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
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
Recent advancements in electrocatalysis have highlighted the exceptional application value of amorphous electrocatalysts. Withtheir unique atomic configurations, these electrocatalysts exhibit superior catalytic perfo...Recent advancements in electrocatalysis have highlighted the exceptional application value of amorphous electrocatalysts. Withtheir unique atomic configurations, these electrocatalysts exhibit superior catalytic performance compared to that of their crystalline coun-terparts. Transition metal(TM) amorphous ribbon-shaped electrocatalysts have recently emerged as a new frontier in the catalysis field.Dealloying is widely considered a fascinating method for enhancing the electrocatalyst performance. In this review, we comprehensivelyexamine the principles of water electrolysis, discuss the prevalent methods for fabricating ribbon-configured electrocatalysts, and providean overview of amorphous alloys. Furthermore, we discuss binary, ternary, and high-entropy amorphous TM-based electrocatalysts,which satisfy the requirements necessary for effective water electrolysis. We also propose strategies to enhance the activity of amorphousTM-based ribbons, including morphology control, defect engineering, composition optimization, and heterostructure creation in differentelectrolytes. Our focus extends to the latest developments in the design of heterogeneous micro/nanostructures, management of prepara-tion techniques, and synthesis of different compositions. Finally, we address the ongoing challenges and provide a perspective on the fu-ture development of broadly applicable, self-supporting TM ribbon-shaped electrocatalysts.展开更多
Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance i...Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.展开更多
Electrochemical water splitting presents a promising,environmentally friendly alternative to fossil fuels for hydrogen production.However,the efficiency is constrained by the sluggish kinetics and high overpotentials ...Electrochemical water splitting presents a promising,environmentally friendly alternative to fossil fuels for hydrogen production.However,the efficiency is constrained by the sluggish kinetics and high overpotentials associated with the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).While noble metal catalysts,such as Pt for HER and Ir for OER,currently offer superior performance,their widespread adoption is hindered by high cost and scarcity.This has spurred research into costeffective alternatives,with a focus on understanding the underlying electrocatalytic mechanisms.MXenes,a class of two-dimensional materials,have emerged as promising candidates for electrocatalytic water splitting due to their unique physical and chemical properties.However,research in this field remains largely experimental,lacking a comprehensive understanding of fundamental mechanisms.This knowledge gap impedes the development of high-efficiency electrocatalysts and necessitates further investigation.This review systematically examines recent advancements in MXene-based nanohybrids for electrocatalytic water splitting,covering synthetic methods,structure-property relationships,and performance enhancement strategies.It encompasses both precious and non-noble metal-based systems for HER,OER,and overall water splitting applications.Additionally,this review addresses current challenges,opportunities,and future research directions for MXene-based nanohybrids.By providing comprehensive insights into the development of high-performance MXene-based electrocatalysts,this review aims to accelerate progress in the field of electrochemical water splitting.It serves as a valuable resource for researchers and engineers working towards more efficient and sustainable hydrogen production technologies,potentially contributing to the broader goal of transitioning away from fossil fuels towards cleaner energy sources.展开更多
In this paper,we propose a rate splitting multiple access(RSMA)based integrated sensing and communication system(ISAC),where the sensing and communication are realized simultaneously with the RSMA signal.Further,recon...In this paper,we propose a rate splitting multiple access(RSMA)based integrated sensing and communication system(ISAC),where the sensing and communication are realized simultaneously with the RSMA signal.Further,reconfigurable holographic surface(RHS)is utilized to replace the traditional antennas for beam generation,expecting to combine the advantages of RSMA and RHS.To maximize the weighted summation of system rate and probing power,an optimization problem is formulated to jointly design the digital beamformer,the holographic beamformer and the message splitting vectors.To solve the non-convex problem,we first decompose it into two subproblems,where one jointly designs the digital beamformer and message splitting vectors,and the other deals with the holographic beamformer.An iterative algorithm,which leverages successive convex approximation and semi-definite relaxation,is proposed to achieve the sub-optimal solution through solving these two subproblems alternatively.Simulations confirm the effectiveness and efficiency of the proposed algorithm.展开更多
