This paper takes Zoomlion （Changsha Zoomlion Heavy Industry Science and Technology Development Co., Ltd） as an example and illustrates the reasons why traditional theories of stock dividends and stock splits cannot ...This paper takes Zoomlion （Changsha Zoomlion Heavy Industry Science and Technology Development Co., Ltd） as an example and illustrates the reasons why traditional theories of stock dividends and stock splits cannot rationally explain the large stock dividend and stock split behavior among Chinese listed companies. The paper offers the following points after analyzing the current situation of China＇s capital market： As many investors seek after the stocks with large stock dividends and stock splits and form a ＂herd effect＂, it greatly pushes up the price of these stocks. Thus, companies＇ managers can cater these investors＇ irrational behavior, and help their companies get more funds from secondary equity offerings, or help their large shareholders and institutional investors to obtain more returns after lifting the sell restriction on their shares.展开更多
The fast solution of linear equations has always been one of the hot spots in scientific computing.A kind of the diagonal matrix splitting iteration methods are provided,which is different from the classical matrix sp...The fast solution of linear equations has always been one of the hot spots in scientific computing.A kind of the diagonal matrix splitting iteration methods are provided,which is different from the classical matrix splitting methods.Taking the decomposition of the diagonal elements for coefficient matrix as the key point,some new preconditioners are constructed.Taking the tri-diagonal coefficient matrix as an example,the convergence domains and optimal relaxation factor of the new method are analyzed theoretically.The presented new iteration methods are applied to solve linear algebraic equations,even 2D and 3D diffusion problems with the fully implicit discretization.The results of numerical experiments are matched with the theoretical analysis,and show that the iteration numbers are reduced greatly.The superiorities of presented iteration methods exceed some classical iteration methods dramatically.展开更多
Electrochemical water splitting represents a sustainable technology for hydrogen(H_(2))production.However,its large-scale implementation is hindered by the high overpotentials required for both the cathodic hydrogen e...Electrochemical water splitting represents a sustainable technology for hydrogen(H_(2))production.However,its large-scale implementation is hindered by the high overpotentials required for both the cathodic hydrogen evolution reaction(HER)and the anodic oxygen evolution reaction(OER).Transition metal-based catalysts have garnered significant research interest as promising alternatives to noble-metal catalysts,owing to their low cost,tunable composition,and noble-metal-like catalytic activity.Nevertheless,systematic reviews on their application as bifunctional catalysts for overall water splitting(OWS)are still limited.This review comprehensively outlines the principal categories of bifunctional transition metal electrocatalysts derived from electrospun nanofibers(NFs),including metals,oxides,phosphides,sulfides,and carbides.Key strategies for enhancing their catalytic performance are systematically summarized,such as heterointerface engineering,heteroatom doping,metal-nonmetal-metal bridging architectures,and single-atom site design.Finally,current challenges and future research directions are discussed,aiming to provide insightful perspectives for the rational design of high-performance electrocatalysts for OWS.展开更多
Two[FeFe]-hydrogenase compounds with 2-cyanobenzyl groups,{Fe_(2)[(SCH_(2)CH_(3))(SR)](CO)_(6)}(1 or 1′,which are the crystalline states from petroleum ether and dichloromethane solution,respectively)and{Fe_(2)[(SCH_...Two[FeFe]-hydrogenase compounds with 2-cyanobenzyl groups,{Fe_(2)[(SCH_(2)CH_(3))(SR)](CO)_(6)}(1 or 1′,which are the crystalline states from petroleum ether and dichloromethane solution,respectively)and{Fe_(2)[(SCH_(2)CH_(3))(SR)](CO)_(5)(PPh_(3))}(2)(R=2-cyanobenzyl),were synthesized and characterized by infrared spectroscopy,UV-Vis spectroscopy,single-crystal diffraction,powder X-ray diffraction,etc.Their performances as photocatalysts for H_(2)production through water splitting were evaluated.The results showed that 316.8μmol of H_(2)was produced on compound 1 after 3 h of illumination,with a catalytic efficiency of 25.1μmol·mg^(-1)·h^(-1)and a turnover number(TON)of 36.8.The replacement of carbonyl with PPh3 could significantly improve the catalytic performance of the complex,and 705.0μmol of H_(2)was produced on 2 after 3 h of illumination,with a catalytic efficiency of 37.9μmol·mg^(-1)·h^(-1)and a TON of 81.8.CCDC:2515700,1;2515702,1′;2515701,2.展开更多
Photoelectrochemical(PEC)water splitting is an effective approach to directly convert solar energy into clean hydrogen fuel.As a visible-light-responsive p-type semiconductor,CuBi_(2)O_(4)possesses a suitable bandgap ...Photoelectrochemical(PEC)water splitting is an effective approach to directly convert solar energy into clean hydrogen fuel.As a visible-light-responsive p-type semiconductor,CuBi_(2)O_(4)possesses a suitable bandgap and good stability.However,its performance is inhibited by high interfacial resistance and severe charge carrier recombination.In this study,a CuO interlayer was introduced between fluorine-doped tin oxide(FTO)and CuBi_(2)O_(4)to construct CuO/CuBi_(2)O_(4)photocathodes,aiming to improve interfacial charge transfer.The results showed that CuO/CuBi_(2)O_(4)-200 exhibited a photocurrent density of−1.71 mA/cm^(2)at 0 V vs.RHE,which was more than 3.5 times higher than that of bare CuBi_(2)O_(4).The incident photon-to-current efficiency(IPCE)at 365 nm was enhanced to~13%and the maximum applied bias photon-to-current efficiency(ABPE)reached 0.17%.Water splitting experiments revealed a hydrogen yield of 2.05μmol/cm^(2),significantly surpassing that of the unmodified photoelectrode.The enhanced PEC performance indicated that the CuO layer established a favorable band alignment,promoted hole transport toward the FTO substrate and effectively suppressed interfacial carrier recombination.This work demonstrated a simple and efficient interfacial engineering strategy,offering new insights and guidance for the design and development of high-performance semiconductor-based PEC photoelectrodes.展开更多
Split Learning(SL)has been promoted as a promising collaborative machine learning technique designed to address data privacy and resource efficiency.Specifically,neural networks are divided into client and server subn...Split Learning(SL)has been promoted as a promising collaborative machine learning technique designed to address data privacy and resource efficiency.Specifically,neural networks are divided into client and server subnetworks in order to mitigate the exposure of sensitive data and reduce the overhead on client devices,thereby making SL particularly suitable for resource-constrained devices.Although SL prevents the direct transmission of raw data,it does not alleviate entirely the risk of privacy breaches.In fact,the data intermediately transmitted to the server sub-model may include patterns or information that could reveal sensitive data.Moreover,achieving a balance between model utility and data privacy has emerged as a challenging problem.In this article,we propose a novel defense approach that combines:(i)Adversarial learning,and(ii)Network channel pruning.In particular,the proposed adversarial learning approach is specifically designed to reduce the risk of private data exposure while maintaining high performance for the utility task.On the other hand,the suggested channel pruning enables the model to adaptively adjust and reactivate pruned channels while conducting adversarial training.The integration of these two techniques reduces the informativeness of the intermediate data transmitted by the client sub-model,thereby enhancing its robustness against attribute inference attacks without adding significant computational overhead,making it wellsuited for IoT devices,mobile platforms,and Internet of Vehicles(IoV)scenarios.The proposed defense approach was evaluated using EfficientNet-B0,a widely adopted compact model,along with three benchmark datasets.The obtained results showcased its superior defense capability against attribute inference attacks compared to existing state-of-the-art methods.This research’s findings demonstrated the effectiveness of the proposed channel pruning-based adversarial training approach in achieving the intended compromise between utility and privacy within SL frameworks.In fact,the classification accuracy attained by the attackers witnessed a drastic decrease of 70%.展开更多
