In igneous-intruded coal seams,coal undergoes significant metamorphism,which critically alters its pore structure and oxygen consumption dynamics,thereby elevating its spontaneous combustion tendency.This study invest...In igneous-intruded coal seams,coal undergoes significant metamorphism,which critically alters its pore structure and oxygen consumption dynamics,thereby elevating its spontaneous combustion tendency.This study investigates the specific surface area,pore volume,structure complexity/connectivity,heterogeneity/local features of pore size distribution,and oxygen consumption dynamics of igneous metamorphic coal through N2/CO2 isothermal adsorption tests and low-temperature oxidation experiments,and elucidates the influence mechanisms of pore structure evolution on oxygen consumption dynamics during low-temperature oxidation.With increasing metamorphic degree,igneous metamorphic coal exhibits a more pronounced reduction in specific surface area during oxidation,while the increase in structure complexity due to coal-oxygen reactions is suppressed.Thermally metamorphic coal demonstrates accelerated oxygen consumption,with oxidation amplifying the difference in reaction rates compared to raw coal.Key mechanisms include oxidation-induced reduction in mesopore complexity and micropore volume,decreased dominance of small-pore-volume apertures,and increased heterogeneity,collectively leading to a lower half-oxygen-consuming temperature and steeper oxygen consumption curves.Simultaneously,increased pore volume/complexity and reduced uniformity/connectivity act synergistically to enhance oxygen consumption capacity,highlighting the coupling between pore structure evolution and oxidation behavior in igneous metamorphic coal.This study provides theoretical insights into the pore-oxygen coupling mechanisms governing coal spontaneous combustion in igneous intrusion areas.展开更多
Porosity is a fundamental parameter in characterizing the pore structure of shale oil reservoirs,as it directly affects the accuracy of shale oil reserve estimations.Despite the availability of various measurement tec...Porosity is a fundamental parameter in characterizing the pore structure of shale oil reservoirs,as it directly affects the accuracy of shale oil reserve estimations.Despite the availability of various measurement techniques,accurately quantifying porosity in such reservoirs remains a significant challenge.In an effort to identify the most effective porosity testing method,this study collected samples from four shale oil reservoir intervals across five sags in three different basins.Five porosity testing methods were employed to detect shale porosity,including helium porosity,low-temperature nitrogen adsorption-desorption(LTNA/D),oil-saturated wetting,and nuclear magnetic resonance(NMR)T2and T1-T2.NMR T2porosity acted as a touchstone against which the other methods were compared.The pros and cons of each evaluation technique were explored to select the optimal analysis method for shale oil reservoirs.Results indicate that LTNA/D porosity,derived from powdered samples,commonly fails to reflect shale porosity effectively.Helium porosity,widely used for detecting nanoscale pores,is constrained by extended equilibration times and the retention of residual pore fluids after oil washing and drying,leading to systematic underestimation.In contrast,oil-saturation wetting and NMR T2exhibit strong agreement,both reflecting pore fluid content.However,residual fluid distribution can also impact the accuracy of NMR T2measurements.NMR T1-T2is an innovative technique for quantitatively evaluating shale oil reservoirs.NMR T1-T2spectrum at the water and oil restoration state can provide accurate shale porosity.NMRT1-T2porosity estimates generally align with those obtained from T2 porosity.When residual pore fluids are not entirely removable,the NMRT1-T2method offers a more realistic porosity assessment.The NMR technique is recommended for evaluating the porosity of shale oil reservoirs,and the combination of T2and T1-T2can accurately determine the effective and total porosity.This research serves as a valuable reference for accurately determining porosity in shale oil reservoirs.展开更多
Silicon/graphite(Si/C)composites,which combine the advantages of Si anodes and commercial graphite anodes,are promising anode materials for high-energy-density lithium-ion batteries(LIBs).Despite experimental and theo...Silicon/graphite(Si/C)composites,which combine the advantages of Si anodes and commercial graphite anodes,are promising anode materials for high-energy-density lithium-ion batteries(LIBs).Despite experimental and theoretical studies on the electrochemical characteristics of different silicon crystal surfaces,there have been limited investigations on the electrochemical and mechanical properties of Si composite anode materials with different graphite crystal planes,such as the electrode interfaces between Si(111)and graphite(0001),as well as amorphous Si and graphite(1010).In this study,models of Si/C anode interfaces for LIBs were constructed to explore the mechanical-electrochemical-low-temperature performance by density functional theory(DFT)calculations and ab initio molecular dynamics(AIMD)simulations.The calculation results indicate that upon Li intercalation into the graphite(1010)surface,the electrical conductivity,electrochemical adsorption,and interfacial mechanical strength of the Si/C composite are significantly enhanced,with a separation work that is 2.3 times higher than that of Si/C on the graphite(0001)surface.More importantly,AIMD simulations at low temperatures reveal that the interface between graphite(1010)and amorphous Si forms a solid electrolyte interphase(SEI)rich in organic components,which significantly improves the Li-diffusion kinetics.This discovery provides new insights for the design and optimization of Si/C anode materials for low-temperature LIBs.展开更多
Protons emerge as superior charge carriers due to the lowest mass-to-charge ratio,ultra-high natural abundance,and the smallest ionic radius.Herein,2.0 M H2 SO4 dissolved in EG(ethylene glycol)/H2O cosolvent ...Protons emerge as superior charge carriers due to the lowest mass-to-charge ratio,ultra-high natural abundance,and the smallest ionic radius.Herein,2.0 M H2 SO4 dissolved in EG(ethylene glycol)/H2O cosolvent is investigated as an aqueous proton battery electrolyte,which not only enhances the cycling performance of MoO3 nanorod anode but also improves its low-temperature electrochemical performance.Specifically,the EG tightly adsorbs onto the surface of MoO3 nanorods,thereby inhibiting the corrosion from H2O molecules in the electrolyte and suppressing the dissolution of MoO3.In addition,EG molecule disturbs the hydrogen-bond network between H2O molecules,which greatly decreases the freezing point of the electrolyte,endowing the MoO3 nanorods with excellent low-temperature electrochemical performance.Therefore,the MoO3 nanorods exhibit a capacity retention of 96.9%after 2000 cycles at a current density of 10 A g-1in a three-electrode system.After assembling with CuHCF cathode,under-40℃,the full battery displays negligible capacity decay for over 2500 cycles at 1 A g-1.These results indicate that the cosolvent strategy has the promising potential in enhancing the performance of aqueous proton batteries.展开更多
This study focused on improving the cathode performance of Ba0.6Sr0.4Co0.85Nb0.15O3-δ(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea0.6Sr0.4Co_(0...This study focused on improving the cathode performance of Ba0.6Sr0.4Co0.85Nb0.15O3-δ(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea0.6Sr0.4Co0.85Nb0.1Mo0.05O3-δ(B S CNM0.05),Ba0.6Sr0.4Co0.85Nb0.05Mo0.1O3-δ(BSCNM0.1),and Ba0.6Sr0.4Co0.85Mo0.15O3-δ(BSCM)—with Mo doping contents of 5mol%,10mol%,and15mol%,respectively,were successfully prepared using the sol-gel method.The effects of Mo doping on the crystal structure,conductivity,thermal expansion coefficient,oxygen reduction reaction(ORR)activity,and electrochemical performance were systematically evaluated using X-ray diffraction analysis,thermally induced characterization,electrochemical impedance spectroscopy,and single-cell performance tests.The results revealed that Mo doping could improve the conductivity of the materials,suppress their thermal expansion effects,and significantly improve the electrochemical performance.Surface chemical state analysis using X-ray photoelectron spectroscopy revealed that 5mol%Mo doping could facilitate a high adsorbed oxygen concentration leading to enhanced ORR activity in the materials.Density functional theory calculations confirmed that Mo doping promoted the ORR activity in the materials.At an operating temperature of 600℃,the BSCNM0.05cathode material exhibited significantly enhanced electrochemical impedance characteristics,with a reduced area specific resistance of 0.048Ω·cm~2,which was lower than that of the undoped BSCN matrix material by 32.39%.At the same operating temperature,an anode-supported single cell using a BSCNM0.05cathode achieved a peak power density of 1477 mW·cm-2,which was 30.71%,56.30%,and 171.50%higher than those of BSCN,BSCNM0.1,and B SCM,respectively.The improved ORR activity and electrochemical performance of BSCNM0.05indicate that it can be used as a cathode material in low-temperature solid oxide fuel cells.展开更多
