The three-dimensional particle electrode system exhibits significant potential for application in the treatment of wastewater.Nonetheless,the advancement of effective granular electrodes characterized by elevated cata...The three-dimensional particle electrode system exhibits significant potential for application in the treatment of wastewater.Nonetheless,the advancement of effective granular electrodes characterized by elevated catalytic activity and minimal energy consumption continues to pose a significant challenge.In this research,Fluorine-doped copper-carbon(F/Cu-GAC)particle electrodes were effectively synthesized through an impregnationcalcination technique,utilizing granular activated carbon as the carrier and fluorinedoped modified copper oxides as the catalytic agents.The particle electrodes were subsequently utilized to promote the degradation of 2,4,6-trichlorophenol(2,4,6-TCP)in a threedimensional electrocatalytic reactor(3DER).The F/Cu-GAC particle electrodes were polarized under the action of electric field,which promoted the heterogeneous Fenton-like reaction in which H2O2 generated by two-electron oxygen reduction reaction(2e-ORR)of O_(2) was catalytically decomposed to·OH.The 3DER equipped with F/Cu-GAC particle electrodes showed 100%removal of 2,4,6-TCP and 79.24%removal of TOC with a specific energy consumption(EC)of approximately 0.019 kWh/g·COD after 2 h of operation.The F/Cu-GAC particle electrodes exhibited an overpotential of 0.38 V and an electrochemically active surface area(ECSA)of 715 cm^(2),as determined through linear sweep voltammetry(LSV)and cyclic voltammetry(CV)assessments.These findings suggest a high level of electrocatalytic performance.Furthermore,the catalytic mechanism of the 3DER equipped with F/Cu-GAC particle electrodes was elucidated through the application of X-ray photoelectron spectroscopy(XPS),electron spin resonance(ESR),and active species capture experiments.This investigation offers a novel approach for the effective degradation of 2,4,6-TCP.展开更多
In order to explore the effect of particle position on the electrocatalytic reaction rate at different positions in three-dimensional electrocatalytic reactor,using methylene blue as the simulated organic wastewater,a...In order to explore the effect of particle position on the electrocatalytic reaction rate at different positions in three-dimensional electrocatalytic reactor,using methylene blue as the simulated organic wastewater,and spherical graphite particles as the particle electrode,the potential distribution in three-dimensional electrocatalytic reactor was simulated by using COMSOL Multiphysics software.A multivariate logarithmic regression model of reaction kinetic constant and position was established by mathematical statistics.The electrocatalytic reaction rates were predicted at different locations in the reactor.The results show that the degradation ability of particle electrode to pollutants is uneven in the electrocatalytic reactor.The increase of electric field intensity and particle size will improve the difference of reaction rate.The closer the particle electrode is to the anode,the stronger the pollutant degradation ability would be.The reaction rate of the same particle electrode at different locations varies greatly,which can be roughly divided into three regions according to the degree of difference,among which the central region of the particle has the highest electrocatalytic reaction efficiency.展开更多
This paper reports the preparation of three di‑iron complexes containing a thiazole moiety.Esterification of complex[Fe_(2)(CO)_(6)(μ‑SCH_(2)CH(CH_(2)OH)S)](1)with 4‑methylthiazole‑5‑carboxylic acid gave the correspo...This paper reports the preparation of three di‑iron complexes containing a thiazole moiety.Esterification of complex[Fe_(2)(CO)_(6)(μ‑SCH_(2)CH(CH_(2)OH)S)](1)with 4‑methylthiazole‑5‑carboxylic acid gave the corresponding ester[Fe_(2)(CO)_(6)(μ‑tedt)](2),where tedt=SCH_(2)CH(CH_(2)OOC(5‑C_(3)HNSCH_(3)))S.Further reactions of complex 2 with tri(ptolyl)phosphine(tp)or tris(4‑fluorophenyl)phosphine(fp)gave the phosphine‑substituted derivatives[Fe_(2)(CO)_(5)(tp)(μ‑tedt)](3)and[Fe_(2)(CO)_(5)(fp)(μ‑tedt)](4).The structures of the newly prepared complexes were elucidated by elemental analysis,NMR,IR,and X‑ray photoelectron spectroscopy.Moreover,single‑crystal X‑ray diffraction analysis confirmed their molecular structures,showing that they contain a di‑iron core ligated by a bridged dithiolate bearing a thiazole moiety and terminal carbonyls.The electrochemical and electrocatalytic proton reduction were probed by cyclic voltammetry,revealing that three complexes can catalyze the reduction of protons to H_(2) under the electrochemical conditions.For comparison,complex 4 possessed the best efficiency with a turnover frequency of 23.5 s^(-1)at 10 mmol·L^(-1)HOAc concentration.In addition,the fungicidal activity of these complexes was also investigated in this study.CCDC:2477511,2;2477512,3;2477513,4.展开更多
CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organ...CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organic frameworks(COFs)are porous crystalline materials formed by connecting organic monomers through covalent bonds.They have the characteristics of functional diversity and rich chemical properties.Their advantages,such as high porosity,a wide range of visible light absorption,and excellent charge separation efficiency,give them good potential in CO_(2)capture,separation,and conversion.Currently,Cu is a key metal in the catalytic CO_(2)reduction reaction(CO_(2)RR)for the preparation of high-value-added chemicals.The preparation of highly stable and large-pore Cu-based COFs using COFs as an ideal sacrificial template for loading Cu can be used to develop high-performance electrocatalysts and photocatalysts.In this review,we discuss the latest advancements in this field,including the development of various Cu-based COFs and their applications as catalysts for CO_(2)RR.Here,we mainly introduce the synthesis strategies,some important characterization information,and the applications of electrocatalytic and photocatalytic CO_(2)conversion using these previously reported Cu-based COFs.展开更多
Under the strategic framework of rural revitalization and agricultural modernization, Xinjiashan Specialty Coffee Base, located in Zaotang Village, Lujiang Town, Longyang District, Baoshan City, has been proactively i...Under the strategic framework of rural revitalization and agricultural modernization, Xinjiashan Specialty Coffee Base, located in Zaotang Village, Lujiang Town, Longyang District, Baoshan City, has been proactively investigating innovative models for agricultural development. Through extensive communication and collaboration, this base has established close partnerships with research institutions including Kunming University of Science and Technology, Baoshan University, and Yunnan Academy of Agricultural Sciences, with a commitment to thoroughly exploring the potential for resource recycling and ecological complementarity. An innovative four-in-one three-dimensional integrated planting system incorporating "coffee, bananas, green manure, and bees" has been implemented. Concurrently, technological and digital management strategies have been comprehensively integrated to improve planting efficiency. Under this model, the proportion of specialty coffee attains 71%, and the per-unit yield is 17% greater than that of the conventional planting model. This approach not only substantially enhances economic returns but also promotes the integrated development of ecological and social benefits, offering a valuable practical example and experiential reference for the specialty and sustainable advancement of the coffee industry in comparable regions.展开更多
