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
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
For efficient electrolysis of water for hydrogen generation or other valueadded chemicals, it is highly relevant to develop low-temperature synthesis of low-cost and high-e ciency metal sulfide electrocatalysts on a l...For efficient electrolysis of water for hydrogen generation or other valueadded chemicals, it is highly relevant to develop low-temperature synthesis of low-cost and high-e ciency metal sulfide electrocatalysts on a large scale. Herein, we construct a new core–branch array and binder-free electrode by growing Ni_3S_2 nanoflake branches on an atomic-layer-deposited(ALD) TiO_2 skeleton. Through induced growth on the ALD-TiO_2 backbone, cross-linked Ni_3S_2 nanoflake branches with exposed { 210} highindex facets are uniformly anchored to the preformed TiO_2 core forming an integrated electrocatalyst. Such a core–branch array structure possesses large active surface area, uniform porous structure, and rich active sites of the exposed { 210 } high-index facet in the Ni_3S_2 nanoflake. Accordingly, the TiO_2@Ni_3S_2 core/branch arrays exhibit remarkable electrocatalytic activities in an alkaline medium, with lower overpotentials for both oxygen evolution reaction(220 mV at 10 mA cm^(-2)) and hydrogen evolution reaction(112 m V at 10 mA cm^(-2)), which are better than those of other Ni_3S_2 counterparts. Stable overall water splitting based on this bifunctional electrolyzer is also demonstrated.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
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
In this article a new approach is considered for implementing operator splitting methods for transport problems, influenced by electric fields. Our motivation came to model PE-CVD (plasma-enhanced chemical vapor depos...In this article a new approach is considered for implementing operator splitting methods for transport problems, influenced by electric fields. Our motivation came to model PE-CVD (plasma-enhanced chemical vapor deposition) processes, means the flow of species to a gas-phase, which are influenced by an electric field. Such a field we can model by wave equations. The main contributions are to improve the standard discretization schemes of each part of the coupling equation. So we discuss an improvement with implicit Runge- Kutta methods instead of the Yee’s algorithm. Further we balance the solver method between the Maxwell and Transport equation.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
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
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
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
Effective utilization of hot electrons generated from the decay of surface plasmon resonance in metal nanoparticles is conductive to improve solar water splitting efficiency.Herein,Ag nanoparticles and reduced graphen...Effective utilization of hot electrons generated from the decay of surface plasmon resonance in metal nanoparticles is conductive to improve solar water splitting efficiency.Herein,Ag nanoparticles and reduced graphene oxide(rGO)co-decorated hierarchical TiO2 nanoring/nanotube arrays(TiO2 R/T)were facilely fabricated by using two-step electrochemical anodization,electrodeposition,and photoreduction methods.Comparative studies were conducted to elucidate the effects of rGO and Ag on the morphology,photoresponse,charge transfer,and photoelectric properties of TiO2.Firstly,scanning electron microscope images confirm that the Ag nanoparticles adhered on TiO2 R/T and TiO2 R/T-rGO have similar diameter of 20 nm except for TiO2 R-rGO/T.Then,the UV-Vis DRS and scatter spectra reveal that the optical property of the Ag-TiO2 R/T-rGO ternary composite is enhanced,ascribing to the visible light absorption of plasmonic Ag nanoparticles and the weakening effect of rGO on light scattering.Meanwhile,intensity-modulated photocurrent spectroscopy and photoluminescence spectra demonstrate that rGO can promote the hot electrons transfer from Ag nanoparticles to Ti substrate,reducing the photogenerated electron-hole recombination.Finally,Ag-TiO2 R/T-rGO photoanode exhibits high photocurrent density(0.98 mA cm?2)and photovoltage(0.90 V),and the stable H2 evolution rate of 413μL h?1 cm?2 within 1.5 h under AM 1.5 which exceeds by 1.30 times than that of pristine TiO2 R/T.In line with the above results,this work provides a reliable route synergizing rGO with plasmonic metal nanoparticles for photocatalysis,in which,rGO presents a broad absorption spectrum and effective photogenerated electrons transfer.展开更多
