Memristive crossbar arrays(MCAs)offer parallel data storage and processing for energy-efficient neuromorphic computing.However,most wafer-scale MCAs that are compatible with complementary metal-oxide-semiconductor(CMO...Memristive crossbar arrays(MCAs)offer parallel data storage and processing for energy-efficient neuromorphic computing.However,most wafer-scale MCAs that are compatible with complementary metal-oxide-semiconductor(CMOS)technology still suffer from substantially larger energy consumption than biological synapses,due to the slow kinetics of forming conductive paths inside the memristive units.Here we report wafer-scale Ag_(2)S-based MCAs realized using CMOS-compatible processes at temperatures below 160℃.Ag_(2)S electrolytes supply highly mobile Ag+ions,and provide the Ag/Ag_(2)S interface with low silver nucleation barrier to form silver filaments at low energy costs.By further enhancing Ag+migration in Ag_(2)S electrolytes via microstructure modulation,the integrated memristors exhibit a record low threshold of approximately−0.1 V,and demonstrate ultra-low switching-energies reaching femtojoule values as observed in biological synapses.The low-temperature process also enables MCA integration on polyimide substrates for applications in flexible electronics.Moreover,the intrinsic nonidealities of the memristive units for deep learning can be compensated by employing an advanced training algorithm.An impressive accuracy of 92.6%in image recognition simulations is demonstrated with the MCAs after the compensation.The demonstrated MCAs provide a promising device option for neuromorphic computing with ultra-high energy-efficiency.展开更多
Growth of high-quality Nb_(3)Sn thin films for superconducting radiofrequency(SRF)applications using the vapor diffusion method requires a uniform distribution of tin nuclei on the niobium(Nb)surface.This study examin...Growth of high-quality Nb_(3)Sn thin films for superconducting radiofrequency(SRF)applications using the vapor diffusion method requires a uniform distribution of tin nuclei on the niobium(Nb)surface.This study examines the mechanism underlying the observed non-uniform distribution of tin nuclei with tin chloride SnCl_(2).Electron backscatter diffraction(EBSD)analysis was used to examine the correlation between the nucleation behavior and orientation of niobium grains in the substrate.The findings of the density functional theory(DFT)simulation are in good agreement with the experimental results,showing that the non-uniform distribution of tin nuclei is the result of the adsorption energy of SnCl_(2)molecules by varied niobium grain orientations.Further analysis indicated that the surface roughness and grain size of niobium also played significant roles in the nucleation behavior.This study provides valuable insights into enhancing the surface pretreatment of niobium substrates during the growth of Nb_(3)Sn thin films using the vapor diffusion method.展开更多
Aqueous zinc-ion batteries (AZIBs) are fundamentally challenged by the instability of the electrode/electrolyte interface,predominantly due to irreversible zinc (Zn) deposition and hydrogen evolution.Particularly,the ...Aqueous zinc-ion batteries (AZIBs) are fundamentally challenged by the instability of the electrode/electrolyte interface,predominantly due to irreversible zinc (Zn) deposition and hydrogen evolution.Particularly,the intricate mechanisms behind the electrochemical discrepancies induced by interfacial Zn^(2+)-solvation and deposition behavior demand comprehensive investigation.Organic molecules endowed with special functional groups (such as hydroxyl,carboxyl,etc.) have the potential to significantly optimize the solvation structure of Zn^(2+)and regulate the interfacial electric double layer (EDL).By increasing nucleation overpotential and decreasing interfacial free energy,these functional groups facilitate a lower critical nucleation radius,thereby forming an asymptotic nucleation model to promote uniform Zn deposition.Herein,this study presents a pioneering approach by introducing trace amounts of n-butanol as solvation regulators to engineer the homogenized Zn (H-Zn) anode with a uniform and dense structure.The interfacial reaction and structure evolution are explored by in/ex-situ experimental techniques,indicating that the H-Zn anode exhibits dendrite-free growth,no by-products,and weak hydrogen evolution,in sharp contrast to the bare Zn.Consequently,the H-Zn anode achieves a remarkable Zn utilization rate of approximately 20% and simultaneously sustains a prolonged cycle life exceeding 500 h.Moreover,the H-Zn//NH_(4)V_(4)O^(10)(NVO) full battery showcases exceptional cycle stability,retaining 95.04%capacity retention after 400 cycles at a large current density of 5 A g^(-1).This study enlightens solvation-regulated additives to develop Zn anode with superior utilization efficiency and extended operational lifespan.展开更多
Sodium metal batteries(SMBs)are rising as viable alternatives to lithium-ion systems due to their superior energy density and sodium's relative abundance.However,SMBs face significant impediments,particularly the ...Sodium metal batteries(SMBs)are rising as viable alternatives to lithium-ion systems due to their superior energy density and sodium's relative abundance.However,SMBs face significant impediments,particularly the exceedingly high negative-to-positive capacity ratios(N/P ratios)which severely encumber energy density and hinder their practical application.Herein,a novel nucleophilic Na_(3)P interphase on aluminum foil has been designed to significantly lower the nucleation energy barrier for sodium atom deposition,resulting in a remarkable reduction of nucleation overpotential and efficient mitigation of dendritic growth at high sodium deposition of 5 mA h cm^(−2).The interphase promotes stable cycling in anode-less SMB configurations with a low N/P ratio of 1.4 and high cathode mass loading of 11.5 mg cm^(−2),and demonstrates a substantial increase in high capacity retention of 92.4%after 500 cycles even under 1 C rate condition.This innovation signifies a promising leap forward in the development of high-energy-density,anode-less SMBs,offering a potential solution to the longstanding issues of cycle stability and energy efficiency.展开更多