Designing a highly active and stable bifunctional catalyst is essential for achieving superior overall water splitting(OWS).In this study,a three-dimensional(3D)core-shell structure Co_(3)S_(4)/CuS@NiFe LDH nanocoral ...Designing a highly active and stable bifunctional catalyst is essential for achieving superior overall water splitting(OWS).In this study,a three-dimensional(3D)core-shell structure Co_(3)S_(4)/CuS@NiFe LDH nanocoral spheres electrocatalyst was constructed on nickel foam(NF)via an interfacial engineering strategy.This 3D core-shell heterostructure maximizes the exposure of active sites,optimizes the charge transport pathway and accelerates gas release rates.The protective shell strategy of NiFe LDH provides favorable stability,which contributes to inhibiting the electrochemical corrosion of the electrocatalyst and mitigating the toxic effects of Cl^(-) and other microorganisms during the seawater splitting process.Moreover,the introduction of NiFe LDH induces a change in the OER mechanism from an adsorption evolution mechanism(AEM)to a lattice oxygen mechanism(LOM),which improves the intrinsic activity of the catalyst.Consequently,Co_(3)S_(4)/CuS@NiFe LDH demonstrates exceptional performance in the oxygen evolution reaction(OER)(η100=251 mV)and in the hydrogen evolution reaction(HER)(η100=254 mV),alongside remarkable stability over 100 h.For OWS,it exhibits a voltage of 1.46 V at 10 mA/cm^(2) and maintain stability for 100 h.Impressively,Co_(3)S_(4)/CuS@NiFe LDH still possesses outstanding activity and stability in natural alkaline seawater.This work proposes interfacial engineering to construct bifunctional catalysts with core-shell heterostructures,providing instructive guidelines for the design of highly efficient electrocatalysts toward seawater electrolysis.展开更多
Herein,we have developed a straightforward wet-chemical method to synthesize a series of Pd-based alloy nanowires(NWs),including Pd Pt NWs,Pd Au NWs,Pd Ir NWs,and Pd Ru NWs,which exhibits high mass activity and turnov...Herein,we have developed a straightforward wet-chemical method to synthesize a series of Pd-based alloy nanowires(NWs),including Pd Pt NWs,Pd Au NWs,Pd Ir NWs,and Pd Ru NWs,which exhibits high mass activity and turnover frequency(TOF) for HER,surpassing Pt/C by 4.6-fold and 1.5-fold in acidic and alkaline electrolytes,respectively.It also demonstrates high stability in alkaline electrolyte at a current density of 220 m A/cm^(2) for 280 h,highlighting its potential for practical applications under industrial current conditions.Pd Pt NWs exhibited ultrathin structures with head-to-tail kinks and inherent defects,significantly increasing the density of active sites and precisely tuning the electronic structure,which could accelerate reaction kinetics and boost water-splitting electrocatalytic performance.This study highlights the potential of Pd Pt NWs as highly efficient catalysts,offering outstanding catalytic performance and stability for practical applications.展开更多
The process of utilizing solar-driven semiconductor water splitting for the production of hydrogen is a vital strategy in the pursuit of a zero-carbon economy.Zn_(0.1)Cd_(0.9)S,a rod-like semiconductor metal sulfide,e...The process of utilizing solar-driven semiconductor water splitting for the production of hydrogen is a vital strategy in the pursuit of a zero-carbon economy.Zn_(0.1)Cd_(0.9)S,a rod-like semiconductor metal sulfide,encounters considerable difficulties stemming from the swift recombination of charge carriers generated by light.Overcoming the coulombic interactions between charge carriers is essential for achieving efficient separation.In this study,we modified Zn_(0.1)Cd_(0.9)S with dodecahedral rare-earth compound CeVO_(4) and employed ultrasonic self-assembly to tightly couple the two materials.This integration established a built-in electric field and constructed an S-scheme heterojunction.Within this configuration,Zn_(0.1)Cd_(0.9)S serves as an electron acceptor while CeVO_(4) functions as an electron donor.Driven by the built-in electric field,electrons rapidly traverse the tightly coupled interface,minimizing their path length.The S-scheme heterojunction preserves the catalyst's strong redox capabilities and facilitates the vectorial separation of photogenerated charge carriers.In situ irradiated X-ray photoelectron spectroscopy(XPS)and electron paramagnetic resonance(EPR)analyses further validated the charge transfer mechanism of the S-scheme heterojunction.Density functional theory calculations elucidated the electronic states and roles of the catalyst,thereby establishing a theoretical framework for the investigation of S-scheme heterojunctions.This work lays a theoretical basis for the design and mechanistic investigation of S-scheme heterojunction catalysts.展开更多
Photocatalytic transfer hydrogenation using water as the proton source has emerged as an attractive and green approach for the catalytic reduction of unsaturated bonds.Herein,we report an oxygen-defective TiO_(2)-supp...Photocatalytic transfer hydrogenation using water as the proton source has emerged as an attractive and green approach for the catalytic reduction of unsaturated bonds.Herein,we report an oxygen-defective TiO_(2)-supported palladium catalyst(Pd-TiO_(2)-Ov)for efficient photocatalytic water-donating transfer hydrogenation of anethole towards 4-n-propylanisole in a high yield of 99.9%,which is significantly higher compared to the pristine TiO_(2)-supported palladium catalyst(Pd-TiO_(2),74%).The enhanced performance is ascribed to the presence of oxygen vacancies,which facilitate light absorption and suppress the recombination of photogenerated electron-hole pairs.Furthermore,the Pd-TiO_(2)-Ov is versatile in hydrogenating various alkene substrates including those with hydroxyl,ether,fluoride,and chloride functional groups in full conversion,thus offering a green method for transfer hydrogenation of alkenes.This study provides new insights and advances in current hydrogenation technology with water as the proton source.展开更多
