In this study,an artificial intelligence-based machine vision system was developed for in-line particle size analysis during the pellet layering process.Drug-layered pellets were produced by coating microcrystalline c...In this study,an artificial intelligence-based machine vision system was developed for in-line particle size analysis during the pellet layering process.Drug-layered pellets were produced by coating microcrystalline cellulose cores with an ibuprofen-containing layering liquid until the target drug content was achieved.Drug content increases with pellet size;therefore,particle size monitoring can ensure product safety and quality.The direct imaging system,consisting of a rigid endoscope,a light source,and a high-speed camera,provides real-time information about pellet size and layer uniformity,enabling timely intervention in the case of out-of-spec products.A convolutional neural network-based instance segmentation algorithm was employed to detect particles in focus,ensuring that pellet size could be accurately determined despite the dense flow of the particles.After training the model,the performance of the developed system was assessed by analysing the particle size distribution of pellet cores with variable sizes within the 250 e850 mm size range.The endoscopic system was tested in-line at a larger scale during the drug layering of inert pellet cores.The particle size data acquired in real time with the endoscopic imaging system corresponded with the reference methods,demonstrating the feasibility of the proposed machine vision-based method as a process analytical technology tool for in-line process monitoring.展开更多
NiFe-layered double hydroxides(NiFe-LDHs)are among the most promising earth-abundant electrocatalysts for the oxygen evolution reaction(OER)in alkaline media.However,their practical application is hindered by intrinsi...NiFe-layered double hydroxides(NiFe-LDHs)are among the most promising earth-abundant electrocatalysts for the oxygen evolution reaction(OER)in alkaline media.However,their practical application is hindered by intrinsic activity limitations and poor stability,primarily due to the asymmetric adsorption of oxygen intermediates.To overcome this,the binding strength must be synergistically tuned to a moderate level to optimize catalytic performance.Here,we engineered NiFeCoCr LDH through Co doping to enhance electrical conductivity and controlled Cr leaching to introduce cationic vacancies for modulating intermediate binding strength in NiFe LDH.X-ray absorption near-edge structure and extended X-ray absorption fine structure analyses reveal that NiFe-LDH with Co doping and Cr vacancies modulates the Ni oxidation state and local coordination environment,leading to a balanced electronic structure and enhanced structural complexity around the Ni sites.Additionally,these vacancies can trap OH^(-)/H_(2)O species,which can serve as a reservoir for OH^(-) transfer,facilitating the rapid formation of OER intermediates and enhancing catalytic performance at high current densities.As a result,V_(Cr)-NiFeCo LDH achieves 1.6 A cm^(-2)current density at 1.7 V vs.RHE while maintaining stable operation for over 1000 h at 500 mA cm^(-2).Density functional theory(DFT)calculations validate the synergistic effects of Co doping and Cr-induced vacancies on intermediate binding energies and improved OER kinetics.Overall,this work presents a rational design strategy to simultaneously enhance the activity and durability of NiFe-based OER catalysts for their application in high-performance alkaline water electrolysis.展开更多
To deepen understanding of the evolution of coal char microstructural properties of coal char during the co-pyrolysis of coking coal with additives,this study incorporated two typical additives,coal tar pitch(CTP)and ...To deepen understanding of the evolution of coal char microstructural properties of coal char during the co-pyrolysis of coking coal with additives,this study incorporated two typical additives,coal tar pitch(CTP)and waste plastic(HDPE),into a blended coal sample and carried out pyrolysis experiments.The pyrolysis process and the microstructure of char were systematically characterized using various analytical techniques,including thermogravimetric analysis(TGA),X-ray diffraction(XRD)and Raman spectroscopy.Data correlation analysis was performed to reveal the mechanism of carbon structural ordering evolution within the critical temperature range(350−600℃)from colloidal layer formation to semi-coke conversion in coking coal,and to elucidate the regulatory effects of different additives on coal pyrolysis pathways.The results indicate that HDPE releases free radicals during high-temperature pyrolysis,accelerating the pyrolysis reaction and increase the yield of volatile components.Conversely,CTP facilitates pyrolysis at low temperatures through its light components,thereby delaying high-temperature reactions due to the colloidal layer’s effect.XRD results indicate that during the process of pyrolysis,there is a progressive decrease in the interlayer spacing of aromatic layers(d002),while the aromatic ring stacking height(L_(c))and lateral size(L_(a))undergo significant of carbon skeleton ordering.Further comparative reveals that CTP partially suppresses structural ordering at low temperatures,whereas HDPE promotes the condensation and alignment of aromatic clusters via a free radical mechanism.Raman spectroscopy reveals a two-stage reorganization mechanism in the microstructure of the coal char:the decrease in the I_(D)/I_(G)ratio between 350 and 550℃is primarily attributed to the cleavage of aliphatic side chains and cross-linking bonds,leading to a reduction in defective structures;whereas the increase in ID/IG between 550 and 600℃is closely associated with enhanced condensation reactions of aromatic structures.Correlation analysis further demonstrates progressive graphitization during pyrolysis,with a significant positive correlation(R^(2)>0.85)observed between d002 and the full width at half maximum of the G-band(FWHM-G).展开更多
Post-quantum transport layer security(PQ-TLS)is capable of effectively defending against quantum threats to current network communications,whereas its larger public key and certificate sizes as well as higher computat...Post-quantum transport layer security(PQ-TLS)is capable of effectively defending against quantum threats to current network communications,whereas its larger public key and certificate sizes as well as higher computational overhead may result in a significant performance reduction compared with conventional TLS.In this paper,we present a systematic evaluation of PQ-TLS performance across diverse deployment scenarios to address the following critical research questions.(1)What is the performance behavior of PQ-TLS across different TLS modes?(2)How does PQ-TLS perform across varying client scales?(3)Which network topology is most suitable for PQ-TLS?(4)How does PQ-TLS perform on personal computers(PCs)compared to embedded IoT devices?To the best of our knowledge,this is the first work to comprehensively address these issues,offering implementers some insights into PQ-TLS performance and guidance for optimizing it across diverse scenarios.展开更多