Nucleation of lithium sulfide(Li_(2)S)induced by electrocatalysts plays a crucial role in mitigating the shut-tle effect.However,short-chain polysulfides on electrocatalysts surfaces tend to re-dissolve into elec-trol...Nucleation of lithium sulfide(Li_(2)S)induced by electrocatalysts plays a crucial role in mitigating the shut-tle effect.However,short-chain polysulfides on electrocatalysts surfaces tend to re-dissolve into elec-trolytes,delaying Li_(2)S supersaturation and its nucleation.In this study,we draw inspiration from the ribosome-driven protein synthesis process in cells to prepare ultrasmall nitrogen-doped MoS_(2) nanocrys-tals anchored on porous nitrogen-doped carbon networks(N-MoS_(2)-NC)electrocatalysts.Excitedly,the ex-situ SEM demonstrates that ribosome-inspired N-MoS_(2)-NC electrocatalysts induce early nucleation and rapid growth of three-dimensional Li_(2)s during discharge.Theoretical calculations reveal that the Li-s bond length in N-MoS_(2)-Li_(2)S(100)is shorter,and the corresponding interfacial formation energy is lower than in MoS_(2)-Li_(2)S(100).This accelerated conversion of lithium polysulfides to Li_(2)S can enhance the utilization of active substances and inhibit the shuttle effect.This study highlights the potential of ribosome-inspired N-MoS_(2)-NC in improving the electrochemical stability of Li-S batteries,providing valuable insights for future electrocatalyst design.展开更多
Solid polymer electrolytes(SPEs)are highly promising for realizing high-capacity,low-cost,and safe Li metal batteries.However,the Li dendritic growth and side reactions between Li and SPEs also plague these systems.He...Solid polymer electrolytes(SPEs)are highly promising for realizing high-capacity,low-cost,and safe Li metal batteries.However,the Li dendritic growth and side reactions between Li and SPEs also plague these systems.Herein,a fluorinated lithium salt coating(FC)with organic-inorganic gradient and soft–rigid feature is introduced on Li surface as an artificial protective layer by the in-situ reaction between Li metal and fluorinated carboxylic acid.The FC layer can improve the interface stability and wettability between Li and SPEs,assist the transport of Li ions,and guide Li nucleation,contributing to a dendrite-free Li deposition and long-lifespan Li metal batteries.The symmetric cell with FC-Li anodes exhibits a high areal capacity of 1 mAh cm^(-2)at 0.5 mA cm^(-2),and an ultra-long lifespan of 2000 h at a current density of 0.1 mA cm^(-2).Moreover,the full cell paired with the LiFePO4 cathode exhibits improved cycling stability,remaining 83.7%capacity after 500 cycles at 1 C.When matching with the S cathode,the FC layer can prevent the shuttle effect,contributing to stable and high-capacity Li–S battery.This work provided a promising way for the construction of stable all-solid-state lithium metal batteries with prolonged lifespan.展开更多
The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode.However,the reve...The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode.However,the reversible Mg electrochemistry suffers from unsatisfied rate capability and lifespan,mainly caused by non-uniform distribution of electrodeposits.In this work,a fresh design concept of threedimensional carbon cloths scaffolds is proposed to overcome the uncontrollable Mg growth via homogenizing electric field and improving magnesiophilicity.A microscopic smooth and nitrogen-containing defective carbonaceous layer is constructed through a facile pyrolysis of ZIF8 on carbon cloths.As revealed by finite element simulation and DFT calculation results,the smooth surface endows with uniform electric field distribution and simultaneously the nitrogen-doping species enable good magnesiophilicity of scaffolds.The fine and uniform Mg nucleus as well as the inner electrodeposit behavior are also disclosed.As a result,an exceptional cycle life of 500 cycles at 4.0 mA cm^(-2) and 4.0 mA h cm^(-2) is firstly realized to our best knowledge.Besides,the functional scaffolds can be cycled for over 2200 h at 2.0 mA cm^(-2) under a normalized capacity of 5.0 mA h cm^(-2),far exceeding previous results.This work offers an effective approach to enable the full potential of carbon cloths-based scaffolds towards metal storage for next generation battery applications.展开更多
In the present work,the focus has been shifted to the relationship between the PANI morphology and the physicochemical properties,controlled by the amount of added ionic liquids,of the polymerization medium instead of...In the present work,the focus has been shifted to the relationship between the PANI morphology and the physicochemical properties,controlled by the amount of added ionic liquids,of the polymerization medium instead of focusing on the structure of the ionic liquids as used to be in the litterature.For that reason,PANI has been synthesized in different weight ratio of[Pyrr][PTS]/water following the standard experimental process.The addition of[Pyrr][PTS]into the polymerization medium controls the morphology of PANI without affecting its structure.Moreover,[Pyrr][PTS]promotes a viscous reaction system without the need of an external source.The viscosity of the polymerization system restricts the diffusion of species that leads to the predominance of the homogeneous nucleation mode during the course of polymerization and,thus,nanostructuring of PANI morphology.As for the ionic conductivity,it reflects the mobility of the ions of the polymerization medium and,thus,the way of its interference with the formed PANI that affects the arrangement and the shape of formed PANI fibers.This relationship between PANI morphology and the physicochemical properties,adjusted by adding ionic liquids,of the polymerization medium is prelaminar and promising.The effect of the ionic liquids on the viscosity as well as on the mobility of the polymerization medium have to be taken into consideration to choose the ionic liquids,which lead to the PANI with desired morphology.展开更多
Through the methods of correlation analysis and main factor analysis, the relationship between the poplar INA bacte-rial canker and circumstances was analyzed and 9 main factors for affecting the disease were selected...Through the methods of correlation analysis and main factor analysis, the relationship between the poplar INA bacte-rial canker and circumstances was analyzed and 9 main factors for affecting the disease were selected. Based on the compre-hensive analysis of main factors and induced factors, the standard for risk grades of this disease was promoted and northeast region of China was divided into 4 districts with different risk grades: seriously occurring district, commonly occurring district, occasionally occurring district, and un-occurring district. Nonlinear regression analysis for six model curves showed that the Richard growth model was suitable for describing the temporal dynamics of poplar INA bacterial canker. By stepwise variable selection method, the multi-variable linear regression forecasting equation was set up to predict the next year抯 disease index, and the GM (1,1) model was also set up by grey method to submit middle or long period forecast.展开更多
