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 H_(2) SO_(4) dissolved in EG(ethylene glycol)/H_(2)O 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 H_(2) SO_(4) dissolved in EG(ethylene glycol)/H_(2)O cosolvent is investigated as an aqueous proton battery electrolyte,which not only enhances the cycling performance of MoO_(3) nanorod anode but also improves its low-temperature electrochemical performance.Specifically,the EG tightly adsorbs onto the surface of MoO_(3) nanorods,thereby inhibiting the corrosion from H_(2)O molecules in the electrolyte and suppressing the dissolution of MoO_(3).In addition,EG molecule disturbs the hydrogen-bond network between H_(2)O molecules,which greatly decreases the freezing point of the electrolyte,endowing the MoO_(3) nanorods with excellent low-temperature electrochemical performance.Therefore,the MoO_(3) nanorods exhibit a capacity retention of 96.9%after 2000 cycles at a current density of 10 A g^(-1)in 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
Among the alloying-type anodes,elemental Sb possesses the suitable yet safe plateau,simple lithiation pathway,small voltage polarization,high conductivity,and superior cycle stability.However,challenge is that its int...Among the alloying-type anodes,elemental Sb possesses the suitable yet safe plateau,simple lithiation pathway,small voltage polarization,high conductivity,and superior cycle stability.However,challenge is that its intrinsic capacity is rather low(660 mAh g^(-1)),<1/6 of silicon.Herein,we propose a seamless integration strategy by merging the voltage and capacity of phosphorus and antimony into a solid solution alloy.Interestingly,the enlistment of P is found greatly enlarge the capacity from 660 to 993 mAh g^(-1) for such Sb_(30)P_(30) solid solution,while maintaining a single and stable discharge plateau(~0.79 V)similar to elemental Sb.Various experimental characterizations including XPS,PDF,Raman,and EDS mapping reveal that in such a material the P and Sb atoms have interacted with each other to form a homogenous solid solution alloy,rather than a simple mixing of the two substances.Thus,the Sb_(30)P_(30) exhibits superior rate performances(807 mAh g^(-1) at 5000 mA g^(-1))and cyclability(821 mAh g^(-1) remained after 300 cycles).Furthermore,such Sb_(60-x)P_(x) alloys can even deliver 621 mAh g^(-1) at30℃,which can be served as the alternative anode materials for high-energy and low-temperature batteries.This unique seamless integration strategy based on solid solution chemistry can be easily leveraged to manipulate the capacity of other electrode materials at similar voltage.展开更多
Sodium-ion batteries (NIBs) have become an ideal alternative to lithium-ion batteries in the field of electrochemical energy storage due to their abundant raw materials and cost-effectiveness. With the progress of hum...Sodium-ion batteries (NIBs) have become an ideal alternative to lithium-ion batteries in the field of electrochemical energy storage due to their abundant raw materials and cost-effectiveness. With the progress of human society, the requirements for energy storage systems in extreme environments, such as deep-sea exploration, aerospace missions, and tunnel operations, have become more stringent. The comprehensive performance of NIBs at low temperatures (LTs) has also become an important consideration. Under LT conditions, challenges such as increased viscosity of electrolyte, abnormal growth of solid electrolyte interface, and poor contact between collector and electrode materials emerge. The aforementioned issues hinder the diffusion kinetics of sodium ions (Na^(+)) at the electrode/electrolyte interface and cause rapid degradation of battery performance. Consequently, the optimization of electrolyte composition and cathode/anode materials becomes an effective approach to improve LT performance. This review discusses the conduction behavior and limiting factors of Na^(+) in both solid electrodes and liquid electrolytes at LT. Furthermore, it systematically reviews the recent research progress of LT NIBs from three aspects: cathode materials, anode materials, and electrolyte components. This review aims to provide a valuable reference for developing high-performance LT NIBs.展开更多
A novel Mo-doped CuO catalyst is developed and used for low-temperature NH_(3)-SCR reaction.Compared with the undoped CuO sample,the Mo doped CuO catalyst shows an increased SCR performance with above 80%NO_(x) conver...A novel Mo-doped CuO catalyst is developed and used for low-temperature NH_(3)-SCR reaction.Compared with the undoped CuO sample,the Mo doped CuO catalyst shows an increased SCR performance with above 80%NO_(x) conversion at 175℃.The XRD and Raman results have confirmed the incorporation of Mo metal ions into CuO lattice to form Mo-O-Cu species which may be related to the enhanced SCR activity.The XPS and UV-vis results reveal the creation of electron interaction between Cu and Mo in this Mo-O-Cu system which provides an increased amount of Lewis and Brønsted acid sites,thereby promoting the adsorption capacity of NH_(3) and NO_(x) as verified by NH_(3)-TPD and NO_(x)-TPD characterization.Besides,it also promotes the formation of oxygen vacancies,leading to the increasing of chemisorbed oxygen species,which improves the NO oxidation to NO_(2) activity.Furthermore,in situ DRIFTS technology was also used to study the reaction mechanism of this Mo doped CuO catalyst.The formed NO_(2) could react with NHx(x=3,2)species to enhance the low-temperature NH_(3)-SCR activity via the"fast-SCR"reaction pathway.The nitrate and nitrite ad-species may react with NH_(3) and NH4^(+)ad-species through the L-H pathway.展开更多