The morphology of active layer plays a critical role in determining the photovoltaic performance of organic solar cells(OSCs).However,binary blends often suffer from suboptimal phase separation,which limits the effici...The morphology of active layer plays a critical role in determining the photovoltaic performance of organic solar cells(OSCs).However,binary blends often suffer from suboptimal phase separation,which limits the efficiency of OSCs.Herein,two bridging polymer acceptors(PAs)—benzodithiophene-(2-ethylhexyl)oxy(BDT-C2C4)and benzodithiophene-octyloxy(BDT-C_(8))—are designed and synthesized by combining a benzodithiophene(BDT)unit as the donor moiety[poly({4,8-bis[5-(2-ethylhexyl)-4-fluorothiophen-2-yl]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl}){5,8-bis[4-(2-butyloctyl)thiophen-2-yl]dithieno[3',2':3,4]},D18],and a 2,2′-((2Z,2′Z)-{[12,13-Bis(2-butyloctyl)-12,13-dihydro-3,9-dinonylthieno[2,3]thieno[3,2-b]pyrrolo[4,5-g]thieno[2,3-b]indole-2,10-diyl]bis(methanylylidene)}bis(3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile(Y6)derivative as the acceptor moiety.BDT-C2C4 and BDT-C_(8) are functionalized with(2-ethylhexyl)oxy and octyloxy side chains on the BDT unit,respectively.Both PAs show complementary absorption and cascaded energy levels with the donor D18 and the acceptor 2,2′-((2Z,2′Z)-{[12,13-bis(3-ethylheptyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2″,3″∶4′,5′]thieno[2′,3′∶4,5]pyrrolo[3,2-g]thieno[2′,3′∶4,5]thieno[3,2-b]indole-2,10-diyl]bis(meth⁃aneylylidene)}bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile(N3),but BDT-C_(8) exhibits better compatibility with D18 and N3 compared to BDT-C2C4.When incorporated as a third component into the D18∶N3 blend,both PAs improve the active layer morphology.In particular,the D18∶N3∶BDT-C_(8) blend shows significantly optimized morphology,featuring reduced phase separation and a fibrous network structure.As a result,the device based on D18∶N3∶BDT-C_(8) achieves a power conversion efficiency of 18.18%,significantly higher than that of the device based on D18∶N3(ca.17.37%).This work presents a compatibilizer strategy for optimizing blend morphology towards high-performance ternary OSCs.展开更多
Layered transition-metal compounds(LTMCs)feature stacked architectures,strong magnetic anisotropy,and tunable magnetic order,making them promising material platforms for low-power spintronic technologies and for enabl...Layered transition-metal compounds(LTMCs)feature stacked architectures,strong magnetic anisotropy,and tunable magnetic order,making them promising material platforms for low-power spintronic technologies and for enabling topological functionalities in the post-Moore era.Here we review recent progress on two-dimensional(2D)magnetism in LTMCs,emphasizing material taxonomy,intrinsic magnetic properties,and external-field controls.This review first presents a classification of LTMCs by crystal structure and chemistry—binary halides,chalcogenides,and ternary families(e.g.,MPX_(3),M_(m)X_(n)Te_(k),MnBi_(2)Te_(4))—followed by a summary of their coupling mechanisms,ordering temperatures,and dimensional effects.It then analyzes the modulation of exchange interactions,magnetic anisotropy,and topological states by electric-field gating,strain engineering,and ion intercalation,with representative experimental demonstrations.Notable advances include room-temperature ferromagnetic metals and semiconductors,observation of the quantum anomalous Hall effect(QAHE)in MnBi2Te4,and synergistic control of magnetic-topological states under multiple external stimuli.Persistent challenges involve the limited availability of intrinsic 2D magnetic semiconductors with high Curie temperatures(Tc),incomplete understanding of the microscopic couplings at interfaces and under quantum confinement,and device-level stability.We conclude by outlining opportunities that lie in the integration of multiscale characterization,first-principles theory,and cross-scale fabrication to precisely co-engineer magnetism,topology,and electronic structure,thereby advancing LTMCs toward spintronic and topological-quantum applications.展开更多
AlGaN-based deep-ultraviolet(DUV)laser diodes(LDs)face performance challenges due to elec-tron leakage and poor hole injection which is often worsened by polarization effects from conventional elec-tron blocking layer...AlGaN-based deep-ultraviolet(DUV)laser diodes(LDs)face performance challenges due to elec-tron leakage and poor hole injection which is often worsened by polarization effects from conventional elec-tron blocking layers(EBLs).To overcome these limitations,we propose an EBL-free DUV LD design incor-porating a 1-nm undoped Al_(0.8)Ga_(0.2)N thin strip layer after the last quantum barrier.Using PICS3D simula-tions,we evaluate the optical and electrical characteristics.Results show a significant increase in effective electron barrier height(from 158.2 meV to 420.7 meV)and a reduction in hole barrier height(from 149.2 meV to 62.8 meV),which enhance hole injection and reduce electron leakage.The optimized structure(LD3)achieves a 14%increase in output power,improved slope efficiency(1.85 W/A),and lower threshold current.This design also reduces the quantum confined Stark effect and forms dual hole accumulation regions,im-proving recombination efficiency.展开更多
[Objective] The aim was to promote color wheat industrialization and meet the demand of people on nutritious grain, making both natural and safe food possible. [Method] Hardness indices of wheat were measured and laye...[Objective] The aim was to promote color wheat industrialization and meet the demand of people on nutritious grain, making both natural and safe food possible. [Method] Hardness indices of wheat were measured and layering peeling and milling technology was adopted to explore nutrients distribution in color wheat and effect of hardness on milling of wheat layers. [Result] The results indicated that total content of amino acid in color wheat was higher than that of common wheat by 13.91%-23.32%; Zhongpu Black 1 and Zhongpu Green 1 exceeded common wheat in Zn, Fe and Ca, but Zhongpu Purple 1 was generally lower; Zhongpu Green 1 was significantly higher in Fe and Ca by 371.80% and 102.86%, respectively. Mean- while, it was found that nutrients distribution of color wheat was similar to that of common ,one, namely, pericarp, testa, aleurone layer and embryo were abundant with nutrients. In addition, color wheat was concluded nutritious one and milling in- dustrialization of wheat layers could be achieved through layer-milling and separation technology. Furthermore, wheat hardness was proved the key element influencing milling of wheat layers. [Conclusion] The research set an example for nutrition development and utilization of color wheat.展开更多