The Internet of Vehicles,or IoV,is expected to lessen pollution,ease traffic,and increase road safety.IoV entities’interconnectedness,however,raises the possibility of cyberattacks,which can have detrimental effects....The Internet of Vehicles,or IoV,is expected to lessen pollution,ease traffic,and increase road safety.IoV entities’interconnectedness,however,raises the possibility of cyberattacks,which can have detrimental effects.IoV systems typically send massive volumes of raw data to central servers,which may raise privacy issues.Additionally,model training on IoV devices with limited resources normally leads to slower training times and reduced service quality.We discuss a privacy-preserving Federated Split Learning with Tiny Machine Learning(TinyML)approach,which operates on IoV edge devices without sharing sensitive raw data.Specifically,we focus on integrating split learning(SL)with federated learning(FL)and TinyML models.FL is a decentralisedmachine learning(ML)technique that enables numerous edge devices to train a standard model while retaining data locally collectively.The article intends to thoroughly discuss the architecture and challenges associated with the increasing prevalence of SL in the IoV domain,coupled with FL and TinyML.The approach starts with the IoV learning framework,which includes edge computing,FL,SL,and TinyML,and then proceeds to discuss how these technologies might be integrated.We elucidate the comprehensive operational principles of Federated and split learning by examining and addressingmany challenges.We subsequently examine the integration of SL with FL and various applications of TinyML.Finally,exploring the potential integration of FL and SL with TinyML in the IoV domain is referred to as FSL-TM.It is a superior method for preserving privacy as it conducts model training on individual devices or edge nodes,thereby obviating the necessity for centralised data aggregation,which presents considerable privacy threats.The insights provided aim to help both researchers and practitioners understand the complicated terrain of FL and SL,hence facilitating advancement in this swiftly progressing domain.展开更多
Drilling and blasting tunneling is a cyclic process in which tunnel rock undergoes repeated blast loading,affecting its dynamic characteristics,energy evolution,and damage progression.To explore the dynamic mechanical...Drilling and blasting tunneling is a cyclic process in which tunnel rock undergoes repeated blast loading,affecting its dynamic characteristics,energy evolution,and damage progression.To explore the dynamic mechanical properties and damage mechanisms of carbonaceous slate under cyclic impact loads of varying intensities,cyclic dynamic tests are conducted using a triaxial split Hopkinson pressure bar.This study analyzes the stress-strain relationship,energy damage evolution,and macro-to-micro failure characteristics.The results show that peak stress and strain are significantly influenced by impact intensity and the number of impacts.The initial dynamic stress is positively correlated with the impact intensity,but with more impact,the dynamic stress decreases while the peak strain increases.Energy evolution follows a pattern of"slow growthfluctuating growthrapid growth,"with the crack initiation stress and its proportion decreasing.CT and SEM analyses reveal that as the impact intensity increases,failure becomes more chaotic,the fracture volume increases,and the fracture mode shifts from interlayer and intergranular to through-layer and trans-granular fractures.These findings provide an experimental basis for soft rock tunnel stability analysis.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
Despite intensive research on solar-driven photocatalytic overall water splitting(POWS),the overall efficiencies remain insufficient to meet commercial standards.As a central challenge in realizing this technology mai...Despite intensive research on solar-driven photocatalytic overall water splitting(POWS),the overall efficiencies remain insufficient to meet commercial standards.As a central challenge in realizing this technology mainly lies in the precise tuning and rational designing of highly efficient materials and photocatalytic systems,which is paramount for its unlocking scalable,practical applications.However,novel materials fabrication and advanced photocatalytic systems are essential for overcoming intrinsic limitations of conventional catalysts by enabling this green technology to resolve global energy crisis.Therefore,this review critically explores the engineering developments in POWS process and novel photocatalyst designing,via shifting from simple bandgap engineering to more advanced charge carrier dynamics control via utilizing one/two-step photocatalytic excitation system,surface phase junctions i.e.,Z-scheme and S-scheme heterojunctions,surface modification,morphological tuning,and the role of co-catalysts,to control sluggish kinetics,promote oxygen evolution reaction(OER)and suppress undesirable H2/O2,backward reaction with superior visible light absorption capacity to produce remarkable energy production.Moreover,we critically discuss the recent trend of POWS from a materials discovery phase to demanding engineering and mechanistic optimization phase with viable economic viability,which requires bridging the gap between excellent lab-scale performance to stringent stability,cost,and high efficiency demands of industrial-scale solar fuel production.In addition,the currents challenges and future directions are also enclosed in detail for sustainable energy production.展开更多
NiFe layered double hydroxide(NiFe LDH)has emerged as a promising catalyst for the oxygen evolution reaction(OER);however,its hydrogen evolution reaction(HER)activity remains suboptimal due to unfavorable electronic s...NiFe layered double hydroxide(NiFe LDH)has emerged as a promising catalyst for the oxygen evolution reaction(OER);however,its hydrogen evolution reaction(HER)activity remains suboptimal due to unfavorable electronic structures,particularly the d-electron density of metal sites,which impede water dissociation and lead to poor hydrogen adsorption/desorption capabilities.Herein,we introduce an efficient cooperative d-electron density regulation(CDDR)engineering to comprehensively optimize the delectron density of NiFe LDH by grafting MoO_(x) -modified NiFe LDH nanosheets onto porous nickel particles(PNPs).The PNPs facilitate d-electron density modulation along the edges of the nanosheets,while the MoO_(x) species enable d-electron density modulation across the plane of the nanosheets,thus cooperatively constructing enriched d-electron density in NiFe LDH.Theoretical studies validate the CDDR process and reveal that the enriched d-electron density accelerates water dissociation and optimizes the hydrogen adsorption behavior of NiFe LDH.As a result,the engineered catalyst exhibits significantly improved HER activity,achieving an ultra-low overpotential of 38 mV at 10 mA cm^(-2)in 1 M KOH.Additionally,the CDDR-optimized catalyst also exhibits good OER performance,demonstrating excellent bifunctional performance for overall water splitting in both alkaline freshwater and seawater electrolytes.This work presents a novel CDDR strategy for engineering NiFe LDH into efficient HER catalysts without compromising its OER activity,potentially paving the way for the development of active and robust electrocatalysts for sustainable energy applications.展开更多