In this work,a multi-core-shell-structured LiFePO_(4)@Na_(3) V_(2)(PO_(4))_(3)@C(LFP@NVP@C) composite was successfully designed and prepared to address inferior low-temperature performance of LiFePO_(4) cathode for li...In this work,a multi-core-shell-structured LiFePO_(4)@Na_(3) V_(2)(PO_(4))_(3)@C(LFP@NVP@C) composite was successfully designed and prepared to address inferior low-temperature performance of LiFePO_(4) cathode for lithium-ion batteries.Transmission electron microscopy(TEM) confirms the inner NVP and outer carbon layers coexisted on the surface of LFP particle.When evaluated at low-temperature operation,LFP@NVP@C composite exhibits an evidently enhanced electrochemical performance in term of higher capacity and lower polarization,compared with LFP@C.Even at-10℃ with 0.5 C,LFP@NVP@C delivers a discharge capacity of ca.96.9 mAh-g^(-1) and discharge voltage of ca.3.3 V,which is attributed to the beneficial contribution of NVP coating.NAS ICON-structured NVP with an open framework for readily insertion/desertion of Li+ will effectively reduce the polarization for the electrochemical reactions of the designed LFP@NVP@C composite.展开更多
Low-temperature performance and high-rate discharge capability of AB5-type non-stoichiometric hydrogen storage are studied. X-ray diffraction(XRD),pressure-composition-temperature(PCT) curves and electrochemical imped...Low-temperature performance and high-rate discharge capability of AB5-type non-stoichiometric hydrogen storage are studied. X-ray diffraction(XRD),pressure-composition-temperature(PCT) curves and electrochemical impedance spectroscopy(EIS) are applied to characterize the electrochemical properties of ABx(x=4.8,4.9,5.0,5.1,5.2) alloys. The results show that the non-stoichiometric alloys exhibit better electrochemical properties compared with that of the AB5 alloy.展开更多
This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0...This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.1)Mo_(0.05)O_(3-δ)(B S CNM_(0.05)),Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.05)Mo_(0.1)O_(3-δ)(BSCNM_(0.1)),and Ba_(0.6)Sr_(0.4)Co_(0.85)Mo_(0.15)O_(3-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 BSCNM_(0.05)cathode 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 BSCNM_(0.05)cathode achieved a peak power density of 1477 mW·cm^(-2),which was 30.71%,56.30%,and 171.50%higher than those of BSCN,BSCNM_(0.1),and B SCM,respectively.The improved ORR activity and electrochemical performance of BSCNM_(0.05)indicate that it can be used as a cathode material in low-temperature solid oxide fuel cells.展开更多
Achieving an in-depth understanding of the nexus between temperature and phase transitions is paramount for advancing the electrochemical efficiency of aqueous zinc ion batteries.Yet,the intricacies of electrochemical...Achieving an in-depth understanding of the nexus between temperature and phase transitions is paramount for advancing the electrochemical efficiency of aqueous zinc ion batteries.Yet,the intricacies of electrochemical interactions,particularly those associated with the structural evolution over extended periods,remain enigmatic.In this research,we leverage V_(2)O_(5) as an initial structural model of crystals to demystify the kinetics of electrode reactions and the decay mechanism of global electrochemical degradation by meticulously controlling the crystal defects via applying different mechanical grounding intensities.It is noted that the grounding V_(2)O_(5)(GVO)can exhibit a stable crystal structure that suppresses the dissolution/shuttling of vanadium and mitigates Zn anodes by-products caused by electrochemical processes.Thus,the GVO is utilized as the cathode material,achieving excellent Zn storage capacity at both room temperature and low temperatures,e.g.,380 and 246 mA h g^(−1) at room temperature and−20℃,respectively.Remarkably,the GVO cathode retains a specific capacity of 160 mA h g^(−1) with a capacity retention rate of 99%after 1500 cycles at−20℃ and 1 A g^(−1).This work provides a novel insight into the electrochemical crosstalk behavior of aqueous zinc-ion batteries(AZIBs)in a wide range of temperatures.展开更多
Because of their excellent low-temperature(−15 to−40℃)tolerance,sodium-ion batteries are emerging as a complement to lithium-ion batteries for use in extremely cold environments(e.g.high-latitude areas).Hard carbon h...Because of their excellent low-temperature(−15 to−40℃)tolerance,sodium-ion batteries are emerging as a complement to lithium-ion batteries for use in extremely cold environments(e.g.high-latitude areas).Hard carbon has a high low-voltage sodium storage capacity and a good initial efficiency,making it one of the most promising anode materials for sodium-ion batteries.It has a complex structure,featuring closed pores,nano graphitic domains,and surface functional groups.The sodium storage sites in hard carbon are reviewed as are the widely accepted sodium storage mechanisms.The main factors contributing to the degradation of the good low-temperature performance in hard carbon anodes are considered,including sodium dendrite formation,low ion diffusion rates,and surface-side reactions.Finally,strategies to increase the low-temperature sodium storage performance of hard carbon anodes are summarized,including bulk structure design,and improvements in interfaces and cut-off voltage.Guidance is provided for improving the low-temperature performance of hard carbon anodes to accelerate the development of these batteries.展开更多
The design and development of high-performance anodes pose significant challenges in the construction of next-generation rechargeable lithium-ion batteries(LIBs).Sodium molybdate dihydrate(Na_(2)MoO_(4)·2H_(2)O)h...The design and development of high-performance anodes pose significant challenges in the construction of next-generation rechargeable lithium-ion batteries(LIBs).Sodium molybdate dihydrate(Na_(2)MoO_(4)·2H_(2)O)has garnered increasing attention due to its cost-effectiveness,non-toxicity and earth abundance.To enhance the Li storage performance of Na_(2)MoO_(4)·2H_(2)O,a crystallographic orientation regulation strategy is proposed in this work.Initially,density functional theory calculations are carried out to demonstrate that the(020)crystal plane of Na_(2)MoO_(4)·2H_(2)O offers the lowest energy barrier for Li^(+)migration.Subsequently,the preferred crystallographic orientation of Na_(2)MoO_(4)·2H_(2)O crystal is tuned through a low-temperature recrystallization method.Furthermore,the microstructure and phase changes of Na_(2)MoO_(4)·2H_(2)O during the lithiation/de-lithiation process are studied using in situ and ex situ XRD tests,ex situ XPS and cyclic voltammetry to unravel its Li^(+)storage mechanism.Upon application as LIBs anode,the Na_(2)MoO_(4)·2H_(2)O single-crystal particles with a preferred(020)surface exhibit superior reversible capacity,high-capacity retention and high cycling stability.The enhanced Li storage performance should be attributed to the regulated crystallographic orientation and small changes in the crystal microstructure during the charge/discharge process,which facilitates Li^(+)migration and bolsters structural stability.Notably,this study introduces a novel concept and a simple synthesis method for the advancement of electrodes in rechargeable batteries.展开更多