Here we report on simultaneous lidar observations of sporadic Ni(Nis)layers and sporadic Na(Nas)layers in the atmosphere over Yanqing,Beijing(40.42°N,116.02°E)from April 2019 to October 2022.During 343 night...Here we report on simultaneous lidar observations of sporadic Ni(Nis)layers and sporadic Na(Nas)layers in the atmosphere over Yanqing,Beijing(40.42°N,116.02°E)from April 2019 to October 2022.During 343 nights of observation,68 Nis and 56 Nas were observed.The seasonal variation of Nis and Nas was also obtained,with the highest occurrence of Nis being in July(43%)and that of Nas being in June(61%).We found that the seasonal variation of Nis is similar to that of Nas and that both occur more frequently in summer than in winter.In addition,we found 23 events in which Nis and Nas occur simultaneously.The average peak altitude of Nas is approximately 1 km higher than that of Nis,and the peak density ratio of Nas to Nis is approximately 5,which is half the density ratio of the two main layers.Additionally,the strength factor for Nas is smaller than that for Nis.Through data analysis of sporadic E layers(Es),we found that Nis and Nas has a significant correlation with Es.The neutralization rates of Ni^(+)/Na^(+)were calculated according to the dissociative recombination reaction of Ni^(+)/Na^(+)and the WACCM-Ni(Whole Atmosphere Community Climate Model of Ni).The production rates of Ni and Na were estimated to be approximately 1:4.4,which is consistent with the density ratio of Nis to Nas.The results showed that the neutralization reaction of Ni+,Na+,and electrons in Es is the main reason for the formation of the Nis layer and the Nas layer.展开更多
If you're tired of megacities that feel like nothing but glass,steel,and constant rush,Guangzhou moves at its own pace.Here,a 19th-century ancestral hall stands next to a 600-meter tower,and the day begins with te...If you're tired of megacities that feel like nothing but glass,steel,and constant rush,Guangzhou moves at its own pace.Here,a 19th-century ancestral hall stands next to a 600-meter tower,and the day begins with tea and delicate steamed treats instead of coffee.展开更多
Interfacial engineering is crucial for developing high-performance Ni-rich layered cathodes for lithiumion batteries.Here,we introduce an interfacial precipitation(IP)strategy,guided by first-principles calculations,t...Interfacial engineering is crucial for developing high-performance Ni-rich layered cathodes for lithiumion batteries.Here,we introduce an interfacial precipitation(IP)strategy,guided by first-principles calculations,to create a functionally graded cathode during precursor synthesis.Based on thermodynamic principles of bulk insolubility and phase separation kinetics,we achieved the selective precipitation of Co onto the surface of a Ni-rich hydroxide precursor.Upon high-temperature lithiation,this engineered precursor spontaneously forms a unique,bifunctional Co-rich spinel-like layer on the final LiNi_(0.88)Co_(0.06)Mn_(0.06)O_(2)(NCM)cathode.This architecture suppresses detrimental Li/Ni cation mixing and protects the active material.Consequently,the IP-driven NCM cathode demonstrates vastly superior rate capability,delivering 140.8 m A h g^(-1)at 5C,compared to 112.9 mA h g^(-1)for its conventionally prepared counterpart.This enhancement is attributed to significantly lower charge-transfer resistance and faster kinetics.Remarkably,in a full-cell configuration,the IP-driven NCM cathode maintains 81.5%capacity after 1000 cycles at an aggressive 5C rate.This work presents a thermodynamically driven,scalable strategy for designing advanced cathodes with exceptional high-power performance and stability.展开更多
Significant progress has been achieved in the field of organic solar cells(OSCs). Most devices with power conversion efficiencies(PCEs) exceeding 20% rely predominantly on active materials that incorporate D18 or its ...Significant progress has been achieved in the field of organic solar cells(OSCs). Most devices with power conversion efficiencies(PCEs) exceeding 20% rely predominantly on active materials that incorporate D18 or its derivatives as the donor. In contrast, the PCEs over 20% have been realized as well for OSCs with the non-D18-based donor materials by simultaneously optimizing material properties, active layer morphologies and interface engineering, thereby demonstrating the potential to outperform D18 counterparts. Therefore, this review summarizes an overview of recent advancements in OSCs with the PCEs over20% utilizing the non-D18-based donor materials, and highlights three critical aspects including molecular design strategies,the active layer morphologies, and the interface optimization. Their synergistic roles are advantageous in enhancing the exciton dissociation, facilitating the charge transport, and suppressing the recombination losses, accordingly supporting the improved PCEs over 20%. Furthermore, the challenges and valuable insights are discussed, which can lead to improved efficiency, scalable fabrication, and enhanced environmental and thermal stability, potentially accelerating the commercialization of OSCs.展开更多
A novel trace nickel(Ni)doped tungsten(W)matrix with coated Ni on W grains was prepared by powder metallurgy method.The introduction of Ni can inhibit the reaction between W and barium-calcium aluminates(Ba-Ca alumina...A novel trace nickel(Ni)doped tungsten(W)matrix with coated Ni on W grains was prepared by powder metallurgy method.The introduction of Ni can inhibit the reaction between W and barium-calcium aluminates(Ba-Ca aluminates)during the impregnation process of the matrix.After cathode activation,the surface Ba:O molar ratio is 0.88:1.00,much higher than the Ba dispenser cathode without Ni doping.The XPS results of the cathode surface showed that the metallic Ba appeared on the activated cathode surface,forming dipoles with oxygen,and effectively reducing the cathode surface work function.The pulse electron emission current density at 1100℃_(b)(brightness temperature)was 18.26 A/cm^(2),and the calculated work function was 1.97 eV.It has a low evaporation rate and the accelerated lifetime test predict a lifetime of over 160000 h.First-principles calculations showed that the charge transfer and dipole moment in the NiW-BaO system were both increased compared to the Ba dispenser cathode,thus improving the emission performance of the Ni-W mixed matrix cathode.展开更多
Zeolite imidazolate framework(ZIF)-derived bimetallic sulfides and layered double hydroxides(LDHs)have emerged as promising electrode materials for supercapacitors,owing to their porous layered structures,high electro...Zeolite imidazolate framework(ZIF)-derived bimetallic sulfides and layered double hydroxides(LDHs)have emerged as promising electrode materials for supercapacitors,owing to their porous layered structures,high electrochemical activity,tun-able molecular architectures,low cost,and high specific capacitance.In this study,a unique composite material comprising ZIF-derived ZnCo bimetallic sulfide and LDH with a honeycomb-like structure was in situ grown on nickel foil(NF)via a con-trolled self-sacrificial template strategy.In contrast to previous reports,the resulting ZnS@Co_(3)S_(4)@MXene@Ni-LDH/NF compos-ite integrates the advantages of MXene,LDH,and sulfides,leading to significantly enhanced conductivity,structural stability,and catalytic activity.The ZnS@Co_(3)S_(4)@MXene@Ni-LDH/NF electrode exhibits a uniform network structure with a thickness of approximately 1μm coated on NF,and delivers a high specific capacitance of 1356.1 F·g^(-1)at a current density of 2 A·g^(-1).Further-more,an asymmetric supercapacitor assembled with ZnS@Co_(3)S_(4)@MXene@Ni-LDH/NF as the positive electrode and activated car-bon as the negative electrode achieves a high energy density of 34.08 Wh·kg^(-1)and a power density of 742.3 W·kg^(-1)at 1 A·g^(-1).This device successfully powers LED lights for 5 min,demonstrating its practical applicability.These results underscore the out-standing electrochemical performance of the ZnS@Co_(3)S_(4)@MXene@Ni-LDH/NF electrode,highlighting its potential for applica-tions in supercapacitors and related energy storage fields.展开更多
