The defect regulation and p-n heterojunction of composites have gained significant attention due to their potential applications.Nitrogen(N)as doping heteroatoms and perylene-3,4,9,10-tetracarboximide(PDINH)as an appr...The defect regulation and p-n heterojunction of composites have gained significant attention due to their potential applications.Nitrogen(N)as doping heteroatoms and perylene-3,4,9,10-tetracarboximide(PDINH)as an appropriate n-type semiconductor were innovatively and reasonably selected to enhance the photocatalytic performance of pristine p-type cuprous oxide(Cu_(2)O).In this study,the defect regula-tion of N doping(1)achieved the small-size effect of Cu_(2)O,(2)optimized the electron features,and(3)improved the kinetics of reactive oxygen species.The p-n heterojunction with PDINH was developed to sharply improve the light utilization of Cu_(2)O,from the UV region to the near-infrared region.As expected,the optimized Cu_(2)N_(x)O_(1–x)/PDINH(x=0.02)exhibited excellent long-term photocatalytic antibacterial ac-tivities,with antibacterial rates exceeding 91%against Staphylococcus aureus and Pseudomonas aeruginosa.Defect regulation and p-n heterojunction of Cu_(2)O-based composites thus provide a great deal of potential for future advancements in photocatalysis.展开更多
Up-and-coming high-temperature materials,refractory high entropy alloys,are suffering from lower oxidation resistance,restricting their applications in the aerospace field.In this study,two novel treatments of Al-depo...Up-and-coming high-temperature materials,refractory high entropy alloys,are suffering from lower oxidation resistance,restricting their applications in the aerospace field.In this study,two novel treatments of Al-deposited and remelted were developed to refine the microstructure and enhance the oxidation resistance of refractory high entropy alloy using electron beam freeform fabrication(EBF3).Finer and short-range ordering structures were observed in the remelted sample,whereas the Al-deposited sample showcased the formation of silicide and intermetallic phases.High-temperature cyclic and isothermal oxidation tests at 1000℃ were carried out.The total weight gain after 60 h of cyclic oxidation decreased by 17.49%and 30.46%for the remelted and deposited samples,respectively,compared to the as-cast state.Oxidation kinetics reveal an evident lower mass gain and oxidation rate in the treated samples.A multilayer oxide consisting of TiO_(2)+Al_(2)O_(3)+SiO_(2)+AlNbO_(4) was studied for its excellent oxidation resistance.The oxidation behavior of rutile,corundum and other oxides was analyzed using first principles calculations and chemical defect analysis.Overall,this research,which introduces novel treatments,offers promising insights for enhancing the inherent oxidation resistance of refractory high entropy alloys.展开更多
Nitrogen-doping of carbon support(N-C)for platinum(Pt)nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction(ORR)in proton exchange...Nitrogen-doping of carbon support(N-C)for platinum(Pt)nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells.For fundamental understanding,clearly identifying the metalsupport effect on enhancement mechanisms of ORR electrocatalysis is definitely needed.In this work,the impact of Pt-support interaction via interfacial Pt-N coordination on electrocatalytic ORR activity and stability in Pt/N-C catalyst is deeply studied through structural/compositional characterizations,electrochemical measurements and theoretical DFT-calculations/AIMD-simulations.The resulting Pt/N-C catalyst exhibits a superior electrocatalytic performance compared to the commercial Pt/C catalyst in both half-cell and H_(2)-O_(2)fuel cell.Experimental and theoretical results reveal that the interfacial Pt-N coordination enables electron transfer from N-C support to Pt nanoparticles,which can weaken the adsorption strength of oxygen intermediates on Pt surface to improve ORR activity and induce the strong Pt-support interaction to enhance electrochemical stability.展开更多
The quest for high-energy-density magnesium-air batteries is hindered by the efficiency-voltage trade-off,ultimately leading to an unsatisfactory energy density.Here,we effectively mitigate the inherent efficiency-vol...The quest for high-energy-density magnesium-air batteries is hindered by the efficiency-voltage trade-off,ultimately leading to an unsatisfactory energy density.Here,we effectively mitigate the inherent efficiency-voltage trade-off by introducing a novel anode material,specifically,Mg-0.5Sn-0.5In-0.5Ga.This anode demonstrates exceptional anodic efficiency,achieving 60.5±2.5%at 1 mA cm^(-2),65.3±2.7%at 10 mA cm^(-2),and 71.4±1.2%at 20 mA cm^(-2).Furthermore,the discharge voltage is significantly enhanced,reaching 1.76±0.01 V at 1 mA cm^(-2),1.44±0.02 V at 10 mA cm^(-2),and 1.21±0.08 V at 20 mA cm^(-2).Consequently,our newly developed anode exhibits a remarkable energy density of 2312±98 W h kg^(-1),placing it among the top-performing magnesium anodes documented in the literature.Density functional theory calculations and experimental investigations have unveiled that the exceptional performance can be attributed to the inhibition of water reduction,facilitated by the hybridization between solute atoms and neighboring Mg atoms.Furthermore,the activation of the second phase,introducing additional galvanic couples,significantly contributes to this performance.This study presents valuable insights that can guide the design of novel anodes,contributing to the advancement of high-performance magnesium-air batteries.展开更多
As a means of quantitative interpretation,forward calculations of the global lithospheric magnetic field in the Spherical Harmonic(SH)domain have been widely used to reveal geophysical,lithological,and geothermal vari...As a means of quantitative interpretation,forward calculations of the global lithospheric magnetic field in the Spherical Harmonic(SH)domain have been widely used to reveal geophysical,lithological,and geothermal variations in the lithosphere.Traditional approaches either do not consider the non-axial dipolar terms of the inducing field and its radial variation or do so by means of complicated formulae.Moreover,existing methods treat the magnetic lithosphere either as an infinitesimally thin layer or as a radially uniform spherical shell of constant thickness.Here,we present alternative forward formulae that account for an arbitrarily high maximum degree of the inducing field and for a magnetic lithosphere of variable thickness.Our simulations based on these formulae suggest that the satellite magnetic anomaly field is sensitive to the non-axial dipolar terms of the inducing field but not to its radial variation.Therefore,in forward and inverse calculations of satellite magnetic anomaly data,the non-axial dipolar terms of the inducing field should not be ignored.Furthermore,our results show that the satellite magnetic anomaly field is sensitive to variability in the lateral thickness of the magnetized shell.In particular,we show that for a given vertically integrated susceptibility distribution,underestimating the thickness of the magnetic layer overestimates the induced magnetic field.This discovery bridges the greatest part of the alleged gap between the susceptibility values measured from rock samples and the susceptibility values required to match the observed magnetic field signal.We expect the formulae and conclusions of this study to be a valuable tool for the quantitative interpretation of the Earth's global lithospheric magnetic field,through an inverse or forward modelling approach.展开更多