Aerial surveys are dynamic and continuous processes,and there are different height distributions of the ground in the measurement area,which leads to problems such as overlapping measurement areas and inaccurate altit...Aerial surveys are dynamic and continuous processes,and there are different height distributions of the ground in the measurement area,which leads to problems such as overlapping measurement areas and inaccurate altitude correction during the survey process.Commonly used terrain correction methods are based on the concept of finite elementization of ground surface radioactive sources,using GPS coordinates,radar altitude,and ground elevation distribution information from aerial surveys,combined with the sourceless efficiency calibration method to construct a response matrix,which is then inverted for surface nuclide content.However,most of the sourceless efficiency calibration methods used are numerical calculations that consider the body detector as a point detector and do not consider the changes in intrinsic detection efficiency under different incident directions of gamma rays.Therefore,when the altitude of the measurement area varies significantly or the flight altitude of the aerial survey is relatively low,such sourceless efficiency calibration method calculations tend to have a large bias,which affects the accuracy of the terrain correction.To address the above problems,this study employs a novel sourceless efficiency calibration method based on the Boolean operation of the ray deposition process and simplifies the traditional body source measurement model to a surface source measurement model to achieve fast and accurate efficiency calibration.Then,through the discretization of the measurement process,the static measurement process is superposed as equivalent to the dynamic measurement process,and the dynamic measurement response matrix is built and optimized based on the calibration method.Finally,the PSO-MLEM algorithm was used to solve the dynamic measurement response matrix to achieve dynamic terrain correction of aerial survey data.Analysis of the Baiyun'ebo test area revealed that,after applying dynamic terrain correction,the inverted anomalies in uranium(eU),thorium(eTh),and potassium(K)concentrations were closer to ground measurements(within 5.72%-30.79%)and exhibited clearer anomaly boundaries compared to traditional height-based corrections.However,owing to the inherent statistical fluctuations and characteristics of matrix inversion,higher measurement values tend to absorb lower ones,potentially enlarging the anomalous regions.Nevertheless,the highanomaly regions after inversion largely coincided with the ground truth validation,demonstrating that the proposed method can effectively correct airborne gamma spectrometry data.展开更多
The two-electron electrochemical oxygen reduction reaction(ORR)affords an appealing alternative for on-site production of hydrogen peroxide(H_(2)O_(2)),which can fulfill the demands of various applications even at low...The two-electron electrochemical oxygen reduction reaction(ORR)affords an appealing alternative for on-site production of hydrogen peroxide(H_(2)O_(2)),which can fulfill the demands of various applications even at low concentrations.Under neutral or near-neutral conditions,the electrolyte environment capable of electrochemically synthesizing H_(2)O_(2) exhibits diversity and holds vast potential for practical applications;however,the electrocatalytic performance is limited without desirable electrode materials.In this contribution,methoxylated nickel hydroxides were proposed for high-performance on-site H_(2)O_(2) electrosynthesis in different potassium fertilizer solutions.The methoxylation compared to pristine Ni(OH)_(2) was demonstrated to optimize the electronic structure with favorable adsorption of reaction intermediates,obviously enhancing the activity and selectivity.In 0.10 M K_(2)SO_(4) solution,H_(2)O_(2) production ranged from 28.1 to 153.6 mg h^(-1) cm^(-2) at current densities of-50 to-250 mA cm^(-2),accompanied by Faradaic efficiency values exceeding 88.0%.An integrated system was devised by combining fertilization,disinfection,and irrigation through the coupling of two-electron ORR with agricultural irrigation,utilizing nutrient solutions as the electrolyte for on-site H_(2)O_(2) electrosynthesis.These findings afford a promising avenue for the practical application of 2e-ORR in neutral environments.展开更多
Elucidating the active site formation mechanism of bismuth(Bi)-based catalysts in electrochemical CO_(2)reduction remains challenging for achieving high activity,selectivity,and long-term stability.Here we confirm thr...Elucidating the active site formation mechanism of bismuth(Bi)-based catalysts in electrochemical CO_(2)reduction remains challenging for achieving high activity,selectivity,and long-term stability.Here we confirm through experimental results that Bi-based catalysts containing halogen ions(I^(-),Cl^(-),Br^(-))and SO_(4)^(2-)maintain the system stability,keeping Faraday efficiency of formic acid above90%in the current range of 50-800 mA cm^(-2).In contrast,anions containing S^(2-)and NO_(3)^(-)in the electrolyte can be reduced to produce by-products.These anions and their by-products could poison the active center,leading to increased side reactions and thus significantly reducing the Faraday efficiency of formic acid.The combination of non-in situ and in situ characterization results revealed that the Bi-based catalysts all underwent the transition from the initial state to the Bi/Bi_(2)O_(2)CO_(3)(BOC)intermediate state in high-concentration KHCO_(3) solution,and the different anions could selectively modulate the degree of exposure of specific crystalline surfaces of BOC.At the late stage of the reaction,BOC was completely converted to metal Bi and became the real active center.Combined with in situ IR and DFT calculations,it is further verified that^(*)OCHO is the key intermediate on the metallic Bi surface,which is most favorable for formic acid formation.This study reveals the key mechanism by which anions affect the formation of active sites via modulating the catalyst reconstruction process,which provides an important theoretical basis for the design and optimization of test conditions of Bi-based catalysts.展开更多
This insightful review explores the electrochemical principles and energy potential of electrocatalytic water splitting(EWS).It highlights recent advancements,identifies key challenges,and underscores the pivotal role...This insightful review explores the electrochemical principles and energy potential of electrocatalytic water splitting(EWS).It highlights recent advancements,identifies key challenges,and underscores the pivotal role of EWS in enabling the transition to sustainable energy systems.This work contextualizes the significance of green hydrogen in global decarbonization pathways and examines the historical progression of electrocatalysis.The fundamental thermodynamics and mechanistic pathways governing both the hydrogen and oxygen evolution reactions(HER and OER)are analyzed,highlighting energy barriers and rate-determining steps.Various electrode architectures and electrochemical cell configurations are evaluated,including a comparative assessment of key electrolyzer technologies and their performance characteristics.Furthermore,we critically examine recent advances and persistent limitations across the landscape of electrocatalysts,spanning noble metal-based materials,earth-abundant transition metal compounds,and emerging materials.Design principles and mechanistic insights drawn from electronic structu re modulation,defect engineering,doping strategies,and na noscale morphology control are elucidated to establish robust structure-property-performance relationships.Major challenges including sluggish oxygen evolution kinetics,catalyst degradation mechanisms,and the integration of devices with intermittent renewable energy sources are thoroughly examined.This work also debates advanced strategies such as hybrid photoelectrochemical systems,flexible device architectures,and the direct utilization of non-traditional water sources(e.g.,seawater,wastewater)as promising pathways for future development.Finally,it is specifically distinguished by its critical focus on bridging the gap between fundamental electrocatalysts development and practical system-level integration,addressing the challenges of scalability and deployment under industrially relevant conditions.This comprehensive review provides a strategic outlook and identifies key scientific priorities for optimizing EWS systems toward efficient,robust,and scalable hydrogen generation.展开更多