The personalized fine-tuning of large languagemodels(LLMs)on edge devices is severely constrained by limited computation resources.Although split federated learning alleviates on-device burdens,its effectiveness dimin...The personalized fine-tuning of large languagemodels(LLMs)on edge devices is severely constrained by limited computation resources.Although split federated learning alleviates on-device burdens,its effectiveness diminishes in few-shot reasoning scenarios due to the low data efficiency of conventional supervised fine-tuning,which leads to excessive communication overhead.To address this,we propose Language-Empowered Split Fine-Tuning(LESFT),a framework that integrates split architectures with a contrastive-inspired fine-tuning paradigm.LESFT simultaneously learns frommultiple logically equivalent but linguistically diverse reasoning chains,providing richer supervisory signals and improving data efficiency.This process-oriented training allows more effective reasoning adaptation with fewer samples.Extensive experiments demonstrate that LESFT consistently outperforms strong baselines such as SplitLoRA in task accuracy.LESFT consistently outperforms strong baselines on GSM8K,CommonsenseQA,and AQUA_RAT,with the largest gains observed on Qwen2.5-3B.These results indicate that LESFT can effectively adapt large language models for reasoning tasks under the computational and communication constraints of edge environments.展开更多
High‐entropy amorphous catalysts(HEACs)integrate multielement synergy with structural disorder,making them promising candidates for water splitting.Their distinctive features—including flexible coordination environm...High‐entropy amorphous catalysts(HEACs)integrate multielement synergy with structural disorder,making them promising candidates for water splitting.Their distinctive features—including flexible coordination environments,tunable electronic structures,abundant unsaturated active sites,and dynamic structural reassembly—collectively enhance electrochemical activity and durability under operating conditions.This review summarizes recent advances in HEACs for hydrogen evolution,oxygen evolution,and overall water splitting,highlighting their disorder-driven advantages over crystalline counterparts.Catalytic performance benchmarks are presented,and mechanistic insights are discussed,focusing on how multimetallic synergy,amorphization effect,and in‐situ reconstruction cooperatively regulate reaction pathways.These insights provide guidance for the rational design of next‐generation amorphous high‐entropy electrocatalysts with improved efficiency and durability.展开更多
Highly active and stable FeOOH cocatalysts are essential for achieving optimal performance of BiVO_(4)(BVO)photoanodes.Despite offering remarkable structural stability,widely used thick FeOOH cocatalysts often suffer ...Highly active and stable FeOOH cocatalysts are essential for achieving optimal performance of BiVO_(4)(BVO)photoanodes.Despite offering remarkable structural stability,widely used thick FeOOH cocatalysts often suffer from insufficient hole transport capability,which hinders the overall activity.The present study demonstrates that a simple photoetching strategy is able to introduce gradient distributed oxygen vacancies(GO_(V))in the thick FeOOH layer and significantly enhances the photogenerated holes transport dynamics.The incorporation of GO_(V)within FeOOH not only realizes the“relay transport”of photogenerated hole through the progressive upward shift of the valence band in the spatial distribution,but also provides abundant oxidation active sites by efficient hole trapping.These improvements effectively improve the oxygen evolution reaction(OER)activities and mitigate photocorrosion by the instantaneous hole extraction.Consequently,the FeOOH-GO_(V)layer enables the BVO/FeOOH-GO_(V)photoanode to achieve an impressive photocurrent density of 5.37 mA cm^(-2)and a robust operational stability up to 160 h at 1.23 VRHE,setting new benchmarks for current density and stability in FeOOH-based BVO photoanodes.This work provides an effective avenue to optimize OER cocatalysts for constructing highly efficient and stable photoelectrochemical water splitting devices.展开更多
Amorphous metal-based catalysts are highly promising for water splitting due to their abundance of unsaturated active sites.Herein,we report a one-step,surfactant-free synthesis of amorphous nickel nanoparticles(NPs)e...Amorphous metal-based catalysts are highly promising for water splitting due to their abundance of unsaturated active sites.Herein,we report a one-step,surfactant-free synthesis of amorphous nickel nanoparticles(NPs)encapsulated in nitrogen-doped carbon shells(A-Ni@NC)via pulsed laser ablation in liquid(PLAL).The synergistic integration of the amorphous Ni core and a defect-rich N-doped carbon shell markedly enhanced the catalytic activities for both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),with low overpotentials of 182 mV for HER and 288 mV for OER at 10 mA cm^(-2)in 1.0 m KOH.Furthermore,the bifunctional catalyst achieved a current density of 10 mA cm^(-2)at 1.63 V and retained 98.9%of its initial performance after 100 h of operation.The nitrogen-rich carbon shell not only offered abundant active sites and structural protection but also promoted charge transport.Density functional theory(DFT)calculations revealed that N-doping optimized intermediate adsorption energies,while the amorphous Ni core facilitated efficient electron transfer.This green and scalable synthesis strategy provides a promising platform for developing a wide range of transition metal@N-doped carbon hybrid catalysts for sustainable energy conversion applications.展开更多
Energy shortage has become one of themost concerning issues in the world today,and improving energy utilization efficiency is a key area of research for experts and scholars worldwide.Small-diameter heat exchangers of...Energy shortage has become one of themost concerning issues in the world today,and improving energy utilization efficiency is a key area of research for experts and scholars worldwide.Small-diameter heat exchangers offer advantages such as reduced material usage,lower refrigerant charge,and compact structure.However,they also face challenges,including increased refrigerant pressure drop and smaller heat transfer area inside the tubes.This paper combines the advantages and disadvantages of both small and large-diameter tubes and proposes a combined-diameter heat exchanger,consisting of large and small diameters,for use in the indoor units of split-type air conditioners.There are relatively few studies in this area.In this paper,A theoretical and numerical computation method is employed to establish a theoretical-numerical calculation model,and its reliability is verified through experiments.Using this model,the optimal combined diameters and flow path design for a combined-diameter heat exchanger using R32 as the working fluid are derived.The results show that the heat transfer performance of all combined diameter configurations improves by 2.79%to 8.26%compared to the baseline design,with the coefficient of performance(COP)increasing from 4.15 to 4.27~4.5.These designs can save copper material,but at the cost of an increase in pressure drop by 66.86%to 131.84%.The scheme IIIH,using R32,is the optimal combined-diameter and flow path configuration that balances both heat transfer performance and economic cost.展开更多
文摘This paper takes Zoomlion （Changsha Zoomlion Heavy Industry Science and Technology Development Co., Ltd） as an example and illustrates the reasons why traditional theories of stock dividends and stock splits cannot rationally explain the large stock dividend and stock split behavior among Chinese listed companies. The paper offers the following points after analyzing the current situation of China＇s capital market： As many investors seek after the stocks with large stock dividends and stock splits and form a ＂herd effect＂, it greatly pushes up the price of these stocks. Thus, companies＇ managers can cater these investors＇ irrational behavior, and help their companies get more funds from secondary equity offerings, or help their large shareholders and institutional investors to obtain more returns after lifting the sell restriction on their shares.
