Methanol oxidation reaction (MOR) at Pt and Pt electrode surface deposited with various amounts of Ru (denoted as PtxRuy, nominal coverage y is 0.17, 0.27, and 0.44 ML) in 0.1 mol/L HClO4+0.5 mol/L MeOH has been ...Methanol oxidation reaction (MOR) at Pt and Pt electrode surface deposited with various amounts of Ru (denoted as PtxRuy, nominal coverage y is 0.17, 0.27, and 0.44 ML) in 0.1 mol/L HClO4+0.5 mol/L MeOH has been studied under potentiostatic conditions by in situ FTIR spectroscopy in attenuated-total-reflection con guration and di erential electro-chemical mass spectrometry under controlled flow conditions. Results reveal that (i) CO is the only methanol-related adsorbate observed by IR spectroscopy at all the Pt and PtRu electrodes examined at potentials from 0.3 V to 0.6 V (vs. RHE); (ii) at Pt0.56Ru0.44, two IR bands, one from CO adsorbed at Ru islands and the other from COL at Pt substrate are detected, while at other electrodes, only a single band for COL adsorbed at Pt is observed; (iii) MOR activity decreases in the order of Pt0.73Ru0.27〉Pt0.56Ru0.44〉Pt0.83Ru0.17〉Pt; (iv) at 0.5 V, MOR at Pt0.73Ru0.27 reaches a current e ciency of 50% for CO2 production, the turn-over frequency from CH3OH to CO2 is ca. 0.1 molecule/(site sec). Suggestions for further improving of PtRu catalysts for MOR are provided.展开更多
Materials exhibiting high-performance electromagnetic wave absorption have garnered considerable scientific and technological attention,yet encounter significant challenges.Developing new materials and innovative stru...Materials exhibiting high-performance electromagnetic wave absorption have garnered considerable scientific and technological attention,yet encounter significant challenges.Developing new materials and innovative structural design concepts is crucial for expanding the application field of electromagnetic wave absorption.Particularly,hierarchical structure engineering has emerged as a promising approach to enhance the physical and chemical properties of materials,providing immense potential for creating versatile electromagnetic wave absorption materials.Herein,an exceptional multi-dimensional hierarchical structure was meticulously devised,unleashing the full microwave attenuation capabilities through in situ growth,selfreduction,and multi-heterogeneous interface integration.The hierarchical structure features a three-dimensional carbon framework,where magnetic nanoparticles grow in situ on the carbon skeleton,creating a necklace-like structure.Furthermore,magnetic nanosheets assemble within this framework.Enhanced impedance matching was achieved by precisely adjusting component proportions,and intelligent integration of diverse interfaces bolstered dielectric polarization.The obtain Fe_(3)O_(4)-Fe nanoparticles/carbon nanofibers/Al-Fe_(3)O_(4)-Fe nanosheets composites demonstrated outstanding performance with a minimum reflection loss(RLmin)value of−59.3 dB and an effective absorption bandwidth(RL≤−10 dB)extending up to 5.6 GHz at 2.2 mm.These notable accomplishments offer fresh insights into the precision design of high-efficient electromagnetic wave absorption materials.展开更多
Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will ben...Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will benefit their quick transition to the next catalysts.Herein,Mo-doped CoOOH was designed as a high-performance model electrocatalyst with durability for 20 h at 10 mAcm−2.Additionally,it had an overpotential of 260 mV(glassy carbon)or 215 mV(nickel foam),which was 78 mV lower than that of IrO_(2)(338 mV).In situ,Raman spectroscopy revealed the transformation process of CoOOH.Calculations using the density functional theory showed that during OER,doped Mo increased the spin-up density of states and shrank the spin-down bandgap of the 3d orbits in the reconstructed CoOOH under the electrochemical activation process,which simultaneously optimized the adsorption and electron conduction of oxygen-related intermediates on Co sites and lowered the OER overpotentials.Our research provides new insights into the methodical planning of the creation of transition-metal oxyhydroxide OER catalysts.展开更多
Direct analysis of copper-base alloys using laser ablation techniques is an increasingly common procedure in cultural heritage studies. However, main discussions remain focused on the possibility of using non-matrix m...Direct analysis of copper-base alloys using laser ablation techniques is an increasingly common procedure in cultural heritage studies. However, main discussions remain focused on the possibility of using non-matrix matched external reference materials. To evaluate the occurrence of matrix effects during in situ microanalysis of copper-base materials, using near infrared femtosecond laser ablation techniques (NIR fs-LA-ICP-MS), two bronzes, i.e., (Sn-Zn)-ternary and (Sn)-binary copper-matrix reference materials, as well as a reference synthetic glass (NIST-SRM-610) have been analyzed. The results have been compared to data obtained on a sulfide-matrix reference material. Similar values in relative sensitivity averages of 63Cu, 118Sn and 66Zn, as well as in 118Sn/63Cu and 66Zn/63Cu ratios were obtained, for all analyzed matrix types, i.e., copper-base-, silicate-, and sulfide-reference materials. Consequently, it is possible to determinate major and minor element concentrations in copper alloys, i.e., Cu, Sn and Zn, using silicate and sulfide reference materials as external calibrators, without any matrix effect and over a wide range of concentrations (from wt.% to ppm). Equally, Cu, Sn and Zn concentrations can be precisely determined in sulfides using homogeneous alloys (reference) materials as an external calibrator. Thus, it is possible to determine Cu, Sn and Zn in copper-base materials and their ore minerals, mostly sulfides, in a single analytical session, without requiring specific external calibrators for each matrix type. In contrast, immiscible elements in copper matrix, such as Pb and Fe show notable differences in their relative sensitivity values and ratios for different matrix-materials analyzed, implying that matrix-matched external calibrations remain to be applied for their trace quantification.展开更多
Dear Editor,Three dimensional(3D)bioprinted extracellular matrix(ECM)can be used to provide both biochemical and biophysical cues to direct mesenchymal stem cells(MSCs)differentiation,and then differentiated cells wer...Dear Editor,Three dimensional(3D)bioprinted extracellular matrix(ECM)can be used to provide both biochemical and biophysical cues to direct mesenchymal stem cells(MSCs)differentiation,and then differentiated cells were isolated for implantation in vivo using surgical procedures.However,the reduced cell activity after cell isolation from 3D constructs and low cell retention in injured sites limit its application[1].Methacrylated gelatin(GelMA)hydrogel has the advantage of fast crosslinking,which could resemble complex architectures of tissue construct in vivo[2].Here,we adopted a noninvasive bioprinting procedure to imitate the regenerative microenvironment that could simultaneously direct the sweat gland(SG)and vascular differentiation from MSCs and ultimately promote the replacement of glandular tissue in situ(Fig.1a).展开更多