AIM:To describe the technique and the outcomes of manual Bowman layer and stroma transplant-onlay(BLST-o)for 2 cases of radial keratotomy(RK).METHODS:Two patients with visual fluctuations and corneal irregularity due ...AIM:To describe the technique and the outcomes of manual Bowman layer and stroma transplant-onlay(BLST-o)for 2 cases of radial keratotomy(RK).METHODS:Two patients with visual fluctuations and corneal irregularity due to RK were offered manual BLST-o as an alternative to penetrating keratoplasty(PKP).Visual acuity,refraction,corneal topography,corneal aberrometry,and corneal optical coherence tomography(OCT)pre-and postoperative were analyzed.Histology was obtained for 1 case.RESULTS:Both patients had corneal anatomical and morphological improvement,with elimination of the visual fluctuations.In one case,a subsequent excimer laser treatment improved corneal shape further,thus improving vision.The other case,whereas initially improved,developed epithelial ingrowth following suture removal.The latter was explanted and had a xenogeneic implant.The explanted sample was sent for histology,showing a viable graft of Bowman layer and anterior stroma.CONCLUSION:Manual BLST-o is a potential option for the management of symptoms post RK.These grafts may facilitate subsequent treatments such as laser corrections,and may not preclude from other interventions after explantation.展开更多
Numerical simulations and theoretical models are developed in this paper for the Detonation-Wave/Boundary-Layer Interactions(DWBLIs)under reflections.Transient flow fields demonstrate the highly non-stationarity of th...Numerical simulations and theoretical models are developed in this paper for the Detonation-Wave/Boundary-Layer Interactions(DWBLIs)under reflections.Transient flow fields demonstrate the highly non-stationarity of the DWBLIs when Mach Reflection(MR)occur,and subsequent analyses show that the subsonic region introduced by the boundary layer exacerbates the instability.Further quantitative analyses show that viscosity has little effect on propulsive performance and the separation wave can be considered as an oblique detonation wave.Influence parameters to DWBLIs such as combustion chamber height,incoming Mach number,equivalence ratio,and inlet channel length are categorized and studied.Besides simulations,theoretical analytical modeling is established for Regular Reflection(RR)and MR of DWBLIs.Multiple formulas for the separation zone length are obtained according to the mass conservation under different transformation type between inviscid and viscid reflections.Comparison with the numerical simulations verifies the validity of the model and it can be further generalized to the curved DWBLIs.The developed model makes the theoretical solution process of DWBLIs possible and provides the key foundation for further analysis and solution.展开更多
Artificial photosynthesis of hydrogen peroxide(H_(2)O_(2))from earth-abundant water and oxygen is a sustainable approach,however current photocatalysts suffer from low production rate and solar-to-chemical conversion ...Artificial photosynthesis of hydrogen peroxide(H_(2)O_(2))from earth-abundant water and oxygen is a sustainable approach,however current photocatalysts suffer from low production rate and solar-to-chemical conversion efficiency(<1.5%).Herein,we report that nickelchromium layered double hydroxide with intercalated nitrate(NiCrOOH-NO_(3))and a thickness of~4.4 nm is an efficient photocatalyst,enabling a H_(2)O_(2)production yield of 28.7 mmol g^(-1)h^(-1)under visible light irradiation with3.92%solar-to-chemical conversion efficiency.Experimental and computational studies have revealed an inherent facet-dependent reduction-oxidation reaction behavior and spatial separation of photogenerated electrons and holes.An unexpected role of intercalated nitrate is demonstrated,which promotes excited electron—hole spatial separation and facilitates the electron transfer to oxygen intermediate via delocalization.This work provides understandings in the impact of nanostructure and anion in the design of advanced photocatalysts,paving the way toward practical synthesis of H_(2)O_(2)using fully solar-driven renewable energy.展开更多
Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthes...Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.展开更多
High-entropy layered hydroxides(HELHs),an emerging frontier in entropy-stabilized materials derived from layered double hydroxides(LDHs),have captivated attention with their unparalleled tunability,thermodynamic stabi...High-entropy layered hydroxides(HELHs),an emerging frontier in entropy-stabilized materials derived from layered double hydroxides(LDHs),have captivated attention with their unparalleled tunability,thermodynamic stability,and electrochemical performance.The integration of the high-entropy concept into LDHs empowers HELHs to surmount the constraints of conventional materials through compositional diversity,structurally disordered configurations,and synergistic multi-element interactions.This review systematically embarks on their synthesis methodologies,functional mechanisms,and applications in energy conversion/storage and biomedicine.Advanced synthesis strategies,such as plasma-assisted hydrothermal methods,facilitate precise control over HELH architectures while supporting scalable production.HELHs demonstrate superior electrochemical performance in critical reactions,including oxygen evolution reaction,water oxidation,hydrogen evolution,and glucose electrooxidation.Future directions encompass integrating in situ characterization with simulations,leveraging machine learning for composition screening,and expanding HELHs application through interdisciplinary collaborations.This work establishes a comprehensive roadmap for advancing HELHs as next-generation multifunctional platforms for sustainable energy and biomedical technologies.展开更多
基金Project no.RRF-2.3.1-21-2022-00015 has been implemented with the support provided by the European Unionsupported by the Agency for Credits and Study Grants coordinated by the Romanian Ministry of National Education from the source of the research grant established through the Government Decision no.118/2023+1 种基金supported by the EKÖP-24-3-BME-103 New National Excellence Program of the Ministry for Culture and Innovation from the source of the National,Research,Development and Innovation Fundsupported by the Doctoral Excellence Fellowship Programme(DCEP)is funded by the National Research Development and Innovation Fund of the Ministry of Culture and Innovation and the Budapest University of Technology and Economics,under a grant agreement with the National Research,Development and Innovation Office.
