nanosecond pulsed laser(wavelength=1064 nm,pulse width=7 ns).For the black-painted samples,the LIBS spectra showed a broad background emission,emission lines unrelated to the target metals,large shot-to-shot variation,and a relatively low signal intensity of the target metal,causing poor classification accuracy even at high shot numbers.Cleaning the black paint layer by ablating over a wide area prior to LIBS analysis resulted in high classification accuracy with fewer shot numbers.A method to determine the number of cleaning shots necessary to obtain high classification accuracy and high throughput is proposed on the basis of the change in LIBS signal intensity during cleaning shots.For the white-painted samples,the paint peeled off the metal surface after the first shot,and strong LIBS signals were measured after the following shot,which were attributed to the nanoparticles generated by the ablation of the paint,allowing an accurate classification after only two shots.The results demonstrate that different approaches must be employed depending on the paint color to achieve high classification accuracy with fewer shot numbers.
基金supported by the National Natural Science Foundation of China(No.U2106216,52331004)the Natural Science Foundation of Shandong Province(No.ZR2022ZD12)+5 种基金the Key R&D Program of Shandong Province,China(2023ZLGX05,2023CXGC010406)the Taishan Scholarship of Climbing Plan(No.tspd20230603)the Fundamental Research Funds for the Central Universities(202461105)the China Postdoctoral Science Foundation(2023M732677)Shandong Province Postdoctoral Innovation Project(SDCX-ZG-202303086)Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education(LOEC-202309).
文摘Solar-driven interfacial evaporation is one of the most attractive approaches to addressing the global freshwater shortage.However,achieving an integrated high evaporation rate,salt harvesting,and multifunctionality in evaporator is still a crucial challenge.Here,a novel composite membrane with biomimetic micronanostructured superhydrophobic surface is designed via ultrafast laser etching technology.Attractively,the double-transition-metal(V_(1/2)Mo_(1/2))_(2)CT_(x)MXene nanomaterials as a photothermal layer,exhibiting the enhanced photothermal conversion performance due to elevated joint densities of states,which enables high populations of photoexcited carrier relaxation and heat release,provides a new insight into the photothermal conversion mechanism for multiple principal element MXene.Hence,the(V_(1/2)Mo_(1/2))_(2)CT_(x)MXene-200 composite membrane can achieve a high evaporation rate of 2.23 kg m^(−2)h^(−1)under one sun,owing to the enhanced“light trap”effect,photothermal conversion,and high-throughput water transfer.Synergetically,the membrane can induce the directed precipitation of salt at the membrane edge,thus enabling salt harvesting for recycling and zero-emission of brine water.Moreover,the composite membrane is endowed with excellent multifunctionality of anti-/de-icing,anti-fouling,and antibacterial,overcoming the disadvantage that versatility is difficult to be compatible.Therefore,the evaporator and the promising strategy hold great potential for the practical application of solar evaporation.