The distributions of framework aluminum(Al)in zeolites critically govern the location and speciation of active copper(Cu)centers,thereby influencing their performance in ammonia selective catalytic reduction(NH_(3)-SC...The distributions of framework aluminum(Al)in zeolites critically govern the location and speciation of active copper(Cu)centers,thereby influencing their performance in ammonia selective catalytic reduction(NH_(3)-SCR)of nitrogen oxides(NO_(x)).Conventional Cu-SSZ-39(Cu-SSZ-39-T)exhibits excellent hydrothermal stability but limited low-temperature activity(150–225℃)due to a low concentration of Al in 8-membered rings(8MRs)that inhibits the formation of active[Cu(OH)]^(+)-Z species.Herein,an SSZ-39 zeolite synthesized with potassium ions(SSZ-39-K)achieved a significantly higher 8MR Al fraction(37.6%).Density functional theory calculations and H_(2)-temperature-programmed reduction analyses confirmed that the increased 8MR Al population facilitated the formation of[Cu(OH)]^(+)-Z species.Aged Cu-SSZ-39-K exhibited nearly twice the NO_(x)conversion of aged Cu-SSZ-39-T in the 150–225℃range while maintaining comparable high-temperature activity(250–550℃)under a gas hourly space velocity of 250,000 h^(-1).Enhanced low-temperature performance is particularly beneficial for mitigating NO_(x)emissions during cold-start phase.Moreover,SSZ-39-K was synthesized with a high crystallization yield(~65%),nearly double the highest yield(33%)reported for direct synthesis routes.This work establishes a robust strategy for tailoring Al distributions in SSZ-39 zeolites,offering an effective pathway to improve low-temperature NH_(3)-SCR performance and promote practical implementation.展开更多
Al/NH_(4)CoF_(3)-Φ(Φ=0.5,1.0,1.5,2.0,and 3.0)binary composites and Al-NH_(4)CoF_(3)@P(VDF-HFP)ternary composites are fabricated via ultrasonication-assisted blending and electrostatic spraying.The effect of equivale...Al/NH_(4)CoF_(3)-Φ(Φ=0.5,1.0,1.5,2.0,and 3.0)binary composites and Al-NH_(4)CoF_(3)@P(VDF-HFP)ternary composites are fabricated via ultrasonication-assisted blending and electrostatic spraying.The effect of equivalence ratio(Φ)on the reaction properties is systematically investigated in the binary Al/NH_(4)CoF_(3)system.For ternary systems,electrostatic spraying allows both components to be efficiently encapsulated by P(VDF-HFP)and to achieve structural stabilization and enhanced reactivity through synergistic interfacial interactions.Morphological analysis using SEM/TEM revealed that P(VDF-HFP)formed a protective layer on Al and NH_(4)CoF_(3)particles,improving dispersion,hydrophobicity(water contact angle increased by 80.5%compared to physically mixed composites),and corrosion resistance.Thermal decomposition of NH_(4)CoF_(3)occurred at 265℃,releasing NH_(3)and HF,which triggered exothermic reactions with Al.The ternary composites exhibited a narrowed main reaction temperature range and concentrated heat release,attributed to improved interfacial contact and polymer decomposition.Combustion tests demonstrated that Al-NH_(4)CoF_(3)@P(VDF-HFP)achieved self-sustaining combustion.In addition,a simple validation was done by replacing the Al component in the aluminium-containing propellant,demonstrating its potential application in the propellant field.This work establishes a novel strategy for designing stable,high-energy composites with potential applications in advanced propulsion systems.展开更多
This study systematically conducted preparation optimization and performance investigations on Co-modified Ce/TiO_(2) catalysts,with a focus on examining how preparation methods and Co loading regulate the catalyst’s...This study systematically conducted preparation optimization and performance investigations on Co-modified Ce/TiO_(2) catalysts,with a focus on examining how preparation methods and Co loading regulate the catalyst’s low-temperature denitrification activity.After identifying optimal preparation parameters via condition screening,multiple characterization techniques-including BET,XRD,XPS,H_(2)-TPR and in situ DRIFTS-were employed to deeply analyze the catalyst’s physicochemical properties and reaction mechanism.Results demonstrated that compared to the impregnation and co-precipitation methods,the Ce-Co_(0.025)/TiO_(2)-SG catalyst(prepared by the sol-gel method with a Co/Ti mass ratio of 0.025)exhibited significantly superior denitrification activity:NO conversion remained stably above 95%in the 225−350℃ temperature range,and it displayed high N_(2) selectivity.Characterization analysis revealed that abundant surface oxygen vacancies,a high proportion of Ce^(3+) species,and prominent acidic sites collectively contributed to enhancing its low-temperature denitrification performance.This work provides reference value for the development of highly efficient low-temperature denitrification catalysts.展开更多
Under the context of global energy transition and carbon neutrality,controlling nitrogen oxide(NO_(x))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(NO_(x))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 Mn_(7)-Cu_(3)/BCN catalyst to construct the Mn_(7)-Cu_(3)-Nb_(x)/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