基金The National Natural Science Foundations of China (12202219)the Natural Science Foundations of Ningxia (2024AAC02009, 2023AAC05001)the Ningxia Youth Top Talents Training Project。
文摘The fast solution of linear equations has always been one of the hot spots in scientific computing.A kind of the diagonal matrix splitting iteration methods are provided,which is different from the classical matrix splitting methods.Taking the decomposition of the diagonal elements for coefficient matrix as the key point,some new preconditioners are constructed.Taking the tri-diagonal coefficient matrix as an example,the convergence domains and optimal relaxation factor of the new method are analyzed theoretically.The presented new iteration methods are applied to solve linear algebraic equations,even 2D and 3D diffusion problems with the fully implicit discretization.The results of numerical experiments are matched with the theoretical analysis,and show that the iteration numbers are reduced greatly.The superiorities of presented iteration methods exceed some classical iteration methods dramatically.
基金Supported by the National Natural Science Foundation of China(No.52273056)the Science and Technology Development Program of Jilin Province,China(No.YDZJ202501ZYTS305)。
文摘Electrochemical water splitting represents a sustainable technology for hydrogen(H_(2))production.However,its large-scale implementation is hindered by the high overpotentials required for both the cathodic hydrogen evolution reaction(HER)and the anodic oxygen evolution reaction(OER).Transition metal-based catalysts have garnered significant research interest as promising alternatives to noble-metal catalysts,owing to their low cost,tunable composition,and noble-metal-like catalytic activity.Nevertheless,systematic reviews on their application as bifunctional catalysts for overall water splitting(OWS)are still limited.This review comprehensively outlines the principal categories of bifunctional transition metal electrocatalysts derived from electrospun nanofibers(NFs),including metals,oxides,phosphides,sulfides,and carbides.Key strategies for enhancing their catalytic performance are systematically summarized,such as heterointerface engineering,heteroatom doping,metal-nonmetal-metal bridging architectures,and single-atom site design.Finally,current challenges and future research directions are discussed,aiming to provide insightful perspectives for the rational design of high-performance electrocatalysts for OWS.
文摘Two[FeFe]-hydrogenase compounds with 2-cyanobenzyl groups,{Fe_(2)[(SCH_(2)CH_(3))(SR)](CO)_(6)}(1 or 1′,which are the crystalline states from petroleum ether and dichloromethane solution,respectively)and{Fe_(2)[(SCH_(2)CH_(3))(SR)](CO)_(5)(PPh_(3))}(2)(R=2-cyanobenzyl),were synthesized and characterized by infrared spectroscopy,UV-Vis spectroscopy,single-crystal diffraction,powder X-ray diffraction,etc.Their performances as photocatalysts for H_(2)production through water splitting were evaluated.The results showed that 316.8μmol of H_(2)was produced on compound 1 after 3 h of illumination,with a catalytic efficiency of 25.1μmol·mg^(-1)·h^(-1)and a turnover number(TON)of 36.8.The replacement of carbonyl with PPh3 could significantly improve the catalytic performance of the complex,and 705.0μmol of H_(2)was produced on 2 after 3 h of illumination,with a catalytic efficiency of 37.9μmol·mg^(-1)·h^(-1)and a TON of 81.8.CCDC:2515700,1;2515702,1′;2515701,2.
基金Supported by Educational Department(JYTMS20230310)Natural Science Foundation of Liaoning Province(2024-MS-215)。
文摘Photoelectrochemical(PEC)water splitting is an effective approach to directly convert solar energy into clean hydrogen fuel.As a visible-light-responsive p-type semiconductor,CuBi_(2)O_(4)possesses a suitable bandgap and good stability.However,its performance is inhibited by high interfacial resistance and severe charge carrier recombination.In this study,a CuO interlayer was introduced between fluorine-doped tin oxide(FTO)and CuBi_(2)O_(4)to construct CuO/CuBi_(2)O_(4)photocathodes,aiming to improve interfacial charge transfer.The results showed that CuO/CuBi_(2)O_(4)-200 exhibited a photocurrent density of−1.71 mA/cm^(2)at 0 V vs.RHE,which was more than 3.5 times higher than that of bare CuBi_(2)O_(4).The incident photon-to-current efficiency(IPCE)at 365 nm was enhanced to~13%and the maximum applied bias photon-to-current efficiency(ABPE)reached 0.17%.Water splitting experiments revealed a hydrogen yield of 2.05μmol/cm^(2),significantly surpassing that of the unmodified photoelectrode.The enhanced PEC performance indicated that the CuO layer established a favorable band alignment,promoted hole transport toward the FTO substrate and effectively suppressed interfacial carrier recombination.This work demonstrated a simple and efficient interfacial engineering strategy,offering new insights and guidance for the design and development of high-performance semiconductor-based PEC photoelectrodes.
基金supported by a grant(No.CRPG-25-2054)under the Cybersecurity Research and Innovation Pioneers Initiative,provided by the National Cybersecurity Authority(NCA)in the Kingdom of Saudi Arabia.