A positive grid bias and a negative substrate bias voltages are applied to the self-made hot filament chemical vapor deposited （HFCVD） system. The high quality nanocrystalline diamond （NCD） film is successfully de...A positive grid bias and a negative substrate bias voltages are applied to the self-made hot filament chemical vapor deposited （HFCVD） system. The high quality nanocrystalline diamond （NCD） film is successfully deposited by double bias voltage nucleation and grid bias voltage growth. The Micro-Raman XRD SEM and AFM are used to investigate the diamond grain size, microstructure, surface morphology, and nucleation density. Results show that the obtained NCD has grain size of about 20 nm. The effect of grid bias voltage on the nucleation and the diamond growth is studied. Experimental results and theoretical analysis show that the positive grid bias increases the plasma density near the hot filaments, enhances the diamond nucleation, keeps the nanometer size of the diamond grains, and improves the quality of diamond film.展开更多
The focus of this study is to investigate the influence of memory effect and the relation of its existence with the dissociation temperature,using gas hydrate formation and dissociation experiments.This is beneficial ...The focus of this study is to investigate the influence of memory effect and the relation of its existence with the dissociation temperature,using gas hydrate formation and dissociation experiments.This is beneficial because memory effect is considered as an effective approach to promote the thermodynamic and dynamic conditions of gas hydrate nucleation.Seven experimental systems （twenty tests in total） were performed in a 1 L pressure cell.Three types of hydrate morphology,namely massive,whiskery and jelly crystals were present in the experiments.The pressures and temperatures at the time when visual hydrate crystals appeared were measured.Furthermore,the influence of memory effect was quantified in terms of pressure-temperature-time （p-T-t） relations.The results revealed that memory effect could promote the thermodynamic conditions and shorten the induction time when the dissociation temperature was not higher than 25℃.In this study,the nucleation superpressure and induction time decrease gradually with time of tests,when the earlier and the later tests are compared.It is assumed that the residual structure of hydrate dissociation,as the source of the memory effect,provides a site for mass transfer between host and guest molecules.Therefore,a driving force is created between the residual structures and its surrounding bulk phase to promote the hydrate nucleation.However,when the dissociation temperature was higher than 25 ℃,the memory effect vanished.These findings provide references for the application of memory effect in hydrate-based technology.展开更多
Using the methods introduced by Bier, X.H., Buchinock, Wang Jing-wen, Shi Rihe et al., different varieties of poplar (poplar-Mei譗ing, Poplar-A100, Poplar-Xiaohe14 et al.) were inoculated with poplar ice nucleation ac...Using the methods introduced by Bier, X.H., Buchinock, Wang Jing-wen, Shi Rihe et al., different varieties of poplar (poplar-Mei譗ing, Poplar-A100, Poplar-Xiaohe14 et al.) were inoculated with poplar ice nucleation active (INA) bacteria respec-tively in 1997-1999. The water content, relative turgidity, lignin content, phenylalanine ammonialyase (PAL) activity, electrolyte effusion rate, and inorganic element content of poplar bark were measured before and after inoculating. The results showed that after the poplar trees were inoculated with INA bacteria, the moisture content of bark decreased but relative turgidity increased, electrolyte effusion rate increased and had a peak at temperatures of 4 and 5 C, lignin content increased and positively cor-related with poplars disease-resistance, and the plenylalanine ammonialyase activity increased and also showed a significant positive correlation with poplars disease-resistance. For the contents of inorganic element, Cu and Fe decreased but K and Zn increased obviously, while Mn, Ca and Mg changed little.展开更多
In the present work we studied the induction periods of hydrate formation of natural gas in pure water, aqueous solutions of surfactants, and in the presence of surfactant together with aluminum oxide nanopowder, the ...In the present work we studied the induction periods of hydrate formation of natural gas in pure water, aqueous solutions of surfactants, and in the presence of surfactant together with aluminum oxide nanopowder, the activity of which as hydrate formation inducer was studied previously. Sodium dodecyl sulfate（SDS） or neonol AF-9-12 were used as the surfactants. It was demonstrated that the addition of either surfactants or aluminum oxide powder under our experimental conditions causes a decrease in the induction period of hydrate formation from;05 min for pure water to 30–35 min for water with additives. In the case of the simultaneous presence of surfactants and aluminum oxide powder in the system, induction period decreased to;0 min. So, the synergistic effect of the combination of surfactant and oxide powder on gas hydrate nucleation was demonstrated. Possible reasons of this effect have been discussed.展开更多
Clathrate hydrate can be used in energy gas storage and transportation, CO2 capture and cool storage etc. However, these technologies are difficult to be used due to the low formation rate and long induction time of h...Clathrate hydrate can be used in energy gas storage and transportation, CO2 capture and cool storage etc. However, these technologies are difficult to be used due to the low formation rate and long induction time of hydrate formation. In this paper, ZIF-61 （zeolite imidazolate framework, ZIF） was first used in hydrate formation to stimulate hydrate nucleation. As an additive of clathrate hydrate, ZIF-61 promoted obviously the acceleration of tetrahydrofuran （THF） hydrate nucleation. It shortened the induction time of THF hydrate formation from 2-5 h to 0.3-1 h mainly due to the template function of ZIF-61 by which the nucleation of THF hydrate has been promoted.展开更多
Dendrite formation severely compromises further development of zinc ion batteries. Increasing the nucleation overpotential plays a crucial role in achieving uniform deposition of metal ions. However, this strategy has...Dendrite formation severely compromises further development of zinc ion batteries. Increasing the nucleation overpotential plays a crucial role in achieving uniform deposition of metal ions. However, this strategy has not yet attracted enough attention from researchers to our knowledge. Here, we propose that thermodynamic nucleation overpotential of Zn deposition can be boosted through complexing agent and select sodium L-tartrate(Na-L) as example. Theoretical and experimental characterization reveals L-tartrate anion can partially replace H_(2)O in the solvation sheath of Zn^(2+), increasing de-solvation energy. Concurrently, the Na^(+) could absorb on the surface of Zn anode preferentially to inhibit the deposition of Zn^(2+) aggregation. In consequence, the overpotential of Zn deposition could increase from 32.2 to 45.1 mV with the help of Na-L. The Zn-Zn cell could achieve a Zn utilization rate of 80% at areal capacity of 20 mAh cm^(-2). Zn-LiMn_(2)O_(4) full cell with Na-L additive delivers improved stability than that with blank electrolyte. This study also provides insight into the regulation of nucleation overpotential to achieve homogeneous Zn deposition.展开更多