The adsorptive denitrification performance of MIL-101(Cr)-0.5 toward pyridine,aniline or quinoline in simulated fuels with basic nitrogen content of 1732μg/g was evaluated separately.Furthermore,the effects of adsorp...The adsorptive denitrification performance of MIL-101(Cr)-0.5 toward pyridine,aniline or quinoline in simulated fuels with basic nitrogen content of 1732μg/g was evaluated separately.Furthermore,the effects of adsorption temperature,adsorption time and adsorbent dosage on their adsorptive denitrification performance were systematically investigated.The experimental results demonstrated that under a fixed adsorbent dosage of 0.05 g and a simulated fuel volume of 10 mL,the optimal removal efficiency for aniline was achieved at 30℃ within 30 min,whereas higher temperatures and longer times(40℃and 40 min)were required for effective removal of pyridine and quinoline.Density Functional Theory(DFT)calculations were conducted via Materials Studio(MS)software to study the adsorptive denitrification mechanism of MIL-101(Cr)toward these three basic nitrogen-containing compounds.The simulation calculation results revealed that the interaction between pyridine and MIL-101(Cr)primarily involved coordination adsorption.In contrast,the interaction between aniline or quinoline and MIL-101(Cr)proceeded mainly through coordination,with additional contributions fromπ-complexation and hydrogen bonding.The overall adsorption strength order is pyridine>aniline>quinoline.During the adsorption process,pyridine and quinoline transfer electrons to the MIL-101(Cr)surface through the H→C→N→Cr^(3+)pathway,while aniline transfers electrons to the MIL-101(Cr)surface through various pathways,including N→Cr^(3+),N→C→Cr^(3+)and N→H→O.Furthermore,adsorption kinetics studies indicated that the adsorption processes for all three basic nitrogen-containing compounds followed the quasi second order kinetic models.The experimental results on the effect of benzene on the adsorptive denitrification performance of MIL-101(Cr)-0.5 demonstrated that benzene exerted a more significant impact on the adsorption of aniline and quinoline.Finally,the adsorbent was regenerated using ethanol washing.It was found that MIL-101(Cr)-0.5 retained stable denitrification performance after two regeneration cycles.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
To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content ...To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content in coal)catalysts were prepared by the incipient wetness impregnation method,followed by acid washing to remove calcium-containing minerals.Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity.Specifically,NO conversion increased from 88.3%of Mn-Ce/De-AC to 91.7%of Mn-Ce/De-AC-1CaCO_(3)(210℃).The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn^(4+)content and Ce^(4+)/Ce^(3+)ratio,an abundance of chemisorbed oxygen and acidic sites,which could strengthen the SCR reaction pathways(richer NH_(3)activated species and bidentate nitrate active species).Therefore,NO removal is enhanced.展开更多
Severe failures of nonstructural components have occurred during previous earthquakes.Claddings are one of the most widely used nonstructural component and are installed in many modern buildings;therefore,an evaluatio...Severe failures of nonstructural components have occurred during previous earthquakes.Claddings are one of the most widely used nonstructural component and are installed in many modern buildings;therefore,an evaluation of their seismic performance is important and cannot be ignored.To investigate the seismic performance of large-sized high performance concrete cladding(HPCC),a series of full-scale experimental tests were conducted using a unidirectional shaking table.A steel supporting frame was used to install the HPCCs and reproduce the effects of the building under earthquake.The tests were divided into two parts:in-plane(IP)testing and out-plane(OP)testing.Three recorded accelerograms,one artificial accelerogram,and one sinusoidal accelerogram were used to conduct the shaking table tests.The results show that the maximum recorded IP responses of acceleration and interstory drift ratio were 1.04 g and 1/97,while the OP responses were 1.02 g and 1/51.The HPCCs functioned well throughout the entire experimental protocol.The fundamental frequency of the HPCCs systems rarely changed after the tests.展开更多
Purpose:ATLAS is a cross-sectional study aiming to investigate environmental and genetic determinants of athletic performance in healthy Greek competitive athletes(CA).This article presents the study design,investigat...Purpose:ATLAS is a cross-sectional study aiming to investigate environmental and genetic determinants of athletic performance in healthy Greek competitive athletes(CA).This article presents the study design,investigates the muscle strength performance(MSP)of 289 adult and teenage CA,exercisers,and physically inactive individuals(PI),and proposes predictive models of MSP for adults.Methods:Muscle maximal,speed,and explosive strength(MMS/MSS/MES)at unilateral maximal concentric flexion and extension contraction(FC/EC)were evaluated using Biodex System 3 PRO^(TM)at 60°/s,180°/s,and 300°/s,while additional performance markers were assessed through field ergometric testing.Participants were interviewed about their lifestyle,dietary habits,physical activity,injury,and medical history.Body composition was assessed via bioelectrical impedance.gDNA was extracted from biochemical samples and then genotyped.Statistical analysis was conducted using IBM SPSS Statistics v21.0 and R.Results:Age,fitness,and sex impacted correlations of MSP with body composition and anthropometric measurements(p<0.05).Among CA,females outperformed males in accuracy(p<0.001)while,males outperformed females in anaerobic power,MSP,speed,and endurance(p<0.001).Adult CA outperformed exercisers and PI in MMS,MSS,and MES(p<0.05).Multiple linear regression models,with predictors age,FFM,body extremity,training load explained the majority of variation in MMS(R^(2)_(adj):71.4%–88.9%),MSS(R^(2)_(adj):64.8%–78.4%),and MES(R^(2)_(adj):52.7%–68.4%)at EC,FC,and their mean(p<0.001).Conclusions:Muscle-strengthening strategies should be customized according to individual fitness levels,body composition,and anthropometric measurements.The innovative sex-specific regression models assessing MMS,MSS,and MES at EC and FC provide a framework for personalizing rehabilitation and skill-specific training strategies.展开更多
