Solid oxide cells(SOCs)are emerging devices for efficient energy storage and conversion.However,during SOC operation,gaseous chromium(Cr)species released from Fe-Cr alloy interconnect can lead to Cr deposition and poi...Solid oxide cells(SOCs)are emerging devices for efficient energy storage and conversion.However,during SOC operation,gaseous chromium(Cr)species released from Fe-Cr alloy interconnect can lead to Cr deposition and poisoning of air electrodes,causing substantial degradation in electrochemical performance and compromising the longterm stability of SOCs.This mini-review examines the mechanism of Cr deposition and poisoning in air electrodes under both fuel-cell and electrolysis modes.Furthermore,emphasis is placed on the recent advancements in strategies to mitigate Cr poisoning,offering insights into the rational design and development of active and Cr-tolerant air electrodes for SOCs.展开更多
The semiconductor photocatalysis are considered as one of the most promising candidates in hydrogen energy source and environmental remediation area.In this paper,flower-shaped SnS,is successfully combined on g-C,Ns,a...The semiconductor photocatalysis are considered as one of the most promising candidates in hydrogen energy source and environmental remediation area.In this paper,flower-shaped SnS,is successfully combined on g-C,Ns,and the well matching band structure successfully constitutes a new Type-II heterojunction.As expected,the photocatalytic hydrogen production experiment showed that the quantity of hydrogen produced on 5% SnS_(2)/C_(3)N_(5)was 922.5μmol/(g.h),which is 3.6 times higher than that of pure g-C_(3)N_(5).Meanwhile,in photocatalytic degradation of methylene blue,5%SnS2/C,Ns composite material can degrade 95% of contaminants within 40 min,showing good photocatalytic degradation performance.The mechanism study indicates that SnS_(2)/C_(3)N_(5)heterojunction improves the photogenerated charge migration rate and reduces the electron-hole recombination rate,and effectively improves the photocatalytic performance of g-C_(3)N_(5).This work provides a new idea for designing C,Ns-based heterojunctions with efficient hydrogen production and degradation performance.展开更多
Liposomes serve as critical carriers for drugs and vaccines,with their biological effects influenced by their size.The microfluidic method,renowned for its precise control,reproducibility,and scalability,has been wide...Liposomes serve as critical carriers for drugs and vaccines,with their biological effects influenced by their size.The microfluidic method,renowned for its precise control,reproducibility,and scalability,has been widely employed for liposome preparation.Although some studies have explored factors affecting liposomal size in microfluidic processes,most focus on small-sized liposomes,predominantly through experimental data analysis.However,the production of larger liposomes,which are equally significant,remains underexplored.In this work,we thoroughly investigate multiple variables influencing liposome size during microfluidic preparation and develop a machine learning(ML)model capable of accurately predicting liposomal size.Experimental validation was conducted using a staggered herringbone micromixer(SHM)chip.Our findings reveal that most investigated variables significantly influence liposomal size,often interrelating in complex ways.We evaluated the predictive performance of several widely-used ML algorithms,including ensemble methods,through cross-validation(CV)for both lipo-some size and polydispersity index(PDI).A standalone dataset was experimentally validated to assess the accuracy of the ML predictions,with results indicating that ensemble algorithms provided the most reliable predictions.Specifically,gradient boosting was selected for size prediction,while random forest was employed for PDI prediction.We successfully produced uniform large(600 nm)and small(100 nm)liposomes using the optimised experimental conditions derived from the ML models.In conclusion,this study presents a robust methodology that enables precise control over liposome size distribution,of-fering valuable insights for medicinal research applications.展开更多
The morphology and dimension of W phases play an important role in determining mechanical properties of Mg-RE-Zn(where RE denotes rare earth elements)alloys.In this study,theγ′platelet and W particle occurred in the...The morphology and dimension of W phases play an important role in determining mechanical properties of Mg-RE-Zn(where RE denotes rare earth elements)alloys.In this study,theγ′platelet and W particle occurred in the aged Mg-2Dy-0.5Zn(at.%)alloys were investigated by aberration-corrected scanning transmission electron microscopy.A novel formation mechanism of W phase was proposed,and its effects on the morphology and dimension of W particle,as well as mechanical properties of Mg-2Dy-0.5Zn alloys,were also discussed particularly.Different from other Mg-RE-Zn alloys,the nucleation and growth of W particle in Mg-Dy-Zn alloys mainly depend on the precipitatedγ′platelet.Primarily,a mass of Dy and Zn solute atoms concentrated nearγ′platelet or between two adjacentγ′platelets can meet the composition requirement of W particle nucleation.Next,the smaller interfacial mismatch between W andγ′facilitates the nucleation and growth of W particle.Thirdly,the growth of W particle can be achieved by consuming the surroundingγ′platelets.The nucleation and growth mechanisms make W particles exhibit rectangular or leaf-like and remain at the nanoscale.The coexistence ofγ′platelets and nanoscale W particles,and some better interfacial relationships between phases,lead to a high strength-ductility synergy of alloy.The findings may provide some fundamental guidelines for the microstructure design and optimization of new-type Mg-based alloys.展开更多
With the rapid development of electric vehicles,hybrid electric vehicles and smart grids,people's demand for large-scale energy storage devices is increasingly intense.As a new type of secondary battery,potassium ...With the rapid development of electric vehicles,hybrid electric vehicles and smart grids,people's demand for large-scale energy storage devices is increasingly intense.As a new type of secondary battery,potassium ion battery is promising to replace the lithium-ion battery in the field of large-scale energy storage by virtue of its low price and environmental friendliness.At present,the research on the anode materials of potassium ion batteries mainly focuses on carbon materials and the design of various nanostructured metal-based materials.Problems such as poor rate performance and inferior cycle life caused by electrode structure comminution during charge and discharge have not been solved.Quantum dots/nanodots materials are a new type of nanomaterials that can effectively improve the utilization of electrode materials and reduce production costs.In addition,quantum dots/nanodots materials can enhance the electrode reaction kinetics,reduce the stress generated in cycling,and effectively alleviate the agglomeration and crushing of electrode materials.In this review,we will systematically introduce the synthesis methods,K+storage properties and K+storage mechanisms of carbon quantum dots and carbon-based transition metal compound quantum dots composites.This review will have significant references for potassium ion battery researchers.展开更多