To prepare the porous NC-based(nitrocellulose-based) gun propellants,the batch foaming process of using supercritical CO_2 as the physical blowing agent is used.The solubilities of CO_2 in the single-base propellants ...To prepare the porous NC-based(nitrocellulose-based) gun propellants,the batch foaming process of using supercritical CO_2 as the physical blowing agent is used.The solubilities of CO_2 in the single-base propellants and TEGDN(trimethyleneglycol dinitrate) propellants are measured by the gravimetric method,and SEM(scanning electron microscope) is used to observe the morphology of foamed propellants.The result shows that a large amount of CO_2 could be dissolved in NC-based propellants.The experimental results also reveal that the energetic plasticizer TEGDN exerts an important influence on the pore structure.The triaxial tensile failure mechanism for solid-state nucleation is used to explain the nucleation of NC-based propellants in the sol id state.Since some specific foaming behaviors of NC-based propellants can not be explained by the failure mechanism,a solid-state nucleation mechanism which revises the triaxial tensile failure mechanism is proposed and discussed.展开更多
Lithium metal anode of lithium batteries,including lithium-ion batteries,has been considered the anode for next-generation batteries with desired high energy densities due to its high theoretical specific capacity(386...Lithium metal anode of lithium batteries,including lithium-ion batteries,has been considered the anode for next-generation batteries with desired high energy densities due to its high theoretical specific capacity(3860 mA h g^(-1))and low standards electrode potential(-3.04 V vs.SHE).However,the highly reactive nature of metallic lithium and its direct contact with the electrolyte could lead to severe chemical reactions,leading to the continuous consumption of the electrolyte and a reduction in the cycle life and Coulombic efficiency.In addition,the solid electrolyte interface formed during battery cycling is mainly inorganic,which is too fragile to withstand the extreme volume change during the plating and stripping of lithium.The uneven flux of lithium ions could lead to excessive lithium deposition at local points,resulting in needle-like lithium dendrites,which could pierce the separator and cause short circuits,battery failure,and safety issues.In the last five years,tremendous efforts have been dedicated to addressing these issues,and the most successful improvements have been related to lithiophilicity optimizations.Thus,this paper comprehensively reviewed the lithiophilicity regulation in lithium metal anode modifications and highlighted the vital effect of lithiophilicity.The remaining challenges faced by the lithiophilicity optimization for lithium metal anodes are discussed with the proposed research directions for overcoming the technical challenges in this subject.展开更多
The nanocrystallization behaviour of a bulk Zr-based metallic glass subjected to compressive stress is investigated in the supercooled liquid region. Compared with annealing treatments without compressive stress, comp...The nanocrystallization behaviour of a bulk Zr-based metallic glass subjected to compressive stress is investigated in the supercooled liquid region. Compared with annealing treatments without compressive stress, compressive deformation promotes the development of nucleation and suppresses the coarsening of nanocrystallites at high temperatures.展开更多
Li-O_(2) batteries provide an attractive and potential strategy for energy conversion and storage with high specific energy densities.However,large over-potential in oxygen evolution reactions (OER) caused by the deco...Li-O_(2) batteries provide an attractive and potential strategy for energy conversion and storage with high specific energy densities.However,large over-potential in oxygen evolution reactions (OER) caused by the decomposition obstacles of Li_(2)O_(2) seriously impedes its electrochemical performances.Herein,a novel N,O,S and F co-doping vesicular carbon was prepared by self-template pyrolysis method and used in LiO_(2) battery to tune the nucleation and decomposition of Li_(2)O_(2).The introduction of F in the carbon matrix with suitable content can regulate the adsorption of intermediates,through which the morphology of Li_(2)O_(2) can be controlled to film,favorable to its decomposition in charge process.The cathode based on the optimized F doped carbon vesicle exhibits improved electrochemical performances including a low over-potential,large capacity and a long-term stability.Density functional theory (DFT) results show that F and C in C–F bond hasve a strong interaction to Li and O in Li_(2)O_(2),respectively,which can enhance the transfer of electrons from Li_(2)O_(2) to the carbon matrix to generate hole polaron and thus accelerate the delithiation and decomposition of Li_(2)O_(2).This work provides a new sight into understanding the mechanism of nucleation and decomposition of Li_(2)O_(2) for the development of high-performance Li-O_(2) batteries.展开更多
This study aims to develop a paraffin-based phase change material(PCM) emulsion with a low extent of supercooling for thermal energy storage(TES) systems to improve the cooling efficiency.Hexadecane-water emulsions we...This study aims to develop a paraffin-based phase change material(PCM) emulsion with a low extent of supercooling for thermal energy storage(TES) systems to improve the cooling efficiency.Hexadecane-water emulsions were prepared and characterized. Multi-wall carbon nanotubes(MWCNTs) were dispersed in the emulsion as a nucleating agent to reduce the supercooling. The MWCNTs were chemically modified with carboxyl groups to improve the dispersion of the tubular particles in the organic liquid. Thermal analyses of the emulsions by differential scanning calorimeter(DSC) indicated that the extent of supercooling was significantly reduced. The concentration of the nucleating agent for an effective supercooling suppression as found to be very low, in agreement with previous findings, and there appeared to be a minimum concentration for the supercooling reduction.展开更多
基金supported by the Swedish Strategic Research Foundation(SSF FFL15-0174 to Zhen Zhang)the Swedish Research Council(VR 2018-06030 and 2019-04690 to Zhen Zhang)+1 种基金the Wallenberg Academy Fellow Extension Program(KAW 2020-0190 to Zhen Zhang)the Olle Engkvist Foundation(Postdoc grant 214-0322 to Zhen Zhang).