The Nuri deposit is the only Cu-W-Mo polymetallic deposit with large-scale WO3 resources in the eastern section of the Gangdese metallogenic belt,Tibet,China.However,the genetic type of this deposit has been controver...The Nuri deposit is the only Cu-W-Mo polymetallic deposit with large-scale WO3 resources in the eastern section of the Gangdese metallogenic belt,Tibet,China.However,the genetic type of this deposit has been controversial since its discovery.Based on a study of the geological characteristics of the deposit,this study presents mineralization stages,focusing on the oxide stage and the quartz-sulfide stage where scheelite is mainly formed,referred to as Sch-A and Sch-B,respectively.Through LA-ICP-MS trace element and Sr isotope analyses,the origin,evolutionary process of the oreforming fluid and genesis of the ore deposit are investigated.Scanning Electron Microscope-Cathodoluminescence(SEMCL)observations reveal that Sch-A consists of three generations,with dark gray homogenous Sch-A1 being replaced by relatively lighter and homogeneous Sch-A2 and Sch-A3,with Sch-A2 displaying a gray CL image color with vague and uneven growth bands and Sch-A3 has a light gray CL image color with hardly any growth band.In contrast,Sch-B exhibits a‘core-rim’structure,with the core part(Sch-B1)being dark gray and displaying a uniform growth band,while the rim part(Sch-B2)is light gray and homogeneous.The normalized distribution pattern of rare earth elements in scheelite and Sr isotope data suggest that the early ore-forming fluid in the Nuri deposit originated from granodiorite porphyry and,later on,some country rock material was mixed in,due to strong water-rock interaction.Combining the O-H isotope data further indicates that the ore-forming fluid in the Nuri deposit originated from magmatic-hydrothermal sources,with contributions from metamorphic water caused by water-rock interaction during the mineralization process,as well as later meteoric water.The intense water-rock interaction likely played a crucial role in the precipitation of scheelite,leading to varying Eu anomalies in different generations of scheelite from the oxide stage to the quartz-sulfide stage,while also causing a gradual decrease in oxygen fugacity(fO2)and a slow rise in pH value.Additionally,the high Mo and low Sr contents in the scheelite are consistent with typical characteristics of magmatic-hydrothermal scheelite.Therefore,considering the geological features of the deposit,the geochemical characteristics of scheelite and the O-H isotope data published previously,it can be concluded that the genesis of the Nuri deposit belongs to porphyry-skarn deposit.展开更多
The Moon provides a unique environment for investigating nearby astrophysical events such as supernovae.Lunar samples retain valuable information from these events,via detectable long-lived“fingerprint”radionuclides...The Moon provides a unique environment for investigating nearby astrophysical events such as supernovae.Lunar samples retain valuable information from these events,via detectable long-lived“fingerprint”radionuclides such as^(60)Fe.In this work,we stepped up the development of an accelerator mass spectrometry(AMS)method for detecting^(60)Fe using the HI-13tandem accelerator at the China Institute of Atomic Energy(CIAE).Since interferences could not be sufficiently removed solely with the existing magnetic systems of the tandem accelerator and the following Q3D magnetic spectrograph,a Wien filter with a maximum voltage of±60 kV and a maximum magnetic field of 0.3 T was installed after the accelerator magnetic systems to lower the detection background for the low abundance nuclide^(60)Fe.A 1μm thick Si_(3)N_(4) foil was installed in front of the Q3D as an energy degrader.For particle detection,a multi-anode gas ionization chamber was mounted at the center of the focal plane of the spectrograph.Finally,an^(60)Fe sample with an abundance of 1.125×10^(-10)was used to test the new AMS system.These results indicate that^(60)Fe can be clearly distinguished from the isobar^(60)Ni.The sensitivity was assessed to be better than 4.3×10^(-14)based on blank sample measurements lasting 5.8 h,and the sensitivity could,in principle,be expected to be approximately 2.5×10^(-15)when the data were accumulated for 100 h,which is feasible for future lunar sample measurements because the main contaminants were sufficiently separated.展开更多
Ex situ characterization techniques in molecular beam epitaxy(MBE)have inherent limitations,such as being prone to sample contamination and unstable surfaces during sample transfer from the MBE chamber.In recent years...Ex situ characterization techniques in molecular beam epitaxy(MBE)have inherent limitations,such as being prone to sample contamination and unstable surfaces during sample transfer from the MBE chamber.In recent years,the need for improved accuracy and reliability in measurement has driven the increasing adoption of in situ characterization techniques.These techniques,such as reflection high-energy electron diffraction,scanning tunneling microscopy,and X-ray photoelectron spectroscopy,allow direct observation of film growth processes in real time without exposing the sample to air,hence offering insights into the growth mechanisms of epitaxial films with controlled properties.By combining multiple in situ characterization techniques with MBE,researchers can better understand film growth processes,realizing novel materials with customized properties and extensive applications.This review aims to overview the benefits and achievements of in situ characterization techniques in MBE and their applications for material science research.In addition,through further analysis of these techniques regarding their challenges and potential solutions,particularly highlighting the assistance of machine learning to correlate in situ characterization with other material information,we hope to provide a guideline for future efforts in the development of novel monitoring and control schemes for MBE growth processes with improved material properties.展开更多
LiNi_(x)Co_(y)Al_(z)O_(2)(NCA)cathode materials are drawing widespread attention,but the huge gap between the ideal and present cyclic stability still hinders their further commercial application,especially for the Ni...LiNi_(x)Co_(y)Al_(z)O_(2)(NCA)cathode materials are drawing widespread attention,but the huge gap between the ideal and present cyclic stability still hinders their further commercial application,especially for the Ni-rich LiNi_(x)Co_(y)Al_(z)O_(2)(x>0.8,x+y+z=1)cathode material,which is owing to the structural degradation and particles'intrinsic fracture.To tackle the problems,Li_(0.5)La_(2)Al_(0.5)O_(4)in situ coated and Mn compensating doped multilayer LiNi_(0.82)Co_(0.14)Al_(0.04)O_(2)was prepared.XRD refinement indicates that La-Mn co-modifying could realize appropriate Li/Ni disorder degree.Calculated results and in situ XRD patterns reveal that the LLAO coating layer could effectively restrain crack in secondary particles benefited from the suppressed internal strain.AFM further improves as NCA-LM2 has superior mechanical property.The SEM,TEM,XPS tests indicate that the cycled cathode with LLAO-Mn modification displays a more complete morphology and less side reaction with electrolyte.DEMS was used to further investigate cathode-electrolyte interface which was reflected by gas evolution.NCA-LM2 releases less CO_(2)than NCA-P indexing on a more stable surface.The modified material presents outstanding capacity retention of 96.2%after 100 cycles in the voltage range of 3.0-4.4 V at 1C,13%higher than that of the pristine and 80.8%at 1 C after 300 cycles.This excellent electrochemical performance could be attributed to the fact that the high chemically stable coating layer of Li_(0.5)La_(2)Al_(0.5)O_(4)(LLAO)could enhance the interface and the Mn doping layer could suppress the influence of the lattice mismatch and distortion.We believe that it can be a useful strategy for the modification of Ni-rich cathode material and other advanced functional material.展开更多
The reaction mechanism for alkylation of benzene with propylene over the β zeolite and the MCM-22 zeolite were investigated respectively by in-situ IR spectrometry. Three types of experiments were carried out. (1) ...The reaction mechanism for alkylation of benzene with propylene over the β zeolite and the MCM-22 zeolite were investigated respectively by in-situ IR spectrometry. Three types of experiments were carried out. (1) IR spectra of the gas-phase propylene, benzene and isopropyl benzene were recorded. (2) IR spectra of the above-mentioned substances as adsorbates that have combined with the zeolite wafer were recorded. (3) IR spectra of the reaction modes were recorded. The test results showed that the alkytation reaction over the zeolite β was ascribed to the mechanism of carbonium ions, whereas the alkylation reaction over the zeolite MCM-22 was ascribed to the synchronous reaction mechanism.展开更多