文摘Split Learning(SL)has been promoted as a promising collaborative machine learning technique designed to address data privacy and resource efficiency.Specifically,neural networks are divided into client and server subnetworks in order to mitigate the exposure of sensitive data and reduce the overhead on client devices,thereby making SL particularly suitable for resource-constrained devices.Although SL prevents the direct transmission of raw data,it does not alleviate entirely the risk of privacy breaches.In fact,the data intermediately transmitted to the server sub-model may include patterns or information that could reveal sensitive data.Moreover,achieving a balance between model utility and data privacy has emerged as a challenging problem.In this article,we propose a novel defense approach that combines:(i)Adversarial learning,and(ii)Network channel pruning.In particular,the proposed adversarial learning approach is specifically designed to reduce the risk of private data exposure while maintaining high performance for the utility task.On the other hand,the suggested channel pruning enables the model to adaptively adjust and reactivate pruned channels while conducting adversarial training.The integration of these two techniques reduces the informativeness of the intermediate data transmitted by the client sub-model,thereby enhancing its robustness against attribute inference attacks without adding significant computational overhead,making it wellsuited for IoT devices,mobile platforms,and Internet of Vehicles(IoV)scenarios.The proposed defense approach was evaluated using EfficientNet-B0,a widely adopted compact model,along with three benchmark datasets.The obtained results showcased its superior defense capability against attribute inference attacks compared to existing state-of-the-art methods.This research’s findings demonstrated the effectiveness of the proposed channel pruning-based adversarial training approach in achieving the intended compromise between utility and privacy within SL frameworks.In fact,the classification accuracy attained by the attackers witnessed a drastic decrease of 70%.
基金supported by the National Natural Science Foundation of China(No.52274304).
文摘Designing a highly active and stable bifunctional catalyst is essential for achieving superior overall water splitting(OWS).In this study,a three-dimensional(3D)core-shell structure Co_(3)S_(4)/CuS@NiFe LDH nanocoral spheres electrocatalyst was constructed on nickel foam(NF)via an interfacial engineering strategy.This 3D core-shell heterostructure maximizes the exposure of active sites,optimizes the charge transport pathway and accelerates gas release rates.The protective shell strategy of NiFe LDH provides favorable stability,which contributes to inhibiting the electrochemical corrosion of the electrocatalyst and mitigating the toxic effects of Cl^(-) and other microorganisms during the seawater splitting process.Moreover,the introduction of NiFe LDH induces a change in the OER mechanism from an adsorption evolution mechanism(AEM)to a lattice oxygen mechanism(LOM),which improves the intrinsic activity of the catalyst.Consequently,Co_(3)S_(4)/CuS@NiFe LDH demonstrates exceptional performance in the oxygen evolution reaction(OER)(η100=251 mV)and in the hydrogen evolution reaction(HER)(η100=254 mV),alongside remarkable stability over 100 h.For OWS,it exhibits a voltage of 1.46 V at 10 mA/cm^(2) and maintain stability for 100 h.Impressively,Co_(3)S_(4)/CuS@NiFe LDH still possesses outstanding activity and stability in natural alkaline seawater.This work proposes interfacial engineering to construct bifunctional catalysts with core-shell heterostructures,providing instructive guidelines for the design of highly efficient electrocatalysts toward seawater electrolysis.
基金the financial support from the National Natural Science Foundation of China (Nos.21805170,22172093)Natural Science Foundation of Shandong Province (Nos.ZR2023QB219,ZR2021QB161)Qingdao Postdoctoral Innovation Project (No.QDBSH20220202031)。
文摘Herein,we have developed a straightforward wet-chemical method to synthesize a series of Pd-based alloy nanowires(NWs),including Pd Pt NWs,Pd Au NWs,Pd Ir NWs,and Pd Ru NWs,which exhibits high mass activity and turnover frequency(TOF) for HER,surpassing Pt/C by 4.6-fold and 1.5-fold in acidic and alkaline electrolytes,respectively.It also demonstrates high stability in alkaline electrolyte at a current density of 220 m A/cm^(2) for 280 h,highlighting its potential for practical applications under industrial current conditions.Pd Pt NWs exhibited ultrathin structures with head-to-tail kinks and inherent defects,significantly increasing the density of active sites and precisely tuning the electronic structure,which could accelerate reaction kinetics and boost water-splitting electrocatalytic performance.This study highlights the potential of Pd Pt NWs as highly efficient catalysts,offering outstanding catalytic performance and stability for practical applications.
基金Project supported by the National Natural Science Foundation of China(22271106,52073286)the Natural Science Foundation of Fujian Province(2006L2005)。
文摘The process of utilizing solar-driven semiconductor water splitting for the production of hydrogen is a vital strategy in the pursuit of a zero-carbon economy.Zn_(0.1)Cd_(0.9)S,a rod-like semiconductor metal sulfide,encounters considerable difficulties stemming from the swift recombination of charge carriers generated by light.Overcoming the coulombic interactions between charge carriers is essential for achieving efficient separation.In this study,we modified Zn_(0.1)Cd_(0.9)S with dodecahedral rare-earth compound CeVO_(4) and employed ultrasonic self-assembly to tightly couple the two materials.This integration established a built-in electric field and constructed an S-scheme heterojunction.Within this configuration,Zn_(0.1)Cd_(0.9)S serves as an electron acceptor while CeVO_(4) functions as an electron donor.Driven by the built-in electric field,electrons rapidly traverse the tightly coupled interface,minimizing their path length.The S-scheme heterojunction preserves the catalyst's strong redox capabilities and facilitates the vectorial separation of photogenerated charge carriers.In situ irradiated X-ray photoelectron spectroscopy(XPS)and electron paramagnetic resonance(EPR)analyses further validated the charge transfer mechanism of the S-scheme heterojunction.Density functional theory calculations elucidated the electronic states and roles of the catalyst,thereby establishing a theoretical framework for the investigation of S-scheme heterojunctions.This work lays a theoretical basis for the design and mechanistic investigation of S-scheme heterojunction catalysts.
基金supported by the National Key Research and Development Program of China(2023YFD2200505)National Natural Science Foundation of China(22202105),Natural Science Foundation of Jiangsu Higher Education Institutions of China(21KJA150003)the Innovation and Entrepreneurship Team Program of Jiangsu Province(JSSCTD202345).
文摘Photocatalytic transfer hydrogenation using water as the proton source has emerged as an attractive and green approach for the catalytic reduction of unsaturated bonds.Herein,we report an oxygen-defective TiO_(2)-supported palladium catalyst(Pd-TiO_(2)-Ov)for efficient photocatalytic water-donating transfer hydrogenation of anethole towards 4-n-propylanisole in a high yield of 99.9%,which is significantly higher compared to the pristine TiO_(2)-supported palladium catalyst(Pd-TiO_(2),74%).The enhanced performance is ascribed to the presence of oxygen vacancies,which facilitate light absorption and suppress the recombination of photogenerated electron-hole pairs.Furthermore,the Pd-TiO_(2)-Ov is versatile in hydrogenating various alkene substrates including those with hydroxyl,ether,fluoride,and chloride functional groups in full conversion,thus offering a green method for transfer hydrogenation of alkenes.This study provides new insights and advances in current hydrogenation technology with water as the proton source.