文摘In this study,an artificial intelligence-based machine vision system was developed for in-line particle size analysis during the pellet layering process.Drug-layered pellets were produced by coating microcrystalline cellulose cores with an ibuprofen-containing layering liquid until the target drug content was achieved.Drug content increases with pellet size;therefore,particle size monitoring can ensure product safety and quality.The direct imaging system,consisting of a rigid endoscope,a light source,and a high-speed camera,provides real-time information about pellet size and layer uniformity,enabling timely intervention in the case of out-of-spec products.A convolutional neural network-based instance segmentation algorithm was employed to detect particles in focus,ensuring that pellet size could be accurately determined despite the dense flow of the particles.After training the model,the performance of the developed system was assessed by analysing the particle size distribution of pellet cores with variable sizes within the 250 e850 mm size range.The endoscopic system was tested in-line at a larger scale during the drug layering of inert pellet cores.The particle size data acquired in real time with the endoscopic imaging system corresponded with the reference methods,demonstrating the feasibility of the proposed machine vision-based method as a process analytical technology tool for in-line process monitoring.
基金supported by the Natural Science Foundation of China Grant No.52272289 and 5240223,and JSPS(Japan Society for the Promotion of Science)of Grant No.22K19088,23H00313,24H02202,and 24H02205。
文摘NiFe-layered double hydroxides(NiFe-LDHs)are among the most promising earth-abundant electrocatalysts for the oxygen evolution reaction(OER)in alkaline media.However,their practical application is hindered by intrinsic activity limitations and poor stability,primarily due to the asymmetric adsorption of oxygen intermediates.To overcome this,the binding strength must be synergistically tuned to a moderate level to optimize catalytic performance.Here,we engineered NiFeCoCr LDH through Co doping to enhance electrical conductivity and controlled Cr leaching to introduce cationic vacancies for modulating intermediate binding strength in NiFe LDH.X-ray absorption near-edge structure and extended X-ray absorption fine structure analyses reveal that NiFe-LDH with Co doping and Cr vacancies modulates the Ni oxidation state and local coordination environment,leading to a balanced electronic structure and enhanced structural complexity around the Ni sites.Additionally,these vacancies can trap OH^(-)/H_(2)O species,which can serve as a reservoir for OH^(-) transfer,facilitating the rapid formation of OER intermediates and enhancing catalytic performance at high current densities.As a result,V_(Cr)-NiFeCo LDH achieves 1.6 A cm^(-2)current density at 1.7 V vs.RHE while maintaining stable operation for over 1000 h at 500 mA cm^(-2).Density functional theory(DFT)calculations validate the synergistic effects of Co doping and Cr-induced vacancies on intermediate binding energies and improved OER kinetics.Overall,this work presents a rational design strategy to simultaneously enhance the activity and durability of NiFe-based OER catalysts for their application in high-performance alkaline water electrolysis.
基金Supported by National Natural Science Foundation of China(22378180,22078141)Education Department Foundation of Liaoning Province(JYTMS20230960)。
文摘To deepen understanding of the evolution of coal char microstructural properties of coal char during the co-pyrolysis of coking coal with additives,this study incorporated two typical additives,coal tar pitch(CTP)and waste plastic(HDPE),into a blended coal sample and carried out pyrolysis experiments.The pyrolysis process and the microstructure of char were systematically characterized using various analytical techniques,including thermogravimetric analysis(TGA),X-ray diffraction(XRD)and Raman spectroscopy.Data correlation analysis was performed to reveal the mechanism of carbon structural ordering evolution within the critical temperature range(350−600℃)from colloidal layer formation to semi-coke conversion in coking coal,and to elucidate the regulatory effects of different additives on coal pyrolysis pathways.The results indicate that HDPE releases free radicals during high-temperature pyrolysis,accelerating the pyrolysis reaction and increase the yield of volatile components.Conversely,CTP facilitates pyrolysis at low temperatures through its light components,thereby delaying high-temperature reactions due to the colloidal layer’s effect.XRD results indicate that during the process of pyrolysis,there is a progressive decrease in the interlayer spacing of aromatic layers(d002),while the aromatic ring stacking height(L_(c))and lateral size(L_(a))undergo significant of carbon skeleton ordering.Further comparative reveals that CTP partially suppresses structural ordering at low temperatures,whereas HDPE promotes the condensation and alignment of aromatic clusters via a free radical mechanism.Raman spectroscopy reveals a two-stage reorganization mechanism in the microstructure of the coal char:the decrease in the I_(D)/I_(G)ratio between 350 and 550℃is primarily attributed to the cleavage of aliphatic side chains and cross-linking bonds,leading to a reduction in defective structures;whereas the increase in ID/IG between 550 and 600℃is closely associated with enhanced condensation reactions of aromatic structures.Correlation analysis further demonstrates progressive graphitization during pyrolysis,with a significant positive correlation(R^(2)>0.85)observed between d002 and the full width at half maximum of the G-band(FWHM-G).
基金Special Fund for Key Technologies in Blockchain of Shanghai Scientific and Technological Committee(23511100300)。
文摘Post-quantum transport layer security(PQ-TLS)is capable of effectively defending against quantum threats to current network communications,whereas its larger public key and certificate sizes as well as higher computational overhead may result in a significant performance reduction compared with conventional TLS.In this paper,we present a systematic evaluation of PQ-TLS performance across diverse deployment scenarios to address the following critical research questions.(1)What is the performance behavior of PQ-TLS across different TLS modes?(2)How does PQ-TLS perform across varying client scales?(3)Which network topology is most suitable for PQ-TLS?(4)How does PQ-TLS perform on personal computers(PCs)compared to embedded IoT devices?To the best of our knowledge,this is the first work to comprehensively address these issues,offering implementers some insights into PQ-TLS performance and guidance for optimizing it across diverse scenarios.