Lunar habitat construction is crucial for successful lunar exploration missions.Due to the limitations of transportation conditions,extensive global research has been conducted on lunar in situ material processing tec...Lunar habitat construction is crucial for successful lunar exploration missions.Due to the limitations of transportation conditions,extensive global research has been conducted on lunar in situ material processing techniques in recent years.The aim of this paper is to provide a comprehensive review,precise classification,and quantitative evaluation of these approaches,focusing specifically on four main approaches:reaction solidification(RS),sintering/melting(SM),bonding solidification(BS),and confinement formation(CF).Eight key indicators have been identified for the construction of low-cost and highperformance systems to assess the feasibility of these methods:in situ material ratio,curing temperature,curing time,implementation conditions,compressive strength,tensile strength,curing dimensions,and environmental adaptability.The scoring thresholds are determined by comparing the construction requirements with the actual capabilities.Among the evaluated methods,regolith bagging has emerged as a promising option due to its high in situ material ratio,low time requirement,lack of hightemperature requirements,and minimal shortcomings,with only the compressive strength falling below the neutral score.The compressive strength still maintains a value of 2–3 MPa.The proposed construction scheme utilizing regolith bags offers numerous advantages,including rapid and large-scale construction,ensured tensile strength,and reduced reliance on equipment and energy.In this study,guidelines for evaluating regolith solidification techniques are provided,and directions for improvement are offered.The proposed lunar habitat design based on regolith bags is a practical reference for future research.展开更多
This study aims to investigate the feasibility of deriving in situ horizontal stresses from the breakout width and depth using the analytical method.Twenty-three breakout data with different borehole sizes were collec...This study aims to investigate the feasibility of deriving in situ horizontal stresses from the breakout width and depth using the analytical method.Twenty-three breakout data with different borehole sizes were collected and three failure criteria were studied.Based on the Kirsch equations,relatively accurate major horizontal stress(sH)estimations from known minor horizontal stress(sh)were achieved with percentage errors ranging from 0.33%to 44.08%using the breakout width.The Mogi-Coulomb failure criterion(average error:13.1%)outperformed modified Wiebols-Cook(average error:19.09%)and modified Lade(average error:18.09%)failure criteria.However,none of the tested constitutive models could yield reasonable sh predictions from known sH using the same approach due to the analytical expression of the redistributed stress and the nature of the constitutive models.In consideration of this issue,the horizontal stress ratio(sH/sh)is suggested as an alternative input,which could estimate both sH and sh with the same level of accuracy.Moreover,the estimation accuracies for both large-scale and laboratory-scale breakouts are comparable,suggesting the applicability of this approach across different breakout sizes.For breakout depth,conformal mapping and complex variable method were used to calculate the stress concentration around the breakout tip,allowing the expression of redistributed stresses using binomials composed of sH and sh.Nevertheless,analysis of the breakout depth stabilisation mechanism indicates that additional parameters are required to utilise normalised breakout depth for stress estimation compared to breakout width.These parameters are challenging to obtain,especially under field conditions,meaning utilising normalised breakout depth analytically in practical applications faces significant challenges and remains infeasible at this stage.Nonetheless,the normalised breakout depth should still be considered a critical input for any empirical and statistical stress estimation method given its significant correlation with horizontal stresses.The outcome of this paper is expected to contribute valuable insights into the breakout stabilisation mechanisms and estimation of in situ stress magnitudes based on borehole breakout geometries.展开更多
The current study comprehensively evaluates four different protein extraction methods based on urea,sodium dodecyl sulfate(SDS),anionic surfactants(BT),and total RNA extractor(Trizol),aiming to optimize the sample pre...The current study comprehensively evaluates four different protein extraction methods based on urea,sodium dodecyl sulfate(SDS),anionic surfactants(BT),and total RNA extractor(Trizol),aiming to optimize the sample preparation workflow for mass spectrometry-based proteomics.Using HeLa cells as an example,we found that the method employing the mass spectrometry-compatible surfactant BT reagent significantly reduces the total time consumed for protein extraction and minimizes protein losses during the sample preparation process.Further integrating the four protein extraction methods,we identified over 7000 proteins from HeLa cells without relying on pre-fractionation techniques,and 2990 of them were quantified using label-free quantification.It is worth noting that the BT and SDS methods demonstrate higher efficiency in extracting membrane proteins,while the Urea and Trizol methods are more effective in extracting proteins from nuclear and cytoplasmic fractions.In summary,this study provides a novel solution for deep proteome coverage,particularly in the context of cellular protein extraction,by integrating mass spectrometry-compatible surfactants with traditional extraction methods to effectively enhance protein identification numbers.展开更多
Profiling the protein composition of bacteria is essential for understanding their biology,physiology and interaction with environment.Mass spectrometry has become a pivotal tool for protein analysis,facilitating the ...Profiling the protein composition of bacteria is essential for understanding their biology,physiology and interaction with environment.Mass spectrometry has become a pivotal tool for protein analysis,facilitating the examination of expression levels,molecular masses and structural modifications.In this study,we compared the performance of three widely-used mass spectrometry methods,i.e.,matrix-assisted laser desorption/ionization(MALDI)protein fingerprinting,top-down proteomics and bottom-up proteomics,in the profiling of bacterial protein composition.It was revealed that bottom-up proteomics provided the highest protein coverage and exhibited the greatest protein profile overlap between bacterial species.In contrast,MALDI protein fingerprinting demonstrated superior detection reproducibility and effectiveness in distinguishing between bacterial species.Although top-down proteomics identified fewer proteins than bottom-up approach,it complemented MALDI fingerprinting in the discovery of bacterial protein markers,both favoring abundant,stable,and hydrophilic bacterial ribosomal proteins.This study represents the most systematic and comprehensive comparison of mass spectrometry-based protein profiling methodologies to date.It provides valuable guidelines for the selection of appropriate profiling strategies for specific analytical purposes.This will facilitate studies across various fields,including infection diagnosis,antimicrobial resistance detection and pharmaceutical target discovery.展开更多
MgH_(2) and TiH_(2) have been extensively studied as potential anode materials due to their high theoretical specific capacities of 2036 and 1024 mAh/g,respectively.However,the large volume changes that these compound...MgH_(2) and TiH_(2) have been extensively studied as potential anode materials due to their high theoretical specific capacities of 2036 and 1024 mAh/g,respectively.However,the large volume changes that these compounds undergo during cycling affects their performance and limits practical applications.The present work demonstrates a novel approach to limiting the volume changes of active materials.This effect is based on mechanical support from an intimate interface generated in situ via the reaction between MgH_(2) and Ti within the electrode prior to lithiation to form Mg and TiH_(2).The resulting Mg can be transformed back to MgH_(2) by reaction with LiH during delithiation.In addition,the TiH_(2) improves the reaction kinetics of MgH_(2) and enhances electrochemical performance.The intimate interface produced in this manner is found to improve the electrochemical properties of a MgH_(2)-Ti-LiH electrode.An exceptional reversible capacity of 800 mAh/g is observed even after 200 cycles with a high current density of 1 mA/cm^(2) and a high proportion of active material(90 wt.%)at an operation temperature of 120℃.This study therefore showcases a new means of improving the performance of electrodes by limiting the volume changes of active materials.展开更多