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 N_(2)/CO_(2) 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
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)。
文摘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 H_(2) SO_(4) dissolved in EG(ethylene glycol)/H_(2)O cosolvent is investigated as an aqueous proton battery electrolyte,which not only enhances the cycling performance of MoO_(3) nanorod anode but also improves its low-temperature electrochemical performance.Specifically,the EG tightly adsorbs onto the surface of MoO_(3) nanorods,thereby inhibiting the corrosion from H_(2)O molecules in the electrolyte and suppressing the dissolution of MoO_(3).In addition,EG molecule disturbs the hydrogen-bond network between H_(2)O molecules,which greatly decreases the freezing point of the electrolyte,endowing the MoO_(3) nanorods with excellent low-temperature electrochemical performance.Therefore,the MoO_(3) nanorods exhibit a capacity retention of 96.9%after 2000 cycles at a current density of 10 A g^(-1)in 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the National Natural Science Foundation of China(Grant No.52072138,21571073,51772115)National Key Research and Development Program of China(Grant No.2018YFE0206900)Hubei Provincial Natural Science Foundation of China(Grant No.2019CFA002)。
文摘Among the alloying-type anodes,elemental Sb possesses the suitable yet safe plateau,simple lithiation pathway,small voltage polarization,high conductivity,and superior cycle stability.However,challenge is that its intrinsic capacity is rather low(660 mAh g^(-1)),<1/6 of silicon.Herein,we propose a seamless integration strategy by merging the voltage and capacity of phosphorus and antimony into a solid solution alloy.Interestingly,the enlistment of P is found greatly enlarge the capacity from 660 to 993 mAh g^(-1) for such Sb_(30)P_(30) solid solution,while maintaining a single and stable discharge plateau(~0.79 V)similar to elemental Sb.Various experimental characterizations including XPS,PDF,Raman,and EDS mapping reveal that in such a material the P and Sb atoms have interacted with each other to form a homogenous solid solution alloy,rather than a simple mixing of the two substances.Thus,the Sb_(30)P_(30) exhibits superior rate performances(807 mAh g^(-1) at 5000 mA g^(-1))and cyclability(821 mAh g^(-1) remained after 300 cycles).Furthermore,such Sb_(60-x)P_(x) alloys can even deliver 621 mAh g^(-1) at30℃,which can be served as the alternative anode materials for high-energy and low-temperature batteries.This unique seamless integration strategy based on solid solution chemistry can be easily leveraged to manipulate the capacity of other electrode materials at similar voltage.
基金Guangdong High-level Innovation Institute Project,Grant/Award Number:2021 B0909050001National Natural Science Foundation(NNSF)of China,Grant/Award Number:22309162GRINM Young Scholar Funding Project,National Natural Science Foundation of China,Grant/Award Number:12104024。
文摘Sodium-ion batteries (NIBs) have become an ideal alternative to lithium-ion batteries in the field of electrochemical energy storage due to their abundant raw materials and cost-effectiveness. With the progress of human society, the requirements for energy storage systems in extreme environments, such as deep-sea exploration, aerospace missions, and tunnel operations, have become more stringent. The comprehensive performance of NIBs at low temperatures (LTs) has also become an important consideration. Under LT conditions, challenges such as increased viscosity of electrolyte, abnormal growth of solid electrolyte interface, and poor contact between collector and electrode materials emerge. The aforementioned issues hinder the diffusion kinetics of sodium ions (Na^(+)) at the electrode/electrolyte interface and cause rapid degradation of battery performance. Consequently, the optimization of electrolyte composition and cathode/anode materials becomes an effective approach to improve LT performance. This review discusses the conduction behavior and limiting factors of Na^(+) in both solid electrodes and liquid electrolytes at LT. Furthermore, it systematically reviews the recent research progress of LT NIBs from three aspects: cathode materials, anode materials, and electrolyte components. This review aims to provide a valuable reference for developing high-performance LT NIBs.
基金supported by the National Natural Science Foundation of China(Nos.21806017,21876019)the Fundamental Research Funds for the Central Universities(No.DUT20RC(4)003)National Key Research and Development Program of China(No.2019YFC1903903).
文摘A novel Mo-doped CuO catalyst is developed and used for low-temperature NH_(3)-SCR reaction.Compared with the undoped CuO sample,the Mo doped CuO catalyst shows an increased SCR performance with above 80%NO_(x) conversion at 175℃.The XRD and Raman results have confirmed the incorporation of Mo metal ions into CuO lattice to form Mo-O-Cu species which may be related to the enhanced SCR activity.The XPS and UV-vis results reveal the creation of electron interaction between Cu and Mo in this Mo-O-Cu system which provides an increased amount of Lewis and Brønsted acid sites,thereby promoting the adsorption capacity of NH_(3) and NO_(x) as verified by NH_(3)-TPD and NO_(x)-TPD characterization.Besides,it also promotes the formation of oxygen vacancies,leading to the increasing of chemisorbed oxygen species,which improves the NO oxidation to NO_(2) activity.Furthermore,in situ DRIFTS technology was also used to study the reaction mechanism of this Mo doped CuO catalyst.The formed NO_(2) could react with NHx(x=3,2)species to enhance the low-temperature NH_(3)-SCR activity via the"fast-SCR"reaction pathway.The nitrate and nitrite ad-species may react with NH_(3) and NH4^(+)ad-species through the L-H pathway.