The paleo-geothermal gradient is a crucial parameter for converting the thermal history to the exhumation history.However,the precise estimation of this parameter has been a challenge.This paper presents a simple two-...The paleo-geothermal gradient is a crucial parameter for converting the thermal history to the exhumation history.However,the precise estimation of this parameter has been a challenge.This paper presents a simple two-step method to model the paleo-geothermal gradient using low-temperature thermochronology.(1)It uses the Monte Carlo approach to generate thermal histories in a vertical section randomly and calculates the entire thermal history within the goodnessof-fit thresholds based on different paleo-geothermal gradients.(2)It selects the optimum paleogeothermal gradient by comparing the entire thermal history within different goodness-of-fit thresholds.We validated the method with apatite(U-Th)/He and fission track data collected from two drill cores in the Haiyuan-Liupanshan region.The result revealed that the best-fit paleo-geothermal gradient was~42℃/km during the Early Cretaceous–Miocene and has decreased rapidly to 20℃/km since~10 Ma.The crust thickening in the study area may explain the rapid reduction in the paleogeothermal gradient since~10 Ma.Our results are consistent with earlier studies in the region,suggesting that our simple and more intuitive approach provides an alternative method for paleogeothermal gradient modeling.展开更多
Aqueous zinc-ion batteries(AZIBs)have emerged as strong contenders for large-scale energy storage solutions,attributed to their cost-effectiveness and enhanced safety profiles.Nevertheless,their widespread adoption is...Aqueous zinc-ion batteries(AZIBs)have emerged as strong contenders for large-scale energy storage solutions,attributed to their cost-effectiveness and enhanced safety profiles.Nevertheless,their widespread adoption is currently hindered by their poor performance in low-temperature conditions.Herein,an electrolyte is developed by utilizing weakly solvated and film-forming molecule dimethyl sulfite(DMS)to achieve smooth de-solvation and high ionic conductivity at low temperature.The DMS disrupts the hydrogen bonding network of water and lowers the freezing point of the electrolyte to-40.9℃.The designed electrolyte achieves ionic conductivity up to 10.75 m S/cm at-30℃.Due to the chemical reactivity of DMS and trifluoromethanesulfonate anions in the Zn2+-solvation shell,a Zn F2-Zn S hybrid solid electrolyte interphase(SEI)is successively generated on Zn metal surface.Mechanistic studies reveal that such robust hybrid interphase can promote Zn2+desolvation and rapid Zn2+transport.In addition,the addition of DMS effectively suppresses the dendritic growth,hydrogen evolution reaction(HER),and corrosioninduced passivation on the anode surface,facilitating long-term cycling at subzero temperatures.At-40℃,the Zn//Zn symmetrical cell cycles for 1200 h at 0.5 m A/cm2and 0.5 m Ah/cm2,and the Zn//NVO cell achieves an ultra-long cycle life of 1000 cycles with a high capacity retention of 82.89%at 1 A/g.展开更多
In order to explore the effects of CaO,lignite dust and sawdust on the drying characteristics ofmunicipal sludge at different concentrations,a three-factor three-level regression experiment was carried out based on th...In order to explore the effects of CaO,lignite dust and sawdust on the drying characteristics ofmunicipal sludge at different concentrations,a three-factor three-level regression experiment was carried out based on the results of thermogravimetric experiment and single factor experiment.By fitting three common mathematical models,the Page model with the highest fitting degree was selected to determine the most suitable mathematical model to describe the municipal sludge drying process.In addition,the Box-Behnken design principle in the response surface method was used to analyze the interaction of three factors on the drying characteristics of municipal sludge.The results of the study show that below 100℃is the optimal drying temperature range for municipal sludge.The results of single factor experiments showed that the order of influence of the three factors on sludge drying time was CaO concentration>sawdust concentration>lignite dust concentration.In the single factor experiment,the optimal process parameterswere CaOconcentration 3%,lignite powder concentration 7%,and sawdust concentration 7%.In themulti-factor interaction analysis,the interaction between CaO and sawdust had the most significant effect on the reduction of drying time,and the order of influence was as follows:CaO interaction with sawdust>lignite dust interaction with sawdust>CaO interaction with lignite powder.Further analysis showed that the optimal process ratio was 3%CaO concentration and 3%sawdust concentration.展开更多
The Beishan Fold-Thrust Belt(BFTB),located in the southern part of the Central Asian Orogenic Belt(CAOB),underwent complex intracontinental deformation during the late Mesozoic and is a key tectonic unit for decipheri...The Beishan Fold-Thrust Belt(BFTB),located in the southern part of the Central Asian Orogenic Belt(CAOB),underwent complex intracontinental deformation during the late Mesozoic and is a key tectonic unit for deciphering the remote effects of plate margin orogenesis.In this study,we selected the Yemaquan region in southern Beishan and conducted remote sensing interpretation,field mapping,seismic profile interpretation and low-temperature thermochronological analyses.The Permian pluton and Carboniferous strata thrust over the Jurassic strata and developed a series of SEE-trending thrusts,NE-striking left strike-slip faults,and several SEE-and NE-trending folds.This area experienced two directions(NE and NW) of compression deformation.Under the joint influence of compression stress and pluton blocking,fold structures related to strike-slip faults also developed(the Big Ear syncline).The above constituted the Yemaquan Fold-Thrust system(YFTS).Zircon(U-Th)/He(ZHe) data reveal cooling events at~175-165 Ma;combining the regional deformation,it may indicate the compression time.We concluded that the intracontinental deformation of the BFTB in the southern CAOB was driven by the far-field effects.NE compression is related to the closure of the Mongol-Okhotsk Ocean and the collision of the Lhasa-Qiangtang block;NW compression is related to westward subduction of the Paleo-Pacific plate.展开更多
The reliable operation of lithium-ion batteries(LIBs)in low temperatures has long been hindered by severe side reactions on graphite anodes.To develop a commercially viable low-temperature electrolyte,we design a solv...The reliable operation of lithium-ion batteries(LIBs)in low temperatures has long been hindered by severe side reactions on graphite anodes.To develop a commercially viable low-temperature electrolyte,we design a solvent-resistant Nitrate-coordinated electrolyte.The practical Ah-level graphite LiNi0.5Co0.2Mn0.3O2 pouch cell with the newly developed electrolyte demonstrates a significant breakthrough in cycling stability,exhibiting negligible capacity fade after 250 cycles at-30℃ and 0.1 C.NO3-,as the functional additive,compresses the electric field around Li+through electrostatic interactions,mimicking the Debye-screening effect and inducing the coordinative exclusion of free ethyl acetate molecules at low temperatures.The transformation from contact ion pairs(CIPs)formed by Pto solventseparated ion pairs is significantly restrained,which mitigates the continuous reactions between the electrolyte and inevitable lithium deposition at low temperature.Additionally,this customized inert CIPs form a solid electrolyte interphase on graphite that exhibits remarkable ionic conductivity and rigidity,preventing excessive Li dendrite growth.This finding offers new insights into the relationship of microstructure-performance for low-temperature electrolytes,demonstrating that relying solely on inert CIPs can also inhibit the decomposition of the interfacial electrolyte,and inspires a unique design concept for high-performance,commercially viable LIBs that operate reliably in sub-zero environments.展开更多