Establishing an energy-saving and affordable hydrogen production route from infinite seawater presents a promising strategy for achieving carbon neutrality and low-carbon development.Compared with the kinetically slug...Establishing an energy-saving and affordable hydrogen production route from infinite seawater presents a promising strategy for achieving carbon neutrality and low-carbon development.Compared with the kinetically sluggish oxygen evolution reaction(OER),the thermodynamically advantageous sulfion oxidation reaction(SOR)enables the S^(2-)pollutants recovery while reducing the energy input of water electrolysis.Here,a nanoporous NiMo alloy ligament(np-NiMo)with AlNi_(3)/Al_(5)Mo heterostructure was prepared for hydrogen evolution reaction(HER,-0.134V versus reversible hydrogen electrode(vs.RHE)at 50mA/cm^(2)),which needs an Al_(89)Ni_(10)Mo_(1)as a precursor and dealloying operation.Further,the np-NiMo alloy was thermal-treated with S powder to generate Mo-doped NiS_(2)(np-NiMo-S)for OER(1.544V vs.RHE at 50mA/cm^(2))and SOR(0.364 V vs.RHE at 50mA/cm^(2)),while still maintaining the nanostructuring advantages.Moreover,for a two-electrode electrolyzer system with np-NiMo cathode(1M KOH+seawater)coupling np-NiMo-S anode(1mol/L KOH+seawater+1 mol/L Na_(2)S),a remarkably ultra-low cell potential of 0.532 V is acquired at 50mA/cm^(2),which is about 1.015 V below that of normal alkaline seawater splitting.The theory calculations confirmed that the AlNi_(3)/Al_(5)Mo heterostructure within np-NiMo promotes H_(2)O dissociation for excellent HER,while the Mo-dopant of np-NiMo-S lowers energy barriers for the rate-determining step from^(*)S_(4)to^(*)S_(8).This work develops two kinds of NiMo alloy with tremendous prominence for achieving energy-efficient hydrogen production from alkaline seawater and sulfur recycling from sulfion-rich sewage.展开更多
The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-...The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.展开更多
INTERNAL DOSE RESEARCH PAPERS INTDOSKIT:An R-Code for Calculation of Dose Coefficients and Studying Their Uncertainties Bastian Breustedt 1,Niranjan Chavan 2,Thomas Makumbi 2(1.Karlsruhe Institute of Technology,Instit...INTERNAL DOSE RESEARCH PAPERS INTDOSKIT:An R-Code for Calculation of Dose Coefficients and Studying Their Uncertainties Bastian Breustedt 1,Niranjan Chavan 2,Thomas Makumbi 2(1.Karlsruhe Institute of Technology,Institute of Biomedical Engineering(IBT),Fritz-Haber-Weg 1,D-76131 Karlsruhe,Germany;2.Karlsruhe Institute of Technology,Institute for Thermal Energy Technology and Safety(ITES),Hermann-von-Helmholtz-Platz 1,76344 EggensteinLeopoldshafen,Germany)Abstract:An R-code,which allows the calculation of the time dependent activity distribution based on ICRP reference models,the number of decays in a commitment period,and the dose coefficients for tissues and organs of the human body,has been developed.R Language was chosen due to its powerful mathematical and statistical modeling features,as well as its graphical capabilities.展开更多
Al-Cu-Mg-Ag alloys have become a research hotspot because of its good heat resistance.Its excellent mechanical properties are inseparable from the regulation of the structure by researchers.The method of material stru...Al-Cu-Mg-Ag alloys have become a research hotspot because of its good heat resistance.Its excellent mechanical properties are inseparable from the regulation of the structure by researchers.The method of material structure simulation has become more and more perfect.This study employs numerical simulation to investigate the microstructure evolution of Al-Cu-Mg-Ag alloys during solidification with the aim of controlling its structure.The size distribution of Ti-containing particles in an Al-Ti-B master alloy was characterized via microstructure observation,serving as a basis for optimizing the nucleation density parameters for particles of varying radii in the phase field model.The addition of refiner inhibited the growth of dendrites and no longer produced coarse dendrites.With the increase of refiner,the grains gradually tended to form cellular morphology.The refined grains were about 100μm in size.Experimental validation of the simulated as-cast grain morphology was conducted.The samples were observed by metallographic microscope and scanning electron microscope.The addition of refiner had a significant effect on the refinement of the alloy,and the average grain size after refinement was also about 100μm.At the same time,the XRD phase identification of the alloy was carried out.The observation of the microstructure morphology under the scanning electron microscope showed that the precipitated phase was mainly concentrated on the grain boundary.The Al_(2)Cu accounted for about 5%,and the matrix phase FCC accounted for about 95%,which also corresponded well with the simulation results.展开更多
Nitric oxide(NO),which generally originates from vehicle exhaust and industrial flue gases,is one of the most serious air pollutants.In this case,the electrochemical NO reduction reaction(NORR)not only removes the atm...Nitric oxide(NO),which generally originates from vehicle exhaust and industrial flue gases,is one of the most serious air pollutants.In this case,the electrochemical NO reduction reaction(NORR)not only removes the atmospheric pollutant NO but also produces valuable ammonia(NH_(3)).Hence,through the synthesis and modification of Fe_(3)C nanocrystal cata-lysts,the as-obtained optimal sample of Fe_(3)C/C-900 was adopted as the NORR catalyst at ambient conditions.As a result,the Fe_(3)C/C-900 catalyst showed an NH_(3)Faraday efficiency of 76.5%and an NH_(3)yield rate of 177.5μmol·h^(-1)·cm^(-2)at the working potentials of-0.8 and-1.2 V versus reversible hydrogen electrode(vs.RHE),respectively.And it delivered a stable NORR activity during the electrolysis.Moreover,we attribute the high NORR properties of Fe_(3)C/C-900 to two aspects:one is the enhanced intrinsic activity of Fe_(3)C nanocrystals,including the lowering of the energy barrier of rate-limiting step(*NOH→*N)and the inhibition of hydrogen evolution;on the other hand,the favorable dispersion of active components,the effective adsorption of gaseous NO,and the release of liquid NH_(3)products facilitated by the porous carbon substrate.展开更多