基金financially supported by the National Natural Science Foundation of China(No.51902036)the Natural Science Foundation of Chongqing Science&Technology Commission(No.cstc2019jcyj-msxm1407)+5 种基金the Natural Science Foundation of Chongqing Technology and Business University(No.1952009)the Science and Technology Research Program of Chongqing Municipal Education Commission(Nos.KJQN201900826 and KJQN201800808)the Venture&Innovation Support Program for Chongqing Overseas Returnees(No.CX2018129)the Innovation Group of New Technologies for Industrial Pollution Control of Chongqing Education Commission(No.CXQT19023)the Engineering and Physical Sciences Research Council(EPSRC)(No.EP/S032886/1)the Key Disciplines of Chemical Engineering and Technology in Chongqing Colleges and Universities during the 13th Five Year Plan。
文摘In this work,a multi-core-shell-structured LiFePO_(4)@Na_(3) V_(2)(PO_(4))_(3)@C(LFP@NVP@C) composite was successfully designed and prepared to address inferior low-temperature performance of LiFePO_(4) cathode for lithium-ion batteries.Transmission electron microscopy(TEM) confirms the inner NVP and outer carbon layers coexisted on the surface of LFP particle.When evaluated at low-temperature operation,LFP@NVP@C composite exhibits an evidently enhanced electrochemical performance in term of higher capacity and lower polarization,compared with LFP@C.Even at-10℃ with 0.5 C,LFP@NVP@C delivers a discharge capacity of ca.96.9 mAh-g^(-1) and discharge voltage of ca.3.3 V,which is attributed to the beneficial contribution of NVP coating.NAS ICON-structured NVP with an open framework for readily insertion/desertion of Li+ will effectively reduce the polarization for the electrochemical reactions of the designed LFP@NVP@C composite.
基金Project(2006AA11A151) supported by the National Hi-Tech Research and Development Program of China
文摘Low-temperature performance and high-rate discharge capability of AB5-type non-stoichiometric hydrogen storage are studied. X-ray diffraction(XRD),pressure-composition-temperature(PCT) curves and electrochemical impedance spectroscopy(EIS) are applied to characterize the electrochemical properties of ABx(x=4.8,4.9,5.0,5.1,5.2) alloys. The results show that the non-stoichiometric alloys exhibit better electrochemical properties compared with that of the AB5 alloy.
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)。
文摘This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.1)Mo_(0.05)O_(3-δ)(B S CNM_(0.05)),Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.05)Mo_(0.1)O_(3-δ)(BSCNM_(0.1)),and Ba_(0.6)Sr_(0.4)Co_(0.85)Mo_(0.15)O_(3-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 BSCNM_(0.05)cathode 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 BSCNM_(0.05)cathode achieved a peak power density of 1477 mW·cm^(-2),which was 30.71%,56.30%,and 171.50%higher than those of BSCN,BSCNM_(0.1),and B SCM,respectively.The improved ORR activity and electrochemical performance of BSCNM_(0.05)indicate that it can be used as a cathode material in low-temperature solid oxide fuel cells.
基金supported by the Natural Science Foundation of Xiamen, China (3502Z202372036)the National Natural Science Foundation of China (52372191, 52073286 (to CZ Lu), 22275185 (to CZ Lu))+4 种基金the Scientific Research Funds of Huaqiao University (20221XD027, 20221XD045)the Xiamen Institute of Rare Earth Materials Haixi Institutes (XMIREM)the Autonomously Deployment Project (2023GG01 (to CZ Lu))the Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China (2021ZZ115 (to CZ Lu))the China Postdoctoral Science Foundation (2022TQ0282)。
文摘Achieving an in-depth understanding of the nexus between temperature and phase transitions is paramount for advancing the electrochemical efficiency of aqueous zinc ion batteries.Yet,the intricacies of electrochemical interactions,particularly those associated with the structural evolution over extended periods,remain enigmatic.In this research,we leverage V_(2)O_(5) as an initial structural model of crystals to demystify the kinetics of electrode reactions and the decay mechanism of global electrochemical degradation by meticulously controlling the crystal defects via applying different mechanical grounding intensities.It is noted that the grounding V_(2)O_(5)(GVO)can exhibit a stable crystal structure that suppresses the dissolution/shuttling of vanadium and mitigates Zn anodes by-products caused by electrochemical processes.Thus,the GVO is utilized as the cathode material,achieving excellent Zn storage capacity at both room temperature and low temperatures,e.g.,380 and 246 mA h g^(−1) at room temperature and−20℃,respectively.Remarkably,the GVO cathode retains a specific capacity of 160 mA h g^(−1) with a capacity retention rate of 99%after 1500 cycles at−20℃ and 1 A g^(−1).This work provides a novel insight into the electrochemical crosstalk behavior of aqueous zinc-ion batteries(AZIBs)in a wide range of temperatures.
文摘Because of their excellent low-temperature(−15 to−40℃)tolerance,sodium-ion batteries are emerging as a complement to lithium-ion batteries for use in extremely cold environments(e.g.high-latitude areas).Hard carbon has a high low-voltage sodium storage capacity and a good initial efficiency,making it one of the most promising anode materials for sodium-ion batteries.It has a complex structure,featuring closed pores,nano graphitic domains,and surface functional groups.The sodium storage sites in hard carbon are reviewed as are the widely accepted sodium storage mechanisms.The main factors contributing to the degradation of the good low-temperature performance in hard carbon anodes are considered,including sodium dendrite formation,low ion diffusion rates,and surface-side reactions.Finally,strategies to increase the low-temperature sodium storage performance of hard carbon anodes are summarized,including bulk structure design,and improvements in interfaces and cut-off voltage.Guidance is provided for improving the low-temperature performance of hard carbon anodes to accelerate the development of these batteries.
基金supported by the Natural Science Foundation of Guizhou Province(No.ZK 2022-044)the Platform of Science and Technology and Talent Team Plan of Guizhou Province(No.GCC[2023]007)+1 种基金the National Science Foundation of China(Nos.52101010 and 11964006)the Fund of Natural Science Special(Special Post)Research Foundation of Guizhou University(No.2021-018).