文摘Memristive crossbar arrays(MCAs)offer parallel data storage and processing for energy-efficient neuromorphic computing.However,most wafer-scale MCAs that are compatible with complementary metal-oxide-semiconductor(CMOS)technology still suffer from substantially larger energy consumption than biological synapses,due to the slow kinetics of forming conductive paths inside the memristive units.Here we report wafer-scale Ag_(2)S-based MCAs realized using CMOS-compatible processes at temperatures below 160℃.Ag_(2)S electrolytes supply highly mobile Ag+ions,and provide the Ag/Ag_(2)S interface with low silver nucleation barrier to form silver filaments at low energy costs.By further enhancing Ag+migration in Ag_(2)S electrolytes via microstructure modulation,the integrated memristors exhibit a record low threshold of approximately−0.1 V,and demonstrate ultra-low switching-energies reaching femtojoule values as observed in biological synapses.The low-temperature process also enables MCA integration on polyimide substrates for applications in flexible electronics.Moreover,the intrinsic nonidealities of the memristive units for deep learning can be compensated by employing an advanced training algorithm.An impressive accuracy of 92.6%in image recognition simulations is demonstrated with the MCAs after the compensation.The demonstrated MCAs provide a promising device option for neuromorphic computing with ultra-high energy-efficiency.
基金supported by the National Natural Science Foundation of China(No.12175283)Youth Innovation Promotion Association of Chinese Academy of Sciences(2020410)Advanced Energy Science and Technology Guangdong Laboratory(HND20TDSPCD,HND22PTDZD).
文摘Growth of high-quality Nb_(3)Sn thin films for superconducting radiofrequency(SRF)applications using the vapor diffusion method requires a uniform distribution of tin nuclei on the niobium(Nb)surface.This study examines the mechanism underlying the observed non-uniform distribution of tin nuclei with tin chloride SnCl_(2).Electron backscatter diffraction(EBSD)analysis was used to examine the correlation between the nucleation behavior and orientation of niobium grains in the substrate.The findings of the density functional theory(DFT)simulation are in good agreement with the experimental results,showing that the non-uniform distribution of tin nuclei is the result of the adsorption energy of SnCl_(2)molecules by varied niobium grain orientations.Further analysis indicated that the surface roughness and grain size of niobium also played significant roles in the nucleation behavior.This study provides valuable insights into enhancing the surface pretreatment of niobium substrates during the growth of Nb_(3)Sn thin films using the vapor diffusion method.
基金National Natural Science Foundation of China (52301273, 52072411)Science and Technology Innovation Program of Hunan Province (2024RC3222)+3 种基金Key project of scientific research project of Hunan Provincial Department of Education (22A0479)China Postdoctoral Science Foundation (2024M753668)Central South University Innovation-Driven Research Programme (2023CXQD038)Hunan Provincial Postgraduate Research Innovation Programme(CX20240970)。
文摘Aqueous zinc-ion batteries (AZIBs) are fundamentally challenged by the instability of the electrode/electrolyte interface,predominantly due to irreversible zinc (Zn) deposition and hydrogen evolution.Particularly,the intricate mechanisms behind the electrochemical discrepancies induced by interfacial Zn^(2+)-solvation and deposition behavior demand comprehensive investigation.Organic molecules endowed with special functional groups (such as hydroxyl,carboxyl,etc.) have the potential to significantly optimize the solvation structure of Zn^(2+)and regulate the interfacial electric double layer (EDL).By increasing nucleation overpotential and decreasing interfacial free energy,these functional groups facilitate a lower critical nucleation radius,thereby forming an asymptotic nucleation model to promote uniform Zn deposition.Herein,this study presents a pioneering approach by introducing trace amounts of n-butanol as solvation regulators to engineer the homogenized Zn (H-Zn) anode with a uniform and dense structure.The interfacial reaction and structure evolution are explored by in/ex-situ experimental techniques,indicating that the H-Zn anode exhibits dendrite-free growth,no by-products,and weak hydrogen evolution,in sharp contrast to the bare Zn.Consequently,the H-Zn anode achieves a remarkable Zn utilization rate of approximately 20% and simultaneously sustains a prolonged cycle life exceeding 500 h.Moreover,the H-Zn//NH_(4)V_(4)O^(10)(NVO) full battery showcases exceptional cycle stability,retaining 95.04%capacity retention after 400 cycles at a large current density of 5 A g^(-1).This study enlightens solvation-regulated additives to develop Zn anode with superior utilization efficiency and extended operational lifespan.
基金funding support from the National Natural Science Foundation of China (22125902, 22109150, 22279126, U2032202, and 21975243)the DNL cooperation Fund, CAS (DNL202020)+1 种基金the National Key R&D Program of China (no. 2022YFA1504101)the Anhui Provincial Natural Science Foundation (2108085QB65)
文摘Sodium metal batteries(SMBs)are rising as viable alternatives to lithium-ion systems due to their superior energy density and sodium's relative abundance.However,SMBs face significant impediments,particularly the exceedingly high negative-to-positive capacity ratios(N/P ratios)which severely encumber energy density and hinder their practical application.Herein,a novel nucleophilic Na_(3)P interphase on aluminum foil has been designed to significantly lower the nucleation energy barrier for sodium atom deposition,resulting in a remarkable reduction of nucleation overpotential and efficient mitigation of dendritic growth at high sodium deposition of 5 mA h cm^(−2).The interphase promotes stable cycling in anode-less SMB configurations with a low N/P ratio of 1.4 and high cathode mass loading of 11.5 mg cm^(−2),and demonstrates a substantial increase in high capacity retention of 92.4%after 500 cycles even under 1 C rate condition.This innovation signifies a promising leap forward in the development of high-energy-density,anode-less SMBs,offering a potential solution to the longstanding issues of cycle stability and energy efficiency.