Fifty agricultural soil samples collected from Fuzhou,southeast China,were first investigated for the occurrence,distribution,and potential risks of twelve organophosphate esters(OPEs).The total concentration of OPEs(...Fifty agricultural soil samples collected from Fuzhou,southeast China,were first investigated for the occurrence,distribution,and potential risks of twelve organophosphate esters(OPEs).The total concentration of OPEs(ΣOPEs)in soil ranged from 1.33 to 96.5 ng/g dry weight(dw),with an average value of 17.1 ng/g dw.Especially,halogenated-OPEs were the predominant group with amean level of 9.75 ng/g dw,and tris(1-chloro-2-propyl)phosphate(TCIPP)was the most abundant OPEs,accounting for 51.1%ofΣOPEs.The concentrations of TCIPP andΣOPEs were found to be significantly higher(P<0.05)in soils of urban areas than those in suburban areas.In addition,the use of agricultural plastic films and total organic carbon had a positive effect on the occurrence of OPE in this study.The positive matrix factorization model suggested complex sources of OPEs in agricultural soils from Fuzhou.The ecological risk assessment demonstrated that tricresyl phosphate presented a medium risk to land-based organisms(0.1≤risk quotient<1.0).Nevertheless,the carcinogenic and noncarcinogenic risks for human exposure to OPEs through soil ingestion and dermal absorption were negligible.These findings would facilitate further investigations into the pollution management and risk control of OPEs.展开更多
Impact of texture type on the magnetic properties of ultrahigh density perpendicular magnetic recording media L1_(0)-FePt thin film was investigated,so were the texture formation and evolution mechanism.Reuss,Voigt,an...Impact of texture type on the magnetic properties of ultrahigh density perpendicular magnetic recording media L1_(0)-FePt thin film was investigated,so were the texture formation and evolution mechanism.Reuss,Voigt,and Hill models were used to determine the anisotropic elastic modulus of L1_(0)-FePt thin film with fiber texture.Then,the elastic strain energies of thin films under various stress conditions were calculated.Results reveal that the stress condition has a significant influence on the fiber texture evolution.When the L1_(0)-FePt thin film is subjected to compressive in-plane strain prior to ordering phase transformation,the formation of{100}fiber texture is promoted.On the contrary,the ordering phase transformation under tensile in-plane strain promotes the{001}fiber texture formation.展开更多
Current research primarily focuses on emerging organic pollutants,with limited attention to emerging inorganic pollutants (EIPs).However,due to advances in detection technology and the escalating environmental and hea...Current research primarily focuses on emerging organic pollutants,with limited attention to emerging inorganic pollutants (EIPs).However,due to advances in detection technology and the escalating environmental and health challenges posed by pollution,there is a growing interest in treating waters contaminated with EIPs.This paper explores biochar characteristics and modification methods,encompassing physical,chemical,and biological approaches for adsorbing EIPs.It offers a comprehensive review of research advancements in employing biochar for EIPs remediation in water,outlines the adsorption mechanisms of EIPs by biochar,and presents an environmental and economic analysis.It can be concluded that using biochar for the adsorption of EIPs in wastewater exhibits promising potential.Nonetheless,it is noteworthy that certain EIPs like Au(III),Rh(III),Ir(III),Ru(III),Os(III),Sc(III),and Y(III),have not been extensively investigated regarding their adsorption onto biochar.This comprehensive review will catalyze further inquiry into the biochar-based adsorption of EIPs,addressing current research deficiencies and advancing the practical implementation of biochar as a potent substrate for EIP removal from wastewater streams.展开更多
In this study,we present the fabrication of vertical SnO/β-Ga_(2)O_(3) heterojunction diode(HJD)via radio frequency(RF)reactive magnetron sputtering.The valence and conduction band offsets betweenβ-Ga_(2)O_(3) and S...In this study,we present the fabrication of vertical SnO/β-Ga_(2)O_(3) heterojunction diode(HJD)via radio frequency(RF)reactive magnetron sputtering.The valence and conduction band offsets betweenβ-Ga_(2)O_(3) and SnO are determined to be 2.65and 0.75 eV,respectively,through X-ray photoelectron spectroscopy,showing a type-Ⅱband alignment.Compared to its Schottky barrier diode(SBD)counterpart,the HJD presents a comparable specific ON-resistances(R_(on,sp))of 2.8 mΩ·cm^(2) and lower reverse leakage current(I_R),leading to an enhanced reverse blocking characteristics with breakdown voltage(BV)of 1675 V and power figure of merit(PFOM)of 1.0 GW/cm~2.This demonstrates the high quality of the SnO/β-Ga_(2)O_(3) heterojunction interface.Silvaco TCAD simulation further reveals that electric field crowding at the edge of anode for the SBD was greatly depressed by the introduction of SnO film,revealing the potential application of SnO/β-Ga_(2)O_(3) heterojunction in the futureβ-Ga_(2)O_(3)-based power devices.data mining,AI training,and similar technologies,are reserved.展开更多
To modify the stable thermodynamics and poor kinetics of magnesium hydride(MgH_(2))for solid-state hydrogen storage,MIL-100(Fe)was in situ fabricated on the surfaces of TiO_(2)nano-sheets(NS)by a self-assembly method,...To modify the stable thermodynamics and poor kinetics of magnesium hydride(MgH_(2))for solid-state hydrogen storage,MIL-100(Fe)was in situ fabricated on the surfaces of TiO_(2)nano-sheets(NS)by a self-assembly method,and the prepared TiO_(2)NS@MIL-100(Fe)presents an excellent catalytic effect on MgH_(2).The MgH_(2)+7wt.%TiO_(2)NS@MIL-100(Fe)composite can release hydrogen at 200℃,achieving a decrease of 150℃ compared to pure MgH_(2).Besides,the activation energy of dehydrogenation is decreased to 70.62 kJ/mol and 4 wt.%H_(2) can be desorbed within 20 min at a low temperature of 235℃.Under conditions of 100℃ and 3 MPa,MgH_(2)+7wt.%TiO_(2)NS@MIL-100(Fe)absorbs 5 wt.%of H_(2) in 10 min.Surprisingly,6.62 wt.%reversible capacity is maintained after 50 cycles.The modification mechanism is confirmed that the presence of oxygen vacancies and the synergistic effect of multivalent titanium in TiO_(2)NS@MIL-100(Fe)greatly enhance the kinetic and thermodynamic properties of MgH_(2).展开更多
Dendritic spines are small protrusions along dendrites that contain most of the excitatory synapses in principal neurons,playing a crucial role in neuronal function by creating a compartmentalized environment for sign...Dendritic spines are small protrusions along dendrites that contain most of the excitatory synapses in principal neurons,playing a crucial role in neuronal function by creating a compartmentalized environment for signal transduction.The plasticity of spine morphologies provides a tunable handle to regulate calcium signal dynamics,allowing rapid regulation of protein expression necessary to establish and maintain synapses(Cornejo et al.,2022).If excitatory inputs were to be located primarily on dendritic shafts,dendrites would frequently short-circuit,preventing voltage signals from propagating(Cornejo et al.,2022).It is thus not surprising that the structural plasticity of dendritic spines is closely linked to synaptic plasticity and memory formation(Berry and Nedivi,2017).While comprehensive in vitro studies have been conducted,in vivo studies that directly tackle the mechanism of dendritic transport and translation in regulating spine plasticity spatiotemporally are limited.展开更多