Phase transition of polycrystalline iron compressed along the Hugoniot is studied by combining laser-driven shock with in situ x-ray diffraction technique.It is suggested that polycrystalline iron changes from an init...Phase transition of polycrystalline iron compressed along the Hugoniot is studied by combining laser-driven shock with in situ x-ray diffraction technique.It is suggested that polycrystalline iron changes from an initial body-centered cubic structure to a hexagonal close-packed structure with increasing pressure(i.e.,a phase transition fromαtoε).The relationship between density and pressure for polycrystalline iron obtained from the present experiments is found to be in good agreement with the gas-gun Hugoniot data.Our results show that experiments with samples at lower temperatures under static loading,such as in a diamond anvil cell,lead to higher densities measured than those found under dynamic loading.This means that extrapolating results of static experiments may not predict the dynamic responses of materials accurately.In addition,neither the face-centered cubic structure seen in previous molecular-dynamics simulations or twophase coexistence are found within our experimental pressure range.展开更多
Interfacial water molecules are the most important participants in the hydrogen evolution reaction(HER).Hence,understanding the behavior and role that interfacial water plays will ultimately reveal the HER mechanism.U...Interfacial water molecules are the most important participants in the hydrogen evolution reaction(HER).Hence,understanding the behavior and role that interfacial water plays will ultimately reveal the HER mechanism.Unfortunately,investigating interfacial water is extremely challenging owing to the interference caused by bulk water molecules and complexity of the interfacial environment.Here,the behaviors of interfacial water in different cationic electrolytes on Pd surfaces were investigated by the electrochemistry,in situ core-shell nanostructure enhanced Raman spectroscopy and theoretical simulation techniques.Direct spectral evidence reveals a red shift in the frequency and a decrease in the intensity of interfacial water as the potential is shifted in the positively direction.When comparing the different cation electrolyte systems at a given potential,the frequency of the interfacial water peak increases in the specified order:Li+<Na^(+)<K^(+)<Ca^(2+)<Sr^(2+).The structure of interfacial water was optimized by adjusting the radius,valence,and concentration of cation to form the two-H down structure.This unique interfacial water structure will improve the charge transfer efficiency between the water and electrode further enhancing the HER performance.Therefore,local cation tuning strategies can be used to improve the HER performance by optimizing the interfacial water structure.展开更多
To prolong the service life of optics,the feasibility of in situ cleaning of the multilayer mirror(MLM)of tin and its oxidized contamination was investigated using hydrogen plasma at different power levels.Granular ti...To prolong the service life of optics,the feasibility of in situ cleaning of the multilayer mirror(MLM)of tin and its oxidized contamination was investigated using hydrogen plasma at different power levels.Granular tin-based contamination consisting of micro-and macroparticles was deposited on silicon via physical vapor deposition(PVD).The electrodedriven hydrogen plasma at different power levels was systematically diagnosed using a Langmuir probe and a retarding field ion energy analyzer(RFEA).Moreover,the magnitude of the self-biasing voltage was measured at different power levels,and the peak ion energy was corrected for the difference between the RFEA measurements and the self-biasing voltage(E_(RFEA)-eV_(self)).XPS analysis of O 1s and Sn 3d peaks demonstrated the chemical reduction process after 1 W cleaning.Analysis of surface and cross-section morphology revealed that holes emerged on the upper part of the macroparticles while its bottom remained smooth.Hills and folds appeared on the upper part of the microparticles,confirming the top-down cleaning mode with hydrogen plasma.This study provides an in situ electrode-driven hydrogen plasma etching process for tin-based contamination and will provide meaningful guidance for understanding the chemical mechanism of reduction and etching.展开更多
In situ surface-enhanced Raman scattering(SERS)is a widely used operando analytical technique,while facing numerous complex factors in applications under aqueous environment,such as low detection sensitivity,poor anti...In situ surface-enhanced Raman scattering(SERS)is a widely used operando analytical technique,while facing numerous complex factors in applications under aqueous environment,such as low detection sensitivity,poor anti-interference capability,etc.,resulting in unreliable detectability.To address these issues,herein a new hydrophobic SERS strategy has been attempted.By comprehensively designing and researching a SERS-active structure of superhydrophobic ZnO/Ag nanowires,we demonstrate that hydrophobicity can not only draw analytes from water onto substrate,but also adjust"hottest spot"from the bottom of the nanowires to the top.As a result,the structure can simultaneously concentrate the dispersed molecules in water and the enhanced electric field in structure into a same zone,while perfecting its own anti-interference ability.The underwater in situ analytical enhancement factor of this platform is as high as 1.67×10^(11),and the operando limited of detection for metronidazole(MNZ)reaches to 10^(-9)M.Most importantly,we also successfully generalized this structure to various real in situ detection scenarios,including on-site detection of MNZ in corrosive urine,real-time warning of wrong dose of MNZ during intravenous therapy,in situ monitoring of MNZ in flowing wastewater with particulate interference,etc.,demonstrating the great application potential of this hydrophobic platform.This work realizes a synergistic promotion for in situ SERS performance under aqueous environment,and also provides a novel view for improving other in situ analytical techniques.展开更多
In conventional isochronous mass spectrometry(IMS)performed on a storage ring,the precision of mass measurements for short-lived nuclei depends on the accurate determination of the revolution times(T)of stored ions.Ho...In conventional isochronous mass spectrometry(IMS)performed on a storage ring,the precision of mass measurements for short-lived nuclei depends on the accurate determination of the revolution times(T)of stored ions.However,the resolution of T inevitably deteriorates due to the magnetic rigidity spread of the ions,limiting the mass-resolving power.In this study,we used the betatron tunes Q(the number of betatron oscillations per revolution)of the ions and established a correlation between T and Q.From this correlation,T was transformed to correspond to a fixed Q with higher resolution.Using these transformed T values,the masses of ^(63)Ge,^(65)As,^(67)Se,and ^(71)Kr agreed well with the mass values measured using the newly developed IMS(Bρ-IMS).We also studied the systematics of Coulomb displacement energies(CDEs)and found that anomalous staggering in CDEs was eliminated using new mass values.This method of T transformation is highly effective for conventional IMS equipped with a single time-of-flight detector.展开更多
文摘Methanol oxidation reaction (MOR) at Pt and Pt electrode surface deposited with various amounts of Ru (denoted as PtxRuy, nominal coverage y is 0.17, 0.27, and 0.44 ML) in 0.1 mol/L HClO4+0.5 mol/L MeOH has been studied under potentiostatic conditions by in situ FTIR spectroscopy in attenuated-total-reflection con guration and di erential electro-chemical mass spectrometry under controlled flow conditions. Results reveal that (i) CO is the only methanol-related adsorbate observed by IR spectroscopy at all the Pt and PtRu electrodes examined at potentials from 0.3 V to 0.6 V (vs. RHE); (ii) at Pt0.56Ru0.44, two IR bands, one from CO adsorbed at Ru islands and the other from COL at Pt substrate are detected, while at other electrodes, only a single band for COL adsorbed at Pt is observed; (iii) MOR activity decreases in the order of Pt0.73Ru0.27〉Pt0.56Ru0.44〉Pt0.83Ru0.17〉Pt; (iv) at 0.5 V, MOR at Pt0.73Ru0.27 reaches a current e ciency of 50% for CO2 production, the turn-over frequency from CH3OH to CO2 is ca. 0.1 molecule/(site sec). Suggestions for further improving of PtRu catalysts for MOR are provided.