基金support from the National Natural Science Foundation of China(Grant Nos.52372083,52173255),the Collaborative Innovation Center for Advanced Micro/nanomaterials and Equipment(Co-constructed by Jiangsu Province and Ministry of Education)support from the Natural Science Foundation of Jiangsu Province,China(Grant No.BK20230538).
文摘Nucleation of lithium sulfide(Li_(2)S)induced by electrocatalysts plays a crucial role in mitigating the shut-tle effect.However,short-chain polysulfides on electrocatalysts surfaces tend to re-dissolve into elec-trolytes,delaying Li_(2)S supersaturation and its nucleation.In this study,we draw inspiration from the ribosome-driven protein synthesis process in cells to prepare ultrasmall nitrogen-doped MoS_(2) nanocrys-tals anchored on porous nitrogen-doped carbon networks(N-MoS_(2)-NC)electrocatalysts.Excitedly,the ex-situ SEM demonstrates that ribosome-inspired N-MoS_(2)-NC electrocatalysts induce early nucleation and rapid growth of three-dimensional Li_(2)s during discharge.Theoretical calculations reveal that the Li-s bond length in N-MoS_(2)-Li_(2)S(100)is shorter,and the corresponding interfacial formation energy is lower than in MoS_(2)-Li_(2)S(100).This accelerated conversion of lithium polysulfides to Li_(2)S can enhance the utilization of active substances and inhibit the shuttle effect.This study highlights the potential of ribosome-inspired N-MoS_(2)-NC in improving the electrochemical stability of Li-S batteries,providing valuable insights for future electrocatalyst design.
基金support by the National Natural Science Foundation of China(grant no.51772206).
文摘Solid polymer electrolytes(SPEs)are highly promising for realizing high-capacity,low-cost,and safe Li metal batteries.However,the Li dendritic growth and side reactions between Li and SPEs also plague these systems.Herein,a fluorinated lithium salt coating(FC)with organic-inorganic gradient and soft–rigid feature is introduced on Li surface as an artificial protective layer by the in-situ reaction between Li metal and fluorinated carboxylic acid.The FC layer can improve the interface stability and wettability between Li and SPEs,assist the transport of Li ions,and guide Li nucleation,contributing to a dendrite-free Li deposition and long-lifespan Li metal batteries.The symmetric cell with FC-Li anodes exhibits a high areal capacity of 1 mAh cm^(-2)at 0.5 mA cm^(-2),and an ultra-long lifespan of 2000 h at a current density of 0.1 mA cm^(-2).Moreover,the full cell paired with the LiFePO4 cathode exhibits improved cycling stability,remaining 83.7%capacity after 500 cycles at 1 C.When matching with the S cathode,the FC layer can prevent the shuttle effect,contributing to stable and high-capacity Li–S battery.This work provided a promising way for the construction of stable all-solid-state lithium metal batteries with prolonged lifespan.
基金supported by the National Natural Science Foundation of China(51972187,22279068,52374306)the Natural Science Foundation of Shandong Province(ZR2021QE166)Qingdao New Energy Shandong Laboratory Open Project(QNESL OP202312)。
文摘The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode.However,the reversible Mg electrochemistry suffers from unsatisfied rate capability and lifespan,mainly caused by non-uniform distribution of electrodeposits.In this work,a fresh design concept of threedimensional carbon cloths scaffolds is proposed to overcome the uncontrollable Mg growth via homogenizing electric field and improving magnesiophilicity.A microscopic smooth and nitrogen-containing defective carbonaceous layer is constructed through a facile pyrolysis of ZIF8 on carbon cloths.As revealed by finite element simulation and DFT calculation results,the smooth surface endows with uniform electric field distribution and simultaneously the nitrogen-doping species enable good magnesiophilicity of scaffolds.The fine and uniform Mg nucleus as well as the inner electrodeposit behavior are also disclosed.As a result,an exceptional cycle life of 500 cycles at 4.0 mA cm^(-2) and 4.0 mA h cm^(-2) is firstly realized to our best knowledge.Besides,the functional scaffolds can be cycled for over 2200 h at 2.0 mA cm^(-2) under a normalized capacity of 5.0 mA h cm^(-2),far exceeding previous results.This work offers an effective approach to enable the full potential of carbon cloths-based scaffolds towards metal storage for next generation battery applications.
基金funded by RESCOLL French society and the Lebanese University。
文摘In the present work,the focus has been shifted to the relationship between the PANI morphology and the physicochemical properties,controlled by the amount of added ionic liquids,of the polymerization medium instead of focusing on the structure of the ionic liquids as used to be in the litterature.For that reason,PANI has been synthesized in different weight ratio of[Pyrr][PTS]/water following the standard experimental process.The addition of[Pyrr][PTS]into the polymerization medium controls the morphology of PANI without affecting its structure.Moreover,[Pyrr][PTS]promotes a viscous reaction system without the need of an external source.The viscosity of the polymerization system restricts the diffusion of species that leads to the predominance of the homogeneous nucleation mode during the course of polymerization and,thus,nanostructuring of PANI morphology.As for the ionic conductivity,it reflects the mobility of the ions of the polymerization medium and,thus,the way of its interference with the formed PANI that affects the arrangement and the shape of formed PANI fibers.This relationship between PANI morphology and the physicochemical properties,adjusted by adding ionic liquids,of the polymerization medium is prelaminar and promising.The effect of the ionic liquids on the viscosity as well as on the mobility of the polymerization medium have to be taken into consideration to choose the ionic liquids,which lead to the PANI with desired morphology.
基金National Foundation of Ninth Five-Year Plan (No. 96-005-04-01-03).