This study aims to enhance the photocatalytic performance of 2D/2D heterojunctions for NO removal from marine vessel effluents.SnS_(2)/g-C_(3)N_(4) composites were successfully constructed via a facile solvothermal me...This study aims to enhance the photocatalytic performance of 2D/2D heterojunctions for NO removal from marine vessel effluents.SnS_(2)/g-C_(3)N_(4) composites were successfully constructed via a facile solvothermal method,demonstrating a significant improvement in photocatalytic NO removal under visible light irradiation.For high-flux simulated flue gas,the composite with 10%SnS_(2)(denoted as SNCN-10)showed exceptional NO removal efficiency,reaching up to 66.8%,along with excellent reusability over five consecutive cycles.Detailed band structure and density of states(DOS)calculations confirmed the formation of a characteristic heterojunction.Spin-trapping ESR spectroscopy identified·O_(2)^(-)−as the key reactive species driving NO oxidation.Additionally,in situ DRIFT spectroscopy revealed that SNCN-10 facilitated the conversion of NO to nitrate through intermediate species,including bridging nitrite and cis-nitrite(N_(2)O_(2)^(2-)).Kinetic studies further indicated that NO oxidation followed the Langmuir-Hinshelwood(L-H)mechanism.Based on density functional theory(DFT)calculations of free energy changes,a comprehensive reaction pathway for NO oxidation was proposed.These findings provide valuable insights for the development of efficient photocatalytic strategies for NO removal.展开更多
Two new transition-metal coordination polymers,{[Cd(oba)(L)_(2)]·H_(2)O}_n(1)and[Cd(4-nph)(L)_(2)]_n(2)(H_(2)oba=4,4'-oxydibenzoic acid,4-H_(2)nph=4-nitrophthalic acid,L=2,2'-biimidazole),were successfull...Two new transition-metal coordination polymers,{[Cd(oba)(L)_(2)]·H_(2)O}_n(1)and[Cd(4-nph)(L)_(2)]_n(2)(H_(2)oba=4,4'-oxydibenzoic acid,4-H_(2)nph=4-nitrophthalic acid,L=2,2'-biimidazole),were successfully synthesized under hydrothermal conditions and characterized structurally by IR spectroscopy,elemental analyses,single-crystal X-ray diffraction,powder X-ray diffraction,and thermogravimetric analysis.The results of single-crystal X-ray diffraction show that complex 1 presents a 1D zigzag chain structure and further extends to a 2D network through N—H…O hydrogen bonds andπ-πstacking interactions.Meanwhile,complex 2 has a zero-dimensional structure and also extends to form a 2D network through N—H…O hydrogen bonds andπ-πstacking interactions.In addition,both 1and 2 exhibited luminescent properties in the solid state.Furthermore,quantum chemical calculations were carried out on the"molecular fragments"extracted from the crystal structures of 1 and 2 using the PBE0/LANL2DZ method constructed by the Gaussian 16 program.The calculated values signify a significant covalent interaction between the coordination atoms and the Cd(Ⅱ)ions.CCDC:2332173,1;2332176,2.展开更多
In the past decade,people have conducted extensive research on the synthesis and application properties of various functionalized pillararenes.Pillararenes show good application prospects in the field of sensors due t...In the past decade,people have conducted extensive research on the synthesis and application properties of various functionalized pillararenes.Pillararenes show good application prospects in the field of sensors due to the rich host-vip recognition in their rigid electron-rich cavities.However,most reported pillararenes are functionalized by alkoxy modification,which results in poor charge transfer nature and weak fluorescence response.A π-conjugated charge-transfer system P5BN was obtained by introducing electron-donating triarylamine(Ar_(3)N)and electron-deficient triarylborane(Ar_(3)B)into pillar[5]arene skeleton,which significantly improved its luminescence behavior and was further used for fluorescence detection applications.The molecular structure showed that P5BN provided a good macrocyclic cavity to encapsulate amino acids molecules of suitable size.It was found that P5BN,as a fluorescent sensor,showed a highly sensitive and selective response to L-arginine(L-Arg),resulting in a significant enhancement of the fluorescence at 408 nm of P5BN with the lowest detection concentration being 2.21×10^(-8) mol/L.The recognition mechanism was demonstrated through experiments and DFT theoretical calculations.展开更多
Heterogeneous solid frustrated-Lewis-pair(FLP)catalyst is of great promise in practical hydrogenation applications.It has been found that all-solid FLPs can be created on ceria via surface oxygen vacancy regulation.Co...Heterogeneous solid frustrated-Lewis-pair(FLP)catalyst is of great promise in practical hydrogenation applications.It has been found that all-solid FLPs can be created on ceria via surface oxygen vacancy regulation.Consequently,it is desired to investigate the mechanisms of the FLP-catalyzed hydrogenation of C=C and C=O and provide insight into the modification of CeO_(2)catalysts for the selective hydrogenation.In this work,the reaction mechanism of the hydrogenation of CH_(2)=CH_(2)and CH_(3)CH=O at the FLP sites constructed on CeO_(2)(110)surface was investigated by density functional theory(DFT),with the classical Lewis acid-base pairs(CLP)site as the reference.The results illustrate that at the CLP site,the dissociated hydride(H^(δ−))forms a stable H−O bond with the surface O atom,while at the FLP site,H^(δ−)is stabilized by Ce,displaying higher activity on the one hand.On the other hand,the electron cloud density of the Ce atom at the FLP site is higher,which can transfer more electrons to the adsorbed C_(C=C)and O_(C=O)atoms,leading to a higher degree of activation for C=C and C=O bonds,as indicated by the Bader charge analysis.Therefore,compared to the CLP site,the FLP site exhibits higher hydrogenation activity for CH_(2)=CH_(2)and CH_(3)CH=O.Furthermore,at the FLP sites,it demonstrates high efficiency in catalyzing the hydrogenation of CH_(2)=CH_(2)with the rate-determining barrier of 1.04 eV,but it shows limited activity for the hydrogenation of CH_(3)CH=O with the rate-determining barrier of 1.94 eV.It means that the selective hydrogenation of C=C can be effectively achieved at the FLP sites concerning selective hydrogenation catalysis.The insights shown in this work help to clarify the reaction mechanism of the hydrogenation of C=C and C=O at FLP site on CeO_(2)(110)and reveal the relationship between the catalytic performance and the nature of the active site,which is of great benefit to development of rational design of heterogeneous FLP catalysts.展开更多