Photosynthesis of hydrogen peroxide(H_(2)O_(2))from H_(2)O and O_(2)is considered to be a promising approach.However,limited to the rapid recombination of photo-generated carriers and sluggish kinetics of O_(2)re-duct...Photosynthesis of hydrogen peroxide(H_(2)O_(2))from H_(2)O and O_(2)is considered to be a promising approach.However,limited to the rapid recombination of photo-generated carriers and sluggish kinetics of O_(2)re-duction to H_(2)O_(2),it is a challenge for polymeric photocatalysts to achieve efficient photocatalytic H_(2)O_(2) production.Herein,Ag single atoms and nitrogen defects decorated carbon nitride(Ag@MCT)are con-structed through self-assembly and pyrolysis methods.The optimized photocatalyst displays exceptional performance in pure water,with an H_(2)O_(2) production rate of as high as 528.4μmol g^(-1) h^(-1) and an apparent quantum yield for H_(2)O_(2)production of 4.5%at 420 nm.Experimental and theoretical results reveal that the Ag atomic sites act as electron mediators that promote the capture and transfer of photo-generated charge carriers,while nitrogen defects as electron collectors and reaction sites to enhance the adsorption and activation of O_(2),accelerating reduction kinetics from O_(2) to H_(2)O_(2).This work presents a re-liable strategy to design excellent photocatalysts by rationally modulating electronic structures and active sites for accelerating photo-generated charge carriers transfer and surface reaction kinetics.展开更多
Hydrogen,as a cheap,clean,and cost-effective secondary energy source,performs an essential role in optimizing today’s energy structure.Magnesium hydride(Mg H_(2))represents an attractive hydrogen carrier for storage ...Hydrogen,as a cheap,clean,and cost-effective secondary energy source,performs an essential role in optimizing today’s energy structure.Magnesium hydride(Mg H_(2))represents an attractive hydrogen carrier for storage and transportation,however,the kinetic behavior and operating temperature remain undesirable.In this work,a dual-phase multi-site alloy(Ms A)anchored on carbon substrates was designed,and its superior catalytic effects on the hydrogen storage properties of MgH_(2) were reported.Mechanism analysis identified that multi-site Fe Ni_(3)/Ni Cu nanoalloys synergistically served as intrinsic drivers for the striking de/hydrogenation performance of the MgH_(2)-Ms A systems.Concretely,the unique multi-metallic site structure attached to the surface of MgH_(2)provided substantial reversible channels and accessible active sites conducive to the adsorption,activation,and nucleation of H atoms.In addition,the coupling system formed by FeNi_(3) and NiCu dual-phase alloys further enhanced the reactivity between Mg/MgH_(2) and H atoms.Hence,the onset dehydrogenation temperature of Mg H_(2)+5 wt%Ms A was reduced to 195℃ and the hydrogen desorption apparent activation energy was reduced to 83.6 k J/mol.5.08 wt%H_(2) could be released at 250℃ in 20 min,reaching a high dehydrogenation rate of 0.254 wt%H_(2)/min,yet that for MgH_(2) at a higher temperature of 335℃ was only 0.145 wt%H_(2)/min.Then,the dehydrogenated Mg H_(2)-Ms A sample could absorb hydrogen from room temperature(30℃)and charge 3.93 wt%H_(2) at 100℃ within20 min under 3.0 MPa H_(2) pressure.Benefiting from carbon substrates,the 5 wt%Ms A doped-MgH_(2) could still maintain 6.36 wt%hydrogen capacity after 20 cycles.In conclusion,this work provides experimental rationale and new insights for the design of efficient catalysts for magnesium-based solid-state hydrogen storage materials.展开更多
In-situ enhanced bioreduction by functional materials is a cost-effective technology to remove chlorinated hydrocarbons in groundwater.Herein,a novel polydopamine(PDA)-modified biochar(BC)-based composite containing n...In-situ enhanced bioreduction by functional materials is a cost-effective technology to remove chlorinated hydrocarbons in groundwater.Herein,a novel polydopamine(PDA)-modified biochar(BC)-based composite containing nanoscale zero-valent iron(n ZVI)and poly-l-lactic acid(PLLA)(PB-PDA-Fe)was synthesized to enhance the removal of 1,1,1-trichloroethane(1,1,1-TCA)in simulated groundwater with actual site sediments.Its impact on functional microbial community structure in system was also investigated.The typical characterizations revealed uniform dispersion of PLA and n ZVI particles on the BC surface,being smoother after PDA coating.The composite exhibited a significantly higher performance on 1,1,1-TCA removal(82.38%,initial concentration 100 mg/L)than Fe-PDA and PB-PDA treatments.The diversity and richness of the microbial community in the composite treatment consistently decreased during incubation due to a synergistic effect between PLLA-BC and n ZVI.Desulfitobaterium,Pedobacter,Sphaerochaeta,Shewanella,and Clostridium were identified as enriched genera by the composite through DNA-stable isotope probing(DNA-SIP),playing a crucial role in the bioreductive dechlorination process.All the above results demonstrate that this novel composite selectively enhances the activity of microorganisms with extracellular respiration functions to efficiently dechlorinate 1,1,1-TCA.These findings could contribute to understanding the responsive microbial community by carbon-iron composites and expedite the application of in-situ enhanced bioreduction for effective remediation of chlorinated hydrocarbon-contaminated groundwater.展开更多
Research on supercontinuum sources on silicon has made significant progress in the past few decades.However,conventional approaches to broaden the spectral bandwidth often rely on complex and critical dispersion engin...Research on supercontinuum sources on silicon has made significant progress in the past few decades.However,conventional approaches to broaden the spectral bandwidth often rely on complex and critical dispersion engineering by optimizing the core thickness or introducing the cladding with special materials and structures.We propose and demonstrate supercontinuum generation using long-periodgrating(LPG)waveguides on silicon with a C-band pump.The LPG waveguide is introduced for quasi-phase matching,and the generated supercontinuum spectrum is improved greatly with grating-induced dispersive waves.In addition,the demonstrated LPG waveguide shows a low propagation loss comparable with regular silicon photonic waveguides without gratings.In experiments,when using a 1550-nm 75-fs pulse pump with a pulse energy of 200 pJ,the supercontinuum spectrum generated with the present LPG waveguide shows an ultrabroad extent from 1150 to 2300 nm,which is much wider by 200 nm than that achieved by dispersionengineered uniform silicon photonic waveguides on the same chip.This provides a promising option for on-chip broadband light source for silicon photonic systems.展开更多
Presetting tensile twins(TTs)can enhance the mechanical properties of magnesium(Mg)alloys.Two as-received(AR)sheets,as-received state-A(AR-A)with fiber texture and nonuniform grains and as-received state-B with basal ...Presetting tensile twins(TTs)can enhance the mechanical properties of magnesium(Mg)alloys.Two as-received(AR)sheets,as-received state-A(AR-A)with fiber texture and nonuniform grains and as-received state-B with basal texture and uniform equiaxial grains are selected to induce TTs via a novel method called corrugated wide limit alignment(CWLA),and the corresponding CWLA-processed sheets are denoted as CWLA-processed state-A(C-A)and CWLA-processed state-B(C-B).The results demonstrate that a larger initial average grain size correlates with a higher fraction of TTs induced in Mg sheets,thereby refining the grains and forming a new rolling direction(RD)tilted texture during CWLA.The ultimate tensile strength increases by 32%from AR-A to C-A,primarily due to refinement strengthening and twinning-induced strain hardening.The recrystallization mechanism of C-A is dominated by twinning-induced dynamic recrystallization(DRX),where DRX grains prefer to inherit the orientation of TTs,resulting in an enhanced RD-tilted texture and the formation of multi-modal texture.The recrystallization mechanism of C-B is mainly discontinuous DRX and continuous DRX,and the DRX grains prefer to inherit the orientation of matrix grains,ultimately forming a basal texture.In summary,the tensile mechanical behavior of pre-twinned Mg sheets significantly depends on the grain size and texture of the AR sheets,so they present similar changing trends during tensile deformation.展开更多