文摘The design and development of high-performance anodes pose significant challenges in the construction of next-generation rechargeable lithium-ion batteries(LIBs).Sodium molybdate dihydrate(Na_(2)MoO_(4)·2H_(2)O)has garnered increasing attention due to its cost-effectiveness,non-toxicity and earth abundance.To enhance the Li storage performance of Na_(2)MoO_(4)·2H_(2)O,a crystallographic orientation regulation strategy is proposed in this work.Initially,density functional theory calculations are carried out to demonstrate that the(020)crystal plane of Na_(2)MoO_(4)·2H_(2)O offers the lowest energy barrier for Li^(+)migration.Subsequently,the preferred crystallographic orientation of Na_(2)MoO_(4)·2H_(2)O crystal is tuned through a low-temperature recrystallization method.Furthermore,the microstructure and phase changes of Na_(2)MoO_(4)·2H_(2)O during the lithiation/de-lithiation process are studied using in situ and ex situ XRD tests,ex situ XPS and cyclic voltammetry to unravel its Li^(+)storage mechanism.Upon application as LIBs anode,the Na_(2)MoO_(4)·2H_(2)O single-crystal particles with a preferred(020)surface exhibit superior reversible capacity,high-capacity retention and high cycling stability.The enhanced Li storage performance should be attributed to the regulated crystallographic orientation and small changes in the crystal microstructure during the charge/discharge process,which facilitates Li^(+)migration and bolsters structural stability.Notably,this study introduces a novel concept and a simple synthesis method for the advancement of electrodes in rechargeable batteries.
文摘The distributions of framework aluminum(Al)in zeolites critically govern the location and speciation of active copper(Cu)centers,thereby influencing their performance in ammonia selective catalytic reduction(NH_(3)-SCR)of nitrogen oxides(NO_(x)).Conventional Cu-SSZ-39(Cu-SSZ-39-T)exhibits excellent hydrothermal stability but limited low-temperature activity(150–225℃)due to a low concentration of Al in 8-membered rings(8MRs)that inhibits the formation of active[Cu(OH)]^(+)-Z species.Herein,an SSZ-39 zeolite synthesized with potassium ions(SSZ-39-K)achieved a significantly higher 8MR Al fraction(37.6%).Density functional theory calculations and H_(2)-temperature-programmed reduction analyses confirmed that the increased 8MR Al population facilitated the formation of[Cu(OH)]^(+)-Z species.Aged Cu-SSZ-39-K exhibited nearly twice the NO_(x)conversion of aged Cu-SSZ-39-T in the 150–225℃range while maintaining comparable high-temperature activity(250–550℃)under a gas hourly space velocity of 250,000 h^(-1).Enhanced low-temperature performance is particularly beneficial for mitigating NO_(x)emissions during cold-start phase.Moreover,SSZ-39-K was synthesized with a high crystallization yield(~65%),nearly double the highest yield(33%)reported for direct synthesis routes.This work establishes a robust strategy for tailoring Al distributions in SSZ-39 zeolites,offering an effective pathway to improve low-temperature NH_(3)-SCR performance and promote practical implementation.
基金supported by the National Natural Science Foundation of China(No.51706105)。
文摘Al/NH_(4)CoF_(3)-Φ(Φ=0.5,1.0,1.5,2.0,and 3.0)binary composites and Al-NH_(4)CoF_(3)@P(VDF-HFP)ternary composites are fabricated via ultrasonication-assisted blending and electrostatic spraying.The effect of equivalence ratio(Φ)on the reaction properties is systematically investigated in the binary Al/NH_(4)CoF_(3)system.For ternary systems,electrostatic spraying allows both components to be efficiently encapsulated by P(VDF-HFP)and to achieve structural stabilization and enhanced reactivity through synergistic interfacial interactions.Morphological analysis using SEM/TEM revealed that P(VDF-HFP)formed a protective layer on Al and NH_(4)CoF_(3)particles,improving dispersion,hydrophobicity(water contact angle increased by 80.5%compared to physically mixed composites),and corrosion resistance.Thermal decomposition of NH_(4)CoF_(3)occurred at 265℃,releasing NH_(3)and HF,which triggered exothermic reactions with Al.The ternary composites exhibited a narrowed main reaction temperature range and concentrated heat release,attributed to improved interfacial contact and polymer decomposition.Combustion tests demonstrated that Al-NH_(4)CoF_(3)@P(VDF-HFP)achieved self-sustaining combustion.In addition,a simple validation was done by replacing the Al component in the aluminium-containing propellant,demonstrating its potential application in the propellant field.This work establishes a novel strategy for designing stable,high-energy composites with potential applications in advanced propulsion systems.
基金Supported by the National Key Research and Development Program of China (2023YFB4102903)。
文摘This study systematically conducted preparation optimization and performance investigations on Co-modified Ce/TiO_(2) catalysts,with a focus on examining how preparation methods and Co loading regulate the catalyst’s low-temperature denitrification activity.After identifying optimal preparation parameters via condition screening,multiple characterization techniques-including BET,XRD,XPS,H_(2)-TPR and in situ DRIFTS-were employed to deeply analyze the catalyst’s physicochemical properties and reaction mechanism.Results demonstrated that compared to the impregnation and co-precipitation methods,the Ce-Co_(0.025)/TiO_(2)-SG catalyst(prepared by the sol-gel method with a Co/Ti mass ratio of 0.025)exhibited significantly superior denitrification activity:NO conversion remained stably above 95%in the 225−350℃ temperature range,and it displayed high N_(2) selectivity.Characterization analysis revealed that abundant surface oxygen vacancies,a high proportion of Ce^(3+) species,and prominent acidic sites collectively contributed to enhancing its low-temperature denitrification performance.This work provides reference value for the development of highly efficient low-temperature denitrification catalysts.