In order to enhance photocatalytic water splitting rates with Pt/TiO2 powder, sufficient agitation of the biphasic medium is required to switch surficial reactions to volumetric reactions. Additionally, agitation is c...In order to enhance photocatalytic water splitting rates with Pt/TiO2 powder, sufficient agitation of the biphasic medium is required to switch surficial reactions to volumetric reactions. Additionally, agitation is conducive to higher diffusion rates of the generated hydrogen and co-produced oxygen, hindering their ability to re-couple to water on Pt loaded to TiO2 powder. In order to create agitation without consuming any electricity, a novel technique utilizing Rayleigh convection was applied, and its ability to enhance photocatalytic water splitting rates was evaluated. Higher Rayleigh convective flow rates resulted in higher photocatalytic water splitting rates. Utilization of Rayleigh convection approximately doubled the photocatalytic water splitting rates, despite relatively low convective flow velocities (obtained through simple thermo-hydrodynamic simulations). The rate enhancement achieved through Rayleigh convection is a result of its ability to disperse the ultrafine Pt/TiO2 particles throughout the whole medium, leading to volumetric reactions.展开更多
Altermagnets represent a newly discovered class of magnetically ordered materials.Among all the candidates,CrSb stands out due to its largest spin splitting energy and highest Néel temperature exceeding 700 K,mak...Altermagnets represent a newly discovered class of magnetically ordered materials.Among all the candidates,CrSb stands out due to its largest spin splitting energy and highest Néel temperature exceeding 700 K,making it promising for room-temperature spintronic applications.Here we have successfully grown high quality CrSb(100)thin film on GaAs(110)substrate by molecular beam epitaxy.Using angle-resolved photoemission spectroscopy,we successfully obtained the three-dimensional electronic structure of the thin film.Moreover,we observed the emergence of the altermagnetic splitting bands corresponding to the calculated results along the low symmetry pathsT-QandP-D.The bands near the Fermi level are only spin splitting bands along theP-Ddirection,with splitting energy reaching as high as 910 meV.This finding provides insights into the magnetic properties of CrSb thin films and paves the way for further studies on their electronic structure and potential applications in spintronics.展开更多
We report the observation of Zeeman splitting in multiple spectral lines emitted by a laser-produced,magnetized plasma(1–3×10^(18)cm^(-3),1–15 eV)in the context of a laboratory astrophysics experiment under a c...We report the observation of Zeeman splitting in multiple spectral lines emitted by a laser-produced,magnetized plasma(1–3×10^(18)cm^(-3),1–15 eV)in the context of a laboratory astrophysics experiment under a controlled magneticfield up to 20T.Nitrogen lines(NII)in the visible range were used to diagnose the magneticfield and plasma conditions.This was performed by coupling our data with(563–574 nm)the Stark–Zeeman line-shape code PPPB.The excellent agreement between experiment and simulations paves the way for a non-intrusive experimental platform to get time-resolved measurements of the local magneticfield in laboratory plasmas.展开更多
Altermagnets,a class of unconventional antiferromagnets with non-relativistic spin-splitting,offer promising potential for antiferromagnetic spintronic devices.While many altermagnets are limited by either low magneti...Altermagnets,a class of unconventional antiferromagnets with non-relativistic spin-splitting,offer promising potential for antiferromagnetic spintronic devices.While many altermagnets are limited by either low magnetic transition temperatures or weak spin splitting,the recently discovered metal CrSb,with high N′eel temperature(T_(N)=710 K)and significant spin-splitting due to its unique spin space group,provides a robust platform for remarkable tunneling magnetoresistance(TMR)in collinear all-antiferromagnetic tunnel junctions(AATJs).This study systematically investigates the spin-polarized Fermi surface of CrSb and spin-dependent electron transport in CrSb-based AATJs.The CrSb/β-InSe/CrSb junction with a three-monolayer InSe barrier exhibits a TMR ratio of approximately 290%,with energy-dependent analysis revealing TMR ratios that may exceed 850%when considering the shift of the Fermi energy.We also demonstrate the angle-dependent TMR of CrSb-based AATJs by adjusting N′eel vector orientations.Our findings might provide strong theoretical support for CrSb as a versatile building block for all-antiferromagnetic memory devices.展开更多
The chemical looping reforming of methane through the nonstoichiometric ceria redox cycle(CeO2/CeO2-δ) has been experimentally investigated in a directly irradiated solar reactor to convert both solar energy and meth...The chemical looping reforming of methane through the nonstoichiometric ceria redox cycle(CeO2/CeO2-δ) has been experimentally investigated in a directly irradiated solar reactor to convert both solar energy and methane to syngas in the temperature range 900–1050 °C. Experiments were carried out with different ceria shapes via two-step redox cycling composed of endothermic partial reduction of ceria with methane and complete exothermic re-oxidation of reduced ceria with H2 O/CO2 at the same operating temperature, thereby demonstrating the capability to operate the cycle isothermally. A parametric study considering