Methanol-assisted water electrolysis presents a promising yet challenging technique for electrochemical hydrogen production,as limited by the easy poisoning issue of Pt active sites.In this study,we successfully synth...Methanol-assisted water electrolysis presents a promising yet challenging technique for electrochemical hydrogen production,as limited by the easy poisoning issue of Pt active sites.In this study,we successfully synthesized an efficient bifunctional catalyst composed of three-dimensional(3D)flower-like MoTe_(2) embedded nitrogen-doped carbon(NC)nanospheres,assembled by nanosheets,to support Pt nanoparticles(Pt-MoTe_(2)/NC)for methanol-assisted water electrolysis.This innovative Pt-MoTe_(2)/NC catalyst demonstrated superior catalytic performance targeting both hydrogen evolution reaction(HER)and methanol oxidation reaction(MOR)due to the strong metal-support interaction and the promotional effect of oxophilic molybdenum telluride.In situ infrared spectroscopy and CO stripping measurements revealed their excellent anti-poisoning ability.In particular,the onset potential of CO oxidation decreased by 130 mV relative to the standard Pt/C electrode.Theoretical calculations indicated the proper H*adsorption energy for HER and weakened CO adsorption energy for MOR in the optimized electronic structure.Therefore,the Pt-MoTe_(2)/NC electrode achieved the highest forward peak current density(76.6 mA·cm^(−2))for MOR,approximately 2.8-fold that of the commercial Pt/C,and only 34 mV was needed to deliver 10 mA·cm^(−2) for HER in acidic electrolyte.When employed as the bifunctional electrode in methanol electrolysis,Pt-MoTe_(2)/NC enabled efficient hydrogen generation with good stability,requiring merely 0.65 V to achieve 10 mA·cm^(−2),approximately 1090 mV less than traditional water electrolysis.This work presents an anti-poisoning catalyst in energy-saving hydrogen production from methanol electrolysis.展开更多
Catalytic doping of magnesium hydride(MgH_(2))to improve its hydrogen ab/desorption kinetic properties is considered to be an effective and feasible method.In solid-phase catalysis,the extent of contact between the ca...Catalytic doping of magnesium hydride(MgH_(2))to improve its hydrogen ab/desorption kinetic properties is considered to be an effective and feasible method.In solid-phase catalysis,the extent of contact between the catalyst and the substrate determines the catalytic reaction in a great sense.With large specific surface area and abundant active sites,two-dimensional(2D)nanomaterials are promising catalysts for MgH_(2)via providing numerous pathways for the diffusion and dissociation of hydrogen.In this regard,2D NiMn-based layered double hydroxide and layered metallic oxide(LMO)are designed and introduced into MgH_(2)to improve its hydrogen storage properties.Simultaneous enhancement in interfacial contact,desorption temperature and kinetics are achieved.The MgH_(2)+9wt%Ni3Mn-LMO composites begin to discharge hydrogen at only 190℃and 6.10wt%H_(2)could be charged in 600 s at 150℃.The activation energy for de/hydrogenation is reduced by 42.43%and 46.56%,respectively,compared to pure MgH_(2).Even at a low operating temperature of 235℃,the modified system was still able to release 4.44wt%H_(2)in an hour,which has rarely been reported in previous studies.Microstructure observations and density functional theory calculations revealed that first,the hydrogen pumping effect of Mg_(2)Ni/Mg_(2)NiH_(4) promotes the adsorption and desorption of hydrogen molecules on the surface of MgH_(2),second,MnOx drew electrons from Mg_(2)Ni,producing a new Density of State structure with a lower d-bond center.This unique change further strengthens the Mg_(2)Ni/Mg_(2)NiH_(4) pump effect on MgH_(2).Our work indicates that the application of 2D metal-based catalysts is a feasible and promising approach towards MgH_(2)for solid-state hydrogen storage to meet technical and scientific requirements.展开更多
The transition metal trichalcogenides(TMTs)with quasi-one-dimensional(quasi-1D)layered crystal structure represent a unique platform to explore intriguing physical properties.Herein,we report the successful growth of ...The transition metal trichalcogenides(TMTs)with quasi-one-dimensional(quasi-1D)layered crystal structure represent a unique platform to explore intriguing physical properties.Herein,we report the successful growth of a new TMT TiSe_(3)single crystal by using a high-pressure and high-temperature technique.The crystal structure of TiSe_(3)was determined by measuring the single-crystal x-ray diffraction and selected area electron diffraction.The 1D chain-like structure along the b-axis is formed by the TiSe_(6)prisms which share their tops and bottoms with each other.TiSe_(3)is a narrow band gap semiconductor with electron-type carriers under ambient conditions identified by the electrical and Hall effect measurements.It exhibits a pressure-induced semiconductor-to-metal transition around 4 GPa.As the pressure further increases to~6 GPa,a pressure-induced Lifshitz transition occurs,as indicated by the electrical transport measurements,high-pressure crystal structure characterizations,and electronic band structure calculations.展开更多
Owing to the orbital hybridization between the transition metal and the B element and the electron-trapping effect of the B ele-ment,transition metal borides are considered very promising materials for energy catalysi...Owing to the orbital hybridization between the transition metal and the B element and the electron-trapping effect of the B ele-ment,transition metal borides are considered very promising materials for energy catalysis.In this work,an amorphous scaly high-entropy boride(HEB)with electron traps was designed and fabricated via a facile reduction method to improve the hydrogen storage properties of magnesium hydride(MgH_(2)).For dehydrogenation,the onset temperature of MgH_(2)+10wt%HEB was dropped to 187.4℃;be-sides,the composite exhibited superior isothermal kinetics and the activation energy of the composite was reduced from(212.78±3.93)to(65.04±2.81)kJ/mol.In addition,MgH_(2)+10wt%HEB could absorb hydrogen at 21.5℃,and 5.02wt%H_(2) was charged in 50 min at 75℃.For reversible hydrogen storage capacity tests,the composite maintained a retention rate of 97%with 6.47wt%hydrogen capacity after 30 cycles.Combining microstructure evidence with hydrogen storage performance,the catalytic mechanism was proposed.During ball milling,scaly high-entropy borides riveted a large number of heterogeneous active sites on the surface of MgH_(2).Driven by the cocktail effect as well as the orbital hybridization of metal borides,numerous active sites steadily enhanced the hydrogen storage reactions in MgH_(2).展开更多
基金supported by National Natural Science Foundation of China(22279018)National Natural Science Foundation of China(22005055)Natural Science Foundation of Fujian Province(2022J01085).
文摘Solid oxide cells(SOCs)are emerging devices for efficient energy storage and conversion.However,during SOC operation,gaseous chromium(Cr)species released from Fe-Cr alloy interconnect can lead to Cr deposition and poisoning of air electrodes,causing substantial degradation in electrochemical performance and compromising the longterm stability of SOCs.This mini-review examines the mechanism of Cr deposition and poisoning in air electrodes under both fuel-cell and electrolysis modes.Furthermore,emphasis is placed on the recent advancements in strategies to mitigate Cr poisoning,offering insights into the rational design and development of active and Cr-tolerant air electrodes for SOCs.