Converting CO2 to CH4 under mild conditions represents a promising strategy for carbon emission reduction and synthetic natural gas production,yet it remains challenging.In this work,we accelerated low-temperatu...Converting CO2 to CH4 under mild conditions represents a promising strategy for carbon emission reduction and synthetic natural gas production,yet it remains challenging.In this work,we accelerated low-temperature CO2 hydrogenation over Ni-CeO2 catalysts by optimizing metal-support interactions through H2-driven reconstruction.The catalyst reduced at 400℃(Ni-CeO2-400R)achieved 84.3%CO2conversion with 100%CH4 selectivity even at a low temperature of 250℃.Various in situ spectroscopic characterizations(X-ray photoelectron spectroscopy(XPS),Raman,and diffused reflectance infrared Fourier transform spectroscopy(DRIFTS))and H2/D2 isotopic exchange experiments reveal that the appropriate interaction in Ni-CeO2 motivates the dispersion of metallic Ni sites and the generation of oxygen vacancies,thereby promoting the activation of H2 and CO2 molecules,respectively.Therefore,CO2 is efficiently adsorbed and converted into reactive intermediates and finally hydrogenated to CH4through carbonyl and formate pathways simultaneously.These findings underscore the critical role of tailored metal-support interactions in designing advanced CO2 hydrogenation catalysts.展开更多
CO2methanation technology has shown great application prospects in carbon neutrality and hydrogen storage due to its extremely high energy efficiency and potential economic benefits.It is highly desirable but chall...CO2methanation technology has shown great application prospects in carbon neutrality and hydrogen storage due to its extremely high energy efficiency and potential economic benefits.It is highly desirable but challenging to design novel catalyst and achieve efficient and stable CO2methanation under mild conditions.Herein,we developed a highly active electron-enriched Y2O3/Ni catalyst,achieving a stable operation with~80.1%CO2conversion and~100%CH4selectivity for 400 h at 0.1 MPa and 220℃,which was a 100℃lower than the conventional supported Ni-based catalysts.Structural characterizations confirmed that the Y2O3/Ni catalyst maintained dynamic redox changes and formed electron-enriched Y2O3-x-Ni interfaces under reaction conditions.Mechanism studies proved that the Y2O3-x-Ni interfaces obviously lowered the energy barrier of*HCO dissociation,and shifted the rate-determining step from*HCO dissociation to*CO hydrogenation.Furthermore,profited by the moderate COx adsorption ability and higher H2coverage at the Y2O3-x-Ni interfaces,the*CO hydrogenation reaction was kinetically promoted.The above factors accounted for the excellent low-temperature CO2methanation activity of the Y2O3/Ni catalyst.展开更多
Converting CO2to CH4 under mild conditions is a promising strategy for solving environmental and energy problems,but also a challenge.In this work,the low-temperature CO2 hydrogenation process over Ni/CeO2 ca...Converting CO2to CH4 under mild conditions is a promising strategy for solving environmental and energy problems,but also a challenge.In this work,the low-temperature CO2 hydrogenation process over Ni/CeO2 catalysts was significantly accelerated by optimizing the H2 dissociation ability of Ni through the size effect,thus A-Ni/CeO2 with an average size of 4.9 nm achieved 83.4%CO2conversion with~100%CH4 selectivity even at 225℃.Systematic H2/D2 isotopic exchange experiments,in situ spectroscopic characterizations,and density functional theory(DFT)calculations reveal that the enhanced H2 activation ability not only promoted the creation of oxygen vacancies and hydroxyl group favorable for CO2 adsorption/activation in the pre-reduction process,but also the simultaneous hydrogenation of reactive intermediates belonging to carbonyl and formate pathway into CH4 in the reaction process.This fundamental understanding of the H2 dissociation effect on CO2 activation and hydrogenation provides critical insights for designing catalysts with considerable low-temperature activity,which significantly reduces energy consumption and operating costs for industrial CO2 conversion.展开更多
Conventional graphite synthesis involves CO2emission and a graphitization process at a high temperature of~3000℃.Herein,we report a new method to synthesize high-performance graphite anode materials from greenhous...Conventional graphite synthesis involves CO2emission and a graphitization process at a high temperature of~3000℃.Herein,we report a new method to synthesize high-performance graphite anode materials from greenhouse CO2gas at an external heating temperature as low as 135℃.Transition metal catalysts are not required for low-temperature synthesis of graphite.Extreme graphitization temperatures are not required as compared to graphite synthesized from petroleum coke-based materials.The graphitization degree of graphite was found to be strongly related to CO2pressure.Graphite was synthesized at a maximum pressure of 20 MPa,whereas semi-graphited carbon was synthesized at a maximum pressure of 6.3 MPa.The synthesized graphite exhibited superior lithium storage kinetics and excellent cycling stability over 3000 cycles,with a capacity retention of~100% at 1.0 A·g-1.This work establishes an integrated sustainable strategy that concurrently addresses greenhouse gas utilization and energy-efficient anode material production.展开更多
Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temp...Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temperature(LT)operation.Therefore,a more comprehensive and systematic understanding of LIB behavior at LT is urgently required.This review article comprehensively reviews recent advancements in electrolyte engineering strategies aimed at improving the low-temperature operational capabilities of LIBs.The study methodically examines critical performance-limiting mechanisms through fundamental analysis of four primary challenges:insufficient ionic conductivity under cryogenic conditions,kinetically hindered charge transfer processes,Li+transport limitations across the solidelectrolyte interphase(SEI),and uncontrolled lithium dendrite growth.The work elaborates on innovative optimization approaches encompassing lithium salt molecular design with tailored dissociation characteristics,solvent matrix optimization through dielectric constant and viscosity regulation,interfacial engineering additives for constructing low-impedance SEI layers,and gel-polymer composite electrolyte systems.Notably,particular emphasis is placed on emerging machine learning-guided electrolyte formulation strategies that enable high-throughput virtual screening of constituent combinations and prediction of structure-property relationships.These artificial intelligence-assisted rational design frameworks demonstrate significant potential for accelerating the development of next-generation LT electrolytes by establishing quantitative composition-performance correlations through advanced data-driven methodologies.展开更多
Under the context of global energy transition and carbon neutrality,controlling nitrogen oxide(NOx)emissions from biomass combustion is of great significance,and the development of high-efficiency low-temperature c...Under the context of global energy transition and carbon neutrality,controlling nitrogen oxide(NOx)emissions from biomass combustion is of great significance,and the development of high-efficiency low-temperature catalysts has become a current research focus.In this study,Nb was used to dope and modify the Mn7-Cu3/BCN catalyst to construct the Mn7-Cu3-Nbx/BCN system.The doping amount was optimized through selective catalytic reduction(SCR)activity tests.The reaction mechanism was explored by combining in situ DRIFTS and density functional theory(DFT)simulations.Experimental findings revealed that the catalyst doped with 0.05%Nb achieved the optimal performance,sustaining a NO conversion efficiency of≥94%within the temperature window of 150−275℃while demonstrating improved resistance to alkali metal K poisoning.Mechanistic analyses showed that at low temperatures,the catalyst facilitated the SCR reaction via both the Eley-Rideal(E-R)and Langmuir-Hinshelwood(L-H)pathways,with the synergistic interaction between multiple active sites driving the efficient conversion of NH3 and NO.DFT calculations further confirmed that both pathways had the characteristics of low reaction energy barriers and significant exothermicity,ensuring the high activity and feasibility of the low-temperature reaction.The findings provided foundational theoretical support for the design of Nb-doped Mn-Cu-supported catalysts and the exploration of the underlying working mechanisms.展开更多