文摘The Internet of Vehicles,or IoV,is expected to lessen pollution,ease traffic,and increase road safety.IoV entities’interconnectedness,however,raises the possibility of cyberattacks,which can have detrimental effects.IoV systems typically send massive volumes of raw data to central servers,which may raise privacy issues.Additionally,model training on IoV devices with limited resources normally leads to slower training times and reduced service quality.We discuss a privacy-preserving Federated Split Learning with Tiny Machine Learning(TinyML)approach,which operates on IoV edge devices without sharing sensitive raw data.Specifically,we focus on integrating split learning(SL)with federated learning(FL)and TinyML models.FL is a decentralisedmachine learning(ML)technique that enables numerous edge devices to train a standard model while retaining data locally collectively.The article intends to thoroughly discuss the architecture and challenges associated with the increasing prevalence of SL in the IoV domain,coupled with FL and TinyML.The approach starts with the IoV learning framework,which includes edge computing,FL,SL,and TinyML,and then proceeds to discuss how these technologies might be integrated.We elucidate the comprehensive operational principles of Federated and split learning by examining and addressingmany challenges.We subsequently examine the integration of SL with FL and various applications of TinyML.Finally,exploring the potential integration of FL and SL with TinyML in the IoV domain is referred to as FSL-TM.It is a superior method for preserving privacy as it conducts model training on individual devices or edge nodes,thereby obviating the necessity for centralised data aggregation,which presents considerable privacy threats.The insights provided aim to help both researchers and practitioners understand the complicated terrain of FL and SL,hence facilitating advancement in this swiftly progressing domain.
基金support from the Joint Funds of the National Natural Science Foundation of China(Grant No.U23A2060)the National Natural Science Foundation of China(Grant Nos.42177143 and 52474150).
文摘Drilling and blasting tunneling is a cyclic process in which tunnel rock undergoes repeated blast loading,affecting its dynamic characteristics,energy evolution,and damage progression.To explore the dynamic mechanical properties and damage mechanisms of carbonaceous slate under cyclic impact loads of varying intensities,cyclic dynamic tests are conducted using a triaxial split Hopkinson pressure bar.This study analyzes the stress-strain relationship,energy damage evolution,and macro-to-micro failure characteristics.The results show that peak stress and strain are significantly influenced by impact intensity and the number of impacts.The initial dynamic stress is positively correlated with the impact intensity,but with more impact,the dynamic stress decreases while the peak strain increases.Energy evolution follows a pattern of"slow growthfluctuating growthrapid growth,"with the crack initiation stress and its proportion decreasing.CT and SEM analyses reveal that as the impact intensity increases,failure becomes more chaotic,the fracture volume increases,and the fracture mode shifts from interlayer and intergranular to through-layer and trans-granular fractures.These findings provide an experimental basis for soft rock tunnel stability analysis.
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the Taizhou University,Zhejiang,China for funding(No.T20250101215)the Deanship of research and Graduate Studies at King Khalid University for funding this work through Large Research Project(R.G.P.2/398/46).
文摘Despite intensive research on solar-driven photocatalytic overall water splitting(POWS),the overall efficiencies remain insufficient to meet commercial standards.As a central challenge in realizing this technology mainly lies in the precise tuning and rational designing of highly efficient materials and photocatalytic systems,which is paramount for its unlocking scalable,practical applications.However,novel materials fabrication and advanced photocatalytic systems are essential for overcoming intrinsic limitations of conventional catalysts by enabling this green technology to resolve global energy crisis.Therefore,this review critically explores the engineering developments in POWS process and novel photocatalyst designing,via shifting from simple bandgap engineering to more advanced charge carrier dynamics control via utilizing one/two-step photocatalytic excitation system,surface phase junctions i.e.,Z-scheme and S-scheme heterojunctions,surface modification,morphological tuning,and the role of co-catalysts,to control sluggish kinetics,promote oxygen evolution reaction(OER)and suppress undesirable H2/O2,backward reaction with superior visible light absorption capacity to produce remarkable energy production.Moreover,we critically discuss the recent trend of POWS from a materials discovery phase to demanding engineering and mechanistic optimization phase with viable economic viability,which requires bridging the gap between excellent lab-scale performance to stringent stability,cost,and high efficiency demands of industrial-scale solar fuel production.In addition,the currents challenges and future directions are also enclosed in detail for sustainable energy production.
基金financially supported from the National Key Research and Development Program of China(2022YFB3803600)the National Natural Science Foundation of China(52301272,22309168,12564025,and 52472205)+7 种基金the Fundamental Research Funds for the Central Universities(CCNU25ZH006)the National College Student Innovation and Entrepreneurship Training Project(202510513082)the Research Program of HBNU(2025X082 and2025Y145)the Foundation of Hubei Key Laboratory of Photoelectric Materials and Devices(PMD202404)the General Program of Open Project of the State Key Laboratory of Precision Welding and Joining of Materials Structures(MSWJ-25M-18)the Key Research Project of Hubei Provincial Department of Education(No.D20252503)the Key Project of Hubei Provincial Natural Science Foundation of China(2025AFD002)the Foundation of National Laboratory of Solid State Microstructures(M37087)。
文摘NiFe layered double hydroxide(NiFe LDH)has emerged as a promising catalyst for the oxygen evolution reaction(OER);however,its hydrogen evolution reaction(HER)activity remains suboptimal due to unfavorable electronic structures,particularly the d-electron density of metal sites,which impede water dissociation and lead to poor hydrogen adsorption/desorption capabilities.Herein,we introduce an efficient cooperative d-electron density regulation(CDDR)engineering to comprehensively optimize the delectron density of NiFe LDH by grafting MoO_(x) -modified NiFe LDH nanosheets onto porous nickel particles(PNPs).The PNPs facilitate d-electron density modulation along the edges of the nanosheets,while the MoO_(x) species enable d-electron density modulation across the plane of the nanosheets,thus cooperatively constructing enriched d-electron density in NiFe LDH.Theoretical studies validate the CDDR process and reveal that the enriched d-electron density accelerates water dissociation and optimizes the hydrogen adsorption behavior of NiFe LDH.As a result,the engineered catalyst exhibits significantly improved HER activity,achieving an ultra-low overpotential of 38 mV at 10 mA cm^(-2)in 1 M KOH.Additionally,the CDDR-optimized catalyst also exhibits good OER performance,demonstrating excellent bifunctional performance for overall water splitting in both alkaline freshwater and seawater electrolytes.This work presents a novel CDDR strategy for engineering NiFe LDH into efficient HER catalysts without compromising its OER activity,potentially paving the way for the development of active and robust electrocatalysts for sustainable energy applications.