Theory and practice have confirmed that the propagation of converted transverse waves in azimuthally anisotropic media results in shear-wave splitting,causing differences in travel time and reflection amplitude betwee...Theory and practice have confirmed that the propagation of converted transverse waves in azimuthally anisotropic media results in shear-wave splitting,causing differences in travel time and reflection amplitude between S1/S2 waves,which reduces the imaging quality and vertical resolution of converted transverse wave.Therefore,eliminating shear-wave splitting is one of the important steps in the imaging processing of converted transverse wave.Due to the limitations of actual data acquisition and signal-tonoise ratio,it is difficult to directly determine a set of orthogonal four components for shear-wave splitting analysis,which cannot achieve good correction processing results.To this end,starting from Alford rotation,an orthogonal four component equation system is derived,and the least squares method is used to stably solve the high signal-to-noise ratio orthogonal four components.Based on this,the crack orientation and fast/slow wave delay are estimated through azimuth and time-delay scanning,and the shear-wave splitting correction and fast/slow wave separation are completed by layer striping from shallow to deep.The synthetic data and actual data calculations show that this method can achieve good azimuthal anisotropy correction,separation of S1/S2 waves,and accurate imaging.展开更多
The development of highly active and easily coupled non-noble metal electrocatalysts for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is of great significance for the H_(2) production by water ele...The development of highly active and easily coupled non-noble metal electrocatalysts for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is of great significance for the H_(2) production by water electrolysis.Here,we have shown an anion-modulated HER and OER activity of 1D Co-Mo based interstitial compound heterojunctions for effective overall water splitting.The Co-Mo based complex nanowires from a one-pot route with high yields can be converted into MoC-Co heterojunction nanowires under N_(2) atmosphere,while a pyrolysis under NH_(3) can give CoMoN-CoN heterostructures.The work function revealed Mott-Schottky effect between interfaces of two heterostructures,which can introduce electron redistribution and thus promote the HER/OER process.The MoC-Co heterojunction nanowires delivers good HER activity at a low overpotential of 39mV to afford a current density of 10mA/cm^(2).Density functional theory calculations show that the heterogeneous interface formed between the Co and MoC optimizes the hydrogen adsorption free energy.Concurrently,CoMoN-CoN heterojunction nanowires exhibits good OER performance with a low overpotential of 260mV to reach 10mA/cm^(2),being superior to RuO_(2).The two catalysts can be coupled to assemble a two-electrode cell with a solarto-hydrogen efficiency of 12.3%at 1.54 V.This work provides an effective means to design easily coupled HER and OER catalysts for H_(2) production by water electrolysis.展开更多
In recent years,the development of wafer-level GaN nanowires photocatalyst loaded onto silicon substrates has progressed rapidly depending on its simplicity of instrumentation,collection and separation from the water....In recent years,the development of wafer-level GaN nanowires photocatalyst loaded onto silicon substrates has progressed rapidly depending on its simplicity of instrumentation,collection and separation from the water.Accordingly,the wafer-level GaN-based nanowires(GaN NWs)photocatalyst can be a fabulous candidate for the application in the field of photocatalytic hydrogen evolution reaction(PHER)and provides a novel route to address the environmental and energy crisis.Herein,a range of innovative strategies to improve the performance of GaN NWs photocatalyst are systematically summarized.Then,the solar-to-hydrogen conversion efficiency,the characteristics of GaN NWs system,the cost of the origin material required,as well as the stability,activity and the corrosion resistance to seawater are discussed in detail as some of the essential conditions for advancing its large-scale industry-friendly application.Last but not least,we provide the potential application of this system for splitting seawater to produce hydrogen and point out the direction for overcoming the barriers to future industrial-scale implementation.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
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
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
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
Bismuth vanadate(BiVO_(4))is regarded as a promising photoanode for photoelectrochemical(PEC)water splitting.Despite its advantage in band gap and visible-light response,the BiVO_(4)exhibits an unsatisfactory achievin...Bismuth vanadate(BiVO_(4))is regarded as a promising photoanode for photoelectrochemical(PEC)water splitting.Despite its advantage in band gap and visible-light response,the BiVO_(4)exhibits an unsatisfactory achieving water splitting due to severe charge recombination.Herein,we elucidate an innovative approach involving the incorporation of single Ru atom with a CoFe-LDH cocatalyst(Ru_(0.51)-CoFe-LDH)and integrating it onto the BiVO_(4)semiconductor substrate.The resulting Ru_(0.51)-CoFe-LDH/BiVO_(4)photoanode film demonstrates commendable charge injection efficiency(76%)and charge collection efficiency(100%).Interestingly,the yield of hydrogen and oxygen increases linearly at a stoichiometric ratio of about 2:1,reaching 158.6 and 67.4μmol after140 min of irradiation,respectively.According to experimental characterization and density functional theory calculation,this remarkable performance results from single Ru atoms triggering the electron rearrangement of Ru_(0.51)-CoFe-LDH to engineer active sites and optimize interfacial energetics.Additionally,the negative shift of Ru_(0.51)-CoFe-LDH band edge gives rise to more conspicuous band bending of the n-n junction formed with BiVO_(4),expediting the separation and transfer of photogenerated electron-hole pairs at the interface.This work furnishes a new preparation perspective for PEC water splitting systems to construct single atoms in the semiconductor substrate.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
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.