We investigated the adsorption mechanisms including physical and chemical adsorption for heavy metals(Cd,Pb,Zn,Co,Cu)on C-lignin using density functional theory(DFT)simulations.Physical adsorption,involving metal atom...We investigated the adsorption mechanisms including physical and chemical adsorption for heavy metals(Cd,Pb,Zn,Co,Cu)on C-lignin using density functional theory(DFT)simulations.Physical adsorption,involving metal atoms near carbon atoms,is found to be endothermic;meanwhile,chemical adsorption,where hydroxyl groups replace metal ions,is exothermic and spontaneous.Pb exhibits the highest physical adsorption potential,while Cu and Co demonstrate the strongest chemical adsorption due to their highly negative adsorption energies.These findings provide valuable insights into the design of eco-friendly nano lignocellulosic composite films for effective heavy metal removal from contaminated water sources.Key words:C-lignin;adsorption;We investigated the adsorption mechanisms including physical and chemical adsorption for heavy metals(Cd,Pb,Zn,Co,Cu)on C-lignin using density functional theory(DFT)simulations.Physical adsorption,involving metal atoms near carbon atoms,is found to be endothermic;meanwhile,chemical adsorption,where hydroxyl groups replace metal ions,is exothermic and spontaneous.Pb exhibits the highest physical adsorption potential,while Cu and Co demonstrate the strongest chemical adsorption due to their highly negative adsorption energies.These findings provide valuable insights into the design of eco-friendly nano lignocellulosic composite films for effective heavy metal removal from contaminated water sources.展开更多
The asymmetric addition of aromatic organometallic compounds to the carbonyl group(C-3)of isatins,catalyzed by transition metals,has emerged as a remarkably efficient method for the synthesis of chiral 3-hydroxyoxindo...The asymmetric addition of aromatic organometallic compounds to the carbonyl group(C-3)of isatins,catalyzed by transition metals,has emerged as a remarkably efficient method for the synthesis of chiral 3-hydroxyoxindoles.Here,an exceptionally enantioselective approach was developed for the first time to achieve a catalytic NHK reaction of isatins with aromatic halides(both aryl and heteroaryl).Utilizing chiral cobalt complexes as catalysts,and the presence of a diboron reagent B_(2)nep_(2)as both a reducing agent and determinant in enantiocontrol,has resulted in the triumphantly achieved synthesis of enantioenriched products.Compared to reported strategies,this approach exhibits remarkable compatibility with substrates bearing sensitive functional groups,such as halides and borate esters,while also eliminating the need for organometallic reagents as required in previous strategies.Through experimental investigations,the presence of aryl-cobalt species during the addition process was confirmed,rather than in-situ generation of an arylboron reagent.Furthermore,the successful attainment of the R absolute configuration through aryl addition was demonstrated.展开更多
As cataract surgery progresses from “restoration of sight” to “refractive correction”, precise prediction of intraocular lens (IOL) power is critical for enhancing postoperative visual quality in patients. IOL pow...As cataract surgery progresses from “restoration of sight” to “refractive correction”, precise prediction of intraocular lens (IOL) power is critical for enhancing postoperative visual quality in patients. IOL power calculation methods have evolved and innovated throughout time, from early theoretical and regression formulas to nonlinear formulas for estimating effective lens position (ELP), multivariable formulas, and innovative formulas that use optical principles and AI-based online formulas. This paper thoroughly discusses the development and iteration of traditional IOL calculation formulas, the emergence of new IOL calculation formulas, and the selection of IOL calculation formulas for different patients in the era of refractive cataract surgery, serving as a reference for “personalized” IOL implantation in clinical practice.展开更多
Based on first-principles calculation framework,the surface model,anodic dissolution,cathodic oxygen absorption reaction,and other related electrochemical corrosion models of Fe-Ce system were constructed,and the infl...Based on first-principles calculation framework,the surface model,anodic dissolution,cathodic oxygen absorption reaction,and other related electrochemical corrosion models of Fe-Ce system were constructed,and the influencing mechanism Ce doping on the corrosion resistance of Fe-Ce system in the Cl medium environment was analyzed.The results show that Ce doping on the first surface and subsurface inhibits the ionization of Fe atoms and greatly promotes the repassivation process of Fe matrix.Ce doping on the first layer is conducive to preventing the detachment of surface Fe atoms from Fe matrix and delaying the occurrence of corrosion.Ce atoms in the subsurface effectively increase the difficulty of Fe atoms detaching from the matrix at high Cl concentrations.When O diffusion is the controlling link of oxygen absorption reaction,Ce doping has no effects on the reaction rate of cathodic oxygen absorption.Ce doping enhances the electrochemical stability of Fe(100)1and reduces the anodic dissolution rate of Fe matrix,thereby improving its corrosion resistance.展开更多
Developing machine learning frameworks with predictive power,interpretability,and transferability is crucial,yet it faces challenges in the field of electrocatalysis.To achieve this,we employed rigorous feature engine...Developing machine learning frameworks with predictive power,interpretability,and transferability is crucial,yet it faces challenges in the field of electrocatalysis.To achieve this,we employed rigorous feature engineering to establish a finely tuned gradient boosting regressor(GBR)model,which adeptly captures the physical complexity from feature space to target variables.We demonstrated that environmental electron effects and atomic number significantly govern the success of the mapping process via global and local explanations.The finely tuned GBR model exhibits exceptional robustness in predicting CO adsorption energies(R_(ave)^(2)=0.937,RMSE=0.153 eV).Moreover,the model demonstrated remarkable transfer learning ability,showing excellent predictive power for OH,NO,and N_(2) adsorption.Importantly,the GBR model exhibits exceptional predictive capability across an extensive search space,thereby demonstrating profound adaptability and versatility.Our research framework significantly enhances the interpretability and transferability of machine learning in electrocatalysis,offering vital insights for further advancements.展开更多
基金supported by the National Natural Science Foundation Joint Fund(Nos.U1806223 and U2106226)the National Natural Science Foundation of China(No.52371081)the Key Technology Research and Development Program of Shandong Province(No.2020CXGC010703).