Renewable energy is critical to building a sustainable society,but its true potential can only be unlocked by developing efficient,environmentally friendly energy storage systems.Advances in storage technologies,inclu...Renewable energy is critical to building a sustainable society,but its true potential can only be unlocked by developing efficient,environmentally friendly energy storage systems.Advances in storage technologies,including cost-effective and green materials,are quickly becoming the cornerstone of sustainable energy solutions.The most effective battery technology available now is lithium-ion batteries(LIBs).However,the sustainability of battery material production and the degradation of LIB functionality at subzero temperatures pose significant challenges,highlighting the urgent need for alternative and sustainable low-temperature(LT)electrode materials.To overcome these issues,a green synthesis approach is proposed to fabricate SnO2 nanoparticles using an aqueous extract of banana peel,while the leftover peel serves as a carbon precursor to produce a SnO2/hard carbon composite.The optimized SnO2/hard carbon(7:3)composite was used as the anode and showcased a remarkable reversible capacity of 1110 mAh g-1 at room temperature and retained about 660 mAh g-1 at-20℃ and 100 mA g-1 after 100 cycles,with a capacity of 383 mAh g-1 even at-30℃.Stable cycling performance was achieved by the synergistic interaction of SnO2 and hard carbon,which improved lithium-ion diffusion and mitigated volume expansion.This eco-friendly and scalable approach shows great promise for developing high-performance anodes for the next generation of LT LIBs.展开更多
With the widespread application of artificial intelligence(AI)computing in low-temperature scenarios such as deep space and deep sea,RRAM-based edge computing has gradually attracted attention.In this paper,an adaptiv...With the widespread application of artificial intelligence(AI)computing in low-temperature scenarios such as deep space and deep sea,RRAM-based edge computing has gradually attracted attention.In this paper,an adaptive reference conductance algorithm(ARCA)is proposed to improve the inference accuracy in low-temperature scenarios due to the conduction drift.The RRAM CIM chips with high read cycles are fabricated based on 28 nm CMOS logic technology,and the read times could reach 1012.By studying the influence of conductance drifting on inference accuracy in low temperature,a model of temperature and optimal reference conductance is proposed.Furthermore,by this model,adaptive selecting optimal reference conductance of analog-to-digital converters(ADCs)to quantize column current of RRAM array under different temperatures.At-40℃,the reference accuracy could increase from 75.43%to 86.8%.展开更多
Traditional marine steel suffers from a ductile-brittle transition temperature,compromising its performance in extremely low temperatures.To enhance low-temperature toughness,research has focused on material heterostr...Traditional marine steel suffers from a ductile-brittle transition temperature,compromising its performance in extremely low temperatures.To enhance low-temperature toughness,research has focused on material heterostructures.A novel marine steel featuring a ferrite-martensite lamellar structure through critical quenching in the dual-phase region and an 85%reduction warm rolling process on quenched and tempered steel was successfully developed.The formation mechanism of this layered structure and its impact on low-temperature toughness were systematically analyzed using multi-scale characterization and mechanical property testing.Findings reveal that the layered heterostructure markedly improves the low-temperature toughness of the steel while preserving strength and plasticity,evidenced by an increase in Charpy impact energy at−60℃by 81.35 J.The enhancement in low-temperature toughness of the tested steel is primarily attributed to grain refinement:Warm rolling markedly refines the grain structure,increasing the high-angle grain boundary density(>15°)from 0.4 to 3.1μm−1.This dense grain boundary network effectively impedes crack propagation,enhancing fracture resistance.Additionally,the ferrite-martensite lamellar structure imparts significant anisotropic characteristics,resulting in a layered structure effect.A distinct orientation difference distribution exists between directions perpendicular and parallel to the rolling direction.This unique microstructure increases the tortuosity of the crack path,significantly boosting low-temperature impact toughness.The lamellar heterostructure notably improves the toughness of the steel with minimal plasticity loss,offering a potential design strategy for optimizing the mechanical properties.展开更多
Sodium-ion batteries(SIBs)are promising for large-scale energy storage due to the abundance and low cost of sodium resources.However,the sluggish kinetics and unstable interface at low temperatures hinder its practica...Sodium-ion batteries(SIBs)are promising for large-scale energy storage due to the abundance and low cost of sodium resources.However,the sluggish kinetics and unstable interface at low temperatures hinder its practical applications.Here,we propose a dual-regulation strategy utilizing polyquaternium-10(PQ-10)to construct an electron-ion synergistic interface.PQ-10 regulates precursor nucleation through electrostatic interactions and simultaneously serves as a nitrogen-containing carbon source during in situ carbonization.The dual regulation enables uniform particle formation and a continuous nitrogen-doped carbon coating,improving interfacial stability and charge transport.The nitrogen-doped carbon layer reduces interfacial impedance,enhances reaction kinetics,and reconfigures interfacial electronic structure,stabilizing the Na3V1.925Mg0.075(PO4)3(NVMP)/carbon interface,promoting Na+extraction/insertion,and accelerating electron/ion transport.At-20℃,the NVMP/C-N@CNT-2 cathode delivers a high specific capacity(103.3 m Ah g-1at 0.1 C,95.9%of room-temperature capacity),exceptional rate capability(67.5 mAh g-1at 30 C),and ultra-stable cycling stability(approximately 100%retention after 5000 cycles at 10 C).This work delivers new insights into interfacial design principles enabling enhanced lowtemperature performance.展开更多
基金supported by the National Natural Science Foundation of China(No.52374247)the Joint Funds of the National Natural Science Foundation of China(No.U24B2042).
摘要In igneous-intruded coal seams,coal undergoes significant metamorphism,which critically alters its pore structure and oxygen consumption dynamics,thereby elevating its spontaneous combustion tendency.This study investigates the specific surface area,pore volume,structure complexity/connectivity,heterogeneity/local features of pore size distribution,and oxygen consumption dynamics of igneous metamorphic coal through N2/CO2 isothermal adsorption tests and low-temperature oxidation experiments,and elucidates the influence mechanisms of pore structure evolution on oxygen consumption dynamics during low-temperature oxidation.With increasing metamorphic degree,igneous metamorphic coal exhibits a more pronounced reduction in specific surface area during oxidation,while the increase in structure complexity due to coal-oxygen reactions is suppressed.Thermally metamorphic coal demonstrates accelerated oxygen consumption,with oxidation amplifying the difference in reaction rates compared to raw coal.Key mechanisms include oxidation-induced reduction in mesopore complexity and micropore volume,decreased dominance of small-pore-volume apertures,and increased heterogeneity,collectively leading to a lower half-oxygen-consuming temperature and steeper oxygen consumption curves.Simultaneously,increased pore volume/complexity and reduced uniformity/connectivity act synergistically to enhance oxygen consumption capacity,highlighting the coupling between pore structure evolution and oxidation behavior in igneous metamorphic coal.This study provides theoretical insights into the pore-oxygen coupling mechanisms governing coal spontaneous combustion in igneous intrusion areas.