文摘The morphology of active layer plays a critical role in determining the photovoltaic performance of organic solar cells(OSCs).However,binary blends often suffer from suboptimal phase separation,which limits the efficiency of OSCs.Herein,two bridging polymer acceptors(PAs)—benzodithiophene-(2-ethylhexyl)oxy(BDT-C2C4)and benzodithiophene-octyloxy(BDT-C_(8))—are designed and synthesized by combining a benzodithiophene(BDT)unit as the donor moiety[poly({4,8-bis[5-(2-ethylhexyl)-4-fluorothiophen-2-yl]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl}){5,8-bis[4-(2-butyloctyl)thiophen-2-yl]dithieno[3',2':3,4]},D18],and a 2,2′-((2Z,2′Z)-{[12,13-Bis(2-butyloctyl)-12,13-dihydro-3,9-dinonylthieno[2,3]thieno[3,2-b]pyrrolo[4,5-g]thieno[2,3-b]indole-2,10-diyl]bis(methanylylidene)}bis(3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile(Y6)derivative as the acceptor moiety.BDT-C2C4 and BDT-C_(8) are functionalized with(2-ethylhexyl)oxy and octyloxy side chains on the BDT unit,respectively.Both PAs show complementary absorption and cascaded energy levels with the donor D18 and the acceptor 2,2′-((2Z,2′Z)-{[12,13-bis(3-ethylheptyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2″,3″∶4′,5′]thieno[2′,3′∶4,5]pyrrolo[3,2-g]thieno[2′,3′∶4,5]thieno[3,2-b]indole-2,10-diyl]bis(meth⁃aneylylidene)}bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile(N3),but BDT-C_(8) exhibits better compatibility with D18 and N3 compared to BDT-C2C4.When incorporated as a third component into the D18∶N3 blend,both PAs improve the active layer morphology.In particular,the D18∶N3∶BDT-C_(8) blend shows significantly optimized morphology,featuring reduced phase separation and a fibrous network structure.As a result,the device based on D18∶N3∶BDT-C_(8) achieves a power conversion efficiency of 18.18%,significantly higher than that of the device based on D18∶N3(ca.17.37%).This work presents a compatibilizer strategy for optimizing blend morphology towards high-performance ternary OSCs.
基金supported by the National KeyR&D Program of China(Grant No.2024YFB3817400)the National Natural Science Foundation of China(Grants No.12274276 and No.U24A6002)+1 种基金the Natural Science Foundation of Shanxi Province(China)(Grant No.202403021223008)Supported by Scientific and Technology Innovation Programs of Higher Education Institutions in Shanxi(Grant No.2024Q017 and No.2025L043).
文摘Layered transition-metal compounds(LTMCs)feature stacked architectures,strong magnetic anisotropy,and tunable magnetic order,making them promising material platforms for low-power spintronic technologies and for enabling topological functionalities in the post-Moore era.Here we review recent progress on two-dimensional(2D)magnetism in LTMCs,emphasizing material taxonomy,intrinsic magnetic properties,and external-field controls.This review first presents a classification of LTMCs by crystal structure and chemistry—binary halides,chalcogenides,and ternary families(e.g.,MPX_(3),M_(m)X_(n)Te_(k),MnBi_(2)Te_(4))—followed by a summary of their coupling mechanisms,ordering temperatures,and dimensional effects.It then analyzes the modulation of exchange interactions,magnetic anisotropy,and topological states by electric-field gating,strain engineering,and ion intercalation,with representative experimental demonstrations.Notable advances include room-temperature ferromagnetic metals and semiconductors,observation of the quantum anomalous Hall effect(QAHE)in MnBi2Te4,and synergistic control of magnetic-topological states under multiple external stimuli.Persistent challenges involve the limited availability of intrinsic 2D magnetic semiconductors with high Curie temperatures(Tc),incomplete understanding of the microscopic couplings at interfaces and under quantum confinement,and device-level stability.We conclude by outlining opportunities that lie in the integration of multiscale characterization,first-principles theory,and cross-scale fabrication to precisely co-engineer magnetism,topology,and electronic structure,thereby advancing LTMCs toward spintronic and topological-quantum applications.
文摘AlGaN-based deep-ultraviolet(DUV)laser diodes(LDs)face performance challenges due to elec-tron leakage and poor hole injection which is often worsened by polarization effects from conventional elec-tron blocking layers(EBLs).To overcome these limitations,we propose an EBL-free DUV LD design incor-porating a 1-nm undoped Al_(0.8)Ga_(0.2)N thin strip layer after the last quantum barrier.Using PICS3D simula-tions,we evaluate the optical and electrical characteristics.Results show a significant increase in effective electron barrier height(from 158.2 meV to 420.7 meV)and a reduction in hole barrier height(from 149.2 meV to 62.8 meV),which enhance hole injection and reduce electron leakage.The optimized structure(LD3)achieves a 14%increase in output power,improved slope efficiency(1.85 W/A),and lower threshold current.This design also reduces the quantum confined Stark effect and forms dual hole accumulation regions,im-proving recombination efficiency.
基金Supported by National Natural Science Foundtion of China in2011(31171789)~~
文摘[Objective] The aim was to promote color wheat industrialization and meet the demand of people on nutritious grain, making both natural and safe food possible. [Method] Hardness indices of wheat were measured and layering peeling and milling technology was adopted to explore nutrients distribution in color wheat and effect of hardness on milling of wheat layers. [Result] The results indicated that total content of amino acid in color wheat was higher than that of common wheat by 13.91%-23.32%; Zhongpu Black 1 and Zhongpu Green 1 exceeded common wheat in Zn, Fe and Ca, but Zhongpu Purple 1 was generally lower; Zhongpu Green 1 was significantly higher in Fe and Ca by 371.80% and 102.86%, respectively. Mean- while, it was found that nutrients distribution of color wheat was similar to that of common ,one, namely, pericarp, testa, aleurone layer and embryo were abundant with nutrients. In addition, color wheat was concluded nutritious one and milling in- dustrialization of wheat layers could be achieved through layer-milling and separation technology. Furthermore, wheat hardness was proved the key element influencing milling of wheat layers. [Conclusion] The research set an example for nutrition development and utilization of color wheat.
基金supported by the Specialized Research Fund for State Key Laboratories,Chinese Meridian Project,the Specialized Research Fund for the State Key Laboratory of Solar Activity and Space Weather,postgraduate Education Reform and Quality Improvement Project of Henan Province(Grant No.YJS2024JD32)Natural Science Foundation Project of Henan Province(Grant No.242300420253)National Natural Science Foundation of China for Young Scientists(Grant No.42504156)funding.