文摘Through the methods of correlation analysis and main factor analysis, the relationship between the poplar INA bacte-rial canker and circumstances was analyzed and 9 main factors for affecting the disease were selected. Based on the compre-hensive analysis of main factors and induced factors, the standard for risk grades of this disease was promoted and northeast region of China was divided into 4 districts with different risk grades: seriously occurring district, commonly occurring district, occasionally occurring district, and un-occurring district. Nonlinear regression analysis for six model curves showed that the Richard growth model was suitable for describing the temporal dynamics of poplar INA bacterial canker. By stepwise variable selection method, the multi-variable linear regression forecasting equation was set up to predict the next year抯 disease index, and the GM (1,1) model was also set up by grey method to submit middle or long period forecast.
文摘A positive grid bias and a negative substrate bias voltages are applied to the self-made hot filament chemical vapor deposited （HFCVD） system. The high quality nanocrystalline diamond （NCD） film is successfully deposited by double bias voltage nucleation and grid bias voltage growth. The Micro-Raman XRD SEM and AFM are used to investigate the diamond grain size, microstructure, surface morphology, and nucleation density. Results show that the obtained NCD has grain size of about 20 nm. The effect of grid bias voltage on the nucleation and the diamond growth is studied. Experimental results and theoretical analysis show that the positive grid bias increases the plasma density near the hot filaments, enhances the diamond nucleation, keeps the nanometer size of the diamond grains, and improves the quality of diamond film.
基金supported by the National Natural Science Foundation(No.50874040,No.50904026)Heilongjiang Provincial Natural Science Foundation(No.B2007-10)Harbin Innovation Talent of Science and Technology Foundation(No.2007RFXXS050,No.2008RFQXG111)
文摘The focus of this study is to investigate the influence of memory effect and the relation of its existence with the dissociation temperature,using gas hydrate formation and dissociation experiments.This is beneficial because memory effect is considered as an effective approach to promote the thermodynamic and dynamic conditions of gas hydrate nucleation.Seven experimental systems （twenty tests in total） were performed in a 1 L pressure cell.Three types of hydrate morphology,namely massive,whiskery and jelly crystals were present in the experiments.The pressures and temperatures at the time when visual hydrate crystals appeared were measured.Furthermore,the influence of memory effect was quantified in terms of pressure-temperature-time （p-T-t） relations.The results revealed that memory effect could promote the thermodynamic conditions and shorten the induction time when the dissociation temperature was not higher than 25℃.In this study,the nucleation superpressure and induction time decrease gradually with time of tests,when the earlier and the later tests are compared.It is assumed that the residual structure of hydrate dissociation,as the source of the memory effect,provides a site for mass transfer between host and guest molecules.Therefore,a driving force is created between the residual structures and its surrounding bulk phase to promote the hydrate nucleation.However,when the dissociation temperature was higher than 25 ℃,the memory effect vanished.These findings provide references for the application of memory effect in hydrate-based technology.
基金This paper was supported by National Foundation of Ninth Five-Year Plan (No. 96-005-04-01-03).
文摘Using the methods introduced by Bier, X.H., Buchinock, Wang Jing-wen, Shi Rihe et al., different varieties of poplar (poplar-Mei譗ing, Poplar-A100, Poplar-Xiaohe14 et al.) were inoculated with poplar ice nucleation active (INA) bacteria respec-tively in 1997-1999. The water content, relative turgidity, lignin content, phenylalanine ammonialyase (PAL) activity, electrolyte effusion rate, and inorganic element content of poplar bark were measured before and after inoculating. The results showed that after the poplar trees were inoculated with INA bacteria, the moisture content of bark decreased but relative turgidity increased, electrolyte effusion rate increased and had a peak at temperatures of 4 and 5 C, lignin content increased and positively cor-related with poplars disease-resistance, and the plenylalanine ammonialyase activity increased and also showed a significant positive correlation with poplars disease-resistance. For the contents of inorganic element, Cu and Fe decreased but K and Zn increased obviously, while Mn, Ca and Mg changed little.
文摘In the present work we studied the induction periods of hydrate formation of natural gas in pure water, aqueous solutions of surfactants, and in the presence of surfactant together with aluminum oxide nanopowder, the activity of which as hydrate formation inducer was studied previously. Sodium dodecyl sulfate（SDS） or neonol AF-9-12 were used as the surfactants. It was demonstrated that the addition of either surfactants or aluminum oxide powder under our experimental conditions causes a decrease in the induction period of hydrate formation from;05 min for pure water to 30–35 min for water with additives. In the case of the simultaneous presence of surfactants and aluminum oxide powder in the system, induction period decreased to;0 min. So, the synergistic effect of the combination of surfactant and oxide powder on gas hydrate nucleation was demonstrated. Possible reasons of this effect have been discussed.
基金supported by the National Natural Science Foundation of China (Grant No. 51106054 and Grant No. 51176051)the National Basic Research Program of China ("973" Program) (Grant No. 2009CB219504-03)
文摘Clathrate hydrate can be used in energy gas storage and transportation, CO2 capture and cool storage etc. However, these technologies are difficult to be used due to the low formation rate and long induction time of hydrate formation. In this paper, ZIF-61 （zeolite imidazolate framework, ZIF） was first used in hydrate formation to stimulate hydrate nucleation. As an additive of clathrate hydrate, ZIF-61 promoted obviously the acceleration of tetrahydrofuran （THF） hydrate nucleation. It shortened the induction time of THF hydrate formation from 2-5 h to 0.3-1 h mainly due to the template function of ZIF-61 by which the nucleation of THF hydrate has been promoted.