文摘The defect regulation and p-n heterojunction of composites have gained significant attention due to their potential applications.Nitrogen(N)as doping heteroatoms and perylene-3,4,9,10-tetracarboximide(PDINH)as an appropriate n-type semiconductor were innovatively and reasonably selected to enhance the photocatalytic performance of pristine p-type cuprous oxide(Cu_(2)O).In this study,the defect regula-tion of N doping(1)achieved the small-size effect of Cu_(2)O,(2)optimized the electron features,and(3)improved the kinetics of reactive oxygen species.The p-n heterojunction with PDINH was developed to sharply improve the light utilization of Cu_(2)O,from the UV region to the near-infrared region.As expected,the optimized Cu_(2)N_(x)O_(1–x)/PDINH(x=0.02)exhibited excellent long-term photocatalytic antibacterial ac-tivities,with antibacterial rates exceeding 91%against Staphylococcus aureus and Pseudomonas aeruginosa.Defect regulation and p-n heterojunction of Cu_(2)O-based composites thus provide a great deal of potential for future advancements in photocatalysis.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFF0609000)National Natural Science Foundation of China(Grant Nos.52171034 and 52101037)Postdoctoral Fellowship Program of CPSFara(No.GZB20230944).
文摘Up-and-coming high-temperature materials,refractory high entropy alloys,are suffering from lower oxidation resistance,restricting their applications in the aerospace field.In this study,two novel treatments of Al-deposited and remelted were developed to refine the microstructure and enhance the oxidation resistance of refractory high entropy alloy using electron beam freeform fabrication(EBF3).Finer and short-range ordering structures were observed in the remelted sample,whereas the Al-deposited sample showcased the formation of silicide and intermetallic phases.High-temperature cyclic and isothermal oxidation tests at 1000℃ were carried out.The total weight gain after 60 h of cyclic oxidation decreased by 17.49%and 30.46%for the remelted and deposited samples,respectively,compared to the as-cast state.Oxidation kinetics reveal an evident lower mass gain and oxidation rate in the treated samples.A multilayer oxide consisting of TiO_(2)+Al_(2)O_(3)+SiO_(2)+AlNbO_(4) was studied for its excellent oxidation resistance.The oxidation behavior of rutile,corundum and other oxides was analyzed using first principles calculations and chemical defect analysis.Overall,this research,which introduces novel treatments,offers promising insights for enhancing the inherent oxidation resistance of refractory high entropy alloys.
基金supported by the National Natural Science Foundation of China(Nos.22272105 and 22002110)Natural Science Foundation of Shanghai(No.23ZR1423900)。
文摘Nitrogen-doping of carbon support(N-C)for platinum(Pt)nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells.For fundamental understanding,clearly identifying the metalsupport effect on enhancement mechanisms of ORR electrocatalysis is definitely needed.In this work,the impact of Pt-support interaction via interfacial Pt-N coordination on electrocatalytic ORR activity and stability in Pt/N-C catalyst is deeply studied through structural/compositional characterizations,electrochemical measurements and theoretical DFT-calculations/AIMD-simulations.The resulting Pt/N-C catalyst exhibits a superior electrocatalytic performance compared to the commercial Pt/C catalyst in both half-cell and H_(2)-O_(2)fuel cell.Experimental and theoretical results reveal that the interfacial Pt-N coordination enables electron transfer from N-C support to Pt nanoparticles,which can weaken the adsorption strength of oxygen intermediates on Pt surface to improve ORR activity and induce the strong Pt-support interaction to enhance electrochemical stability.
基金the R&D Program of Beijing Municipal Education Commission(No.KM202310005010)the National Natural Science Foundation of China(No.52001015)for their financial support.
文摘The quest for high-energy-density magnesium-air batteries is hindered by the efficiency-voltage trade-off,ultimately leading to an unsatisfactory energy density.Here,we effectively mitigate the inherent efficiency-voltage trade-off by introducing a novel anode material,specifically,Mg-0.5Sn-0.5In-0.5Ga.This anode demonstrates exceptional anodic efficiency,achieving 60.5±2.5%at 1 mA cm^(-2),65.3±2.7%at 10 mA cm^(-2),and 71.4±1.2%at 20 mA cm^(-2).Furthermore,the discharge voltage is significantly enhanced,reaching 1.76±0.01 V at 1 mA cm^(-2),1.44±0.02 V at 10 mA cm^(-2),and 1.21±0.08 V at 20 mA cm^(-2).Consequently,our newly developed anode exhibits a remarkable energy density of 2312±98 W h kg^(-1),placing it among the top-performing magnesium anodes documented in the literature.Density functional theory calculations and experimental investigations have unveiled that the exceptional performance can be attributed to the inhibition of water reduction,facilitated by the hybridization between solute atoms and neighboring Mg atoms.Furthermore,the activation of the second phase,introducing additional galvanic couples,significantly contributes to this performance.This study presents valuable insights that can guide the design of novel anodes,contributing to the advancement of high-performance magnesium-air batteries.