different ceria macrostructure variants(ceria packed powder, ceria packed powder mixed with inert Al2 O3 particles, and ceria reticulated porous foam) and operating parameters(methane flow-rate, reduction temperature, or sintering temperature) was conducted in order to unravel their impact on the bed-averaged oxygen non-stoichiometry(δ), syngas yield, methane conversion, and solar reactor performance. The ceria cycling stability was also experimentally investigated to demonstrate repeatable syngas production by alternating the flow between CH4 and H2 O(or CO2). A decrease in sintering temperature of the ceria foam was beneficial for increasing syngas selectivity, methane conversion,and reactor performance. Increasing both CH4 concentration and reduction temperature enhanced δ with the maximum value up to 0.41 but concomitantly favored CH4 cracking reaction. The ceria reticulated porous foam showed better performance in terms of effective heat transfer, due to volumetric absorption of concentrated solar radiation and uniform heating with lower solar power consumption, thereby promoting the solar-to-fuel energy conversion efficiency that reached up to 5.60%. The energy upgrade factor achieved during cycle was up to 1.19. Stable patterns in the δ and syngas yield for consecutive cycles with the ceria foam validated material performance stability.展开更多
Altermagnets,a new type of collinear antiferromagnet,exhibiting non-degenerate electron and magnon dispersion in momentum space have attracted intensive research attention.We theoretically analyze the origin and featu...Altermagnets,a new type of collinear antiferromagnet,exhibiting non-degenerate electron and magnon dispersion in momentum space have attracted intensive research attention.We theoretically analyze the origin and feature of chiral magnon splitting in representative altermagnets including tetragonal RuO_(2),hexagonal MnTe,and orthorhombic LaMnO_(3).The magnon spin transport properties including spin Seebeck and spin Nernst coefcients have been investigated.Through these materials,we demonstrate the diference of chiral splitting in d-wave and g-wave antiferromagnet on magnon transport.RuO2with planar magnon splitting exhibits signifcant magnon spin Nernst and magnon spin Seebeck anisotropy in(110)and(001)planes,whereas MnTe,due to its bulk-like magnon splitting,is incapable of producing magnon spin Nernst efect.Our work may provide in-depth understanding on the mechanisms of nonrelativistic magnon splitting and thermal spin transport in altermagnets.展开更多
The two-dimensional electron gas(2DEG)formed at the interface between two oxide insulators provides new opportunities for electronics and spintronics.The broken inversion symmetry at the heterointerface results in a R...The two-dimensional electron gas(2DEG)formed at the interface between two oxide insulators provides new opportunities for electronics and spintronics.The broken inversion symmetry at the heterointerface results in a Rashba spin-orbit coupling(RSOC)effect that enables the conversion between spin and charge currents.However,conducting oxide interfaces that simultaneously exhibit strong RSOC and high carrier mobility-a combination query for achieving high spin-to-charge inter-conversion efficiencies-remain scarce.Herein,we report a correlated 2DEG with giant Rashba splitting and high electron mobility in(111)-oriented EuTiO_(3)/KTaO_(3)(ETO/KTO)heterostructures under light illumination.Upon light modulation,a unique carrier-dependent giant anomalous Hall effect,the signature of spin-polarized 2DEG,emerges with a sign crossover at a carrier density of approximately 5.0×10^(13)cm^(-2),highlighting dramatic changes in the band topology of KTO(111)interface.Furthermore,at 2 K,the carrier mobility is enhanced from 103 cm^(2)·V^(-1)·s^(-1)to 1800 cm^(2)·V^(-1)·s^(-1),a remarkable enhancement of approximately 20 times.Accompanying with a giant Rashba coefficient αR up to 360meV·˚A,this high mobility ferromagnetic 5d oxide 2DEG is predicted to achieve a giant spin-to-charge conversion efficiency ofλ~10 nm,showing great potential for designing low-power spin-orbitronic devices.展开更多
Generally,the catalytic overpotentials of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)are unavoidable because of the low charge transfer.In this work,two strategies of alloying of Co with Ni and ...Generally,the catalytic overpotentials of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)are unavoidable because of the low charge transfer.In this work,two strategies of alloying of Co with Ni and enclosing of electrocatalysts with carbonaceous materials were both used to accelerate the catalytic efficiency of cobalt selenide for water splitting.The nitrogen-doped carbon(NC)layer improves the reaction kinetics by efficient charge transfer.The alloying of metal into composited electrocatalysts can modify the electronic properties of host materials,thereby tuning the adsorption behavior of intermediate and improving the electrocatalytic activity.As expected,Nyquist plots reveal that the charge-transfer resistance(Rct)of nickel cobalt selenide encapsulated into nitrogen-doped carbon layer(CoNiSe/NC-3,Co:Ni=1:1)are just 5 and 9 for HER and OER,respectively,which are much lower than those of CoSe/NC-1(Co:Ni=1:0)(81 and 138)and CoNiSe/NC-3 without NC(CoNiSe-3)(54 and 25).With the high charge transfer and porous structure,CoNiSe/NC-3 shows good performance for both HER and OER.When current density reaches 10 m A cm-2,only 100 and 270 mV overpotentials are required for HER and OER,respectively.With the potential of 1.65 V,full water splitting also can be catalyzed by Co Ni Se/NC-3 with current density of 20 m A cm-2,suggesting that CoNiSe/NC-3 could be used as replacement for noble metal electrocatalysts.展开更多