基金financially supported by the PhD Scientific Research and Innovation Foundation of the Education Department of Hainan Province Joint Project of Sanya Yazhou Bay Science and Technology City(HSPHDSRF202407-001)the Project of Sanya Yazhou Bay Science and Technology City(SCKJ-JYRC-2023-01)+1 种基金the National Natural Science Foundation of China(42302160)Educational Reform of Hainan Higher Education Institutions(Hnjg2024-276)。
摘要Porosity is a fundamental parameter in characterizing the pore structure of shale oil reservoirs,as it directly affects the accuracy of shale oil reserve estimations.Despite the availability of various measurement techniques,accurately quantifying porosity in such reservoirs remains a significant challenge.In an effort to identify the most effective porosity testing method,this study collected samples from four shale oil reservoir intervals across five sags in three different basins.Five porosity testing methods were employed to detect shale porosity,including helium porosity,low-temperature nitrogen adsorption-desorption(LTNA/D),oil-saturated wetting,and nuclear magnetic resonance(NMR)T2and T1-T2.NMR T2porosity acted as a touchstone against which the other methods were compared.The pros and cons of each evaluation technique were explored to select the optimal analysis method for shale oil reservoirs.Results indicate that LTNA/D porosity,derived from powdered samples,commonly fails to reflect shale porosity effectively.Helium porosity,widely used for detecting nanoscale pores,is constrained by extended equilibration times and the retention of residual pore fluids after oil washing and drying,leading to systematic underestimation.In contrast,oil-saturation wetting and NMR T2exhibit strong agreement,both reflecting pore fluid content.However,residual fluid distribution can also impact the accuracy of NMR T2measurements.NMR T1-T2is an innovative technique for quantitatively evaluating shale oil reservoirs.NMR T1-T2spectrum at the water and oil restoration state can provide accurate shale porosity.NMRT1-T2porosity estimates generally align with those obtained from T2 porosity.When residual pore fluids are not entirely removable,the NMRT1-T2method offers a more realistic porosity assessment.The NMR technique is recommended for evaluating the porosity of shale oil reservoirs,and the combination of T2and T1-T2can accurately determine the effective and total porosity.This research serves as a valuable reference for accurately determining porosity in shale oil reservoirs.
基金supported by the National Natural Science Foundation of China(Nos.U22A20420,52203292,52203291)the Program for International S&T Cooperation Projects of Changzhou City(No.CZ20240026)。
摘要Silicon/graphite(Si/C)composites,which combine the advantages of Si anodes and commercial graphite anodes,are promising anode materials for high-energy-density lithium-ion batteries(LIBs).Despite experimental and theoretical studies on the electrochemical characteristics of different silicon crystal surfaces,there have been limited investigations on the electrochemical and mechanical properties of Si composite anode materials with different graphite crystal planes,such as the electrode interfaces between Si(111)and graphite(0001),as well as amorphous Si and graphite(1010).In this study,models of Si/C anode interfaces for LIBs were constructed to explore the mechanical-electrochemical-low-temperature performance by density functional theory(DFT)calculations and ab initio molecular dynamics(AIMD)simulations.The calculation results indicate that upon Li intercalation into the graphite(1010)surface,the electrical conductivity,electrochemical adsorption,and interfacial mechanical strength of the Si/C composite are significantly enhanced,with a separation work that is 2.3 times higher than that of Si/C on the graphite(0001)surface.More importantly,AIMD simulations at low temperatures reveal that the interface between graphite(1010)and amorphous Si forms a solid electrolyte interphase(SEI)rich in organic components,which significantly improves the Li-diffusion kinetics.This discovery provides new insights for the design and optimization of Si/C anode materials for low-temperature LIBs.
基金supported by the National Natural Science Foundation of China(22409071)Natural Foundation of Shandong Province(ZR2024QB120)+2 种基金Youth Innovation Group Plan of Shandong Province(2024KJG046)Higher-Level Talent Initial Scientific Research and Discipline Construction Fund(511/1009530)Joint Funds of the National Natural Science Foundation of China(No.U22A20140)。
摘要Protons emerge as superior charge carriers due to the lowest mass-to-charge ratio,ultra-high natural abundance,and the smallest ionic radius.Herein,2.0 M H2 SO4 dissolved in EG(ethylene glycol)/H2O cosolvent is investigated as an aqueous proton battery electrolyte,which not only enhances the cycling performance of MoO3 nanorod anode but also improves its low-temperature electrochemical performance.Specifically,the EG tightly adsorbs onto the surface of MoO3 nanorods,thereby inhibiting the corrosion from H2O molecules in the electrolyte and suppressing the dissolution of MoO3.In addition,EG molecule disturbs the hydrogen-bond network between H2O molecules,which greatly decreases the freezing point of the electrolyte,endowing the MoO3 nanorods with excellent low-temperature electrochemical performance.Therefore,the MoO3 nanorods exhibit a capacity retention of 96.9%after 2000 cycles at a current density of 10 A g-1in a three-electrode system.After assembling with CuHCF cathode,under-40℃,the full battery displays negligible capacity decay for over 2500 cycles at 1 A g-1.These results indicate that the cosolvent strategy has the promising potential in enhancing the performance of aqueous proton batteries.
基金financially supported by the National Natural Science Foundation of China(No.22309067)the Open Project Program of the State Key Laboratory of Materials-Oriented Chemical Engineering,China(No.KL21-05)the Marine Equipment and Technology Institute,Jiangsu University of Science and Technology,China(No.XTCX202404)。
摘要This study focused on improving the cathode performance of Ba0.6Sr0.4Co0.85Nb0.15O3-δ(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea0.6Sr0.4Co0.85Nb0.1Mo0.05O3-δ(B S CNM0.05),Ba0.6Sr0.4Co0.85Nb0.05Mo0.1O3-δ(BSCNM0.1),and Ba0.6Sr0.4Co0.85Mo0.15O3-δ(BSCM)—with Mo doping contents of 5mol%,10mol%,and15mol%,respectively,were successfully prepared using the sol-gel method.The effects of Mo doping on the crystal structure,conductivity,thermal expansion coefficient,oxygen reduction reaction(ORR)activity,and electrochemical performance were systematically evaluated using X-ray diffraction analysis,thermally induced characterization,electrochemical impedance spectroscopy,and single-cell performance tests.The results revealed that Mo doping could improve the conductivity of the materials,suppress their thermal expansion effects,and significantly improve the electrochemical performance.Surface chemical state analysis using X-ray photoelectron spectroscopy revealed that 5mol%Mo doping could facilitate a high adsorbed oxygen concentration leading to enhanced ORR activity in the materials.Density functional theory calculations confirmed that Mo doping promoted the ORR activity in the materials.At an operating temperature of 600℃,the BSCNM0.05cathode material exhibited significantly enhanced electrochemical impedance characteristics,with a reduced area specific resistance of 0.048Ω·cm~2,which was lower than that of the undoped BSCN matrix material by 32.39%.At the same operating temperature,an anode-supported single cell using a BSCNM0.05cathode achieved a peak power density of 1477 mW·cm-2,which was 30.71%,56.30%,and 171.50%higher than those of BSCN,BSCNM0.1,and B SCM,respectively.The improved ORR activity and electrochemical performance of BSCNM0.05indicate that it can be used as a cathode material in low-temperature solid oxide fuel cells.