基金supported by the National Natural Science Foundation of China(Grant Nos.42250103 and 42174090)the Opening Fund of Key Laboratory of Geological Survey and Evaluation of Ministry of Education(Grant No.GLAB2023ZR02)the Ministry of Science and Technology(MOST)Special Fund from the State Key Laboratory of Geological Processes and Mineral Resources(Grant No.MSFGPMR2022-4)。
文摘As a means of quantitative interpretation,forward calculations of the global lithospheric magnetic field in the Spherical Harmonic(SH)domain have been widely used to reveal geophysical,lithological,and geothermal variations in the lithosphere.Traditional approaches either do not consider the non-axial dipolar terms of the inducing field and its radial variation or do so by means of complicated formulae.Moreover,existing methods treat the magnetic lithosphere either as an infinitesimally thin layer or as a radially uniform spherical shell of constant thickness.Here,we present alternative forward formulae that account for an arbitrarily high maximum degree of the inducing field and for a magnetic lithosphere of variable thickness.Our simulations based on these formulae suggest that the satellite magnetic anomaly field is sensitive to the non-axial dipolar terms of the inducing field but not to its radial variation.Therefore,in forward and inverse calculations of satellite magnetic anomaly data,the non-axial dipolar terms of the inducing field should not be ignored.Furthermore,our results show that the satellite magnetic anomaly field is sensitive to variability in the lateral thickness of the magnetized shell.In particular,we show that for a given vertically integrated susceptibility distribution,underestimating the thickness of the magnetic layer overestimates the induced magnetic field.This discovery bridges the greatest part of the alleged gap between the susceptibility values measured from rock samples and the susceptibility values required to match the observed magnetic field signal.We expect the formulae and conclusions of this study to be a valuable tool for the quantitative interpretation of the Earth's global lithospheric magnetic field,through an inverse or forward modelling approach.
基金financially supported by the Guangxi Natural Science Fund for Distinguished Young Scholars(No.2024GXNSFFA010008)the Natural Science Foundation of Jilin Province of China(No.20240101098JC)the National Natural Science Foundation of China(No.22469002)。
文摘Establishing an energy-saving and affordable hydrogen production route from infinite seawater presents a promising strategy for achieving carbon neutrality and low-carbon development.Compared with the kinetically sluggish oxygen evolution reaction(OER),the thermodynamically advantageous sulfion oxidation reaction(SOR)enables the S^(2-)pollutants recovery while reducing the energy input of water electrolysis.Here,a nanoporous NiMo alloy ligament(np-NiMo)with AlNi_(3)/Al_(5)Mo heterostructure was prepared for hydrogen evolution reaction(HER,-0.134V versus reversible hydrogen electrode(vs.RHE)at 50mA/cm^(2)),which needs an Al_(89)Ni_(10)Mo_(1)as a precursor and dealloying operation.Further,the np-NiMo alloy was thermal-treated with S powder to generate Mo-doped NiS_(2)(np-NiMo-S)for OER(1.544V vs.RHE at 50mA/cm^(2))and SOR(0.364 V vs.RHE at 50mA/cm^(2)),while still maintaining the nanostructuring advantages.Moreover,for a two-electrode electrolyzer system with np-NiMo cathode(1M KOH+seawater)coupling np-NiMo-S anode(1mol/L KOH+seawater+1 mol/L Na_(2)S),a remarkably ultra-low cell potential of 0.532 V is acquired at 50mA/cm^(2),which is about 1.015 V below that of normal alkaline seawater splitting.The theory calculations confirmed that the AlNi_(3)/Al_(5)Mo heterostructure within np-NiMo promotes H_(2)O dissociation for excellent HER,while the Mo-dopant of np-NiMo-S lowers energy barriers for the rate-determining step from^(*)S_(4)to^(*)S_(8).This work develops two kinds of NiMo alloy with tremendous prominence for achieving energy-efficient hydrogen production from alkaline seawater and sulfur recycling from sulfion-rich sewage.
基金sponsored by the National Natural Science Foundation of China(Nos.5210125 and 52375422)the Science Research Project of Hebei Education Department(No.BJK2023058)the Natural Science Foundation of Hebei Province(Nos.E2020208069,B2020208083 and E202320801).
文摘The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.
文摘INTERNAL DOSE RESEARCH PAPERS INTDOSKIT:An R-Code for Calculation of Dose Coefficients and Studying Their Uncertainties Bastian Breustedt 1,Niranjan Chavan 2,Thomas Makumbi 2(1.Karlsruhe Institute of Technology,Institute of Biomedical Engineering(IBT),Fritz-Haber-Weg 1,D-76131 Karlsruhe,Germany;2.Karlsruhe Institute of Technology,Institute for Thermal Energy Technology and Safety(ITES),Hermann-von-Helmholtz-Platz 1,76344 EggensteinLeopoldshafen,Germany)Abstract:An R-code,which allows the calculation of the time dependent activity distribution based on ICRP reference models,the number of decays in a commitment period,and the dose coefficients for tissues and organs of the human body,has been developed.R Language was chosen due to its powerful mathematical and statistical modeling features,as well as its graphical capabilities.
文摘Al-Cu-Mg-Ag alloys have become a research hotspot because of its good heat resistance.Its excellent mechanical properties are inseparable from the regulation of the structure by researchers.The method of material structure simulation has become more and more perfect.This study employs numerical simulation to investigate the microstructure evolution of Al-Cu-Mg-Ag alloys during solidification with the aim of controlling its structure.The size distribution of Ti-containing particles in an Al-Ti-B master alloy was characterized via microstructure observation,serving as a basis for optimizing the nucleation density parameters for particles of varying radii in the phase field model.The addition of refiner inhibited the growth of dendrites and no longer produced coarse dendrites.With the increase of refiner,the grains gradually tended to form cellular morphology.The refined grains were about 100μm in size.Experimental validation of the simulated as-cast grain morphology was conducted.The samples were observed by metallographic microscope and scanning electron microscope.The addition of refiner had a significant effect on the refinement of the alloy,and the average grain size after refinement was also about 100μm.At the same time,the XRD phase identification of the alloy was carried out.The observation of the microstructure morphology under the scanning electron microscope showed that the precipitated phase was mainly concentrated on the grain boundary.The Al_(2)Cu accounted for about 5%,and the matrix phase FCC accounted for about 95%,which also corresponded well with the simulation results.
基金supported by the Guangxi Natural Science Fund for Distinguished Young Scholars(2024GXNSFFA010008)Shenzhen Science and Technology Program(JCYJ20230807112503008).