基金funded by the National Natural Science Foundation of China(No.51873004).
文摘Materials exhibiting high-performance electromagnetic wave absorption have garnered considerable scientific and technological attention,yet encounter significant challenges.Developing new materials and innovative structural design concepts is crucial for expanding the application field of electromagnetic wave absorption.Particularly,hierarchical structure engineering has emerged as a promising approach to enhance the physical and chemical properties of materials,providing immense potential for creating versatile electromagnetic wave absorption materials.Herein,an exceptional multi-dimensional hierarchical structure was meticulously devised,unleashing the full microwave attenuation capabilities through in situ growth,selfreduction,and multi-heterogeneous interface integration.The hierarchical structure features a three-dimensional carbon framework,where magnetic nanoparticles grow in situ on the carbon skeleton,creating a necklace-like structure.Furthermore,magnetic nanosheets assemble within this framework.Enhanced impedance matching was achieved by precisely adjusting component proportions,and intelligent integration of diverse interfaces bolstered dielectric polarization.The obtain Fe_(3)O_(4)-Fe nanoparticles/carbon nanofibers/Al-Fe_(3)O_(4)-Fe nanosheets composites demonstrated outstanding performance with a minimum reflection loss(RLmin)value of−59.3 dB and an effective absorption bandwidth(RL≤−10 dB)extending up to 5.6 GHz at 2.2 mm.These notable accomplishments offer fresh insights into the precision design of high-efficient electromagnetic wave absorption materials.
基金The National Natural Science Foundation of China(Grant Nos.52072114 and 51922008)the 111 Project(Grant No.D17007),the Henan Center for Outstanding Overseas Scientists(Grant No.GZS2018003)+2 种基金Xinxiang Major Science and Technology Projects(Grant No.21ZD001)Guangdong Innovative and Entrepreneurial Research Team Program(2016ZT06N500)Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(2018B030322001)all provided financial support for this work.
文摘Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will benefit their quick transition to the next catalysts.Herein,Mo-doped CoOOH was designed as a high-performance model electrocatalyst with durability for 20 h at 10 mAcm−2.Additionally,it had an overpotential of 260 mV(glassy carbon)or 215 mV(nickel foam),which was 78 mV lower than that of IrO_(2)(338 mV).In situ,Raman spectroscopy revealed the transformation process of CoOOH.Calculations using the density functional theory showed that during OER,doped Mo increased the spin-up density of states and shrank the spin-down bandgap of the 3d orbits in the reconstructed CoOOH under the electrochemical activation process,which simultaneously optimized the adsorption and electron conduction of oxygen-related intermediates on Co sites and lowered the OER overpotentials.Our research provides new insights into the methodical planning of the creation of transition-metal oxyhydroxide OER catalysts.
文摘Direct analysis of copper-base alloys using laser ablation techniques is an increasingly common procedure in cultural heritage studies. However, main discussions remain focused on the possibility of using non-matrix matched external reference materials. To evaluate the occurrence of matrix effects during in situ microanalysis of copper-base materials, using near infrared femtosecond laser ablation techniques (NIR fs-LA-ICP-MS), two bronzes, i.e., (Sn-Zn)-ternary and (Sn)-binary copper-matrix reference materials, as well as a reference synthetic glass (NIST-SRM-610) have been analyzed. The results have been compared to data obtained on a sulfide-matrix reference material. Similar values in relative sensitivity averages of 63Cu, 118Sn and 66Zn, as well as in 118Sn/63Cu and 66Zn/63Cu ratios were obtained, for all analyzed matrix types, i.e., copper-base-, silicate-, and sulfide-reference materials. Consequently, it is possible to determinate major and minor element concentrations in copper alloys, i.e., Cu, Sn and Zn, using silicate and sulfide reference materials as external calibrators, without any matrix effect and over a wide range of concentrations (from wt.% to ppm). Equally, Cu, Sn and Zn concentrations can be precisely determined in sulfides using homogeneous alloys (reference) materials as an external calibrator. Thus, it is possible to determine Cu, Sn and Zn in copper-base materials and their ore minerals, mostly sulfides, in a single analytical session, without requiring specific external calibrators for each matrix type. In contrast, immiscible elements in copper matrix, such as Pb and Fe show notable differences in their relative sensitivity values and ratios for different matrix-materials analyzed, implying that matrix-matched external calibrations remain to be applied for their trace quantification.
基金supported by the Science Fund for National Defense Distinguished Young Scholars(2022-JCJQ-ZQ-016)the Key Basic Research Projects of the Foundation Strengthening Plan(2022-JCJQZD-096-00)+2 种基金the National Key Research and Development Program of China(2022YFA1104604)the National Natural Science Foundation of China(32000969)the Key Support Program for Growth Factor Research(SZYZ-TR-03).
文摘Dear Editor,Three dimensional(3D)bioprinted extracellular matrix(ECM)can be used to provide both biochemical and biophysical cues to direct mesenchymal stem cells(MSCs)differentiation,and then differentiated cells were isolated for implantation in vivo using surgical procedures.However,the reduced cell activity after cell isolation from 3D constructs and low cell retention in injured sites limit its application[1].Methacrylated gelatin(GelMA)hydrogel has the advantage of fast crosslinking,which could resemble complex architectures of tissue construct in vivo[2].Here,we adopted a noninvasive bioprinting procedure to imitate the regenerative microenvironment that could simultaneously direct the sweat gland(SG)and vascular differentiation from MSCs and ultimately promote the replacement of glandular tissue in situ(Fig.1a).
基金financially supported by the National Key Research and Development Program of China(Grant No.2021YFC2901903)the Geological Comprehensive Research Project of China’s Metallurgical Geology Bureau(Grant No.[2022]CMGBDZYJ005),the National Natural Science Foundation of China(Grant No.42002097)the Geological Investigation Project(Grant Nos.DD20230031,DD20221690,DD20230049,DD20230337).