The efficient electrocatalytic oxidation of glycerol(GLY)is one of the most promising routes for the valorization of GLY.Doping has emerged as a powerful strategy to tailor the electrocatalytic performance of silver n...The efficient electrocatalytic oxidation of glycerol(GLY)is one of the most promising routes for the valorization of GLY.Doping has emerged as a powerful strategy to tailor the electrocatalytic performance of silver nanoclusters(Ag NCs),yet the effects of doping mode(surface vs.core)and the interface environment(e.g.,electrolyte concentration)on the electrocatalytic performance for Ag NCs toward GLY oxidation remain understood.In this work,surface-doped Ag_(4)M_(2)(SR)_(8) and core-doped Ag_(24)M(SR)_(18)(M=Ni,Pd,Pt;SR=SPhMe_(2))NCs were synthesized for electrocatalytic GLY oxidation.The results revealed a strong dependence of selectivity on doping mode and electrolyte concentration:under low KOH concentration,Pd-and Pt-doped Ag_(4)M_(2) NCs exhibited 100%selectivity toward oxalic acid(OA),whereas Pd-and Pt-doped Ag_(24)M NCs delivered>95%selectivity for formic acid(FA).In contrast,under high KOH concentration,Pd-and Pt-doped Ag_(4)M_(2) NCs gave rise to>80%FA,while Pd-and Pt-doped Ag_(24)M NCs produced>45%FA.Mechanism studies indicated that Ni doping predominantly enhanced catalytic activity via lowering the activation barrier of the initial reaction step(GLY→glyceraldehyde),whereas Pd and Pt doping modulated selectivity through reducing the energy barrier of the selective branch step(glyceric acid→OA,OA→FA).High KOH concentration promoted the oxidation by increasing the electrochemical active surface area and facilitating electron transfer of Ag NCs.This study provides clear guidance for designing high-performance Ag-based electrocatalysts for biomass valorization.展开更多
Cuprous oxide(Cu_(2)O) is one of the most promising catalysts for electrochemical conversion of CO_(2) into value-added C_(2) products.The efficiency of CO_(2)-to-C_(2) conversion is highly dependent on the Cu_(2)O cr...Cuprous oxide(Cu_(2)O) is one of the most promising catalysts for electrochemical conversion of CO_(2) into value-added C_(2) products.The efficiency of CO_(2)-to-C_(2) conversion is highly dependent on the Cu_(2)O crystal plane orientation and the corresponding adsorbed ^(*)CO species.Herein,we constructed high-index crystal planes(311) in Cu_(2)O(CO-Cu_(2)O) via a facile self-selective CO-induced strategy under a CO atmosphere,which was verified by high-resolution transmission electron microscopy(HR-TEM) and atomic force microscopy(AFM) results.By exploiting the high surface energy of the high index crystal planes,^(*)CO species are stabilized in CO-Cu_(2)O during CO_(2)RR,resulting in exceptional catalytic performance for CO_(2)-to-C_(2)products.In situ infrared spectroscopy revealed that both atop-type(^(*)CO_(atop)) and hollow-type(^(*)CO_(hollow)) adsorption of ^(*)CO species occurred on the CO-Cu_(2)O.The asymmetric C-C coupling energy barrier between ^(*)CO_(atop) and ^(*)CO_(hollow) in(311) crystal plane decreases by 47.8 % compared to the symmetric coupling of ^(*)CO_(atop) in conventional(100) crystal planes.Consequently,the Faradaic efficiency of C_(2) products generated with CO-Cu_(2)O was increased by as high as 100 % compared to that with pristine Cu_(2)O.展开更多
According to the Mindlin plate theory and the first-order piston theory,this work obtains accurate closed-form eigensolutions for the flutter problem of three-dimensional(3D)rectangular laminated panels.The governing ...According to the Mindlin plate theory and the first-order piston theory,this work obtains accurate closed-form eigensolutions for the flutter problem of three-dimensional(3D)rectangular laminated panels.The governing differential equations are derived by the Hamilton's variational principle,and then solved by the iterative Separation-of-Variable(i SOV)method,which are applicable to arbitrary combinations of homogeneous Boundary Conditions(BCs).However,only the simply-support,clamped and cantilever panels are considered in this work for the sake of clarity.With the closed-form eigensolutions,the flutter frequency,flutter mode and flutter boundary are presented,and the effect of shear deformation and aerodynamic damping on flutter frequencies is investigated.Besides,the relation between panel energy and the work of aerodynamic load is discussed.The numerical comparisons reveal the following.(A)The flutter eigenvalues obtained by the present method are accurate,validated by the Finite Element Method(FEM)and the Galerkin method.(B)When the span-chord ratio is larger than 3,simplifying a 3D panel to 2D(two-dimensional)panel is reasonable and the relative differences of the flutter points predicted by the two models are less than one percent.(C)The reciprocal relationship between the mechanical energy of the panel and the work done by aerodynamic load is verified by using the present flutter eigenvalues and modes,further indicating the high accuracy of the present solutions.(D)The coupling of shear deformation and aerodynamic damping prevents frequency coalescing.展开更多
Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances ar...Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.展开更多
Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g...Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g-C_(3)N_(4) heterojunctions to improve process cost-effectiveness.The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction demonstrated an effective removal of 93.6%thiamphenicol(TAP)within 45 min,with the rate constant(0.0584 min^(-1))that was 2.4 and 2.8 times that of Co_(3)O_(4) and g-C_(3)N_(4) alone,respectively.The formation of heterojunctions facilitated electron transfer,enriched the electron density on Co_(3)O_(4),and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates.The enhanced production of atomic hydrogen(H*)of Co_(3)O_(4)/g-C_(3)N_(4),which increased by 13.6-28.2 times,contributed more to pollutant removal(64.0%),much higher than that of Co_(3)O_(4)(37.3%)and g-C_(3)N_(4)(6.1%).The energy barrier for H_(2) formation on Co_(3)O_(4)/g-C_(3)N_(4)(0.75 eV)was higher than that on Co_(3)O_(4)(-1.84 eV),supporting that it could stabilize H*and inhibit the formation of H_(2).The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction exhibited stable performance with less impact by pH and co-existing ions,and posed effectiveness for the dechlorination of typical chlorinated antibiotics.This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.展开更多
To address the problem of multi-missile cooperative interception against maneuvering targets at a prespecified impact time and desired Line-of-Sight(LOS)angles in ThreeDimensional(3D)space,this paper proposes a 3D lea...To address the problem of multi-missile cooperative interception against maneuvering targets at a prespecified impact time and desired Line-of-Sight(LOS)angles in ThreeDimensional(3D)space,this paper proposes a 3D leader-following cooperative interception guidance law.First,in the LOS direction of the leader,an impact time-controlled guidance law is derived based on the fixed-time stability theory,which enables the leader to complete the interception task at a prespecified impact time.Next,in the LOS direction of the followers,by introducing a time consensus tracking error function,a fixed-time consensus tracking guidance law is investigated to guarantee the consensus tracking convergence of the time-to-go.Then,in the direction normal to the LOS,by combining the designed global integral sliding mode surface and the second-order Sliding Mode Control(SMC)theory,an innovative 3D LOS-angle-constrained interception guidance law is developed,which eliminates the reaching phase in the traditional sliding mode guidance laws and effectively saves energy consumption.Moreover,it effectively suppresses the chattering phenomenon while avoiding the singularity issue,and compensates for unknown interference caused by target maneuvering online,making it convenient for practical engineering applications.Finally,theoretical proof analysis and multiple sets of numerical simulation results verify the effectiveness,superiority,and robustness of the investigated guidance law.展开更多
Structural regulation of Pd-based electrocatalytic hydrodechlorination(EHDC)catalyst for constructing high-efficient cathode materials with low noble metal content and high atom utilization is crucial but still challe...Structural regulation of Pd-based electrocatalytic hydrodechlorination(EHDC)catalyst for constructing high-efficient cathode materials with low noble metal content and high atom utilization is crucial but still challenging.Herein,a support electron inductive effect of Pd-Mn/Ni foam catalyst was proposed via in-situ Mn doping to optimize the electronic structure of the Ni foam(NF),which can inductive regulation of Pd for improving the EHDC performance.The mass activity and current efficiency of Pd-Mn/NF catalyst are 2.91 and 1.34 times superior to that of Pd/NF with 2,4-dichlorophenol as model compound,respectively.The Mn-doped interlayer optimized the electronic structure of Pd by bringing the d-state closer to the Fermi level than Pd on the NF surface,which optimizied the binding of EHDC intermediates.Additionally,the Mn-doped interlayer acted as a promoter for generating H∗and accelerating the EHDC reaction.This work presents a simple and effective regulation strategy for constructing high-efficient cathode catalyst for the EHDC of chlorinated organic compounds.展开更多