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financially supported by the Yancheng Polytechnic College School-Level Scientific Research, China (No. ygy1903)the National Natural Science Foundation of China (Nos. 52001163, 52075237, and 52371157)+2 种基金the Open Project of Taihu Laboratory of Deep-Sea Technology Science, Key Research and Development Plan of Jiangsu Province, China (No. BE2019119)supported by the Priority Academic Program Development of Jiangsu Higher Education Institution (PAPD), Chinathe research funding for the Jiangsu Specially-Appointed Professor Program, China。
文摘Recent advancements in electrocatalysis have highlighted the exceptional application value of amorphous electrocatalysts. Withtheir unique atomic configurations, these electrocatalysts exhibit superior catalytic performance compared to that of their crystalline coun-terparts. Transition metal(TM) amorphous ribbon-shaped electrocatalysts have recently emerged as a new frontier in the catalysis field.Dealloying is widely considered a fascinating method for enhancing the electrocatalyst performance. In this review, we comprehensivelyexamine the principles of water electrolysis, discuss the prevalent methods for fabricating ribbon-configured electrocatalysts, and providean overview of amorphous alloys. Furthermore, we discuss binary, ternary, and high-entropy amorphous TM-based electrocatalysts,which satisfy the requirements necessary for effective water electrolysis. We also propose strategies to enhance the activity of amorphousTM-based ribbons, including morphology control, defect engineering, composition optimization, and heterostructure creation in differentelectrolytes. Our focus extends to the latest developments in the design of heterogeneous micro/nanostructures, management of prepara-tion techniques, and synthesis of different compositions. Finally, we address the ongoing challenges and provide a perspective on the fu-ture development of broadly applicable, self-supporting TM ribbon-shaped electrocatalysts.
基金supported by Multi-Year Research Grants from the University of Macao(MYRG-GRG2023-00010-IAPME,MYRG-GRG2024-00038-IAPME,MYRG2022-00026-IAPME)the Science and Technology Development Fund(FDCT)from Macao SAR(0023/2023/AFJ,0050/2023/RIB2,006/2022/ALC,0087/2024/AFJ,0111/2022/A2).
文摘Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.