文摘The Nuri deposit is the only Cu-W-Mo polymetallic deposit with large-scale WO3 resources in the eastern section of the Gangdese metallogenic belt,Tibet,China.However,the genetic type of this deposit has been controversial since its discovery.Based on a study of the geological characteristics of the deposit,this study presents mineralization stages,focusing on the oxide stage and the quartz-sulfide stage where scheelite is mainly formed,referred to as Sch-A and Sch-B,respectively.Through LA-ICP-MS trace element and Sr isotope analyses,the origin,evolutionary process of the oreforming fluid and genesis of the ore deposit are investigated.Scanning Electron Microscope-Cathodoluminescence(SEMCL)observations reveal that Sch-A consists of three generations,with dark gray homogenous Sch-A1 being replaced by relatively lighter and homogeneous Sch-A2 and Sch-A3,with Sch-A2 displaying a gray CL image color with vague and uneven growth bands and Sch-A3 has a light gray CL image color with hardly any growth band.In contrast,Sch-B exhibits a‘core-rim’structure,with the core part(Sch-B1)being dark gray and displaying a uniform growth band,while the rim part(Sch-B2)is light gray and homogeneous.The normalized distribution pattern of rare earth elements in scheelite and Sr isotope data suggest that the early ore-forming fluid in the Nuri deposit originated from granodiorite porphyry and,later on,some country rock material was mixed in,due to strong water-rock interaction.Combining the O-H isotope data further indicates that the ore-forming fluid in the Nuri deposit originated from magmatic-hydrothermal sources,with contributions from metamorphic water caused by water-rock interaction during the mineralization process,as well as later meteoric water.The intense water-rock interaction likely played a crucial role in the precipitation of scheelite,leading to varying Eu anomalies in different generations of scheelite from the oxide stage to the quartz-sulfide stage,while also causing a gradual decrease in oxygen fugacity(fO2)and a slow rise in pH value.Additionally,the high Mo and low Sr contents in the scheelite are consistent with typical characteristics of magmatic-hydrothermal scheelite.Therefore,considering the geological features of the deposit,the geochemical characteristics of scheelite and the O-H isotope data published previously,it can be concluded that the genesis of the Nuri deposit belongs to porphyry-skarn deposit.
基金supported by the National Natural Science Foundation of China(Nos.12125509,12222514,11961141003,and 12005304)National Key Research and Development Project(No.2022YFA1602301)+1 种基金CAST Young Talent Support Planthe CNNC Science Fund for Talented Young Scholars Continuous support for basic scientific research projects。
文摘The Moon provides a unique environment for investigating nearby astrophysical events such as supernovae.Lunar samples retain valuable information from these events,via detectable long-lived“fingerprint”radionuclides such as^(60)Fe.In this work,we stepped up the development of an accelerator mass spectrometry(AMS)method for detecting^(60)Fe using the HI-13tandem accelerator at the China Institute of Atomic Energy(CIAE).Since interferences could not be sufficiently removed solely with the existing magnetic systems of the tandem accelerator and the following Q3D magnetic spectrograph,a Wien filter with a maximum voltage of±60 kV and a maximum magnetic field of 0.3 T was installed after the accelerator magnetic systems to lower the detection background for the low abundance nuclide^(60)Fe.A 1μm thick Si_(3)N_(4) foil was installed in front of the Q3D as an energy degrader.For particle detection,a multi-anode gas ionization chamber was mounted at the center of the focal plane of the spectrograph.Finally,an^(60)Fe sample with an abundance of 1.125×10^(-10)was used to test the new AMS system.These results indicate that^(60)Fe can be clearly distinguished from the isobar^(60)Ni.The sensitivity was assessed to be better than 4.3×10^(-14)based on blank sample measurements lasting 5.8 h,and the sensitivity could,in principle,be expected to be approximately 2.5×10^(-15)when the data were accumulated for 100 h,which is feasible for future lunar sample measurements because the main contaminants were sufficiently separated.
基金supported by the National Key R&D Program of China(Grant No.2021YFB2206503)National Natural Science Foundation of China(Grant No.62274159)+1 种基金CAS Project for Young Scientists in Basic Research(Grant No.YSBR-056)the“Strategic Priority Research Program”of the Chinese Academy of Sciences(Grant No.XDB43010102).
文摘Ex situ characterization techniques in molecular beam epitaxy(MBE)have inherent limitations,such as being prone to sample contamination and unstable surfaces during sample transfer from the MBE chamber.In recent years,the need for improved accuracy and reliability in measurement has driven the increasing adoption of in situ characterization techniques.These techniques,such as reflection high-energy electron diffraction,scanning tunneling microscopy,and X-ray photoelectron spectroscopy,allow direct observation of film growth processes in real time without exposing the sample to air,hence offering insights into the growth mechanisms of epitaxial films with controlled properties.By combining multiple in situ characterization techniques with MBE,researchers can better understand film growth processes,realizing novel materials with customized properties and extensive applications.This review aims to overview the benefits and achievements of in situ characterization techniques in MBE and their applications for material science research.In addition,through further analysis of these techniques regarding their challenges and potential solutions,particularly highlighting the assistance of machine learning to correlate in situ characterization with other material information,we hope to provide a guideline for future efforts in the development of novel monitoring and control schemes for MBE growth processes with improved material properties.
基金supported in part by the High Performance Computing Center of Central South Universitythe financial support from the Government of Chongzuo,Guangxi Zhuang Autonomous Region(Fund No.FA2020011FA20210713)
文摘LiNi_(x)Co_(y)Al_(z)O_(2)(NCA)cathode materials are drawing widespread attention,but the huge gap between the ideal and present cyclic stability still hinders their further commercial application,especially for the Ni-rich LiNi_(x)Co_(y)Al_(z)O_(2)(x>0.8,x+y+z=1)cathode material,which is owing to the structural degradation and particles'intrinsic fracture.To tackle the problems,Li_(0.5)La_(2)Al_(0.5)O_(4)in situ coated and Mn compensating doped multilayer LiNi_(0.82)Co_(0.14)Al_(0.04)O_(2)was prepared.XRD refinement indicates that La-Mn co-modifying could realize appropriate Li/Ni disorder degree.Calculated results and in situ XRD patterns reveal that the LLAO coating layer could effectively restrain crack in secondary particles benefited from the suppressed internal strain.AFM further improves as NCA-LM2 has superior mechanical property.The SEM,TEM,XPS tests indicate that the cycled cathode with LLAO-Mn modification displays a more complete morphology and less side reaction with electrolyte.DEMS was used to further investigate cathode-electrolyte interface which was reflected by gas evolution.NCA-LM2 releases less CO_(2)than NCA-P indexing on a more stable surface.The modified material presents outstanding capacity retention of 96.2%after 100 cycles in the voltage range of 3.0-4.4 V at 1C,13%higher than that of the pristine and 80.8%at 1 C after 300 cycles.This excellent electrochemical performance could be attributed to the fact that the high chemically stable coating layer of Li_(0.5)La_(2)Al_(0.5)O_(4)(LLAO)could enhance the interface and the Mn doping layer could suppress the influence of the lattice mismatch and distortion.We believe that it can be a useful strategy for the modification of Ni-rich cathode material and other advanced functional material.