基金supported by the National Natural Science Foundation of China(Nos.42072229,42030301,41102131,41972049,41972302 and 41977231)the Guangdong Basic and Applied Basic Research Foundation(No.2025A1515010724)+3 种基金the Guangdong Natural Science Foundation(No.2021A1515011658)the Science and Technology Program of Guangzhou(No.202002030184)the Special Fund for Basic Scientific Research of Central Colleges,Chang'an University(No.300102260502)the Deep Earth Probe and Mineral Resources Exploration-National Science and Technology Major Project(No.2024ZD1001003)。
摘要The paleo-geothermal gradient is a crucial parameter for converting the thermal history to the exhumation history.However,the precise estimation of this parameter has been a challenge.This paper presents a simple two-step method to model the paleo-geothermal gradient using low-temperature thermochronology.(1)It uses the Monte Carlo approach to generate thermal histories in a vertical section randomly and calculates the entire thermal history within the goodnessof-fit thresholds based on different paleo-geothermal gradients.(2)It selects the optimum paleogeothermal gradient by comparing the entire thermal history within different goodness-of-fit thresholds.We validated the method with apatite(U-Th)/He and fission track data collected from two drill cores in the Haiyuan-Liupanshan region.The result revealed that the best-fit paleo-geothermal gradient was~42℃/km during the Early Cretaceous–Miocene and has decreased rapidly to 20℃/km since~10 Ma.The crust thickening in the study area may explain the rapid reduction in the paleogeothermal gradient since~10 Ma.Our results are consistent with earlier studies in the region,suggesting that our simple and more intuitive approach provides an alternative method for paleogeothermal gradient modeling.
基金financially supported by the National Natural Science Foundation of China(No.52377222)Natural Science Foundation of Hunan Province(No.2023JJ20064)。
摘要Aqueous zinc-ion batteries(AZIBs)have emerged as strong contenders for large-scale energy storage solutions,attributed to their cost-effectiveness and enhanced safety profiles.Nevertheless,their widespread adoption is currently hindered by their poor performance in low-temperature conditions.Herein,an electrolyte is developed by utilizing weakly solvated and film-forming molecule dimethyl sulfite(DMS)to achieve smooth de-solvation and high ionic conductivity at low temperature.The DMS disrupts the hydrogen bonding network of water and lowers the freezing point of the electrolyte to-40.9℃.The designed electrolyte achieves ionic conductivity up to 10.75 m S/cm at-30℃.Due to the chemical reactivity of DMS and trifluoromethanesulfonate anions in the Zn2+-solvation shell,a Zn F2-Zn S hybrid solid electrolyte interphase(SEI)is successively generated on Zn metal surface.Mechanistic studies reveal that such robust hybrid interphase can promote Zn2+desolvation and rapid Zn2+transport.In addition,the addition of DMS effectively suppresses the dendritic growth,hydrogen evolution reaction(HER),and corrosioninduced passivation on the anode surface,facilitating long-term cycling at subzero temperatures.At-40℃,the Zn//Zn symmetrical cell cycles for 1200 h at 0.5 m A/cm2and 0.5 m Ah/cm2,and the Zn//NVO cell achieves an ultra-long cycle life of 1000 cycles with a high capacity retention of 82.89%at 1 A/g.
基金the National Natural Science Foundation of China,grant number 52406074the China Postdoctoral Science Foundation under Grant Number 2025T180171+1 种基金the Natural Science Foundation of Guangdong Province(2025A1515011270)the China Southern Power Grid Technology Project(GDKJXM20231415/030100KC23120104).
摘要In order to explore the effects of CaO,lignite dust and sawdust on the drying characteristics ofmunicipal sludge at different concentrations,a three-factor three-level regression experiment was carried out based on the results of thermogravimetric experiment and single factor experiment.By fitting three common mathematical models,the Page model with the highest fitting degree was selected to determine the most suitable mathematical model to describe the municipal sludge drying process.In addition,the Box-Behnken design principle in the response surface method was used to analyze the interaction of three factors on the drying characteristics of municipal sludge.The results of the study show that below 100℃is the optimal drying temperature range for municipal sludge.The results of single factor experiments showed that the order of influence of the three factors on sludge drying time was CaO concentration>sawdust concentration>lignite dust concentration.In the single factor experiment,the optimal process parameterswere CaOconcentration 3%,lignite powder concentration 7%,and sawdust concentration 7%.In themulti-factor interaction analysis,the interaction between CaO and sawdust had the most significant effect on the reduction of drying time,and the order of influence was as follows:CaO interaction with sawdust>lignite dust interaction with sawdust>CaO interaction with lignite powder.Further analysis showed that the optimal process ratio was 3%CaO concentration and 3%sawdust concentration.
基金financially supported by the Deep Earth Probe and Mineral Resources Exploration-National Science and Technology Major Project of China(No.2024ZD1001106)the China Geological Survey(Nos.DD20160083 and DD20190011)。
摘要The Beishan Fold-Thrust Belt(BFTB),located in the southern part of the Central Asian Orogenic Belt(CAOB),underwent complex intracontinental deformation during the late Mesozoic and is a key tectonic unit for deciphering the remote effects of plate margin orogenesis.In this study,we selected the Yemaquan region in southern Beishan and conducted remote sensing interpretation,field mapping,seismic profile interpretation and low-temperature thermochronological analyses.The Permian pluton and Carboniferous strata thrust over the Jurassic strata and developed a series of SEE-trending thrusts,NE-striking left strike-slip faults,and several SEE-and NE-trending folds.This area experienced two directions(NE and NW) of compression deformation.Under the joint influence of compression stress and pluton blocking,fold structures related to strike-slip faults also developed(the Big Ear syncline).The above constituted the Yemaquan Fold-Thrust system(YFTS).Zircon(U-Th)/He(ZHe) data reveal cooling events at~175-165 Ma;combining the regional deformation,it may indicate the compression time.We concluded that the intracontinental deformation of the BFTB in the southern CAOB was driven by the far-field effects.NE compression is related to the closure of the Mongol-Okhotsk Ocean and the collision of the Lhasa-Qiangtang block;NW compression is related to westward subduction of the Paleo-Pacific plate.