基金support from the National Natural Science Foundation of China(Nos.22278364,22208296,U22A20432,22211530045,22178308,22208076)the development project of Zhejiang Province’s"Jianbing"and"Lingyan"(No.2023C01226)+7 种基金Science Foundation of Donghai Laboratory(No.DH2022ZY0009)National Key Research and Development Program of China(No.2022YFB4002100)the Zhejiang Province Basic Public Welfare Research Program(Nos.LQ24B030007,LQ23B060001)the Fundamental Research Funds for the Central Universities(Nos.226–2022–00044,226–2024–00060)the Research Funds of Institute of Zhejiang University-Quzhou(Nos.IZQ2021RCZX026,IZQ2021KJ2008)Key Technology Breakthrough Program of Ningbo“Science and Innovation Yongjiang 2035”(No.2024H024)the Hubei Provincial Natural Science Foundation of China(No.2024AFB1036)the Doctoral Scientific Research Foundation of Hubei University of Automotive Technology(No.BK202354)。
文摘Electrochemical water splitting presents a promising,environmentally friendly alternative to fossil fuels for hydrogen production.However,the efficiency is constrained by the sluggish kinetics and high overpotentials associated with the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).While noble metal catalysts,such as Pt for HER and Ir for OER,currently offer superior performance,their widespread adoption is hindered by high cost and scarcity.This has spurred research into costeffective alternatives,with a focus on understanding the underlying electrocatalytic mechanisms.MXenes,a class of two-dimensional materials,have emerged as promising candidates for electrocatalytic water splitting due to their unique physical and chemical properties.However,research in this field remains largely experimental,lacking a comprehensive understanding of fundamental mechanisms.This knowledge gap impedes the development of high-efficiency electrocatalysts and necessitates further investigation.This review systematically examines recent advancements in MXene-based nanohybrids for electrocatalytic water splitting,covering synthetic methods,structure-property relationships,and performance enhancement strategies.It encompasses both precious and non-noble metal-based systems for HER,OER,and overall water splitting applications.Additionally,this review addresses current challenges,opportunities,and future research directions for MXene-based nanohybrids.By providing comprehensive insights into the development of high-performance MXene-based electrocatalysts,this review aims to accelerate progress in the field of electrochemical water splitting.It serves as a valuable resource for researchers and engineers working towards more efficient and sustainable hydrogen production technologies,potentially contributing to the broader goal of transitioning away from fossil fuels towards cleaner energy sources.
基金supported by the Joint Funds of the National Natural Science Foundation of China(No.U23A20277)the Joint Funds of the National Natural Science Foundation of China(No.U22A2003).
文摘In this paper,we propose a rate splitting multiple access(RSMA)based integrated sensing and communication system(ISAC),where the sensing and communication are realized simultaneously with the RSMA signal.Further,reconfigurable holographic surface(RHS)is utilized to replace the traditional antennas for beam generation,expecting to combine the advantages of RSMA and RHS.To maximize the weighted summation of system rate and probing power,an optimization problem is formulated to jointly design the digital beamformer,the holographic beamformer and the message splitting vectors.To solve the non-convex problem,we first decompose it into two subproblems,where one jointly designs the digital beamformer and message splitting vectors,and the other deals with the holographic beamformer.An iterative algorithm,which leverages successive convex approximation and semi-definite relaxation,is proposed to achieve the sub-optimal solution through solving these two subproblems alternatively.Simulations confirm the effectiveness and efficiency of the proposed algorithm.
基金supported by Sinopec Science and Technology Research Project(P23098,P25152).
文摘Theory and practice have confirmed that the propagation of converted transverse waves in azimuthally anisotropic media results in shear-wave splitting,causing differences in travel time and reflection amplitude between S1/S2 waves,which reduces the imaging quality and vertical resolution of converted transverse wave.Therefore,eliminating shear-wave splitting is one of the important steps in the imaging processing of converted transverse wave.Due to the limitations of actual data acquisition and signal-tonoise ratio,it is difficult to directly determine a set of orthogonal four components for shear-wave splitting analysis,which cannot achieve good correction processing results.To this end,starting from Alford rotation,an orthogonal four component equation system is derived,and the least squares method is used to stably solve the high signal-to-noise ratio orthogonal four components.Based on this,the crack orientation and fast/slow wave delay are estimated through azimuth and time-delay scanning,and the shear-wave splitting correction and fast/slow wave separation are completed by layer striping from shallow to deep.The synthetic data and actual data calculations show that this method can achieve good azimuthal anisotropy correction,separation of S1/S2 waves,and accurate imaging.
基金support of this research by the National Natural Science Foundation of China(No.91961111)the Natural Science Foundation of Heilongjiang Province(No.ZD2021B003)Fundamental Research Funds for the Central Universities(No.2572022BU05).