文摘The reaction mechanism for alkylation of benzene with propylene over the β zeolite and the MCM-22 zeolite were investigated respectively by in-situ IR spectrometry. Three types of experiments were carried out. (1) IR spectra of the gas-phase propylene, benzene and isopropyl benzene were recorded. (2) IR spectra of the above-mentioned substances as adsorbates that have combined with the zeolite wafer were recorded. (3) IR spectra of the reaction modes were recorded. The test results showed that the alkytation reaction over the zeolite β was ascribed to the mechanism of carbonium ions, whereas the alkylation reaction over the zeolite MCM-22 was ascribed to the synchronous reaction mechanism.
基金supported by the National Natural Science Foundation of China(42241109)the Guoqiang Institute,Tsinghua University(2021GQG1001)the New Cornerstone Science Foundation through the XPLORER PRIZE.
文摘Lunar habitat construction is crucial for successful lunar exploration missions.Due to the limitations of transportation conditions,extensive global research has been conducted on lunar in situ material processing techniques in recent years.The aim of this paper is to provide a comprehensive review,precise classification,and quantitative evaluation of these approaches,focusing specifically on four main approaches:reaction solidification(RS),sintering/melting(SM),bonding solidification(BS),and confinement formation(CF).Eight key indicators have been identified for the construction of low-cost and highperformance systems to assess the feasibility of these methods:in situ material ratio,curing temperature,curing time,implementation conditions,compressive strength,tensile strength,curing dimensions,and environmental adaptability.The scoring thresholds are determined by comparing the construction requirements with the actual capabilities.Among the evaluated methods,regolith bagging has emerged as a promising option due to its high in situ material ratio,low time requirement,lack of hightemperature requirements,and minimal shortcomings,with only the compressive strength falling below the neutral score.The compressive strength still maintains a value of 2–3 MPa.The proposed construction scheme utilizing regolith bags offers numerous advantages,including rapid and large-scale construction,ensured tensile strength,and reduced reliance on equipment and energy.In this study,guidelines for evaluating regolith solidification techniques are provided,and directions for improvement are offered.The proposed lunar habitat design based on regolith bags is a practical reference for future research.
基金funded by the Australian Coal Industry’s Research Program(ACARP,Grant No.C26063).
文摘This study aims to investigate the feasibility of deriving in situ horizontal stresses from the breakout width and depth using the analytical method.Twenty-three breakout data with different borehole sizes were collected and three failure criteria were studied.Based on the Kirsch equations,relatively accurate major horizontal stress(sH)estimations from known minor horizontal stress(sh)were achieved with percentage errors ranging from 0.33%to 44.08%using the breakout width.The Mogi-Coulomb failure criterion(average error:13.1%)outperformed modified Wiebols-Cook(average error:19.09%)and modified Lade(average error:18.09%)failure criteria.However,none of the tested constitutive models could yield reasonable sh predictions from known sH using the same approach due to the analytical expression of the redistributed stress and the nature of the constitutive models.In consideration of this issue,the horizontal stress ratio(sH/sh)is suggested as an alternative input,which could estimate both sH and sh with the same level of accuracy.Moreover,the estimation accuracies for both large-scale and laboratory-scale breakouts are comparable,suggesting the applicability of this approach across different breakout sizes.For breakout depth,conformal mapping and complex variable method were used to calculate the stress concentration around the breakout tip,allowing the expression of redistributed stresses using binomials composed of sH and sh.Nevertheless,analysis of the breakout depth stabilisation mechanism indicates that additional parameters are required to utilise normalised breakout depth for stress estimation compared to breakout width.These parameters are challenging to obtain,especially under field conditions,meaning utilising normalised breakout depth analytically in practical applications faces significant challenges and remains infeasible at this stage.Nonetheless,the normalised breakout depth should still be considered a critical input for any empirical and statistical stress estimation method given its significant correlation with horizontal stresses.The outcome of this paper is expected to contribute valuable insights into the breakout stabilisation mechanisms and estimation of in situ stress magnitudes based on borehole breakout geometries.
文摘The current study comprehensively evaluates four different protein extraction methods based on urea,sodium dodecyl sulfate(SDS),anionic surfactants(BT),and total RNA extractor(Trizol),aiming to optimize the sample preparation workflow for mass spectrometry-based proteomics.Using HeLa cells as an example,we found that the method employing the mass spectrometry-compatible surfactant BT reagent significantly reduces the total time consumed for protein extraction and minimizes protein losses during the sample preparation process.Further integrating the four protein extraction methods,we identified over 7000 proteins from HeLa cells without relying on pre-fractionation techniques,and 2990 of them were quantified using label-free quantification.It is worth noting that the BT and SDS methods demonstrate higher efficiency in extracting membrane proteins,while the Urea and Trizol methods are more effective in extracting proteins from nuclear and cytoplasmic fractions.In summary,this study provides a novel solution for deep proteome coverage,particularly in the context of cellular protein extraction,by integrating mass spectrometry-compatible surfactants with traditional extraction methods to effectively enhance protein identification numbers.
文摘Profiling the protein composition of bacteria is essential for understanding their biology,physiology and interaction with environment.Mass spectrometry has become a pivotal tool for protein analysis,facilitating the examination of expression levels,molecular masses and structural modifications.In this study,we compared the performance of three widely-used mass spectrometry methods,i.e.,matrix-assisted laser desorption/ionization(MALDI)protein fingerprinting,top-down proteomics and bottom-up proteomics,in the profiling of bacterial protein composition.It was revealed that bottom-up proteomics provided the highest protein coverage and exhibited the greatest protein profile overlap between bacterial species.In contrast,MALDI protein fingerprinting demonstrated superior detection reproducibility and effectiveness in distinguishing between bacterial species.Although top-down proteomics identified fewer proteins than bottom-up approach,it complemented MALDI fingerprinting in the discovery of bacterial protein markers,both favoring abundant,stable,and hydrophilic bacterial ribosomal proteins.This study represents the most systematic and comprehensive comparison of mass spectrometry-based protein profiling methodologies to date.It provides valuable guidelines for the selection of appropriate profiling strategies for specific analytical purposes.This will facilitate studies across various fields,including infection diagnosis,antimicrobial resistance detection and pharmaceutical target discovery.