文摘Nitric oxide(NO),which generally originates from vehicle exhaust and industrial flue gases,is one of the most serious air pollutants.In this case,the electrochemical NO reduction reaction(NORR)not only removes the atmospheric pollutant NO but also produces valuable ammonia(NH_(3)).Hence,through the synthesis and modification of Fe_(3)C nanocrystal cata-lysts,the as-obtained optimal sample of Fe_(3)C/C-900 was adopted as the NORR catalyst at ambient conditions.As a result,the Fe_(3)C/C-900 catalyst showed an NH_(3)Faraday efficiency of 76.5%and an NH_(3)yield rate of 177.5μmol·h^(-1)·cm^(-2)at the working potentials of-0.8 and-1.2 V versus reversible hydrogen electrode(vs.RHE),respectively.And it delivered a stable NORR activity during the electrolysis.Moreover,we attribute the high NORR properties of Fe_(3)C/C-900 to two aspects:one is the enhanced intrinsic activity of Fe_(3)C nanocrystals,including the lowering of the energy barrier of rate-limiting step(*NOH→*N)and the inhibition of hydrogen evolution;on the other hand,the favorable dispersion of active components,the effective adsorption of gaseous NO,and the release of liquid NH_(3)products facilitated by the porous carbon substrate.
基金The project was supported by Natural Science Foundation of Shandong Province(ZR2021MB104)National Natural Science Foundation of China(22078174).
文摘This study aims to enhance the photocatalytic performance of 2D/2D heterojunctions for NO removal from marine vessel effluents.SnS_(2)/g-C_(3)N_(4) composites were successfully constructed via a facile solvothermal method,demonstrating a significant improvement in photocatalytic NO removal under visible light irradiation.For high-flux simulated flue gas,the composite with 10%SnS_(2)(denoted as SNCN-10)showed exceptional NO removal efficiency,reaching up to 66.8%,along with excellent reusability over five consecutive cycles.Detailed band structure and density of states(DOS)calculations confirmed the formation of a characteristic heterojunction.Spin-trapping ESR spectroscopy identified·O_(2)^(-)−as the key reactive species driving NO oxidation.Additionally,in situ DRIFT spectroscopy revealed that SNCN-10 facilitated the conversion of NO to nitrate through intermediate species,including bridging nitrite and cis-nitrite(N_(2)O_(2)^(2-)).Kinetic studies further indicated that NO oxidation followed the Langmuir-Hinshelwood(L-H)mechanism.Based on density functional theory(DFT)calculations of free energy changes,a comprehensive reaction pathway for NO oxidation was proposed.These findings provide valuable insights for the development of efficient photocatalytic strategies for NO removal.
文摘Two new transition-metal coordination polymers,{[Cd(oba)(L)_(2)]·H_(2)O}_n(1)and[Cd(4-nph)(L)_(2)]_n(2)(H_(2)oba=4,4'-oxydibenzoic acid,4-H_(2)nph=4-nitrophthalic acid,L=2,2'-biimidazole),were successfully synthesized under hydrothermal conditions and characterized structurally by IR spectroscopy,elemental analyses,single-crystal X-ray diffraction,powder X-ray diffraction,and thermogravimetric analysis.The results of single-crystal X-ray diffraction show that complex 1 presents a 1D zigzag chain structure and further extends to a 2D network through N—H…O hydrogen bonds andπ-πstacking interactions.Meanwhile,complex 2 has a zero-dimensional structure and also extends to form a 2D network through N—H…O hydrogen bonds andπ-πstacking interactions.In addition,both 1and 2 exhibited luminescent properties in the solid state.Furthermore,quantum chemical calculations were carried out on the"molecular fragments"extracted from the crystal structures of 1 and 2 using the PBE0/LANL2DZ method constructed by the Gaussian 16 program.The calculated values signify a significant covalent interaction between the coordination atoms and the Cd(Ⅱ)ions.CCDC:2332173,1;2332176,2.
文摘In the past decade,people have conducted extensive research on the synthesis and application properties of various functionalized pillararenes.Pillararenes show good application prospects in the field of sensors due to the rich host-vip recognition in their rigid electron-rich cavities.However,most reported pillararenes are functionalized by alkoxy modification,which results in poor charge transfer nature and weak fluorescence response.A π-conjugated charge-transfer system P5BN was obtained by introducing electron-donating triarylamine(Ar_(3)N)and electron-deficient triarylborane(Ar_(3)B)into pillar[5]arene skeleton,which significantly improved its luminescence behavior and was further used for fluorescence detection applications.The molecular structure showed that P5BN provided a good macrocyclic cavity to encapsulate amino acids molecules of suitable size.It was found that P5BN,as a fluorescent sensor,showed a highly sensitive and selective response to L-arginine(L-Arg),resulting in a significant enhancement of the fluorescence at 408 nm of P5BN with the lowest detection concentration being 2.21×10^(-8) mol/L.The recognition mechanism was demonstrated through experiments and DFT theoretical calculations.
基金supported by the National Natural Science Foundation of China(22302115,22072079)the Fundamental Research Program of Shanxi Province(202303021221056).
文摘Heterogeneous solid frustrated-Lewis-pair(FLP)catalyst is of great promise in practical hydrogenation applications.It has been found that all-solid FLPs can be created on ceria via surface oxygen vacancy regulation.Consequently,it is desired to investigate the mechanisms of the FLP-catalyzed hydrogenation of C=C and C=O and provide insight into the modification of CeO_(2)catalysts for the selective hydrogenation.In this work,the reaction mechanism of the hydrogenation of CH_(2)=CH_(2)and CH_(3)CH=O at the FLP sites constructed on CeO_(2)(110)surface was investigated by density functional theory(DFT),with the classical Lewis acid-base pairs(CLP)site as the reference.The results illustrate that at the CLP site,the dissociated hydride(H^(δ−))forms a stable H−O bond with the surface O atom,while at the FLP site,H^(δ−)is stabilized by Ce,displaying higher activity on the one hand.On the other hand,the electron cloud density of the Ce atom at the FLP site is higher,which can transfer more electrons to the adsorbed C_(C=C)and O_(C=O)atoms,leading to a higher degree of activation for C=C and C=O bonds,as indicated by the Bader charge analysis.Therefore,compared to the CLP site,the FLP site exhibits higher hydrogenation activity for CH_(2)=CH_(2)and CH_(3)CH=O.Furthermore,at the FLP sites,it demonstrates high efficiency in catalyzing the hydrogenation of CH_(2)=CH_(2)with the rate-determining barrier of 1.04 eV,but it shows limited activity for the hydrogenation of CH_(3)CH=O with the rate-determining barrier of 1.94 eV.It means that the selective hydrogenation of C=C can be effectively achieved at the FLP sites concerning selective hydrogenation catalysis.The insights shown in this work help to clarify the reaction mechanism of the hydrogenation of C=C and C=O at FLP site on CeO_(2)(110)and reveal the relationship between the catalytic performance and the nature of the active site,which is of great benefit to development of rational design of heterogeneous FLP catalysts.