基金This project was supported by the Fundamental Research Program of Shanxi Province(202303021221058)。
文摘The semiconductor photocatalysis are considered as one of the most promising candidates in hydrogen energy source and environmental remediation area.In this paper,flower-shaped SnS,is successfully combined on g-C,Ns,and the well matching band structure successfully constitutes a new Type-II heterojunction.As expected,the photocatalytic hydrogen production experiment showed that the quantity of hydrogen produced on 5% SnS_(2)/C_(3)N_(5)was 922.5μmol/(g.h),which is 3.6 times higher than that of pure g-C_(3)N_(5).Meanwhile,in photocatalytic degradation of methylene blue,5%SnS2/C,Ns composite material can degrade 95% of contaminants within 40 min,showing good photocatalytic degradation performance.The mechanism study indicates that SnS_(2)/C_(3)N_(5)heterojunction improves the photogenerated charge migration rate and reduces the electron-hole recombination rate,and effectively improves the photocatalytic performance of g-C_(3)N_(5).This work provides a new idea for designing C,Ns-based heterojunctions with efficient hydrogen production and degradation performance.
基金supported by the National Key Research and Development Plan of the Ministry of Science and Technology,China(Grant No.:2022YFE0125300)the National Natural Science Foundation of China(Grant No:81690262)+2 种基金the National Science and Technology Major Project,China(Grant No.:2017ZX09201004-021)the Open Project of National facility for Translational Medicine(Shanghai),China(Grant No.:TMSK-2021-104)Shanghai Jiao Tong University STAR Grant,China(Grant Nos.:YG2022ZD024 and YG2022QN111).
文摘Liposomes serve as critical carriers for drugs and vaccines,with their biological effects influenced by their size.The microfluidic method,renowned for its precise control,reproducibility,and scalability,has been widely employed for liposome preparation.Although some studies have explored factors affecting liposomal size in microfluidic processes,most focus on small-sized liposomes,predominantly through experimental data analysis.However,the production of larger liposomes,which are equally significant,remains underexplored.In this work,we thoroughly investigate multiple variables influencing liposome size during microfluidic preparation and develop a machine learning(ML)model capable of accurately predicting liposomal size.Experimental validation was conducted using a staggered herringbone micromixer(SHM)chip.Our findings reveal that most investigated variables significantly influence liposomal size,often interrelating in complex ways.We evaluated the predictive performance of several widely-used ML algorithms,including ensemble methods,through cross-validation(CV)for both lipo-some size and polydispersity index(PDI).A standalone dataset was experimentally validated to assess the accuracy of the ML predictions,with results indicating that ensemble algorithms provided the most reliable predictions.Specifically,gradient boosting was selected for size prediction,while random forest was employed for PDI prediction.We successfully produced uniform large(600 nm)and small(100 nm)liposomes using the optimised experimental conditions derived from the ML models.In conclusion,this study presents a robust methodology that enables precise control over liposome size distribution,of-fering valuable insights for medicinal research applications.
基金supported by Natural Science Foundation of Liaoning Province of China under Grant No.2020-MS-085。
文摘The morphology and dimension of W phases play an important role in determining mechanical properties of Mg-RE-Zn(where RE denotes rare earth elements)alloys.In this study,theγ′platelet and W particle occurred in the aged Mg-2Dy-0.5Zn(at.%)alloys were investigated by aberration-corrected scanning transmission electron microscopy.A novel formation mechanism of W phase was proposed,and its effects on the morphology and dimension of W particle,as well as mechanical properties of Mg-2Dy-0.5Zn alloys,were also discussed particularly.Different from other Mg-RE-Zn alloys,the nucleation and growth of W particle in Mg-Dy-Zn alloys mainly depend on the precipitatedγ′platelet.Primarily,a mass of Dy and Zn solute atoms concentrated nearγ′platelet or between two adjacentγ′platelets can meet the composition requirement of W particle nucleation.Next,the smaller interfacial mismatch between W andγ′facilitates the nucleation and growth of W particle.Thirdly,the growth of W particle can be achieved by consuming the surroundingγ′platelets.The nucleation and growth mechanisms make W particles exhibit rectangular or leaf-like and remain at the nanoscale.The coexistence ofγ′platelets and nanoscale W particles,and some better interfacial relationships between phases,lead to a high strength-ductility synergy of alloy.The findings may provide some fundamental guidelines for the microstructure design and optimization of new-type Mg-based alloys.
基金financial support from the Doctoral Foundation of Henan University of Engineering(No.D2022025)National Natural Science Foundation of China(No.U2004162)+1 种基金National Natural Science Foundation of China(No.52302138)Key Project for Science and Technology Development of Henan Province(No.232102320221)。
文摘With the rapid development of electric vehicles,hybrid electric vehicles and smart grids,people's demand for large-scale energy storage devices is increasingly intense.As a new type of secondary battery,potassium ion battery is promising to replace the lithium-ion battery in the field of large-scale energy storage by virtue of its low price and environmental friendliness.At present,the research on the anode materials of potassium ion batteries mainly focuses on carbon materials and the design of various nanostructured metal-based materials.Problems such as poor rate performance and inferior cycle life caused by electrode structure comminution during charge and discharge have not been solved.Quantum dots/nanodots materials are a new type of nanomaterials that can effectively improve the utilization of electrode materials and reduce production costs.In addition,quantum dots/nanodots materials can enhance the electrode reaction kinetics,reduce the stress generated in cycling,and effectively alleviate the agglomeration and crushing of electrode materials.In this review,we will systematically introduce the synthesis methods,K+storage properties and K+storage mechanisms of carbon quantum dots and carbon-based transition metal compound quantum dots composites.This review will have significant references for potassium ion battery researchers.
基金supported by the Open Fund of the Laboratory for Earth Surface Processes,Ministry of Education,Peking University,Beijing,China,and the Cultivation Fund Program for Excellent Dissertation in Fujian Normal University,China(No.LWPYS202315)the Research Start-up Fund of Fujian Normal University,China(No.Y0720304X13).
文摘Fifty agricultural soil samples collected from Fuzhou,southeast China,were first investigated for the occurrence,distribution,and potential risks of twelve organophosphate esters(OPEs).The total concentration of OPEs(ΣOPEs)in soil ranged from 1.33 to 96.5 ng/g dry weight(dw),with an average value of 17.1 ng/g dw.Especially,halogenated-OPEs were the predominant group with amean level of 9.75 ng/g dw,and tris(1-chloro-2-propyl)phosphate(TCIPP)was the most abundant OPEs,accounting for 51.1%ofΣOPEs.The concentrations of TCIPP andΣOPEs were found to be significantly higher(P<0.05)in soils of urban areas than those in suburban areas.In addition,the use of agricultural plastic films and total organic carbon had a positive effect on the occurrence of OPE in this study.The positive matrix factorization model suggested complex sources of OPEs in agricultural soils from Fuzhou.The ecological risk assessment demonstrated that tricresyl phosphate presented a medium risk to land-based organisms(0.1≤risk quotient<1.0).Nevertheless,the carcinogenic and noncarcinogenic risks for human exposure to OPEs through soil ingestion and dermal absorption were negligible.These findings would facilitate further investigations into the pollution management and risk control of OPEs.