基金supported by the National Key R&D Program of China (2022YFB3305400)Beijing Natural Science Foundation (Z220021)+3 种基金Science and Technology Innovation Program Talent Cultivation Project of Beijing Institute of Technology (2021CX01012)the National Natural Science Foundation of China (51972030, 22202011)Beijing Outstanding Young Scientists Program (BJJWZYJH01201910007023)Natural Science Foundation of Shandong Province (ZR2022QB056)。
文摘Dendrite formation severely compromises further development of zinc ion batteries. Increasing the nucleation overpotential plays a crucial role in achieving uniform deposition of metal ions. However, this strategy has not yet attracted enough attention from researchers to our knowledge. Here, we propose that thermodynamic nucleation overpotential of Zn deposition can be boosted through complexing agent and select sodium L-tartrate(Na-L) as example. Theoretical and experimental characterization reveals L-tartrate anion can partially replace H_(2)O in the solvation sheath of Zn^(2+), increasing de-solvation energy. Concurrently, the Na^(+) could absorb on the surface of Zn anode preferentially to inhibit the deposition of Zn^(2+) aggregation. In consequence, the overpotential of Zn deposition could increase from 32.2 to 45.1 mV with the help of Na-L. The Zn-Zn cell could achieve a Zn utilization rate of 80% at areal capacity of 20 mAh cm^(-2). Zn-LiMn_(2)O_(4) full cell with Na-L additive delivers improved stability than that with blank electrolyte. This study also provides insight into the regulation of nucleation overpotential to achieve homogeneous Zn deposition.
基金funded by the priority academic program development of Jiangsu Higher Education Institutions
文摘To prepare the porous NC-based(nitrocellulose-based) gun propellants,the batch foaming process of using supercritical CO_2 as the physical blowing agent is used.The solubilities of CO_2 in the single-base propellants and TEGDN(trimethyleneglycol dinitrate) propellants are measured by the gravimetric method,and SEM(scanning electron microscope) is used to observe the morphology of foamed propellants.The result shows that a large amount of CO_2 could be dissolved in NC-based propellants.The experimental results also reveal that the energetic plasticizer TEGDN exerts an important influence on the pore structure.The triaxial tensile failure mechanism for solid-state nucleation is used to explain the nucleation of NC-based propellants in the sol id state.Since some specific foaming behaviors of NC-based propellants can not be explained by the failure mechanism,a solid-state nucleation mechanism which revises the triaxial tensile failure mechanism is proposed and discussed.
基金supported by the National Natural Science Foundation of China(52072217,22179071)the Joint Funds of the National Natural Science Foundation of China(U20A20249)the Major Technological Innovation Project of Hubei Science and Technology Department(2019AAA164)。
文摘Lithium metal anode of lithium batteries,including lithium-ion batteries,has been considered the anode for next-generation batteries with desired high energy densities due to its high theoretical specific capacity(3860 mA h g^(-1))and low standards electrode potential(-3.04 V vs.SHE).However,the highly reactive nature of metallic lithium and its direct contact with the electrolyte could lead to severe chemical reactions,leading to the continuous consumption of the electrolyte and a reduction in the cycle life and Coulombic efficiency.In addition,the solid electrolyte interface formed during battery cycling is mainly inorganic,which is too fragile to withstand the extreme volume change during the plating and stripping of lithium.The uneven flux of lithium ions could lead to excessive lithium deposition at local points,resulting in needle-like lithium dendrites,which could pierce the separator and cause short circuits,battery failure,and safety issues.In the last five years,tremendous efforts have been dedicated to addressing these issues,and the most successful improvements have been related to lithiophilicity optimizations.Thus,this paper comprehensively reviewed the lithiophilicity regulation in lithium metal anode modifications and highlighted the vital effect of lithiophilicity.The remaining challenges faced by the lithiophilicity optimization for lithium metal anodes are discussed with the proposed research directions for overcoming the technical challenges in this subject.
基金Supported by the Science Foundation for Excellent Young Scholars of Heilongjiang Province under Grant No JC-05-11, the Program for New Century Excellent Talents in University of China under Grant No NCET-04-0322, and the Specialized Research Fund for the Doctoral Programme of Higher Education of China under Grant No 20040213049）
文摘The nanocrystallization behaviour of a bulk Zr-based metallic glass subjected to compressive stress is investigated in the supercooled liquid region. Compared with annealing treatments without compressive stress, compressive deformation promotes the development of nucleation and suppresses the coarsening of nanocrystallites at high temperatures.
基金financially supported by the National Natural Science Foundation of China(Grant No.21701145)the China Postdoctoral Science Foundation(Grant Nos.2017M610459,2018T110739)。
文摘Li-O_(2) batteries provide an attractive and potential strategy for energy conversion and storage with high specific energy densities.However,large over-potential in oxygen evolution reactions (OER) caused by the decomposition obstacles of Li_(2)O_(2) seriously impedes its electrochemical performances.Herein,a novel N,O,S and F co-doping vesicular carbon was prepared by self-template pyrolysis method and used in LiO_(2) battery to tune the nucleation and decomposition of Li_(2)O_(2).The introduction of F in the carbon matrix with suitable content can regulate the adsorption of intermediates,through which the morphology of Li_(2)O_(2) can be controlled to film,favorable to its decomposition in charge process.The cathode based on the optimized F doped carbon vesicle exhibits improved electrochemical performances including a low over-potential,large capacity and a long-term stability.Density functional theory (DFT) results show that F and C in C–F bond hasve a strong interaction to Li and O in Li_(2)O_(2),respectively,which can enhance the transfer of electrons from Li_(2)O_(2) to the carbon matrix to generate hole polaron and thus accelerate the delithiation and decomposition of Li_(2)O_(2).This work provides a new sight into understanding the mechanism of nucleation and decomposition of Li_(2)O_(2) for the development of high-performance Li-O_(2) batteries.
基金Supported by the Research Grant Council of the Hong Kong SAR government(GRF PolyU 5241/11E)
文摘This study aims to develop a paraffin-based phase change material(PCM) emulsion with a low extent of supercooling for thermal energy storage(TES) systems to improve the cooling efficiency.Hexadecane-water emulsions were prepared and characterized. Multi-wall carbon nanotubes(MWCNTs) were dispersed in the emulsion as a nucleating agent to reduce the supercooling. The MWCNTs were chemically modified with carboxyl groups to improve the dispersion of the tubular particles in the organic liquid. Thermal analyses of the emulsions by differential scanning calorimeter(DSC) indicated that the extent of supercooling was significantly reduced. The concentration of the nucleating agent for an effective supercooling suppression as found to be very low, in agreement with previous findings, and there appeared to be a minimum concentration for the supercooling reduction.