基金supported in part by the National Natural Science Foundation of China(NSFC)under Grant 62276109The authors extend their appreciation to the Deanship of Scientific Research at King Saud University for funding this work through the Research Group Project number(ORF-2025-585).
文摘The personalized fine-tuning of large languagemodels(LLMs)on edge devices is severely constrained by limited computation resources.Although split federated learning alleviates on-device burdens,its effectiveness diminishes in few-shot reasoning scenarios due to the low data efficiency of conventional supervised fine-tuning,which leads to excessive communication overhead.To address this,we propose Language-Empowered Split Fine-Tuning(LESFT),a framework that integrates split architectures with a contrastive-inspired fine-tuning paradigm.LESFT simultaneously learns frommultiple logically equivalent but linguistically diverse reasoning chains,providing richer supervisory signals and improving data efficiency.This process-oriented training allows more effective reasoning adaptation with fewer samples.Extensive experiments demonstrate that LESFT consistently outperforms strong baselines such as SplitLoRA in task accuracy.LESFT consistently outperforms strong baselines on GSM8K,CommonsenseQA,and AQUA_RAT,with the largest gains observed on Qwen2.5-3B.These results indicate that LESFT can effectively adapt large language models for reasoning tasks under the computational and communication constraints of edge environments.
基金supported by the Australian Research Council(ARC)Projects(DP220101139,DP220101142,and LP240100542).
文摘High‐entropy amorphous catalysts(HEACs)integrate multielement synergy with structural disorder,making them promising candidates for water splitting.Their distinctive features—including flexible coordination environments,tunable electronic structures,abundant unsaturated active sites,and dynamic structural reassembly—collectively enhance electrochemical activity and durability under operating conditions.This review summarizes recent advances in HEACs for hydrogen evolution,oxygen evolution,and overall water splitting,highlighting their disorder-driven advantages over crystalline counterparts.Catalytic performance benchmarks are presented,and mechanistic insights are discussed,focusing on how multimetallic synergy,amorphization effect,and in‐situ reconstruction cooperatively regulate reaction pathways.These insights provide guidance for the rational design of next‐generation amorphous high‐entropy electrocatalysts with improved efficiency and durability.
基金supported by the State Key Laboratory of Solidification Processing in NWPU(SKLSP202407)the National Natural Science Foundation of China(52402130)+2 种基金the Natural Science Basis Research Plan in Shaanxi Province of China(2024JC-YBQN-0384)the Shaanxi Science and Technology Innovation Team(2023-CX-TD-44)the National Natural Science Foundation of China(52301015).
文摘Highly active and stable FeOOH cocatalysts are essential for achieving optimal performance of BiVO_(4)(BVO)photoanodes.Despite offering remarkable structural stability,widely used thick FeOOH cocatalysts often suffer from insufficient hole transport capability,which hinders the overall activity.The present study demonstrates that a simple photoetching strategy is able to introduce gradient distributed oxygen vacancies(GO_(V))in the thick FeOOH layer and significantly enhances the photogenerated holes transport dynamics.The incorporation of GO_(V)within FeOOH not only realizes the“relay transport”of photogenerated hole through the progressive upward shift of the valence band in the spatial distribution,but also provides abundant oxidation active sites by efficient hole trapping.These improvements effectively improve the oxygen evolution reaction(OER)activities and mitigate photocorrosion by the instantaneous hole extraction.Consequently,the FeOOH-GO_(V)layer enables the BVO/FeOOH-GO_(V)photoanode to achieve an impressive photocurrent density of 5.37 mA cm^(-2)and a robust operational stability up to 160 h at 1.23 VRHE,setting new benchmarks for current density and stability in FeOOH-based BVO photoanodes.This work provides an effective avenue to optimize OER cocatalysts for constructing highly efficient and stable photoelectrochemical water splitting devices.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(NRF-2023R1A2C1005419).
文摘Amorphous metal-based catalysts are highly promising for water splitting due to their abundance of unsaturated active sites.Herein,we report a one-step,surfactant-free synthesis of amorphous nickel nanoparticles(NPs)encapsulated in nitrogen-doped carbon shells(A-Ni@NC)via pulsed laser ablation in liquid(PLAL).The synergistic integration of the amorphous Ni core and a defect-rich N-doped carbon shell markedly enhanced the catalytic activities for both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),with low overpotentials of 182 mV for HER and 288 mV for OER at 10 mA cm^(-2)in 1.0 m KOH.Furthermore,the bifunctional catalyst achieved a current density of 10 mA cm^(-2)at 1.63 V and retained 98.9%of its initial performance after 100 h of operation.The nitrogen-rich carbon shell not only offered abundant active sites and structural protection but also promoted charge transport.Density functional theory(DFT)calculations revealed that N-doping optimized intermediate adsorption energies,while the amorphous Ni core facilitated efficient electron transfer.This green and scalable synthesis strategy provides a promising platform for developing a wide range of transition metal@N-doped carbon hybrid catalysts for sustainable energy conversion applications.
基金supported by Supported by the Scientific Research Foundation for High-Level Talents of Zhoukou Normal University(ZKNUC2024018).
文摘Energy shortage has become one of themost concerning issues in the world today,and improving energy utilization efficiency is a key area of research for experts and scholars worldwide.Small-diameter heat exchangers offer advantages such as reduced material usage,lower refrigerant charge,and compact structure.However,they also face challenges,including increased refrigerant pressure drop and smaller heat transfer area inside the tubes.This paper combines the advantages and disadvantages of both small and large-diameter tubes and proposes a combined-diameter heat exchanger,consisting of large and small diameters,for use in the indoor units of split-type air conditioners.There are relatively few studies in this area.In this paper,A theoretical and numerical computation method is employed to establish a theoretical-numerical calculation model,and its reliability is verified through experiments.Using this model,the optimal combined diameters and flow path design for a combined-diameter heat exchanger using R32 as the working fluid are derived.The results show that the heat transfer performance of all combined diameter configurations improves by 2.79%to 8.26%compared to the baseline design,with the coefficient of performance(COP)increasing from 4.15 to 4.27~4.5.These designs can save copper material,but at the cost of an increase in pressure drop by 66.86%to 131.84%.The scheme IIIH,using R32,is the optimal combined-diameter and flow path configuration that balances both heat transfer performance and economic cost.