基金Inner Mongolia Natural Science Foundation Project(2020LH05028)。
文摘Impact of texture type on the magnetic properties of ultrahigh density perpendicular magnetic recording media L1_(0)-FePt thin film was investigated,so were the texture formation and evolution mechanism.Reuss,Voigt,and Hill models were used to determine the anisotropic elastic modulus of L1_(0)-FePt thin film with fiber texture.Then,the elastic strain energies of thin films under various stress conditions were calculated.Results reveal that the stress condition has a significant influence on the fiber texture evolution.When the L1_(0)-FePt thin film is subjected to compressive in-plane strain prior to ordering phase transformation,the formation of{100}fiber texture is promoted.On the contrary,the ordering phase transformation under tensile in-plane strain promotes the{001}fiber texture formation.
基金support from the earmarked fund for XJARS(No.XJARS-06)the Bingtuan Science and Technology Program(Nos.2021DB019,2022CB001-01)+1 种基金the National Natural Science Foundation of China(No.42275014)the Guangdong Foundation for Program of Science and Technology Research,China(No.2023B1212060044)。
文摘Current research primarily focuses on emerging organic pollutants,with limited attention to emerging inorganic pollutants (EIPs).However,due to advances in detection technology and the escalating environmental and health challenges posed by pollution,there is a growing interest in treating waters contaminated with EIPs.This paper explores biochar characteristics and modification methods,encompassing physical,chemical,and biological approaches for adsorbing EIPs.It offers a comprehensive review of research advancements in employing biochar for EIPs remediation in water,outlines the adsorption mechanisms of EIPs by biochar,and presents an environmental and economic analysis.It can be concluded that using biochar for the adsorption of EIPs in wastewater exhibits promising potential.Nonetheless,it is noteworthy that certain EIPs like Au(III),Rh(III),Ir(III),Ru(III),Os(III),Sc(III),and Y(III),have not been extensively investigated regarding their adsorption onto biochar.This comprehensive review will catalyze further inquiry into the biochar-based adsorption of EIPs,addressing current research deficiencies and advancing the practical implementation of biochar as a potent substrate for EIP removal from wastewater streams.
基金supported by the National Natural Science Foundation of China(NSFC,No.62074048)the Key Research and Development Plan of Anhui Province(No.2022f04020007)the Natural Science Foundation of Anhui Province(No.2208085MF177)。
文摘In this study,we present the fabrication of vertical SnO/β-Ga_(2)O_(3) heterojunction diode(HJD)via radio frequency(RF)reactive magnetron sputtering.The valence and conduction band offsets betweenβ-Ga_(2)O_(3) and SnO are determined to be 2.65and 0.75 eV,respectively,through X-ray photoelectron spectroscopy,showing a type-Ⅱband alignment.Compared to its Schottky barrier diode(SBD)counterpart,the HJD presents a comparable specific ON-resistances(R_(on,sp))of 2.8 mΩ·cm^(2) and lower reverse leakage current(I_R),leading to an enhanced reverse blocking characteristics with breakdown voltage(BV)of 1675 V and power figure of merit(PFOM)of 1.0 GW/cm~2.This demonstrates the high quality of the SnO/β-Ga_(2)O_(3) heterojunction interface.Silvaco TCAD simulation further reveals that electric field crowding at the edge of anode for the SBD was greatly depressed by the introduction of SnO film,revealing the potential application of SnO/β-Ga_(2)O_(3) heterojunction in the futureβ-Ga_(2)O_(3)-based power devices.data mining,AI training,and similar technologies,are reserved.
基金financial support from the National Natural Science Foundation of China(No.51801078).
文摘To modify the stable thermodynamics and poor kinetics of magnesium hydride(MgH_(2))for solid-state hydrogen storage,MIL-100(Fe)was in situ fabricated on the surfaces of TiO_(2)nano-sheets(NS)by a self-assembly method,and the prepared TiO_(2)NS@MIL-100(Fe)presents an excellent catalytic effect on MgH_(2).The MgH_(2)+7wt.%TiO_(2)NS@MIL-100(Fe)composite can release hydrogen at 200℃,achieving a decrease of 150℃ compared to pure MgH_(2).Besides,the activation energy of dehydrogenation is decreased to 70.62 kJ/mol and 4 wt.%H_(2) can be desorbed within 20 min at a low temperature of 235℃.Under conditions of 100℃ and 3 MPa,MgH_(2)+7wt.%TiO_(2)NS@MIL-100(Fe)absorbs 5 wt.%of H_(2) in 10 min.Surprisingly,6.62 wt.%reversible capacity is maintained after 50 cycles.The modification mechanism is confirmed that the presence of oxygen vacancies and the synergistic effect of multivalent titanium in TiO_(2)NS@MIL-100(Fe)greatly enhance the kinetic and thermodynamic properties of MgH_(2).
基金supported by the National Natural Science Foundation of China(NSFC/RGC/JRF N_HKU735/21)Research Grant Council of Hong Kong,China(17102120,17108821,17103922,C1024-22GF,C7074-21G)+1 种基金Health and Medical Research Fund(HMRF 09200966)(to CSWL)FRQS Postdoctoral Fellowship(to AHKF).
文摘Dendritic spines are small protrusions along dendrites that contain most of the excitatory synapses in principal neurons,playing a crucial role in neuronal function by creating a compartmentalized environment for signal transduction.The plasticity of spine morphologies provides a tunable handle to regulate calcium signal dynamics,allowing rapid regulation of protein expression necessary to establish and maintain synapses(Cornejo et al.,2022).If excitatory inputs were to be located primarily on dendritic shafts,dendrites would frequently short-circuit,preventing voltage signals from propagating(Cornejo et al.,2022).It is thus not surprising that the structural plasticity of dendritic spines is closely linked to synaptic plasticity and memory formation(Berry and Nedivi,2017).While comprehensive in vitro studies have been conducted,in vivo studies that directly tackle the mechanism of dendritic transport and translation in regulating spine plasticity spatiotemporally are limited.
基金supported by the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China(No.52488201)the National Natural Science Foundation of China(No.52276213)+1 种基金the Key Research and Development Program of Shaanxi Province(No.2024GX-YBXM-459)the Fundamental Research Funds for the Central Universities.
文摘Photosynthesis of hydrogen peroxide(H_(2)O_(2))from H_(2)O and O_(2)is considered to be a promising approach.However,limited to the rapid recombination of photo-generated carriers and sluggish kinetics of O_(2)re-duction to H_(2)O_(2),it is a challenge for polymeric photocatalysts to achieve efficient photocatalytic H_(2)O_(2) production.Herein,Ag single atoms and nitrogen defects decorated carbon nitride(Ag@MCT)are con-structed through self-assembly and pyrolysis methods.The optimized photocatalyst displays exceptional performance in pure water,with an H_(2)O_(2) production rate of as high as 528.4μmol g^(-1) h^(-1) and an apparent quantum yield for H_(2)O_(2)production of 4.5%at 420 nm.Experimental and theoretical results reveal that the Ag atomic sites act as electron mediators that promote the capture and transfer of photo-generated charge carriers,while nitrogen defects as electron collectors and reaction sites to enhance the adsorption and activation of O_(2),accelerating reduction kinetics from O_(2) to H_(2)O_(2).This work presents a re-liable strategy to design excellent photocatalysts by rationally modulating electronic structures and active sites for accelerating photo-generated charge carriers transfer and surface reaction kinetics.