Three-dimensional(3D)urban structures play a critical role in informing climate mitigation strategies aimed at the built environment and facilitating sustainable urban development.Regrettably,there exists a significan...Three-dimensional(3D)urban structures play a critical role in informing climate mitigation strategies aimed at the built environment and facilitating sustainable urban development.Regrettably,there exists a significant gap in detailed and consistent data on 3D building space structures with global coverage due to the challenges inherent in the data collection and model calibration processes.In this study,we constructed a global urban structure(GUS-3D)dataset,including building volume,height,and footprint information,at a 500 m spatial resolution using extensive satellite observation products and numerous reference building samples.Our analysis indicated that the total volume of buildings worldwide in2015 exceeded 1×10^(12)m^(3).Over the 1985 to 2015 period,we observed a slight increase in the magnitude of 3D building volume growth(i.e.,it increased from 166.02 km3 during the 1985–2000 period to 175.08km3 during the 2000–2015 period),while the expansion magnitudes of the two-dimensional(2D)building footprint(22.51×10^(3) vs 13.29×10^(3)km^(2))and urban extent(157×10^(3) vs 133.8×10^(3)km^(2))notably decreased.This trend highlights the significant increase in intensive vertical utilization of urban land.Furthermore,we identified significant heterogeneity in building space provision and inequality across cities worldwide.This inequality is particularly pronounced in many populous Asian cities,which has been overlooked in previous studies on economic inequality.The GUS-3D dataset shows great potential to deepen our understanding of the urban environment and creates new horizons for numerous 3D urban studies.展开更多
Electrocatalytic CO_(2)reduction(ECR)to produce value-added fuels and chemicals using renewable electricity is an emerging strategy to mitigate global warming and decrease reliance on fossil fuels.Among various ECR pr...Electrocatalytic CO_(2)reduction(ECR)to produce value-added fuels and chemicals using renewable electricity is an emerging strategy to mitigate global warming and decrease reliance on fossil fuels.Among various ECR products,liquid oxygenates(Oxys)are especially attractive due to their high energy density,high safety and transportability that could be adapted to the existing infrastructure and transportation system.However,efficiently generating these highly reduced oxygen-containing products by ECR remains challenging due to the complexity of coupled proton and electron transfer processes.In recent years,in-depth studies of reaction mechanisms have advanced the design of catalysts and the regulation of reaction systems for ECR to produce Oxys,Here,by focusing on the production of typical Oxys,such as methanol,acetic acid,ethanol,acetone,n-propanol,and isopropanol,we outline various reaction paths and key intermediates for the electrochemical conversion of CO_(2)into these target products.We also summarize the current research status and recent advances in catalysts based on their elemental composition,and consider recent studies on the change of catalyst geometry and electronic structure,as well as the optimization of reaction systems to increase ECR performance.Finally,we analyze the challenges in the field of ECR to Oxys and provide an outlook on future directions for high-efficiency catalyst prediction and design,as well as the development of advanced reaction systems.展开更多
BACKGROUND Inguinal hernias are common after surgery.Tension-free repair is widely accepted as the main method for managing inguinal hernias.Adequate exposure,coverage,and repair of the myopectineal orifice(MPO)are ne...BACKGROUND Inguinal hernias are common after surgery.Tension-free repair is widely accepted as the main method for managing inguinal hernias.Adequate exposure,coverage,and repair of the myopectineal orifice(MPO)are necessary.However,due to differences in race and sex,people’s body shapes vary.According to European guidelines,the patch should measure 10 cm×15 cm.If any part of the MPO is dissected,injury to the nerves,vascular network,or organs may occur during surgery,thereby leading to inguinal discomfort,pain,and seroma formation after surgery.Therefore,accurate localization and measurement of the boundary of the MPO are crucial for selecting the optimal patch for inguinal hernia repair.AIM To compare the size of the MPO measured on three-dimensional multislice spiral computed tomography(CT)with that measured via laparoscopy and explore the relevant factors influencing the size of the MPO.METHODS Clinical data from 74 patients who underwent laparoscopic tension-free inguinal hernia repair at the General Surgery Department of the First Affiliated Hospital of Anhui University of Science and Technology between September 2022 and July 2024 were collected and analyzed retrospectively.Transabdominal preperitoneal was performed.Sixty-four males and 10 females,with an average age of 58.30±12.32 years,were included.The clinical data of the patients were collected.The boundary of the MPO was measured on three-dimensional CT images before surgery and then again during transabdominal preperitoneal.All the preoperative and intraoperative data were analyzed via paired t-tests.A t-test was used for comparisons of age,body mass index,and sex between the groups.In the comparative analysis,a P value less than 0.05 indicated a significant difference.RESULTS The boundaries of the MPO on 3-dimensional CT images measured 7.05±0.47 cm and 6.27±0.61 cm,and the area of the MPO was 19.54±3.33 cm^(2).The boundaries of the MPO during surgery were 7.18±0.51 cm and 6.17±0.40 cm.The errors were not statistically significant.However,the intraoperative BD(the width of the MPO,P=0.024,P<0.05)and preoperative AC(the length of the MPO,P=0.045,P<0.05)significantly differed according to sex.The AC and BD measurements before and during surgery were not significantly different according to age,body mass index,hernia side or hernia type(P>0.05).CONCLUSION The application of this technology can aid in determining the most appropriate dissection range and patch size.展开更多
The electrochemical conversion of nitrate,a widespread water pollutant,into valuable ammonia represents a green and decentralized approach to ammonia synthesis.However,the sluggish multielectronproton coupling path an...The electrochemical conversion of nitrate,a widespread water pollutant,into valuable ammonia represents a green and decentralized approach to ammonia synthesis.However,the sluggish multielectronproton coupling path and the low reactive species(nitrate and proton)concentration at the catalyst interface inhibit the efficiency of ammonia production from nitrate reduction reaction(NitRR).Herein,we introduce a novel iron-based tandem catalyst encapsulated by reduced graphene oxide(denoted as Fe-rGO),with a superior ammonia production rate of 47.815 mg h^(-1)mg_(ca)^(t-1)and a high Faraday efficiency(FE)of 96.51%at an applied potential of-0.5 V.It also delivers a robust stability with FE above90%under a current density of 250 mA cm^(-2)for 50 h.In situ X-ray absorption spectroscopy reveals that the FeO_(x)is dynamically translated to Fe~0 site concurrently with the enhancement of the NH_(3)production rate,suggesting the Fe^(0) site as hydrogenation active center.The asymmetric distribution of surface charges of rGO not only enriches nitrate ions at the catalytic interface and promotes the hydrogenation process in NitRR,but also protects the iron species and ensures their stability during electrolysis.The Zn-NO_(3)^(-)battery demonstrates an impressive FE of 88.6%,highlighting its exceptional potential for practical applications.展开更多
基金supported by Guangxi Science and Technology Major Program(No.AA23073008)Hubei Key Laboratory of Water System Science for Sponge City Construction(Wuhan University)(No.2023–05)Nanning Innovation and Entrepreneur Leading Talent Project(No.2021001).