文摘The development of highly active and easily coupled non-noble metal electrocatalysts for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is of great significance for the H_(2) production by water electrolysis.Here,we have shown an anion-modulated HER and OER activity of 1D Co-Mo based interstitial compound heterojunctions for effective overall water splitting.The Co-Mo based complex nanowires from a one-pot route with high yields can be converted into MoC-Co heterojunction nanowires under N_(2) atmosphere,while a pyrolysis under NH_(3) can give CoMoN-CoN heterostructures.The work function revealed Mott-Schottky effect between interfaces of two heterostructures,which can introduce electron redistribution and thus promote the HER/OER process.The MoC-Co heterojunction nanowires delivers good HER activity at a low overpotential of 39mV to afford a current density of 10mA/cm^(2).Density functional theory calculations show that the heterogeneous interface formed between the Co and MoC optimizes the hydrogen adsorption free energy.Concurrently,CoMoN-CoN heterojunction nanowires exhibits good OER performance with a low overpotential of 260mV to reach 10mA/cm^(2),being superior to RuO_(2).The two catalysts can be coupled to assemble a two-electrode cell with a solarto-hydrogen efficiency of 12.3%at 1.54 V.This work provides an effective means to design easily coupled HER and OER catalysts for H_(2) production by water electrolysis.
基金supported by the Natural Science Foundation of China(No.51902101,22479079)Innovation Support Programme(Soft Science Research)Project Achievements of Jiangsu Province(BK20231514)+3 种基金the Youth Natural Science Foundation of Hunan Province(No.2021JJ40044)Natural Science Foundation of Jiangsu Province(No.BK20201381)Science Foundation of Nanjing University of Posts and Telecommunications(Nos.NY219144,NY221046)the National College Student Innovation and Entrepre-neurship Training Program(No.202210293083Y).
文摘In recent years,the development of wafer-level GaN nanowires photocatalyst loaded onto silicon substrates has progressed rapidly depending on its simplicity of instrumentation,collection and separation from the water.Accordingly,the wafer-level GaN-based nanowires(GaN NWs)photocatalyst can be a fabulous candidate for the application in the field of photocatalytic hydrogen evolution reaction(PHER)and provides a novel route to address the environmental and energy crisis.Herein,a range of innovative strategies to improve the performance of GaN NWs photocatalyst are systematically summarized.Then,the solar-to-hydrogen conversion efficiency,the characteristics of GaN NWs system,the cost of the origin material required,as well as the stability,activity and the corrosion resistance to seawater are discussed in detail as some of the essential conditions for advancing its large-scale industry-friendly application.Last but not least,we provide the potential application of this system for splitting seawater to produce hydrogen and point out the direction for overcoming the barriers to future industrial-scale implementation.
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financially supported by the Hunan Provincial Natural Science Foundation for Distinguished Young Scholars(2025JJ20019)the National Key R&D Program of China(2025YFE0107600)。
文摘Bismuth vanadate(BiVO_(4))is regarded as a promising photoanode for photoelectrochemical(PEC)water splitting.Despite its advantage in band gap and visible-light response,the BiVO_(4)exhibits an unsatisfactory achieving water splitting due to severe charge recombination.Herein,we elucidate an innovative approach involving the incorporation of single Ru atom with a CoFe-LDH cocatalyst(Ru_(0.51)-CoFe-LDH)and integrating it onto the BiVO_(4)semiconductor substrate.The resulting Ru_(0.51)-CoFe-LDH/BiVO_(4)photoanode film demonstrates commendable charge injection efficiency(76%)and charge collection efficiency(100%).Interestingly,the yield of hydrogen and oxygen increases linearly at a stoichiometric ratio of about 2:1,reaching 158.6 and 67.4μmol after140 min of irradiation,respectively.According to experimental characterization and density functional theory calculation,this remarkable performance results from single Ru atoms triggering the electron rearrangement of Ru_(0.51)-CoFe-LDH to engineer active sites and optimize interfacial energetics.Additionally,the negative shift of Ru_(0.51)-CoFe-LDH band edge gives rise to more conspicuous band bending of the n-n junction formed with BiVO_(4),expediting the separation and transfer of photogenerated electron-hole pairs at the interface.This work furnishes a new preparation perspective for PEC water splitting systems to construct single atoms in the semiconductor substrate.
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.
