Lithium metal batteries have been considered as one of the most promising next-generation power-support devices due to their high specific energy and output voltage.However,the uncontrollable side-reaction and lithium...Lithium metal batteries have been considered as one of the most promising next-generation power-support devices due to their high specific energy and output voltage.However,the uncontrollable side-reaction and lithium dendrite growth lead to the limited serving life and hinder the practical application of lithium metal batteries.Here,a tri-monomer copolymerized gel polymer electrolyte(TGPE)with a cross-linked reticulation structure was prepared by introducing a cross-linker(polyurethane group)into the acrylate-based in situ polymerization system.The soft segment of polyurethane in TGPE enables the far migration of lithium ions,and the-NH forms hydrogen bonds in the hard segment to build a stable cross-linked framework.This system hinders anion migration and leads to a high Li^(+)migration number(t_(Li^(+))=0.65),which achieves uniform lithium deposition and effectively inhibits lithium dendrite growth.As a result,the assembled symmetric cell shows robust reversibility over 5500 h at a current density of 1 mA cm^(-2).The LFP∷TGPE∷Li cell has a capacity retention of 89.8%after cycling 800 times at a rate of 1C.In summary,in situ polymerization of TGPE electrolytes is expected to be a candidate material for high-energy-density lithium metal batteries.展开更多
Lithium-metal anodes(LMAs)have been recognized as the ultimate anodes for next-generation batteries with high energy density,but stringent assembly-environment conditions derived from the poor moisture stability drama...Lithium-metal anodes(LMAs)have been recognized as the ultimate anodes for next-generation batteries with high energy density,but stringent assembly-environment conditions derived from the poor moisture stability dramatically hinder the transformation of LMAs from laboratory to industry.Herein,an in situ formed cross-linked polymer layer on LMAs is designed and constructed by a facile thiol-acrylate click chemistry reaction between poly(ethylene glycol)diacrylate(PEGDA)and the crosslinker containing multi thiol groups under UV irradiation.Owing to the hydrophobic nature of the layer,the treated LMAs demonstrate remarkable humid stability for more than 3 h in ambient air(70%relative humidity).The coating humid-resistant protective layer also possesses a dual-functional characterization as solid polymer electrolytes by introducing lithium bis(trifluoromethanesulfonyl)imide in the system in advance.The intimate contact between the polymer layer and LMAs reduces interfacial resistance in the assembled Li/LiFePO_(4)or Li/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)full cell effectively,and endows the cell with an outstanding cycle performance.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
High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)M...High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.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
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
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
In situ direct reprogramming technology can directly convert endogenous glial cells into functional neurons in vivo for central nervous system repair. Polypyrimidine tract-binding protein 1(PTB) knockdown has been sho...In situ direct reprogramming technology can directly convert endogenous glial cells into functional neurons in vivo for central nervous system repair. Polypyrimidine tract-binding protein 1(PTB) knockdown has been shown to reprogram astrocytes to functional neurons in situ. In this study, we used AAV-PHP.e B-GFAP-sh PTB to knockdown PTB in a mouse model of ischemic stroke induced by endothelin-1, and investigated the effects of GFAP-sh PTB-mediated direct reprogramming to neurons. Our results showed that in the mouse model of ischemic stroke, PTB knockdown effectively reprogrammed GFAP-positive cells to neurons in ischemic foci, restored neural tissue structure, reduced inflammatory response, and improved behavioral function. These findings validate the effectiveness of in situ transdifferentiation of astrocytes, and suggest that the approach may be a promising strategy for stroke treatment.展开更多
AIM:To observe the effects of femtosecond laserassisted excimer laser in situ keratomileusis combined with accelerated corneal cross-linking(FS-LASIK Xtra)on corneal densitometry after correcting for high myopia.METHO...AIM:To observe the effects of femtosecond laserassisted excimer laser in situ keratomileusis combined with accelerated corneal cross-linking(FS-LASIK Xtra)on corneal densitometry after correcting for high myopia.METHODS:In this prospectively study,130 patients underwent FS-LASIK or FS-LASIK Xtra for high myopia.Their right eyes were selected for inclusion in the study,of which 65 cases of 65 eyes in the FS-LASIK group,65 patients with 65 eyes in the FS-LASIK Xtra group.Patients were evaluated for corneal densitometry at 1,3,and 6mo postoperatively using Pentacam Scheimpflug imaging.RESULTS:Preoperative differences in corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups in different ranges were not statistically significant(P>0.05).Layer-by-layer analysis revealed statistically significant differences in the anterior(120μm),central,and total layer corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups at 1 and 3mo postoperatively(all P<0.05),the FS-LASIK Xtra group is higher than that of the FS-LASIK group.Analysis of different diameter ranges showed statistically significant differences between the FS-LASIK group and the FS-LASIK Xtra group at 1mo postoperatively in the ranges of 0–2,2–6,and 6–10 mm(both P<0.05);At 3mo postoperatively,the FS-LASIK Xtra group is higher than that of the FS-LASIK group in the ranges of 0–2 and 2–6 mm(P<0.05).At 6mo postoperatively,there were no statistically significant differences in corneal densitometry between the FS-LASIK group and the FS-LASIK Xtra group in different diameter ranges(all P>0.05).CONCLUSION:There is an increase in internal corneal densitometry during the early postoperative period after FS-LASIK Xtra for correction of high myopia.However,the densitometry values decreased to the level of conventional FS-LASIK at 6mo after surgery,with the most significant changes observed in the superficial central zone.展开更多
Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked pol...Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.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
In various industries,particularly in the chemical and pharmaceutical fields,Fourier transform infrared spectroscopy(FTIR)spectroscopy provides a unique capacity to detect and characterise complex chemicals while mini...In various industries,particularly in the chemical and pharmaceutical fields,Fourier transform infrared spectroscopy(FTIR)spectroscopy provides a unique capacity to detect and characterise complex chemicals while minimising environmental damage by minimal waste generation and reducing the need for extensive sample preparation or use of harmful reagents.This review showcases the versatility of ex situ and in situ FTIR applications for substance identification,analysis,and dynamic monitoring.Ex situ FTIR spectroscopy’s accuracy in identifying impurities,monitoring crystallisation processes,and regulating medication release patterns improves product quality,safety,and efficacy.Furthermore,its quantification capabilities enable more effective drug development,dosage procedures,and quality control practices,all of which are consistent with green analytical principles.On the other hand,in situ FTIR spectroscopy appears to be a novel tool for the real-time investigation of molecular changes during reactions and processes,allowing for the monitoring of drug release kinetics,crystallisation dynamics,and surface contacts,as well as providing vital insights into material behaviour.The combination of ex situ FTIR precision and in situ FTIR dynamic capabilities gives a comprehensive analytical framework for developing green practices,quality control,and innovation in the chemical and pharmaceutical industries.This review presents the wide range of applications of ex situ and in situ FTIR spectroscopy in chemical,pharmaceutical and medical fields as an analytical green chemistry tool.However,further study is required to fully realise FTIR’s potential and develop new applications that improve sustainability in these areas.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
Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium ...Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.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
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
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
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
基金support from the National Natural Science Foundation of China(52077096)
文摘Lithium metal batteries have been considered as one of the most promising next-generation power-support devices due to their high specific energy and output voltage.However,the uncontrollable side-reaction and lithium dendrite growth lead to the limited serving life and hinder the practical application of lithium metal batteries.Here,a tri-monomer copolymerized gel polymer electrolyte(TGPE)with a cross-linked reticulation structure was prepared by introducing a cross-linker(polyurethane group)into the acrylate-based in situ polymerization system.The soft segment of polyurethane in TGPE enables the far migration of lithium ions,and the-NH forms hydrogen bonds in the hard segment to build a stable cross-linked framework.This system hinders anion migration and leads to a high Li^(+)migration number(t_(Li^(+))=0.65),which achieves uniform lithium deposition and effectively inhibits lithium dendrite growth.As a result,the assembled symmetric cell shows robust reversibility over 5500 h at a current density of 1 mA cm^(-2).The LFP∷TGPE∷Li cell has a capacity retention of 89.8%after cycling 800 times at a rate of 1C.In summary,in situ polymerization of TGPE electrolytes is expected to be a candidate material for high-energy-density lithium metal batteries.
基金the Science and Technology Department of Henan Province of China(Grant No.222102240060 and 222300420541)the Education Department of Henan Province of China(Grant No.22B430023)supported by the Program for Innovative Research Team(in Science and Technology)in University of Henan Province(Grant No.23IRTSTHN009)。
文摘Lithium-metal anodes(LMAs)have been recognized as the ultimate anodes for next-generation batteries with high energy density,but stringent assembly-environment conditions derived from the poor moisture stability dramatically hinder the transformation of LMAs from laboratory to industry.Herein,an in situ formed cross-linked polymer layer on LMAs is designed and constructed by a facile thiol-acrylate click chemistry reaction between poly(ethylene glycol)diacrylate(PEGDA)and the crosslinker containing multi thiol groups under UV irradiation.Owing to the hydrophobic nature of the layer,the treated LMAs demonstrate remarkable humid stability for more than 3 h in ambient air(70%relative humidity).The coating humid-resistant protective layer also possesses a dual-functional characterization as solid polymer electrolytes by introducing lithium bis(trifluoromethanesulfonyl)imide in the system in advance.The intimate contact between the polymer layer and LMAs reduces interfacial resistance in the assembled Li/LiFePO_(4)or Li/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)full cell effectively,and endows the cell with an outstanding cycle performance.
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supported by the National Natural Science Foundation of China(52162030)the Yunnan Major Scientific and Technological Projects(202202AG050003)+4 种基金the Key Research and Development Program of Yunnan Province(202103AA080019)the Scientific Research Foundation of Kunming University of Science and Technology(20220122)the Graduate Student Top Innovative Talent Program of Kunming University of Science and Technology(CA23107M139A)the Analysis and Testing Foundation of Kunming University of Science and Technology(2023T20220122)the Shenzhen Science and Technology Program(KCXST20221021111201003)。
文摘High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.