文摘The three-dimensional particle electrode system exhibits significant potential for application in the treatment of wastewater.Nonetheless,the advancement of effective granular electrodes characterized by elevated catalytic activity and minimal energy consumption continues to pose a significant challenge.In this research,Fluorine-doped copper-carbon(F/Cu-GAC)particle electrodes were effectively synthesized through an impregnationcalcination technique,utilizing granular activated carbon as the carrier and fluorinedoped modified copper oxides as the catalytic agents.The particle electrodes were subsequently utilized to promote the degradation of 2,4,6-trichlorophenol(2,4,6-TCP)in a threedimensional electrocatalytic reactor(3DER).The F/Cu-GAC particle electrodes were polarized under the action of electric field,which promoted the heterogeneous Fenton-like reaction in which H2O2 generated by two-electron oxygen reduction reaction(2e-ORR)of O_(2) was catalytically decomposed to·OH.The 3DER equipped with F/Cu-GAC particle electrodes showed 100%removal of 2,4,6-TCP and 79.24%removal of TOC with a specific energy consumption(EC)of approximately 0.019 kWh/g·COD after 2 h of operation.The F/Cu-GAC particle electrodes exhibited an overpotential of 0.38 V and an electrochemically active surface area(ECSA)of 715 cm^(2),as determined through linear sweep voltammetry(LSV)and cyclic voltammetry(CV)assessments.These findings suggest a high level of electrocatalytic performance.Furthermore,the catalytic mechanism of the 3DER equipped with F/Cu-GAC particle electrodes was elucidated through the application of X-ray photoelectron spectroscopy(XPS),electron spin resonance(ESR),and active species capture experiments.This investigation offers a novel approach for the effective degradation of 2,4,6-TCP.
文摘In order to explore the effect of particle position on the electrocatalytic reaction rate at different positions in three-dimensional electrocatalytic reactor,using methylene blue as the simulated organic wastewater,and spherical graphite particles as the particle electrode,the potential distribution in three-dimensional electrocatalytic reactor was simulated by using COMSOL Multiphysics software.A multivariate logarithmic regression model of reaction kinetic constant and position was established by mathematical statistics.The electrocatalytic reaction rates were predicted at different locations in the reactor.The results show that the degradation ability of particle electrode to pollutants is uneven in the electrocatalytic reactor.The increase of electric field intensity and particle size will improve the difference of reaction rate.The closer the particle electrode is to the anode,the stronger the pollutant degradation ability would be.The reaction rate of the same particle electrode at different locations varies greatly,which can be roughly divided into three regions according to the degree of difference,among which the central region of the particle has the highest electrocatalytic reaction efficiency.
文摘This paper reports the preparation of three di‑iron complexes containing a thiazole moiety.Esterification of complex[Fe_(2)(CO)_(6)(μ‑SCH_(2)CH(CH_(2)OH)S)](1)with 4‑methylthiazole‑5‑carboxylic acid gave the corresponding ester[Fe_(2)(CO)_(6)(μ‑tedt)](2),where tedt=SCH_(2)CH(CH_(2)OOC(5‑C_(3)HNSCH_(3)))S.Further reactions of complex 2 with tri(ptolyl)phosphine(tp)or tris(4‑fluorophenyl)phosphine(fp)gave the phosphine‑substituted derivatives[Fe_(2)(CO)_(5)(tp)(μ‑tedt)](3)and[Fe_(2)(CO)_(5)(fp)(μ‑tedt)](4).The structures of the newly prepared complexes were elucidated by elemental analysis,NMR,IR,and X‑ray photoelectron spectroscopy.Moreover,single‑crystal X‑ray diffraction analysis confirmed their molecular structures,showing that they contain a di‑iron core ligated by a bridged dithiolate bearing a thiazole moiety and terminal carbonyls.The electrochemical and electrocatalytic proton reduction were probed by cyclic voltammetry,revealing that three complexes can catalyze the reduction of protons to H_(2) under the electrochemical conditions.For comparison,complex 4 possessed the best efficiency with a turnover frequency of 23.5 s^(-1)at 10 mmol·L^(-1)HOAc concentration.In addition,the fungicidal activity of these complexes was also investigated in this study.CCDC:2477511,2;2477512,3;2477513,4.
文摘CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organic frameworks(COFs)are porous crystalline materials formed by connecting organic monomers through covalent bonds.They have the characteristics of functional diversity and rich chemical properties.Their advantages,such as high porosity,a wide range of visible light absorption,and excellent charge separation efficiency,give them good potential in CO_(2)capture,separation,and conversion.Currently,Cu is a key metal in the catalytic CO_(2)reduction reaction(CO_(2)RR)for the preparation of high-value-added chemicals.The preparation of highly stable and large-pore Cu-based COFs using COFs as an ideal sacrificial template for loading Cu can be used to develop high-performance electrocatalysts and photocatalysts.In this review,we discuss the latest advancements in this field,including the development of various Cu-based COFs and their applications as catalysts for CO_(2)RR.Here,we mainly introduce the synthesis strategies,some important characterization information,and the applications of electrocatalytic and photocatalytic CO_(2)conversion using these previously reported Cu-based COFs.
文摘Under the strategic framework of rural revitalization and agricultural modernization, Xinjiashan Specialty Coffee Base, located in Zaotang Village, Lujiang Town, Longyang District, Baoshan City, has been proactively investigating innovative models for agricultural development. Through extensive communication and collaboration, this base has established close partnerships with research institutions including Kunming University of Science and Technology, Baoshan University, and Yunnan Academy of Agricultural Sciences, with a commitment to thoroughly exploring the potential for resource recycling and ecological complementarity. An innovative four-in-one three-dimensional integrated planting system incorporating "coffee, bananas, green manure, and bees" has been implemented. Concurrently, technological and digital management strategies have been comprehensively integrated to improve planting efficiency. Under this model, the proportion of specialty coffee attains 71%, and the per-unit yield is 17% greater than that of the conventional planting model. This approach not only substantially enhances economic returns but also promotes the integrated development of ecological and social benefits, offering a valuable practical example and experiential reference for the specialty and sustainable advancement of the coffee industry in comparable regions.
基金supported by the National Key Research and Development Program(No.2022YFC2807400)the National Natural Science Foundation of China(Nos.12265003 and 12205044)。
文摘Aerial surveys are dynamic and continuous processes,and there are different height distributions of the ground in the measurement area,which leads to problems such as overlapping measurement areas and inaccurate altitude correction during the survey process.Commonly used terrain correction methods are based on the concept of finite elementization of ground surface radioactive sources,using GPS coordinates,radar altitude,and ground elevation distribution information from aerial surveys,combined with the sourceless efficiency calibration method to construct a response matrix,which is then inverted for surface nuclide content.However,most of the sourceless efficiency calibration methods used are numerical calculations that consider the body detector as a point detector and do not consider the changes in intrinsic detection efficiency under different incident directions of gamma rays.Therefore,when the altitude of the measurement area varies significantly or the flight altitude of the aerial survey is relatively low,such sourceless efficiency calibration method calculations tend to have a large bias,which affects the accuracy of the terrain correction.To address the above problems,this study employs a novel sourceless efficiency calibration method based on the Boolean operation of the ray deposition process and simplifies the traditional body source measurement model to a surface source measurement model to achieve fast and accurate efficiency calibration.Then,through the discretization of the measurement process,the static measurement process is superposed as equivalent to the dynamic measurement process,and the dynamic measurement response matrix is built and optimized based on the calibration method.Finally,the PSO-MLEM algorithm was used to solve the dynamic measurement response matrix to achieve dynamic terrain correction of aerial survey data.Analysis of the Baiyun'ebo test area revealed that,after applying dynamic terrain correction,the inverted anomalies in uranium(eU),thorium(eTh),and potassium(K)concentrations were closer to ground measurements(within 5.72%-30.79%)and exhibited clearer anomaly boundaries compared to traditional height-based corrections.However,owing to the inherent statistical fluctuations and characteristics of matrix inversion,higher measurement values tend to absorb lower ones,potentially enlarging the anomalous regions.Nevertheless,the highanomaly regions after inversion largely coincided with the ground truth validation,demonstrating that the proposed method can effectively correct airborne gamma spectrometry data.