基金support from the Heilongjiang Touyan Innovation Team Program(HITTY-20190033)National Natural Science Foundation of China(22278096)Innovation Special Project on Science and Technology for Carbon Peaking and Carbon Neutrality in Jiangsu Province(WSSJH20230015)。
摘要The reliable operation of lithium-ion batteries(LIBs)in low temperatures has long been hindered by severe side reactions on graphite anodes.To develop a commercially viable low-temperature electrolyte,we design a solvent-resistant Nitrate-coordinated electrolyte.The practical Ah-level graphite LiNi0.5Co0.2Mn0.3O2 pouch cell with the newly developed electrolyte demonstrates a significant breakthrough in cycling stability,exhibiting negligible capacity fade after 250 cycles at-30℃ and 0.1 C.NO3-,as the functional additive,compresses the electric field around Li+through electrostatic interactions,mimicking the Debye-screening effect and inducing the coordinative exclusion of free ethyl acetate molecules at low temperatures.The transformation from contact ion pairs(CIPs)formed by Pto solventseparated ion pairs is significantly restrained,which mitigates the continuous reactions between the electrolyte and inevitable lithium deposition at low temperature.Additionally,this customized inert CIPs form a solid electrolyte interphase on graphite that exhibits remarkable ionic conductivity and rigidity,preventing excessive Li dendrite growth.This finding offers new insights into the relationship of microstructure-performance for low-temperature electrolytes,demonstrating that relying solely on inert CIPs can also inhibit the decomposition of the interfacial electrolyte,and inspires a unique design concept for high-performance,commercially viable LIBs that operate reliably in sub-zero environments.
基金Project supported by the National Natural Science Foundation of China(52370114)the Science and Technology Project of Southwest United Graduate School of Yunnan Province(202302AQ370002)。
摘要Converting CO2 to CH4 under mild conditions represents a promising strategy for carbon emission reduction and synthetic natural gas production,yet it remains challenging.In this work,we accelerated low-temperature CO2 hydrogenation over Ni-CeO2 catalysts by optimizing metal-support interactions through H2-driven reconstruction.The catalyst reduced at 400℃(Ni-CeO2-400R)achieved 84.3%CO2conversion with 100%CH4 selectivity even at a low temperature of 250℃.Various in situ spectroscopic characterizations(X-ray photoelectron spectroscopy(XPS),Raman,and diffused reflectance infrared Fourier transform spectroscopy(DRIFTS))and H2/D2 isotopic exchange experiments reveal that the appropriate interaction in Ni-CeO2 motivates the dispersion of metallic Ni sites and the generation of oxygen vacancies,thereby promoting the activation of H2 and CO2 molecules,respectively.Therefore,CO2 is efficiently adsorbed and converted into reactive intermediates and finally hydrogenated to CH4through carbonyl and formate pathways simultaneously.These findings underscore the critical role of tailored metal-support interactions in designing advanced CO2 hydrogenation catalysts.
摘要CO2methanation technology has shown great application prospects in carbon neutrality and hydrogen storage due to its extremely high energy efficiency and potential economic benefits.It is highly desirable but challenging to design novel catalyst and achieve efficient and stable CO2methanation under mild conditions.Herein,we developed a highly active electron-enriched Y2O3/Ni catalyst,achieving a stable operation with~80.1%CO2conversion and~100%CH4selectivity for 400 h at 0.1 MPa and 220℃,which was a 100℃lower than the conventional supported Ni-based catalysts.Structural characterizations confirmed that the Y2O3/Ni catalyst maintained dynamic redox changes and formed electron-enriched Y2O3-x-Ni interfaces under reaction conditions.Mechanism studies proved that the Y2O3-x-Ni interfaces obviously lowered the energy barrier of*HCO dissociation,and shifted the rate-determining step from*HCO dissociation to*CO hydrogenation.Furthermore,profited by the moderate COx adsorption ability and higher H2coverage at the Y2O3-x-Ni interfaces,the*CO hydrogenation reaction was kinetically promoted.The above factors accounted for the excellent low-temperature CO2methanation activity of the Y2O3/Ni catalyst.
基金financially supported by the Science and Technology Project of Southwest United Graduate School of Yunnan Province(Grant No.202302AQ370002)the project of the National Natural Science Foundation of China(Grant Nos.52370114 and 22276081)。
摘要Converting CO2to CH4 under mild conditions is a promising strategy for solving environmental and energy problems,but also a challenge.In this work,the low-temperature CO2 hydrogenation process over Ni/CeO2 catalysts was significantly accelerated by optimizing the H2 dissociation ability of Ni through the size effect,thus A-Ni/CeO2 with an average size of 4.9 nm achieved 83.4%CO2conversion with~100%CH4 selectivity even at 225℃.Systematic H2/D2 isotopic exchange experiments,in situ spectroscopic characterizations,and density functional theory(DFT)calculations reveal that the enhanced H2 activation ability not only promoted the creation of oxygen vacancies and hydroxyl group favorable for CO2 adsorption/activation in the pre-reduction process,but also the simultaneous hydrogenation of reactive intermediates belonging to carbonyl and formate pathway into CH4 in the reaction process.This fundamental understanding of the H2 dissociation effect on CO2 activation and hydrogenation provides critical insights for designing catalysts with considerable low-temperature activity,which significantly reduces energy consumption and operating costs for industrial CO2 conversion.
基金financed by the National Natural Science Foundation of China(Nos.52377216 and 52072342)the National Key R&D Program of China(No.2022YFB2502000)。
摘要Conventional graphite synthesis involves CO2emission and a graphitization process at a high temperature of~3000℃.Herein,we report a new method to synthesize high-performance graphite anode materials from greenhouse CO2gas at an external heating temperature as low as 135℃.Transition metal catalysts are not required for low-temperature synthesis of graphite.Extreme graphitization temperatures are not required as compared to graphite synthesized from petroleum coke-based materials.The graphitization degree of graphite was found to be strongly related to CO2pressure.Graphite was synthesized at a maximum pressure of 20 MPa,whereas semi-graphited carbon was synthesized at a maximum pressure of 6.3 MPa.The synthesized graphite exhibited superior lithium storage kinetics and excellent cycling stability over 3000 cycles,with a capacity retention of~100% at 1.0 A·g-1.This work establishes an integrated sustainable strategy that concurrently addresses greenhouse gas utilization and energy-efficient anode material production.
基金the financial support from the Key Project of Shaanxi Provincial Natural Science Foundation-Key Project of Laboratory(2025SYS-SYSZD-117)the Natural Science Basic Research Program of Shaanxi(2025JCYBQN-125)+8 种基金Young Talent Fund of Xi'an Association for Science and Technology(0959202513002)the Key Industrial Chain Technology Research Program of Xi'an(24ZDCYJSGG0048)the Key Research and Development Program of Xianyang(L2023-ZDYF-SF-077)Postdoctoral Fellowship Program of CPSF(GZC20241442)Shaanxi Postdoctoral Science Foundation(2024BSHSDZZ070)Research Funds for the Interdisciplinary Projects,CHU(300104240913)the Fundamental Research Funds for the Central Universities,CHU(300102385739,300102384201,300102384103)the Scientific Innovation Practice Project of Postgraduate of Chang'an University(300103725063)the financial support from the Australian Research Council。
摘要Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temperature(LT)operation.Therefore,a more comprehensive and systematic understanding of LIB behavior at LT is urgently required.This review article comprehensively reviews recent advancements in electrolyte engineering strategies aimed at improving the low-temperature operational capabilities of LIBs.The study methodically examines critical performance-limiting mechanisms through fundamental analysis of four primary challenges:insufficient ionic conductivity under cryogenic conditions,kinetically hindered charge transfer processes,Li+transport limitations across the solidelectrolyte interphase(SEI),and uncontrolled lithium dendrite growth.The work elaborates on innovative optimization approaches encompassing lithium salt molecular design with tailored dissociation characteristics,solvent matrix optimization through dielectric constant and viscosity regulation,interfacial engineering additives for constructing low-impedance SEI layers,and gel-polymer composite electrolyte systems.Notably,particular emphasis is placed on emerging machine learning-guided electrolyte formulation strategies that enable high-throughput virtual screening of constituent combinations and prediction of structure-property relationships.These artificial intelligence-assisted rational design frameworks demonstrate significant potential for accelerating the development of next-generation LT electrolytes by establishing quantitative composition-performance correlations through advanced data-driven methodologies.