基金supported in part by JSPS KAKENHI grants (nos. JP21K05243 and JP22H04621grants-in-aid for Scientific Research on Innovative Areas “Interface Ionics”)+1 种基金by a JST grant (no. JPMJFS2132,for the establishment of university fellowships toward the creation of science technology innovation)by the Suzuki foundation
文摘MgH_(2) and TiH_(2) have been extensively studied as potential anode materials due to their high theoretical specific capacities of 2036 and 1024 mAh/g,respectively.However,the large volume changes that these compounds undergo during cycling affects their performance and limits practical applications.The present work demonstrates a novel approach to limiting the volume changes of active materials.This effect is based on mechanical support from an intimate interface generated in situ via the reaction between MgH_(2) and Ti within the electrode prior to lithiation to form Mg and TiH_(2).The resulting Mg can be transformed back to MgH_(2) by reaction with LiH during delithiation.In addition,the TiH_(2) improves the reaction kinetics of MgH_(2) and enhances electrochemical performance.The intimate interface produced in this manner is found to improve the electrochemical properties of a MgH_(2)-Ti-LiH electrode.An exceptional reversible capacity of 800 mAh/g is observed even after 200 cycles with a high current density of 1 mA/cm^(2) and a high proportion of active material(90 wt.%)at an operation temperature of 120℃.This study therefore showcases a new means of improving the performance of electrodes by limiting the volume changes of active materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.12304033,12072328,and 11991073).
文摘Phase transition of polycrystalline iron compressed along the Hugoniot is studied by combining laser-driven shock with in situ x-ray diffraction technique.It is suggested that polycrystalline iron changes from an initial body-centered cubic structure to a hexagonal close-packed structure with increasing pressure(i.e.,a phase transition fromαtoε).The relationship between density and pressure for polycrystalline iron obtained from the present experiments is found to be in good agreement with the gas-gun Hugoniot data.Our results show that experiments with samples at lower temperatures under static loading,such as in a diamond anvil cell,lead to higher densities measured than those found under dynamic loading.This means that extrapolating results of static experiments may not predict the dynamic responses of materials accurately.In addition,neither the face-centered cubic structure seen in previous molecular-dynamics simulations or twophase coexistence are found within our experimental pressure range.
基金the National Key Research and Development Program of China(2019YFA0705400)the National Natural Science Foundation of China(T2293692,21925404,22021001,21991151,and 22002036)+1 种基金the Natural Science Foundation of Fujian Province of China(2021J06001)the National Natural Science Foundation of Henan province(232300421081).
文摘Interfacial water molecules are the most important participants in the hydrogen evolution reaction(HER).Hence,understanding the behavior and role that interfacial water plays will ultimately reveal the HER mechanism.Unfortunately,investigating interfacial water is extremely challenging owing to the interference caused by bulk water molecules and complexity of the interfacial environment.Here,the behaviors of interfacial water in different cationic electrolytes on Pd surfaces were investigated by the electrochemistry,in situ core-shell nanostructure enhanced Raman spectroscopy and theoretical simulation techniques.Direct spectral evidence reveals a red shift in the frequency and a decrease in the intensity of interfacial water as the potential is shifted in the positively direction.When comparing the different cation electrolyte systems at a given potential,the frequency of the interfacial water peak increases in the specified order:Li+<Na^(+)<K^(+)<Ca^(2+)<Sr^(2+).The structure of interfacial water was optimized by adjusting the radius,valence,and concentration of cation to form the two-H down structure.This unique interfacial water structure will improve the charge transfer efficiency between the water and electrode further enhancing the HER performance.Therefore,local cation tuning strategies can be used to improve the HER performance by optimizing the interfacial water structure.
基金funded by the Institutional Research Fund from Sichuan University(No.2020SCUNL211)。
文摘To prolong the service life of optics,the feasibility of in situ cleaning of the multilayer mirror(MLM)of tin and its oxidized contamination was investigated using hydrogen plasma at different power levels.Granular tin-based contamination consisting of micro-and macroparticles was deposited on silicon via physical vapor deposition(PVD).The electrodedriven hydrogen plasma at different power levels was systematically diagnosed using a Langmuir probe and a retarding field ion energy analyzer(RFEA).Moreover,the magnitude of the self-biasing voltage was measured at different power levels,and the peak ion energy was corrected for the difference between the RFEA measurements and the self-biasing voltage(E_(RFEA)-eV_(self)).XPS analysis of O 1s and Sn 3d peaks demonstrated the chemical reduction process after 1 W cleaning.Analysis of surface and cross-section morphology revealed that holes emerged on the upper part of the macroparticles while its bottom remained smooth.Hills and folds appeared on the upper part of the microparticles,confirming the top-down cleaning mode with hydrogen plasma.This study provides an in situ electrode-driven hydrogen plasma etching process for tin-based contamination and will provide meaningful guidance for understanding the chemical mechanism of reduction and etching.
基金the National Natural Science Foundation of China(No.11974222 and 11904214)the Natural Science Foundation of Shandong Province(No.ZR2020KA004 and ZR2019YQ09)for financial support
文摘In situ surface-enhanced Raman scattering(SERS)is a widely used operando analytical technique,while facing numerous complex factors in applications under aqueous environment,such as low detection sensitivity,poor anti-interference capability,etc.,resulting in unreliable detectability.To address these issues,herein a new hydrophobic SERS strategy has been attempted.By comprehensively designing and researching a SERS-active structure of superhydrophobic ZnO/Ag nanowires,we demonstrate that hydrophobicity can not only draw analytes from water onto substrate,but also adjust"hottest spot"from the bottom of the nanowires to the top.As a result,the structure can simultaneously concentrate the dispersed molecules in water and the enhanced electric field in structure into a same zone,while perfecting its own anti-interference ability.The underwater in situ analytical enhancement factor of this platform is as high as 1.67×10^(11),and the operando limited of detection for metronidazole(MNZ)reaches to 10^(-9)M.Most importantly,we also successfully generalized this structure to various real in situ detection scenarios,including on-site detection of MNZ in corrosive urine,real-time warning of wrong dose of MNZ during intravenous therapy,in situ monitoring of MNZ in flowing wastewater with particulate interference,etc.,demonstrating the great application potential of this hydrophobic platform.This work realizes a synergistic promotion for in situ SERS performance under aqueous environment,and also provides a novel view for improving other in situ analytical techniques.
基金supported in part by the National Key R&D Program of China (No. 2023YFA1606401)CAS Project for Young Scientists in Basic Research (No. YSBR-002)+3 种基金Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB34000000)the NSFC (Nos. 12305126, 12135017, 12121005)the support from the Youth Innovation Promotion Association of the Chinese Academy of Sciences (No. 2021419)the support from the Yong Scholar of Regional Development,CAS (No.[2023]15)
文摘In conventional isochronous mass spectrometry(IMS)performed on a storage ring,the precision of mass measurements for short-lived nuclei depends on the accurate determination of the revolution times(T)of stored ions.However,the resolution of T inevitably deteriorates due to the magnetic rigidity spread of the ions,limiting the mass-resolving power.In this study,we used the betatron tunes Q(the number of betatron oscillations per revolution)of the ions and established a correlation between T and Q.From this correlation,T was transformed to correspond to a fixed Q with higher resolution.Using these transformed T values,the masses of ^(63)Ge,^(65)As,^(67)Se,and ^(71)Kr agreed well with the mass values measured using the newly developed IMS(Bρ-IMS).We also studied the systematics of Coulomb displacement energies(CDEs)and found that anomalous staggering in CDEs was eliminated using new mass values.This method of T transformation is highly effective for conventional IMS equipped with a single time-of-flight detector.