文摘Here we report on simultaneous lidar observations of sporadic Ni(Nis)layers and sporadic Na(Nas)layers in the atmosphere over Yanqing,Beijing(40.42°N,116.02°E)from April 2019 to October 2022.During 343 nights of observation,68 Nis and 56 Nas were observed.The seasonal variation of Nis and Nas was also obtained,with the highest occurrence of Nis being in July(43%)and that of Nas being in June(61%).We found that the seasonal variation of Nis is similar to that of Nas and that both occur more frequently in summer than in winter.In addition,we found 23 events in which Nis and Nas occur simultaneously.The average peak altitude of Nas is approximately 1 km higher than that of Nis,and the peak density ratio of Nas to Nis is approximately 5,which is half the density ratio of the two main layers.Additionally,the strength factor for Nas is smaller than that for Nis.Through data analysis of sporadic E layers(Es),we found that Nis and Nas has a significant correlation with Es.The neutralization rates of Ni^(+)/Na^(+)were calculated according to the dissociative recombination reaction of Ni^(+)/Na^(+)and the WACCM-Ni(Whole Atmosphere Community Climate Model of Ni).The production rates of Ni and Na were estimated to be approximately 1:4.4,which is consistent with the density ratio of Nis to Nas.The results showed that the neutralization reaction of Ni+,Na+,and electrons in Es is the main reason for the formation of the Nis layer and the Nas layer.
文摘If you're tired of megacities that feel like nothing but glass,steel,and constant rush,Guangzhou moves at its own pace.Here,a 19th-century ancestral hall stands next to a 600-meter tower,and the day begins with tea and delicate steamed treats instead of coffee.
基金supported by grants from the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(MSIT)(RS-2024-00407116)+1 种基金by the Ministry of Education(NRF-2018R1A6A1A03024231)support from the NRF grant funded by the MSIT(RS-2024-00406724)。
文摘Interfacial engineering is crucial for developing high-performance Ni-rich layered cathodes for lithiumion batteries.Here,we introduce an interfacial precipitation(IP)strategy,guided by first-principles calculations,to create a functionally graded cathode during precursor synthesis.Based on thermodynamic principles of bulk insolubility and phase separation kinetics,we achieved the selective precipitation of Co onto the surface of a Ni-rich hydroxide precursor.Upon high-temperature lithiation,this engineered precursor spontaneously forms a unique,bifunctional Co-rich spinel-like layer on the final LiNi_(0.88)Co_(0.06)Mn_(0.06)O_(2)(NCM)cathode.This architecture suppresses detrimental Li/Ni cation mixing and protects the active material.Consequently,the IP-driven NCM cathode demonstrates vastly superior rate capability,delivering 140.8 m A h g^(-1)at 5C,compared to 112.9 mA h g^(-1)for its conventionally prepared counterpart.This enhancement is attributed to significantly lower charge-transfer resistance and faster kinetics.Remarkably,in a full-cell configuration,the IP-driven NCM cathode maintains 81.5%capacity after 1000 cycles at an aggressive 5C rate.This work presents a thermodynamically driven,scalable strategy for designing advanced cathodes with exceptional high-power performance and stability.
基金support from the National Key Research and Development Program of China (2022YFB3803300)the National Natural Science Foundation of China (U23A20138 and 52173192)Hunan Provincial Major Basic Research Project (2025JC0004)。
文摘Significant progress has been achieved in the field of organic solar cells(OSCs). Most devices with power conversion efficiencies(PCEs) exceeding 20% rely predominantly on active materials that incorporate D18 or its derivatives as the donor. In contrast, the PCEs over 20% have been realized as well for OSCs with the non-D18-based donor materials by simultaneously optimizing material properties, active layer morphologies and interface engineering, thereby demonstrating the potential to outperform D18 counterparts. Therefore, this review summarizes an overview of recent advancements in OSCs with the PCEs over20% utilizing the non-D18-based donor materials, and highlights three critical aspects including molecular design strategies,the active layer morphologies, and the interface optimization. Their synergistic roles are advantageous in enhancing the exciton dissociation, facilitating the charge transport, and suppressing the recombination losses, accordingly supporting the improved PCEs over 20%. Furthermore, the challenges and valuable insights are discussed, which can lead to improved efficiency, scalable fabrication, and enhanced environmental and thermal stability, potentially accelerating the commercialization of OSCs.
基金supported by the National Natural Science Foundation of China(Nos.U2341209 and 52130407).
文摘A novel trace nickel(Ni)doped tungsten(W)matrix with coated Ni on W grains was prepared by powder metallurgy method.The introduction of Ni can inhibit the reaction between W and barium-calcium aluminates(Ba-Ca aluminates)during the impregnation process of the matrix.After cathode activation,the surface Ba:O molar ratio is 0.88:1.00,much higher than the Ba dispenser cathode without Ni doping.The XPS results of the cathode surface showed that the metallic Ba appeared on the activated cathode surface,forming dipoles with oxygen,and effectively reducing the cathode surface work function.The pulse electron emission current density at 1100℃_(b)(brightness temperature)was 18.26 A/cm^(2),and the calculated work function was 1.97 eV.It has a low evaporation rate and the accelerated lifetime test predict a lifetime of over 160000 h.First-principles calculations showed that the charge transfer and dipole moment in the NiW-BaO system were both increased compared to the Ba dispenser cathode,thus improving the emission performance of the Ni-W mixed matrix cathode.
基金support by NSFC(No.61704047)Natural Science Foundation of Henan Province(No.242300420271)Key Research Project of Henan Provincial Higher Education(No.24A430008).