基金the support from the National Natural Science Foundation of China(22478221)China Postdoctoral Science Foundation(2023M741920 and GZC20231259)+1 种基金Huaneng Group Science and Technology Research Project(HNKJ23-H71)Department of Chemical Engineering-iBHE Cooperation Joint Fund Project(DCE-iBHE-2025-3)。
文摘The two-electron electrochemical oxygen reduction reaction(ORR)affords an appealing alternative for on-site production of hydrogen peroxide(H_(2)O_(2)),which can fulfill the demands of various applications even at low concentrations.Under neutral or near-neutral conditions,the electrolyte environment capable of electrochemically synthesizing H_(2)O_(2) exhibits diversity and holds vast potential for practical applications;however,the electrocatalytic performance is limited without desirable electrode materials.In this contribution,methoxylated nickel hydroxides were proposed for high-performance on-site H_(2)O_(2) electrosynthesis in different potassium fertilizer solutions.The methoxylation compared to pristine Ni(OH)_(2) was demonstrated to optimize the electronic structure with favorable adsorption of reaction intermediates,obviously enhancing the activity and selectivity.In 0.10 M K_(2)SO_(4) solution,H_(2)O_(2) production ranged from 28.1 to 153.6 mg h^(-1) cm^(-2) at current densities of-50 to-250 mA cm^(-2),accompanied by Faradaic efficiency values exceeding 88.0%.An integrated system was devised by combining fertilization,disinfection,and irrigation through the coupling of two-electron ORR with agricultural irrigation,utilizing nutrient solutions as the electrolyte for on-site H_(2)O_(2) electrosynthesis.These findings afford a promising avenue for the practical application of 2e-ORR in neutral environments.
基金funded by the“Pioneer”and“Leading Goose”R&D Program of Zhejiang(No.2023C03017)China Postdoctoral Science Foundation(No.GZC20230373)+5 种基金Zhejiang Provincial Natural Science Foundation of China(No.LQ24B070010)CMA Key Open Laboratory of Transforming Climate Resources to Economy(No.2024004K)Natural Science Foundation of Huzhou City(No.2024YZ19)the National Natural Science Foundation of China(Nos.22202032,22406020 and 22406019)the Key Research and Development Projects of Xinjiang Uygur Autonomous Region,China(No.2022B02031)Joint Fund of the Zhejiang Provincial Natural Science Foundation of China(No.LBMHY25E060009)。
文摘Elucidating the active site formation mechanism of bismuth(Bi)-based catalysts in electrochemical CO_(2)reduction remains challenging for achieving high activity,selectivity,and long-term stability.Here we confirm through experimental results that Bi-based catalysts containing halogen ions(I^(-),Cl^(-),Br^(-))and SO_(4)^(2-)maintain the system stability,keeping Faraday efficiency of formic acid above90%in the current range of 50-800 mA cm^(-2).In contrast,anions containing S^(2-)and NO_(3)^(-)in the electrolyte can be reduced to produce by-products.These anions and their by-products could poison the active center,leading to increased side reactions and thus significantly reducing the Faraday efficiency of formic acid.The combination of non-in situ and in situ characterization results revealed that the Bi-based catalysts all underwent the transition from the initial state to the Bi/Bi_(2)O_(2)CO_(3)(BOC)intermediate state in high-concentration KHCO_(3) solution,and the different anions could selectively modulate the degree of exposure of specific crystalline surfaces of BOC.At the late stage of the reaction,BOC was completely converted to metal Bi and became the real active center.Combined with in situ IR and DFT calculations,it is further verified that^(*)OCHO is the key intermediate on the metallic Bi surface,which is most favorable for formic acid formation.This study reveals the key mechanism by which anions affect the formation of active sites via modulating the catalyst reconstruction process,which provides an important theoretical basis for the design and optimization of test conditions of Bi-based catalysts.
基金Higher Education Commission(HEC)of Pakistan for financial support under grants#377-IPFP-Ⅱ/Batch-1st/SRGP-NAHE/HEC-2022-27 along with ASIP-Support Award Letter#ASIP/R&D/HEC/2024/10006/83387/127。
文摘This insightful review explores the electrochemical principles and energy potential of electrocatalytic water splitting(EWS).It highlights recent advancements,identifies key challenges,and underscores the pivotal role of EWS in enabling the transition to sustainable energy systems.This work contextualizes the significance of green hydrogen in global decarbonization pathways and examines the historical progression of electrocatalysis.The fundamental thermodynamics and mechanistic pathways governing both the hydrogen and oxygen evolution reactions(HER and OER)are analyzed,highlighting energy barriers and rate-determining steps.Various electrode architectures and electrochemical cell configurations are evaluated,including a comparative assessment of key electrolyzer technologies and their performance characteristics.Furthermore,we critically examine recent advances and persistent limitations across the landscape of electrocatalysts,spanning noble metal-based materials,earth-abundant transition metal compounds,and emerging materials.Design principles and mechanistic insights drawn from electronic structu re modulation,defect engineering,doping strategies,and na noscale morphology control are elucidated to establish robust structure-property-performance relationships.Major challenges including sluggish oxygen evolution kinetics,catalyst degradation mechanisms,and the integration of devices with intermittent renewable energy sources are thoroughly examined.This work also debates advanced strategies such as hybrid photoelectrochemical systems,flexible device architectures,and the direct utilization of non-traditional water sources(e.g.,seawater,wastewater)as promising pathways for future development.Finally,it is specifically distinguished by its critical focus on bridging the gap between fundamental electrocatalysts development and practical system-level integration,addressing the challenges of scalability and deployment under industrially relevant conditions.This comprehensive review provides a strategic outlook and identifies key scientific priorities for optimizing EWS systems toward efficient,robust,and scalable hydrogen generation.
基金support from the Jiangsu Natural Science Foundation of China(BK20230329)the National Natural Science Foundation of China(22401147,22361132540,and 22178161)the Russian Science Foundation(23-73-30007).
文摘The efficient electrocatalytic oxidation of glycerol(GLY)is one of the most promising routes for the valorization of GLY.Doping has emerged as a powerful strategy to tailor the electrocatalytic performance of silver nanoclusters(Ag NCs),yet the effects of doping mode(surface vs.core)and the interface environment(e.g.,electrolyte concentration)on the electrocatalytic performance for Ag NCs toward GLY oxidation remain understood.In this work,surface-doped Ag_(4)M_(2)(SR)_(8) and core-doped Ag_(24)M(SR)_(18)(M=Ni,Pd,Pt;SR=SPhMe_(2))NCs were synthesized for electrocatalytic GLY oxidation.The results revealed a strong dependence of selectivity on doping mode and electrolyte concentration:under low KOH concentration,Pd-and Pt-doped Ag_(4)M_(2) NCs exhibited 100%selectivity toward oxalic acid(OA),whereas Pd-and Pt-doped Ag_(24)M NCs delivered>95%selectivity for formic acid(FA).In contrast,under high KOH concentration,Pd-and Pt-doped Ag_(4)M_(2) NCs gave rise to>80%FA,while Pd-and Pt-doped Ag_(24)M NCs produced>45%FA.Mechanism studies indicated that Ni doping predominantly enhanced catalytic activity via lowering the activation barrier of the initial reaction step(GLY→glyceraldehyde),whereas Pd and Pt doping modulated selectivity through reducing the energy barrier of the selective branch step(glyceric acid→OA,OA→FA).High KOH concentration promoted the oxidation by increasing the electrochemical active surface area and facilitating electron transfer of Ag NCs.This study provides clear guidance for designing high-performance Ag-based electrocatalysts for biomass valorization.