基金Supported by National Key Research and Development Program of China(2020YFD1100302)。
摘要Under the context of global energy transition and carbon neutrality,controlling nitrogen oxide(NOx)emissions from biomass combustion is of great significance,and the development of high-efficiency low-temperature catalysts has become a current research focus.In this study,Nb was used to dope and modify the Mn7-Cu3/BCN catalyst to construct the Mn7-Cu3-Nbx/BCN system.The doping amount was optimized through selective catalytic reduction(SCR)activity tests.The reaction mechanism was explored by combining in situ DRIFTS and density functional theory(DFT)simulations.Experimental findings revealed that the catalyst doped with 0.05%Nb achieved the optimal performance,sustaining a NO conversion efficiency of≥94%within the temperature window of 150−275℃while demonstrating improved resistance to alkali metal K poisoning.Mechanistic analyses showed that at low temperatures,the catalyst facilitated the SCR reaction via both the Eley-Rideal(E-R)and Langmuir-Hinshelwood(L-H)pathways,with the synergistic interaction between multiple active sites driving the efficient conversion of NH3 and NO.DFT calculations further confirmed that both pathways had the characteristics of low reaction energy barriers and significant exothermicity,ensuring the high activity and feasibility of the low-temperature reaction.The findings provided foundational theoretical support for the design of Nb-doped Mn-Cu-supported catalysts and the exploration of the underlying working mechanisms.
基金funded by the projects AP19578472“Electrophoretic deposition of composite multilayer gel-polymer electrolyte for 3D lithium-ion batteries”the Research Targeted Programs BR24992766“Development of methods and technologies for environmentally friendly“green”processing of polymer waste for energy storage”from the Ministry of ScienceHigher Education of the Republic of Kazakhstan and 111024CRP2010 and 20122022FD4135 from Nazarbayev University。
摘要Renewable energy is critical to building a sustainable society,but its true potential can only be unlocked by developing efficient,environmentally friendly energy storage systems.Advances in storage technologies,including cost-effective and green materials,are quickly becoming the cornerstone of sustainable energy solutions.The most effective battery technology available now is lithium-ion batteries(LIBs).However,the sustainability of battery material production and the degradation of LIB functionality at subzero temperatures pose significant challenges,highlighting the urgent need for alternative and sustainable low-temperature(LT)electrode materials.To overcome these issues,a green synthesis approach is proposed to fabricate SnO2 nanoparticles using an aqueous extract of banana peel,while the leftover peel serves as a carbon precursor to produce a SnO2/hard carbon composite.The optimized SnO2/hard carbon(7:3)composite was used as the anode and showcased a remarkable reversible capacity of 1110 mAh g-1 at room temperature and retained about 660 mAh g-1 at-20℃ and 100 mA g-1 after 100 cycles,with a capacity of 383 mAh g-1 even at-30℃.Stable cycling performance was achieved by the synergistic interaction of SnO2 and hard carbon,which improved lithium-ion diffusion and mitigated volume expansion.This eco-friendly and scalable approach shows great promise for developing high-performance anodes for the next generation of LT LIBs.
基金supported in part by the Brain Science and Brain-like Intelligence Technology-National Science and Technology Major Project(Grant No.2021ZD0201203)in part by the NSFC(Grants Nos.62504248,62322412,92464201,62488101)in part by the Youth innovation Promotion Association CAS。
摘要With the widespread application of artificial intelligence(AI)computing in low-temperature scenarios such as deep space and deep sea,RRAM-based edge computing has gradually attracted attention.In this paper,an adaptive reference conductance algorithm(ARCA)is proposed to improve the inference accuracy in low-temperature scenarios due to the conduction drift.The RRAM CIM chips with high read cycles are fabricated based on 28 nm CMOS logic technology,and the read times could reach 1012.By studying the influence of conductance drifting on inference accuracy in low temperature,a model of temperature and optimal reference conductance is proposed.Furthermore,by this model,adaptive selecting optimal reference conductance of analog-to-digital converters(ADCs)to quantize column current of RRAM array under different temperatures.At-40℃,the reference accuracy could increase from 75.43%to 86.8%.
基金support from National Key Research and Development Program of China(2022YFB4201502)the Hubei Province Key Research and Development Program(2023BAA019-4)the Postgraduate Innovation and Entrepreneurship Fund Project of Wuhan University of Science and Technology(JCX2024001).
摘要Traditional marine steel suffers from a ductile-brittle transition temperature,compromising its performance in extremely low temperatures.To enhance low-temperature toughness,research has focused on material heterostructures.A novel marine steel featuring a ferrite-martensite lamellar structure through critical quenching in the dual-phase region and an 85%reduction warm rolling process on quenched and tempered steel was successfully developed.The formation mechanism of this layered structure and its impact on low-temperature toughness were systematically analyzed using multi-scale characterization and mechanical property testing.Findings reveal that the layered heterostructure markedly improves the low-temperature toughness of the steel while preserving strength and plasticity,evidenced by an increase in Charpy impact energy at−60℃by 81.35 J.The enhancement in low-temperature toughness of the tested steel is primarily attributed to grain refinement:Warm rolling markedly refines the grain structure,increasing the high-angle grain boundary density(>15°)from 0.4 to 3.1μm−1.This dense grain boundary network effectively impedes crack propagation,enhancing fracture resistance.Additionally,the ferrite-martensite lamellar structure imparts significant anisotropic characteristics,resulting in a layered structure effect.A distinct orientation difference distribution exists between directions perpendicular and parallel to the rolling direction.This unique microstructure increases the tortuosity of the crack path,significantly boosting low-temperature impact toughness.The lamellar heterostructure notably improves the toughness of the steel with minimal plasticity loss,offering a potential design strategy for optimizing the mechanical properties.
基金supported by the National Natural Science Foundation of China(NSFC Grants 52574464)the State Grid Heilongjiang Electric Power Co.,Ltd.,Technology Project Funding(52243723000C)。
摘要Sodium-ion batteries(SIBs)are promising for large-scale energy storage due to the abundance and low cost of sodium resources.However,the sluggish kinetics and unstable interface at low temperatures hinder its practical applications.Here,we propose a dual-regulation strategy utilizing polyquaternium-10(PQ-10)to construct an electron-ion synergistic interface.PQ-10 regulates precursor nucleation through electrostatic interactions and simultaneously serves as a nitrogen-containing carbon source during in situ carbonization.The dual regulation enables uniform particle formation and a continuous nitrogen-doped carbon coating,improving interfacial stability and charge transport.The nitrogen-doped carbon layer reduces interfacial impedance,enhances reaction kinetics,and reconfigures interfacial electronic structure,stabilizing the Na3V1.925Mg0.075(PO4)3(NVMP)/carbon interface,promoting Na+extraction/insertion,and accelerating electron/ion transport.At-20℃,the NVMP/C-N@CNT-2 cathode delivers a high specific capacity(103.3 m Ah g-1at 0.1 C,95.9%of room-temperature capacity),exceptional rate capability(67.5 mAh g-1at 30 C),and ultra-stable cycling stability(approximately 100%retention after 5000 cycles at 10 C).This work delivers new insights into interfacial design principles enabling enhanced lowtemperature performance.