基金financial supports from the National Key R&D Program of China(No.2020YFA0406204)the National Natural Science Foundation of China(No.51801078)。
文摘Hydrogen,as a cheap,clean,and cost-effective secondary energy source,performs an essential role in optimizing today’s energy structure.Magnesium hydride(Mg H_(2))represents an attractive hydrogen carrier for storage and transportation,however,the kinetic behavior and operating temperature remain undesirable.In this work,a dual-phase multi-site alloy(Ms A)anchored on carbon substrates was designed,and its superior catalytic effects on the hydrogen storage properties of MgH_(2) were reported.Mechanism analysis identified that multi-site Fe Ni_(3)/Ni Cu nanoalloys synergistically served as intrinsic drivers for the striking de/hydrogenation performance of the MgH_(2)-Ms A systems.Concretely,the unique multi-metallic site structure attached to the surface of MgH_(2)provided substantial reversible channels and accessible active sites conducive to the adsorption,activation,and nucleation of H atoms.In addition,the coupling system formed by FeNi_(3) and NiCu dual-phase alloys further enhanced the reactivity between Mg/MgH_(2) and H atoms.Hence,the onset dehydrogenation temperature of Mg H_(2)+5 wt%Ms A was reduced to 195℃ and the hydrogen desorption apparent activation energy was reduced to 83.6 k J/mol.5.08 wt%H_(2) could be released at 250℃ in 20 min,reaching a high dehydrogenation rate of 0.254 wt%H_(2)/min,yet that for MgH_(2) at a higher temperature of 335℃ was only 0.145 wt%H_(2)/min.Then,the dehydrogenated Mg H_(2)-Ms A sample could absorb hydrogen from room temperature(30℃)and charge 3.93 wt%H_(2) at 100℃ within20 min under 3.0 MPa H_(2) pressure.Benefiting from carbon substrates,the 5 wt%Ms A doped-MgH_(2) could still maintain 6.36 wt%hydrogen capacity after 20 cycles.In conclusion,this work provides experimental rationale and new insights for the design of efficient catalysts for magnesium-based solid-state hydrogen storage materials.
基金supported by the National Natural Science Foundation of China(No.41877425)the Shanghai Municipal Natural Science Foundation,China(No.21ZR1446800)+4 种基金the State Environmental Protection Key Laboratory of Synergetic Control and Joint Remediation for Soil&Water Pollution(No.GHBK-2022-005)the Key Lab of Eco-restoration of Regional Contaminated Environment(Shenyang University)Ministry of Education(No.KF-22-04)the Fundamental Research Funds for the Central Universities(No.2262022-00084)the open fund from the Shanghai Key Lab for Urban Ecological Processes and Eco-Restoration(No.SHUES2022A04)。
文摘In-situ enhanced bioreduction by functional materials is a cost-effective technology to remove chlorinated hydrocarbons in groundwater.Herein,a novel polydopamine(PDA)-modified biochar(BC)-based composite containing nanoscale zero-valent iron(n ZVI)and poly-l-lactic acid(PLLA)(PB-PDA-Fe)was synthesized to enhance the removal of 1,1,1-trichloroethane(1,1,1-TCA)in simulated groundwater with actual site sediments.Its impact on functional microbial community structure in system was also investigated.The typical characterizations revealed uniform dispersion of PLA and n ZVI particles on the BC surface,being smoother after PDA coating.The composite exhibited a significantly higher performance on 1,1,1-TCA removal(82.38%,initial concentration 100 mg/L)than Fe-PDA and PB-PDA treatments.The diversity and richness of the microbial community in the composite treatment consistently decreased during incubation due to a synergistic effect between PLLA-BC and n ZVI.Desulfitobaterium,Pedobacter,Sphaerochaeta,Shewanella,and Clostridium were identified as enriched genera by the composite through DNA-stable isotope probing(DNA-SIP),playing a crucial role in the bioreductive dechlorination process.All the above results demonstrate that this novel composite selectively enhances the activity of microorganisms with extracellular respiration functions to efficiently dechlorinate 1,1,1-TCA.These findings could contribute to understanding the responsive microbial community by carbon-iron composites and expedite the application of in-situ enhanced bioreduction for effective remediation of chlorinated hydrocarbon-contaminated groundwater.
基金supported by the UK’s Engineering and Physical Sciences Research Council(Grant Nos.EP/V000624/1,EP/X03495X/1,EP/X041166/1,and EP/T02643X/1)the Royal Society(Grant No.RG\R2\232531).
文摘Research on supercontinuum sources on silicon has made significant progress in the past few decades.However,conventional approaches to broaden the spectral bandwidth often rely on complex and critical dispersion engineering by optimizing the core thickness or introducing the cladding with special materials and structures.We propose and demonstrate supercontinuum generation using long-periodgrating(LPG)waveguides on silicon with a C-band pump.The LPG waveguide is introduced for quasi-phase matching,and the generated supercontinuum spectrum is improved greatly with grating-induced dispersive waves.In addition,the demonstrated LPG waveguide shows a low propagation loss comparable with regular silicon photonic waveguides without gratings.In experiments,when using a 1550-nm 75-fs pulse pump with a pulse energy of 200 pJ,the supercontinuum spectrum generated with the present LPG waveguide shows an ultrabroad extent from 1150 to 2300 nm,which is much wider by 200 nm than that achieved by dispersionengineered uniform silicon photonic waveguides on the same chip.This provides a promising option for on-chip broadband light source for silicon photonic systems.
基金supported by the National Natural Science Foundation of China(No.52005362)the Fundamental Research Program of Shanxi Province(Nos.202303021221005 and 202303021211045)+1 种基金the Patent Commercialization Program of Shanxi Province(No.202402003)the Key Research and Development Plan of Xinzhou City.
文摘Presetting tensile twins(TTs)can enhance the mechanical properties of magnesium(Mg)alloys.Two as-received(AR)sheets,as-received state-A(AR-A)with fiber texture and nonuniform grains and as-received state-B with basal texture and uniform equiaxial grains are selected to induce TTs via a novel method called corrugated wide limit alignment(CWLA),and the corresponding CWLA-processed sheets are denoted as CWLA-processed state-A(C-A)and CWLA-processed state-B(C-B).The results demonstrate that a larger initial average grain size correlates with a higher fraction of TTs induced in Mg sheets,thereby refining the grains and forming a new rolling direction(RD)tilted texture during CWLA.The ultimate tensile strength increases by 32%from AR-A to C-A,primarily due to refinement strengthening and twinning-induced strain hardening.The recrystallization mechanism of C-A is dominated by twinning-induced dynamic recrystallization(DRX),where DRX grains prefer to inherit the orientation of TTs,resulting in an enhanced RD-tilted texture and the formation of multi-modal texture.The recrystallization mechanism of C-B is mainly discontinuous DRX and continuous DRX,and the DRX grains prefer to inherit the orientation of matrix grains,ultimately forming a basal texture.In summary,the tensile mechanical behavior of pre-twinned Mg sheets significantly depends on the grain size and texture of the AR sheets,so they present similar changing trends during tensile deformation.