基金the financial support from the National Natural Science Foundation of China (Nos.U23A20677,22022610 and 52400137)"Pioneer" and "Leading Goose" R&D Program of Zhejiang (Nos.2022C03146 and 2023C03017)+2 种基金China Postdoctoral Science Foundation (No.2024T170805)Zhejiang Provincial Natural Science Foundation of China (No.LDT23E06015B06)the support of the Research Computing Center in College of Chemical and Biological Engineering at Zhejiang University for assistance with the calculations。
文摘Cuprous oxide(Cu_(2)O) is one of the most promising catalysts for electrochemical conversion of CO_(2) into value-added C_(2) products.The efficiency of CO_(2)-to-C_(2) conversion is highly dependent on the Cu_(2)O crystal plane orientation and the corresponding adsorbed ^(*)CO species.Herein,we constructed high-index crystal planes(311) in Cu_(2)O(CO-Cu_(2)O) via a facile self-selective CO-induced strategy under a CO atmosphere,which was verified by high-resolution transmission electron microscopy(HR-TEM) and atomic force microscopy(AFM) results.By exploiting the high surface energy of the high index crystal planes,^(*)CO species are stabilized in CO-Cu_(2)O during CO_(2)RR,resulting in exceptional catalytic performance for CO_(2)-to-C_(2)products.In situ infrared spectroscopy revealed that both atop-type(^(*)CO_(atop)) and hollow-type(^(*)CO_(hollow)) adsorption of ^(*)CO species occurred on the CO-Cu_(2)O.The asymmetric C-C coupling energy barrier between ^(*)CO_(atop) and ^(*)CO_(hollow) in(311) crystal plane decreases by 47.8 % compared to the symmetric coupling of ^(*)CO_(atop) in conventional(100) crystal planes.Consequently,the Faradaic efficiency of C_(2) products generated with CO-Cu_(2)O was increased by as high as 100 % compared to that with pristine Cu_(2)O.
基金support of the National Natural Science Foundation of China(No.12172023)。
文摘According to the Mindlin plate theory and the first-order piston theory,this work obtains accurate closed-form eigensolutions for the flutter problem of three-dimensional(3D)rectangular laminated panels.The governing differential equations are derived by the Hamilton's variational principle,and then solved by the iterative Separation-of-Variable(i SOV)method,which are applicable to arbitrary combinations of homogeneous Boundary Conditions(BCs).However,only the simply-support,clamped and cantilever panels are considered in this work for the sake of clarity.With the closed-form eigensolutions,the flutter frequency,flutter mode and flutter boundary are presented,and the effect of shear deformation and aerodynamic damping on flutter frequencies is investigated.Besides,the relation between panel energy and the work of aerodynamic load is discussed.The numerical comparisons reveal the following.(A)The flutter eigenvalues obtained by the present method are accurate,validated by the Finite Element Method(FEM)and the Galerkin method.(B)When the span-chord ratio is larger than 3,simplifying a 3D panel to 2D(two-dimensional)panel is reasonable and the relative differences of the flutter points predicted by the two models are less than one percent.(C)The reciprocal relationship between the mechanical energy of the panel and the work done by aerodynamic load is verified by using the present flutter eigenvalues and modes,further indicating the high accuracy of the present solutions.(D)The coupling of shear deformation and aerodynamic damping prevents frequency coalescing.
基金funding support from General Research Fund[Project No.14300525]from the Research Grants Council(RGC)of Hong Kong SAR,Chinafunding support from Natural Science Foundation of China(NSFC)Young Scientists Fund(Project No.22305203)+2 种基金NSFC Projects Nos.22309123,22422303,22303011,22033002,92261112 and U21A20328support from the Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM)at City University of Hong Kongsupport from Young Collaborative Research Grant[Project No.C1003-23Y]support from RGC of Hong Kong SAR,China.
文摘Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.
基金supported by Natural Science Foundation of China(Nos.U23B20165 and 52170085)National Key R&D Program International Cooperation Project(No.2023YFE0108100)+1 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Fundamental Research Funds for the Central Universities,Nankai University.
文摘Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g-C_(3)N_(4) heterojunctions to improve process cost-effectiveness.The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction demonstrated an effective removal of 93.6%thiamphenicol(TAP)within 45 min,with the rate constant(0.0584 min^(-1))that was 2.4 and 2.8 times that of Co_(3)O_(4) and g-C_(3)N_(4) alone,respectively.The formation of heterojunctions facilitated electron transfer,enriched the electron density on Co_(3)O_(4),and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates.The enhanced production of atomic hydrogen(H*)of Co_(3)O_(4)/g-C_(3)N_(4),which increased by 13.6-28.2 times,contributed more to pollutant removal(64.0%),much higher than that of Co_(3)O_(4)(37.3%)and g-C_(3)N_(4)(6.1%).The energy barrier for H_(2) formation on Co_(3)O_(4)/g-C_(3)N_(4)(0.75 eV)was higher than that on Co_(3)O_(4)(-1.84 eV),supporting that it could stabilize H*and inhibit the formation of H_(2).The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction exhibited stable performance with less impact by pH and co-existing ions,and posed effectiveness for the dechlorination of typical chlorinated antibiotics.This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.
文摘To address the problem of multi-missile cooperative interception against maneuvering targets at a prespecified impact time and desired Line-of-Sight(LOS)angles in ThreeDimensional(3D)space,this paper proposes a 3D leader-following cooperative interception guidance law.First,in the LOS direction of the leader,an impact time-controlled guidance law is derived based on the fixed-time stability theory,which enables the leader to complete the interception task at a prespecified impact time.Next,in the LOS direction of the followers,by introducing a time consensus tracking error function,a fixed-time consensus tracking guidance law is investigated to guarantee the consensus tracking convergence of the time-to-go.Then,in the direction normal to the LOS,by combining the designed global integral sliding mode surface and the second-order Sliding Mode Control(SMC)theory,an innovative 3D LOS-angle-constrained interception guidance law is developed,which eliminates the reaching phase in the traditional sliding mode guidance laws and effectively saves energy consumption.Moreover,it effectively suppresses the chattering phenomenon while avoiding the singularity issue,and compensates for unknown interference caused by target maneuvering online,making it convenient for practical engineering applications.Finally,theoretical proof analysis and multiple sets of numerical simulation results verify the effectiveness,superiority,and robustness of the investigated guidance law.
基金supported by the National Natural Science Foundation of China(Nos.22178388 and 22108306)Taishan Scholars Program of Shandong Province(No.tsqn201909065)Chongqing Science and Technology Bureau(No.cstc2019jscx-gksb X0032).
文摘Structural regulation of Pd-based electrocatalytic hydrodechlorination(EHDC)catalyst for constructing high-efficient cathode materials with low noble metal content and high atom utilization is crucial but still challenging.Herein,a support electron inductive effect of Pd-Mn/Ni foam catalyst was proposed via in-situ Mn doping to optimize the electronic structure of the Ni foam(NF),which can inductive regulation of Pd for improving the EHDC performance.The mass activity and current efficiency of Pd-Mn/NF catalyst are 2.91 and 1.34 times superior to that of Pd/NF with 2,4-dichlorophenol as model compound,respectively.The Mn-doped interlayer optimized the electronic structure of Pd by bringing the d-state closer to the Fermi level than Pd on the NF surface,which optimizied the binding of EHDC intermediates.Additionally,the Mn-doped interlayer acted as a promoter for generating H∗and accelerating the EHDC reaction.This work presents a simple and effective regulation strategy for constructing high-efficient cathode catalyst for the EHDC of chlorinated organic compounds.