基金Funded by the Hubei Province Key Research Foundation for Water Resources,China(No.HBSLKY2023035)the National College Students’Innovation and Entrepreneurship Training Program,China(No.202310500012)the Wuhan Talents Outstanding Young Talents Program。
文摘We investigated the adsorption mechanisms including physical and chemical adsorption for heavy metals(Cd,Pb,Zn,Co,Cu)on C-lignin using density functional theory(DFT)simulations.Physical adsorption,involving metal atoms near carbon atoms,is found to be endothermic;meanwhile,chemical adsorption,where hydroxyl groups replace metal ions,is exothermic and spontaneous.Pb exhibits the highest physical adsorption potential,while Cu and Co demonstrate the strongest chemical adsorption due to their highly negative adsorption energies.These findings provide valuable insights into the design of eco-friendly nano lignocellulosic composite films for effective heavy metal removal from contaminated water sources.Key words:C-lignin;adsorption;We investigated the adsorption mechanisms including physical and chemical adsorption for heavy metals(Cd,Pb,Zn,Co,Cu)on C-lignin using density functional theory(DFT)simulations.Physical adsorption,involving metal atoms near carbon atoms,is found to be endothermic;meanwhile,chemical adsorption,where hydroxyl groups replace metal ions,is exothermic and spontaneous.Pb exhibits the highest physical adsorption potential,while Cu and Co demonstrate the strongest chemical adsorption due to their highly negative adsorption energies.These findings provide valuable insights into the design of eco-friendly nano lignocellulosic composite films for effective heavy metal removal from contaminated water sources.
基金the National Key R&D Program of China(No.2022YFA1503200)the National Natural Science Foundation of China(Nos.22025104,22171134,and 21972064)the Fundamental Research Funds for the Central Universities(No.020514380254)is greatly appreciated.
文摘The asymmetric addition of aromatic organometallic compounds to the carbonyl group(C-3)of isatins,catalyzed by transition metals,has emerged as a remarkably efficient method for the synthesis of chiral 3-hydroxyoxindoles.Here,an exceptionally enantioselective approach was developed for the first time to achieve a catalytic NHK reaction of isatins with aromatic halides(both aryl and heteroaryl).Utilizing chiral cobalt complexes as catalysts,and the presence of a diboron reagent B_(2)nep_(2)as both a reducing agent and determinant in enantiocontrol,has resulted in the triumphantly achieved synthesis of enantioenriched products.Compared to reported strategies,this approach exhibits remarkable compatibility with substrates bearing sensitive functional groups,such as halides and borate esters,while also eliminating the need for organometallic reagents as required in previous strategies.Through experimental investigations,the presence of aryl-cobalt species during the addition process was confirmed,rather than in-situ generation of an arylboron reagent.Furthermore,the successful attainment of the R absolute configuration through aryl addition was demonstrated.
文摘As cataract surgery progresses from “restoration of sight” to “refractive correction”, precise prediction of intraocular lens (IOL) power is critical for enhancing postoperative visual quality in patients. IOL power calculation methods have evolved and innovated throughout time, from early theoretical and regression formulas to nonlinear formulas for estimating effective lens position (ELP), multivariable formulas, and innovative formulas that use optical principles and AI-based online formulas. This paper thoroughly discusses the development and iteration of traditional IOL calculation formulas, the emergence of new IOL calculation formulas, and the selection of IOL calculation formulas for different patients in the era of refractive cataract surgery, serving as a reference for “personalized” IOL implantation in clinical practice.
基金Project supported by the National Natural Science Foundation of China(52364044,52204364)Scientific Research Special Project for First-Class Disciplines of Education Department of Inner Mongolia Autonomous Region(YLXKZX-NKD-001,YLXKZX-NKD-011)Basic Scientific Research Business Expenses of Colleges and Universities of Inner Mongolia Autonomous Region(2023QNJS011)。
文摘Based on first-principles calculation framework,the surface model,anodic dissolution,cathodic oxygen absorption reaction,and other related electrochemical corrosion models of Fe-Ce system were constructed,and the influencing mechanism Ce doping on the corrosion resistance of Fe-Ce system in the Cl medium environment was analyzed.The results show that Ce doping on the first surface and subsurface inhibits the ionization of Fe atoms and greatly promotes the repassivation process of Fe matrix.Ce doping on the first layer is conducive to preventing the detachment of surface Fe atoms from Fe matrix and delaying the occurrence of corrosion.Ce atoms in the subsurface effectively increase the difficulty of Fe atoms detaching from the matrix at high Cl concentrations.When O diffusion is the controlling link of oxygen absorption reaction,Ce doping has no effects on the reaction rate of cathodic oxygen absorption.Ce doping enhances the electrochemical stability of Fe(100)1and reduces the anodic dissolution rate of Fe matrix,thereby improving its corrosion resistance.
基金supported by the Research Grants Council of Hong Kong(CityU 11305919 and 11308620)and NSFC/RGC Joint Research Scheme N_CityU104/19Hong Kong Research Grant Council Collaborative Research Fund:C1002-21G and C1017-22Gsupported by the Hong Kong Research Grant Council Collaborative Research Fund:C6021-19E.
文摘Developing machine learning frameworks with predictive power,interpretability,and transferability is crucial,yet it faces challenges in the field of electrocatalysis.To achieve this,we employed rigorous feature engineering to establish a finely tuned gradient boosting regressor(GBR)model,which adeptly captures the physical complexity from feature space to target variables.We demonstrated that environmental electron effects and atomic number significantly govern the success of the mapping process via global and local explanations.The finely tuned GBR model exhibits exceptional robustness in predicting CO adsorption energies(R_(ave)^(2)=0.937,RMSE=0.153 eV).Moreover,the model demonstrated remarkable transfer learning ability,showing excellent predictive power for OH,NO,and N_(2) adsorption.Importantly,the GBR model exhibits exceptional predictive capability across an extensive search space,thereby demonstrating profound adaptability and versatility.Our research framework significantly enhances the interpretability and transferability of machine learning in electrocatalysis,offering vital insights for further advancements.