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.
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 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.
基金supported by the National Natural Science Foundation of China,No.82071418the Natural Science Foundation of Fujian Province,No.2020J01612 (both to EH)。
文摘In situ direct reprogramming technology can directly convert endogenous glial cells into functional neurons in vivo for central nervous system repair. Polypyrimidine tract-binding protein 1(PTB) knockdown has been shown to reprogram astrocytes to functional neurons in situ. In this study, we used AAV-PHP.e B-GFAP-sh PTB to knockdown PTB in a mouse model of ischemic stroke induced by endothelin-1, and investigated the effects of GFAP-sh PTB-mediated direct reprogramming to neurons. Our results showed that in the mouse model of ischemic stroke, PTB knockdown effectively reprogrammed GFAP-positive cells to neurons in ischemic foci, restored neural tissue structure, reduced inflammatory response, and improved behavioral function. These findings validate the effectiveness of in situ transdifferentiation of astrocytes, and suggest that the approach may be a promising strategy for stroke treatment.
基金Supported by Shandong Province Medical Staff Science and Technology Innovation Program Project(No.SDYWZGKCJH2022021).
文摘AIM:To observe the effects of femtosecond laserassisted excimer laser in situ keratomileusis combined with accelerated corneal cross-linking(FS-LASIK Xtra)on corneal densitometry after correcting for high myopia.METHODS:In this prospectively study,130 patients underwent FS-LASIK or FS-LASIK Xtra for high myopia.Their right eyes were selected for inclusion in the study,of which 65 cases of 65 eyes in the FS-LASIK group,65 patients with 65 eyes in the FS-LASIK Xtra group.Patients were evaluated for corneal densitometry at 1,3,and 6mo postoperatively using Pentacam Scheimpflug imaging.RESULTS:Preoperative differences in corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups in different ranges were not statistically significant(P>0.05).Layer-by-layer analysis revealed statistically significant differences in the anterior(120μm),central,and total layer corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups at 1 and 3mo postoperatively(all P<0.05),the FS-LASIK Xtra group is higher than that of the FS-LASIK group.Analysis of different diameter ranges showed statistically significant differences between the FS-LASIK group and the FS-LASIK Xtra group at 1mo postoperatively in the ranges of 0–2,2–6,and 6–10 mm(both P<0.05);At 3mo postoperatively,the FS-LASIK Xtra group is higher than that of the FS-LASIK group in the ranges of 0–2 and 2–6 mm(P<0.05).At 6mo postoperatively,there were no statistically significant differences in corneal densitometry between the FS-LASIK group and the FS-LASIK Xtra group in different diameter ranges(all P>0.05).CONCLUSION:There is an increase in internal corneal densitometry during the early postoperative period after FS-LASIK Xtra for correction of high myopia.However,the densitometry values decreased to the level of conventional FS-LASIK at 6mo after surgery,with the most significant changes observed in the superficial central zone.
基金financially supported by the National Natural Science Foundation of China(Grant No.22325405,22321002,22279153)Liaoning Revitalization Talents Program(XLYC1807207,XLYC2203134)DICP I202104。
文摘Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.
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supported by the Large Research Grant from the Doctoral School,funded by statutory funds from Poznan University of Medical Sciences,Poland(Grant No.:85/2023).
文摘In various industries,particularly in the chemical and pharmaceutical fields,Fourier transform infrared spectroscopy(FTIR)spectroscopy provides a unique capacity to detect and characterise complex chemicals while minimising environmental damage by minimal waste generation and reducing the need for extensive sample preparation or use of harmful reagents.This review showcases the versatility of ex situ and in situ FTIR applications for substance identification,analysis,and dynamic monitoring.Ex situ FTIR spectroscopy’s accuracy in identifying impurities,monitoring crystallisation processes,and regulating medication release patterns improves product quality,safety,and efficacy.Furthermore,its quantification capabilities enable more effective drug development,dosage procedures,and quality control practices,all of which are consistent with green analytical principles.On the other hand,in situ FTIR spectroscopy appears to be a novel tool for the real-time investigation of molecular changes during reactions and processes,allowing for the monitoring of drug release kinetics,crystallisation dynamics,and surface contacts,as well as providing vital insights into material behaviour.The combination of ex situ FTIR precision and in situ FTIR dynamic capabilities gives a comprehensive analytical framework for developing green practices,quality control,and innovation in the chemical and pharmaceutical industries.This review presents the wide range of applications of ex situ and in situ FTIR spectroscopy in chemical,pharmaceutical and medical fields as an analytical green chemistry tool.However,further study is required to fully realise FTIR’s potential and develop new applications that improve sustainability in these areas.
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.
基金supported by the National Key Research and Development Program of China(2022YFB4101800)National Natural Science Foundation of China(22278077,22108040)+2 种基金Key Program of Qingyuan Innovation Laboratory(00221004)Research Program of Qingyuan Innovation Laboratory(00523006)Natural Science Foundation of Fujian Province(2022J02019)。
文摘Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.
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.