基金supported by the National Science Fund for Distinguished Young Scholars(42225107)the National Natural Science Foundation of China(42001326,42371414,42171409,and 42271419)+1 种基金the Natural Science Foundation of Guangdong Province of China(2022A1515012207)the Basic and Applied Basic Research Project of Guangzhou Science and Technology Planning(202201011539)。
文摘Three-dimensional(3D)urban structures play a critical role in informing climate mitigation strategies aimed at the built environment and facilitating sustainable urban development.Regrettably,there exists a significant gap in detailed and consistent data on 3D building space structures with global coverage due to the challenges inherent in the data collection and model calibration processes.In this study,we constructed a global urban structure(GUS-3D)dataset,including building volume,height,and footprint information,at a 500 m spatial resolution using extensive satellite observation products and numerous reference building samples.Our analysis indicated that the total volume of buildings worldwide in2015 exceeded 1×10^(12)m^(3).Over the 1985 to 2015 period,we observed a slight increase in the magnitude of 3D building volume growth(i.e.,it increased from 166.02 km3 during the 1985–2000 period to 175.08km3 during the 2000–2015 period),while the expansion magnitudes of the two-dimensional(2D)building footprint(22.51×10^(3) vs 13.29×10^(3)km^(2))and urban extent(157×10^(3) vs 133.8×10^(3)km^(2))notably decreased.This trend highlights the significant increase in intensive vertical utilization of urban land.Furthermore,we identified significant heterogeneity in building space provision and inequality across cities worldwide.This inequality is particularly pronounced in many populous Asian cities,which has been overlooked in previous studies on economic inequality.The GUS-3D dataset shows great potential to deepen our understanding of the urban environment and creates new horizons for numerous 3D urban studies.
基金financial supports from the National Natural Science Foundation of China(52201237)the Talent Introduction Project of Chinese Academy of Sciences(E344011)+4 种基金the Shenzhen High Level Talent Team Project(KQTD2022110109364705)the Joint Research Project of China Merchants Group and SIAT(E2Z1521)the Cross Institute Joint Research Youth Team Project of SIAT(E25427)National Natural Science Foundation of China(52402136)the China Postdoctoral Science Foundation(E325281005)。
文摘Electrocatalytic CO_(2)reduction(ECR)to produce value-added fuels and chemicals using renewable electricity is an emerging strategy to mitigate global warming and decrease reliance on fossil fuels.Among various ECR products,liquid oxygenates(Oxys)are especially attractive due to their high energy density,high safety and transportability that could be adapted to the existing infrastructure and transportation system.However,efficiently generating these highly reduced oxygen-containing products by ECR remains challenging due to the complexity of coupled proton and electron transfer processes.In recent years,in-depth studies of reaction mechanisms have advanced the design of catalysts and the regulation of reaction systems for ECR to produce Oxys,Here,by focusing on the production of typical Oxys,such as methanol,acetic acid,ethanol,acetone,n-propanol,and isopropanol,we outline various reaction paths and key intermediates for the electrochemical conversion of CO_(2)into these target products.We also summarize the current research status and recent advances in catalysts based on their elemental composition,and consider recent studies on the change of catalyst geometry and electronic structure,as well as the optimization of reaction systems to increase ECR performance.Finally,we analyze the challenges in the field of ECR to Oxys and provide an outlook on future directions for high-efficiency catalyst prediction and design,as well as the development of advanced reaction systems.
基金Supported by the 2022 Provincial Quality Engineering Project for Higher Education Institutions,No.2022sx031the 2023 Provincial Quality Engineering Project for Higher Education Institutions,No.2023jyxm1071.
文摘BACKGROUND Inguinal hernias are common after surgery.Tension-free repair is widely accepted as the main method for managing inguinal hernias.Adequate exposure,coverage,and repair of the myopectineal orifice(MPO)are necessary.However,due to differences in race and sex,people’s body shapes vary.According to European guidelines,the patch should measure 10 cm×15 cm.If any part of the MPO is dissected,injury to the nerves,vascular network,or organs may occur during surgery,thereby leading to inguinal discomfort,pain,and seroma formation after surgery.Therefore,accurate localization and measurement of the boundary of the MPO are crucial for selecting the optimal patch for inguinal hernia repair.AIM To compare the size of the MPO measured on three-dimensional multislice spiral computed tomography(CT)with that measured via laparoscopy and explore the relevant factors influencing the size of the MPO.METHODS Clinical data from 74 patients who underwent laparoscopic tension-free inguinal hernia repair at the General Surgery Department of the First Affiliated Hospital of Anhui University of Science and Technology between September 2022 and July 2024 were collected and analyzed retrospectively.Transabdominal preperitoneal was performed.Sixty-four males and 10 females,with an average age of 58.30±12.32 years,were included.The clinical data of the patients were collected.The boundary of the MPO was measured on three-dimensional CT images before surgery and then again during transabdominal preperitoneal.All the preoperative and intraoperative data were analyzed via paired t-tests.A t-test was used for comparisons of age,body mass index,and sex between the groups.In the comparative analysis,a P value less than 0.05 indicated a significant difference.RESULTS The boundaries of the MPO on 3-dimensional CT images measured 7.05±0.47 cm and 6.27±0.61 cm,and the area of the MPO was 19.54±3.33 cm^(2).The boundaries of the MPO during surgery were 7.18±0.51 cm and 6.17±0.40 cm.The errors were not statistically significant.However,the intraoperative BD(the width of the MPO,P=0.024,P<0.05)and preoperative AC(the length of the MPO,P=0.045,P<0.05)significantly differed according to sex.The AC and BD measurements before and during surgery were not significantly different according to age,body mass index,hernia side or hernia type(P>0.05).CONCLUSION The application of this technology can aid in determining the most appropriate dissection range and patch size.
基金supported by the National Natural Science Foundation of China(12205300(H.S.),12405377(M.H.L))the Postdoctoral Science Foundation of China(2024M763694(M.H.L))+3 种基金the Natural Science Foundation of Hunan Province(2024JJ4027(H.S.))the Postdoctoral Fellowship Program of CPSF under Grant Number GZB20240859(M.H.L)financial support from the Hunan Normal University Program(grant05311204666)financial support from the 2024 Large Instrument Testing Open Fund of Hunan Normal University(24CSY033,24CSY086)。
文摘The electrochemical conversion of nitrate,a widespread water pollutant,into valuable ammonia represents a green and decentralized approach to ammonia synthesis.However,the sluggish multielectronproton coupling path and the low reactive species(nitrate and proton)concentration at the catalyst interface inhibit the efficiency of ammonia production from nitrate reduction reaction(NitRR).Herein,we introduce a novel iron-based tandem catalyst encapsulated by reduced graphene oxide(denoted as Fe-rGO),with a superior ammonia production rate of 47.815 mg h^(-1)mg_(ca)^(t-1)and a high Faraday efficiency(FE)of 96.51%at an applied potential of-0.5 V.It also delivers a robust stability with FE above90%under a current density of 250 mA cm^(-2)for 50 h.In situ X-ray absorption spectroscopy reveals that the FeO_(x)is dynamically translated to Fe~0 site concurrently with the enhancement of the NH_(3)production rate,suggesting the Fe^(0) site as hydrogenation active center.The asymmetric distribution of surface charges of rGO not only enriches nitrate ions at the catalytic interface and promotes the hydrogenation process in NitRR,but also protects the iron species and ensures their stability during electrolysis.The Zn-NO_(3)^(-)battery demonstrates an impressive FE of 88.6%,highlighting its exceptional potential for practical applications.