基金Supported by National Key Research and Development Program of China(2020YFD1100302)。
文摘Under the context of global energy transition and carbon neutrality,controlling nitrogen oxide(NO_(x))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 Mn_(7)-Cu_(3)/BCN catalyst to construct the Mn_(7)-Cu_(3)-Nb_(x)/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Supported by Basic Scientific Research Project of the Liaoning Provincial Department of Education Has Been Unveiled to Facilitate Local Project Funding (JYTMS20230835)Enhanced Scientific Research Project Funded by the Departmentof Higher Education in Liaoning Province (General program)(JYTMS20230852)。
文摘The adsorptive denitrification performance of MIL-101(Cr)-0.5 toward pyridine,aniline or quinoline in simulated fuels with basic nitrogen content of 1732μg/g was evaluated separately.Furthermore,the effects of adsorption temperature,adsorption time and adsorbent dosage on their adsorptive denitrification performance were systematically investigated.The experimental results demonstrated that under a fixed adsorbent dosage of 0.05 g and a simulated fuel volume of 10 mL,the optimal removal efficiency for aniline was achieved at 30℃ within 30 min,whereas higher temperatures and longer times(40℃and 40 min)were required for effective removal of pyridine and quinoline.Density Functional Theory(DFT)calculations were conducted via Materials Studio(MS)software to study the adsorptive denitrification mechanism of MIL-101(Cr)toward these three basic nitrogen-containing compounds.The simulation calculation results revealed that the interaction between pyridine and MIL-101(Cr)primarily involved coordination adsorption.In contrast,the interaction between aniline or quinoline and MIL-101(Cr)proceeded mainly through coordination,with additional contributions fromπ-complexation and hydrogen bonding.The overall adsorption strength order is pyridine>aniline>quinoline.During the adsorption process,pyridine and quinoline transfer electrons to the MIL-101(Cr)surface through the H→C→N→Cr^(3+)pathway,while aniline transfers electrons to the MIL-101(Cr)surface through various pathways,including N→Cr^(3+),N→C→Cr^(3+)and N→H→O.Furthermore,adsorption kinetics studies indicated that the adsorption processes for all three basic nitrogen-containing compounds followed the quasi second order kinetic models.The experimental results on the effect of benzene on the adsorptive denitrification performance of MIL-101(Cr)-0.5 demonstrated that benzene exerted a more significant impact on the adsorption of aniline and quinoline.Finally,the adsorbent was regenerated using ethanol washing.It was found that MIL-101(Cr)-0.5 retained stable denitrification performance after two regeneration cycles.
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)。
文摘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Supported by the Science and Technology Cooperation and Exchange special project of Cooperation of Shanxi Province(202404041101014)the Fundamental Research Program of Shanxi Province(202403021212333)+3 种基金the Joint Funds of the National Natural Science Foundation of China(U24A20555)the Lvliang Key R&D of University-Local Cooperation(2023XDHZ10)the Initiation Fund for Doctoral Research of Taiyuan University of Science and Technology(20242026)the Outstanding Doctor Funding Award of Shanxi Province(20242080).
文摘To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content in coal)catalysts were prepared by the incipient wetness impregnation method,followed by acid washing to remove calcium-containing minerals.Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity.Specifically,NO conversion increased from 88.3%of Mn-Ce/De-AC to 91.7%of Mn-Ce/De-AC-1CaCO_(3)(210℃).The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn^(4+)content and Ce^(4+)/Ce^(3+)ratio,an abundance of chemisorbed oxygen and acidic sites,which could strengthen the SCR reaction pathways(richer NH_(3)activated species and bidentate nitrate active species).Therefore,NO removal is enhanced.
基金National Key R&D Program of China under Grant No.2024YFD1600404。
文摘Severe failures of nonstructural components have occurred during previous earthquakes.Claddings are one of the most widely used nonstructural component and are installed in many modern buildings;therefore,an evaluation of their seismic performance is important and cannot be ignored.To investigate the seismic performance of large-sized high performance concrete cladding(HPCC),a series of full-scale experimental tests were conducted using a unidirectional shaking table.A steel supporting frame was used to install the HPCCs and reproduce the effects of the building under earthquake.The tests were divided into two parts:in-plane(IP)testing and out-plane(OP)testing.Three recorded accelerograms,one artificial accelerogram,and one sinusoidal accelerogram were used to conduct the shaking table tests.The results show that the maximum recorded IP responses of acceleration and interstory drift ratio were 1.04 g and 1/97,while the OP responses were 1.02 g and 1/51.The HPCCs functioned well throughout the entire experimental protocol.The fundamental frequency of the HPCCs systems rarely changed after the tests.
文摘Purpose:ATLAS is a cross-sectional study aiming to investigate environmental and genetic determinants of athletic performance in healthy Greek competitive athletes(CA).This article presents the study design,investigates the muscle strength performance(MSP)of 289 adult and teenage CA,exercisers,and physically inactive individuals(PI),and proposes predictive models of MSP for adults.Methods:Muscle maximal,speed,and explosive strength(MMS/MSS/MES)at unilateral maximal concentric flexion and extension contraction(FC/EC)were evaluated using Biodex System 3 PRO^(TM)at 60°/s,180°/s,and 300°/s,while additional performance markers were assessed through field ergometric testing.Participants were interviewed about their lifestyle,dietary habits,physical activity,injury,and medical history.Body composition was assessed via bioelectrical impedance.gDNA was extracted from biochemical samples and then genotyped.Statistical analysis was conducted using IBM SPSS Statistics v21.0 and R.Results:Age,fitness,and sex impacted correlations of MSP with body composition and anthropometric measurements(p<0.05).Among CA,females outperformed males in accuracy(p<0.001)while,males outperformed females in anaerobic power,MSP,speed,and endurance(p<0.001).Adult CA outperformed exercisers and PI in MMS,MSS,and MES(p<0.05).Multiple linear regression models,with predictors age,FFM,body extremity,training load explained the majority of variation in MMS(R^(2)_(adj):71.4%–88.9%),MSS(R^(2)_(adj):64.8%–78.4%),and MES(R^(2)_(adj):52.7%–68.4%)at EC,FC,and their mean(p<0.001).Conclusions:Muscle-strengthening strategies should be customized according to individual fitness levels,body composition,and anthropometric measurements.The innovative sex-specific regression models assessing MMS,MSS,and MES at EC and FC provide a framework for personalizing rehabilitation and skill-specific training strategies.
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).
文摘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 N_(2)/CO_(2) 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.