文摘Zeolite imidazolate framework(ZIF)-derived bimetallic sulfides and layered double hydroxides(LDHs)have emerged as promising electrode materials for supercapacitors,owing to their porous layered structures,high electrochemical activity,tun-able molecular architectures,low cost,and high specific capacitance.In this study,a unique composite material comprising ZIF-derived ZnCo bimetallic sulfide and LDH with a honeycomb-like structure was in situ grown on nickel foil(NF)via a con-trolled self-sacrificial template strategy.In contrast to previous reports,the resulting ZnS@Co_(3)S_(4)@MXene@Ni-LDH/NF compos-ite integrates the advantages of MXene,LDH,and sulfides,leading to significantly enhanced conductivity,structural stability,and catalytic activity.The ZnS@Co_(3)S_(4)@MXene@Ni-LDH/NF electrode exhibits a uniform network structure with a thickness of approximately 1μm coated on NF,and delivers a high specific capacitance of 1356.1 F·g^(-1)at a current density of 2 A·g^(-1).Further-more,an asymmetric supercapacitor assembled with ZnS@Co_(3)S_(4)@MXene@Ni-LDH/NF as the positive electrode and activated car-bon as the negative electrode achieves a high energy density of 34.08 Wh·kg^(-1)and a power density of 742.3 W·kg^(-1)at 1 A·g^(-1).This device successfully powers LED lights for 5 min,demonstrating its practical applicability.These results underscore the out-standing electrochemical performance of the ZnS@Co_(3)S_(4)@MXene@Ni-LDH/NF electrode,highlighting its potential for applica-tions in supercapacitors and related energy storage fields.
文摘AIM:To describe the technique and the outcomes of manual Bowman layer and stroma transplant-onlay(BLST-o)for 2 cases of radial keratotomy(RK).METHODS:Two patients with visual fluctuations and corneal irregularity due to RK were offered manual BLST-o as an alternative to penetrating keratoplasty(PKP).Visual acuity,refraction,corneal topography,corneal aberrometry,and corneal optical coherence tomography(OCT)pre-and postoperative were analyzed.Histology was obtained for 1 case.RESULTS:Both patients had corneal anatomical and morphological improvement,with elimination of the visual fluctuations.In one case,a subsequent excimer laser treatment improved corneal shape further,thus improving vision.The other case,whereas initially improved,developed epithelial ingrowth following suture removal.The latter was explanted and had a xenogeneic implant.The explanted sample was sent for histology,showing a viable graft of Bowman layer and anterior stroma.CONCLUSION:Manual BLST-o is a potential option for the management of symptoms post RK.These grafts may facilitate subsequent treatments such as laser corrections,and may not preclude from other interventions after explantation.
基金support of the National Natural Science Foundation of China(Nos.U20A2069,U21B6003,12302389 and 12472337)the Advanced Aero-Power Innovation Workstation,China(No.HKCX2024-01-017)。
文摘Numerical simulations and theoretical models are developed in this paper for the Detonation-Wave/Boundary-Layer Interactions(DWBLIs)under reflections.Transient flow fields demonstrate the highly non-stationarity of the DWBLIs when Mach Reflection(MR)occur,and subsequent analyses show that the subsonic region introduced by the boundary layer exacerbates the instability.Further quantitative analyses show that viscosity has little effect on propulsive performance and the separation wave can be considered as an oblique detonation wave.Influence parameters to DWBLIs such as combustion chamber height,incoming Mach number,equivalence ratio,and inlet channel length are categorized and studied.Besides simulations,theoretical analytical modeling is established for Regular Reflection(RR)and MR of DWBLIs.Multiple formulas for the separation zone length are obtained according to the mass conservation under different transformation type between inviscid and viscid reflections.Comparison with the numerical simulations verifies the validity of the model and it can be further generalized to the curved DWBLIs.The developed model makes the theoretical solution process of DWBLIs possible and provides the key foundation for further analysis and solution.
基金support from the National Natural Science Foundation of China(NSFC 21905092,22475072 and 22075085)the Fundamental Research Funds for the Central Universities+1 种基金supported by the Shanghai Frontiers Science Center of Molecule Intelligent SynthesesEast China Normal University Multifunctional Platform for Innovation(004)。
文摘Artificial photosynthesis of hydrogen peroxide(H_(2)O_(2))from earth-abundant water and oxygen is a sustainable approach,however current photocatalysts suffer from low production rate and solar-to-chemical conversion efficiency(<1.5%).Herein,we report that nickelchromium layered double hydroxide with intercalated nitrate(NiCrOOH-NO_(3))and a thickness of~4.4 nm is an efficient photocatalyst,enabling a H_(2)O_(2)production yield of 28.7 mmol g^(-1)h^(-1)under visible light irradiation with3.92%solar-to-chemical conversion efficiency.Experimental and computational studies have revealed an inherent facet-dependent reduction-oxidation reaction behavior and spatial separation of photogenerated electrons and holes.An unexpected role of intercalated nitrate is demonstrated,which promotes excited electron—hole spatial separation and facilitates the electron transfer to oxygen intermediate via delocalization.This work provides understandings in the impact of nanostructure and anion in the design of advanced photocatalysts,paving the way toward practical synthesis of H_(2)O_(2)using fully solar-driven renewable energy.
基金supported by the National Natural Science Foundation of China (No.52274304)。
文摘Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.
基金the financial support by Advanced Materials-National Science and Technology Major Project(2024ZD0607400)the National Natural Science Foundation of China(No.52402305)+4 种基金the high-level innovation and entrepreneurship talent project of Qinchuangyuan(No.QCYRCXM-2023-084)the Postdoctoral Fellowship Program of CPSF under Grant Number GZB20230570 and 2024M752552Key projects of Shaanxi Province,China(2023GXLH-001)Natural Science Basic Research Program of Shaanxi(Program No.2024JCYBQN-0494,No.2022TD-27)the State Key Laboratory for Electrical Insulation and Power Equipment(No.EIPE23125)。
文摘High-entropy layered hydroxides(HELHs),an emerging frontier in entropy-stabilized materials derived from layered double hydroxides(LDHs),have captivated attention with their unparalleled tunability,thermodynamic stability,and electrochemical performance.The integration of the high-entropy concept into LDHs empowers HELHs to surmount the constraints of conventional materials through compositional diversity,structurally disordered configurations,and synergistic multi-element interactions.This review systematically embarks on their synthesis methodologies,functional mechanisms,and applications in energy conversion/storage and biomedicine.Advanced synthesis strategies,such as plasma-assisted hydrothermal methods,facilitate precise control over HELH architectures while supporting scalable production.HELHs demonstrate superior electrochemical performance in critical reactions,including oxygen evolution reaction,water oxidation,hydrogen evolution,and glucose electrooxidation.Future directions encompass integrating in situ characterization with simulations,leveraging machine learning for composition screening,and expanding HELHs application through interdisciplinary collaborations.This work establishes a comprehensive roadmap for advancing HELHs as next-generation multifunctional platforms for sustainable energy and biomedical technologies.