基金supported by the National Natural Science Foundation of China(Nos.22302168 and 22272148).
文摘Methanol-assisted water electrolysis presents a promising yet challenging technique for electrochemical hydrogen production,as limited by the easy poisoning issue of Pt active sites.In this study,we successfully synthesized an efficient bifunctional catalyst composed of three-dimensional(3D)flower-like MoTe_(2) embedded nitrogen-doped carbon(NC)nanospheres,assembled by nanosheets,to support Pt nanoparticles(Pt-MoTe_(2)/NC)for methanol-assisted water electrolysis.This innovative Pt-MoTe_(2)/NC catalyst demonstrated superior catalytic performance targeting both hydrogen evolution reaction(HER)and methanol oxidation reaction(MOR)due to the strong metal-support interaction and the promotional effect of oxophilic molybdenum telluride.In situ infrared spectroscopy and CO stripping measurements revealed their excellent anti-poisoning ability.In particular,the onset potential of CO oxidation decreased by 130 mV relative to the standard Pt/C electrode.Theoretical calculations indicated the proper H*adsorption energy for HER and weakened CO adsorption energy for MOR in the optimized electronic structure.Therefore,the Pt-MoTe_(2)/NC electrode achieved the highest forward peak current density(76.6 mA·cm^(−2))for MOR,approximately 2.8-fold that of the commercial Pt/C,and only 34 mV was needed to deliver 10 mA·cm^(−2) for HER in acidic electrolyte.When employed as the bifunctional electrode in methanol electrolysis,Pt-MoTe_(2)/NC enabled efficient hydrogen generation with good stability,requiring merely 0.65 V to achieve 10 mA·cm^(−2),approximately 1090 mV less than traditional water electrolysis.This work presents an anti-poisoning catalyst in energy-saving hydrogen production from methanol electrolysis.
基金supports from the National Key R&D Program of China(2020YFA0406204)the National Natural Science Foundation of China(Grant No 51801078).
文摘Catalytic doping of magnesium hydride(MgH_(2))to improve its hydrogen ab/desorption kinetic properties is considered to be an effective and feasible method.In solid-phase catalysis,the extent of contact between the catalyst and the substrate determines the catalytic reaction in a great sense.With large specific surface area and abundant active sites,two-dimensional(2D)nanomaterials are promising catalysts for MgH_(2)via providing numerous pathways for the diffusion and dissociation of hydrogen.In this regard,2D NiMn-based layered double hydroxide and layered metallic oxide(LMO)are designed and introduced into MgH_(2)to improve its hydrogen storage properties.Simultaneous enhancement in interfacial contact,desorption temperature and kinetics are achieved.The MgH_(2)+9wt%Ni3Mn-LMO composites begin to discharge hydrogen at only 190℃and 6.10wt%H_(2)could be charged in 600 s at 150℃.The activation energy for de/hydrogenation is reduced by 42.43%and 46.56%,respectively,compared to pure MgH_(2).Even at a low operating temperature of 235℃,the modified system was still able to release 4.44wt%H_(2)in an hour,which has rarely been reported in previous studies.Microstructure observations and density functional theory calculations revealed that first,the hydrogen pumping effect of Mg_(2)Ni/Mg_(2)NiH_(4) promotes the adsorption and desorption of hydrogen molecules on the surface of MgH_(2),second,MnOx drew electrons from Mg_(2)Ni,producing a new Density of State structure with a lower d-bond center.This unique change further strengthens the Mg_(2)Ni/Mg_(2)NiH_(4) pump effect on MgH_(2).Our work indicates that the application of 2D metal-based catalysts is a feasible and promising approach towards MgH_(2)for solid-state hydrogen storage to meet technical and scientific requirements.
基金the National Key R&D Program of China(Grant Nos.2023YFA1406100 and 2024YFA1400066)the Open Research Fund of Beijing National Laboratory for Condensed Matter Physics(Grant No.2023BNLCMPKF002)+6 种基金supported by the National Natural Science Foundation of China(Grant Nos.52288102 and 52090020)the S&T Program of Hebei(Grant No.225A1102D)the Open Projects from the State Key Laboratory of Metastable Materials Science and Technology,Yanshan University(Grant No.202301)carried out at the Synergetic Extreme Condition User Facility(SE-CUF)of the Chinese Academy of Sciencessupport from the Analytical Instrumentation Center(Grant No.SPST-AIC10112914)School of Physical Science and Technology(SPST),ShanghaiTech Universitysupported by the Double First-Class Initiative Fund of ShanghaiTech University.
文摘The transition metal trichalcogenides(TMTs)with quasi-one-dimensional(quasi-1D)layered crystal structure represent a unique platform to explore intriguing physical properties.Herein,we report the successful growth of a new TMT TiSe_(3)single crystal by using a high-pressure and high-temperature technique.The crystal structure of TiSe_(3)was determined by measuring the single-crystal x-ray diffraction and selected area electron diffraction.The 1D chain-like structure along the b-axis is formed by the TiSe_(6)prisms which share their tops and bottoms with each other.TiSe_(3)is a narrow band gap semiconductor with electron-type carriers under ambient conditions identified by the electrical and Hall effect measurements.It exhibits a pressure-induced semiconductor-to-metal transition around 4 GPa.As the pressure further increases to~6 GPa,a pressure-induced Lifshitz transition occurs,as indicated by the electrical transport measurements,high-pressure crystal structure characterizations,and electronic band structure calculations.
基金supported by the National Natural Science Foundation of China(No.22179054)the Jiangsu Province Innovation Support Project,China(No.BZ2023010)+1 种基金the Project of Jiangsu University High-Tech Ship Collaborative Innovation Center(No.1174871801-11)the Ministry of Science and Technology of the People’s Republic of China(No.G2023014022L).
文摘Owing to the orbital hybridization between the transition metal and the B element and the electron-trapping effect of the B ele-ment,transition metal borides are considered very promising materials for energy catalysis.In this work,an amorphous scaly high-entropy boride(HEB)with electron traps was designed and fabricated via a facile reduction method to improve the hydrogen storage properties of magnesium hydride(MgH_(2)).For dehydrogenation,the onset temperature of MgH_(2)+10wt%HEB was dropped to 187.4℃;be-sides,the composite exhibited superior isothermal kinetics and the activation energy of the composite was reduced from(212.78±3.93)to(65.04±2.81)kJ/mol.In addition,MgH_(2)+10wt%HEB could absorb hydrogen at 21.5℃,and 5.02wt%H_(2) was charged in 50 min at 75℃.For reversible hydrogen storage capacity tests,the composite maintained a retention rate of 97%with 6.47wt%hydrogen capacity after 30 cycles.Combining microstructure evidence with hydrogen storage performance,the catalytic mechanism was proposed.During ball milling,scaly high-entropy borides riveted a large number of heterogeneous active sites on the surface of MgH_(2).Driven by the cocktail effect as well as the orbital hybridization of metal borides,numerous active sites steadily enhanced the hydrogen storage reactions in MgH_(2).