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supported by National Natural Science Foundation of China (Grant Nos. 51728204 and 51772272)Fundamental Research Funds for the Central Universities (Grant No. 2018QNA4011)+2 种基金Qianjiang Talents Plan D (QJD1602029)Startup Foundation for Hundred-Talent Program of Zhejiang Universitythe Fundamental Research Funds for the Central Universities (2015XZZX010-02)
文摘For efficient electrolysis of water for hydrogen generation or other valueadded chemicals, it is highly relevant to develop low-temperature synthesis of low-cost and high-e ciency metal sulfide electrocatalysts on a large scale. Herein, we construct a new core–branch array and binder-free electrode by growing Ni_3S_2 nanoflake branches on an atomic-layer-deposited(ALD) TiO_2 skeleton. Through induced growth on the ALD-TiO_2 backbone, cross-linked Ni_3S_2 nanoflake branches with exposed { 210} highindex facets are uniformly anchored to the preformed TiO_2 core forming an integrated electrocatalyst. Such a core–branch array structure possesses large active surface area, uniform porous structure, and rich active sites of the exposed { 210 } high-index facet in the Ni_3S_2 nanoflake. Accordingly, the TiO_2@Ni_3S_2 core/branch arrays exhibit remarkable electrocatalytic activities in an alkaline medium, with lower overpotentials for both oxygen evolution reaction(220 mV at 10 mA cm^(-2)) and hydrogen evolution reaction(112 m V at 10 mA cm^(-2)), which are better than those of other Ni_3S_2 counterparts. Stable overall water splitting based on this bifunctional electrolyzer is also demonstrated.
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.
文摘In this article a new approach is considered for implementing operator splitting methods for transport problems, influenced by electric fields. Our motivation came to model PE-CVD (plasma-enhanced chemical vapor deposition) processes, means the flow of species to a gas-phase, which are influenced by an electric field. Such a field we can model by wave equations. The main contributions are to improve the standard discretization schemes of each part of the coupling equation. So we discuss an improvement with implicit Runge- Kutta methods instead of the Yee’s algorithm. Further we balance the solver method between the Maxwell and Transport equation.
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 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the National Natural Science Foundation of China(Grant No.51776009)for the financial support.
文摘Effective utilization of hot electrons generated from the decay of surface plasmon resonance in metal nanoparticles is conductive to improve solar water splitting efficiency.Herein,Ag nanoparticles and reduced graphene oxide(rGO)co-decorated hierarchical TiO2 nanoring/nanotube arrays(TiO2 R/T)were facilely fabricated by using two-step electrochemical anodization,electrodeposition,and photoreduction methods.Comparative studies were conducted to elucidate the effects of rGO and Ag on the morphology,photoresponse,charge transfer,and photoelectric properties of TiO2.Firstly,scanning electron microscope images confirm that the Ag nanoparticles adhered on TiO2 R/T and TiO2 R/T-rGO have similar diameter of 20 nm except for TiO2 R-rGO/T.Then,the UV-Vis DRS and scatter spectra reveal that the optical property of the Ag-TiO2 R/T-rGO ternary composite is enhanced,ascribing to the visible light absorption of plasmonic Ag nanoparticles and the weakening effect of rGO on light scattering.Meanwhile,intensity-modulated photocurrent spectroscopy and photoluminescence spectra demonstrate that rGO can promote the hot electrons transfer from Ag nanoparticles to Ti substrate,reducing the photogenerated electron-hole recombination.Finally,Ag-TiO2 R/T-rGO photoanode exhibits high photocurrent density(0.98 mA cm?2)and photovoltage(0.90 V),and the stable H2 evolution rate of 413μL h?1 cm?2 within 1.5 h under AM 1.5 which exceeds by 1.30 times than that of pristine TiO2 R/T.In line with the above results,this work provides a reliable route synergizing rGO with plasmonic metal nanoparticles for photocatalysis,in which,rGO presents a broad absorption spectrum and effective photogenerated electrons transfer.
文摘In order to enhance photocatalytic water splitting rates with Pt/TiO2 powder, sufficient agitation of the biphasic medium is required to switch surficial reactions to volumetric reactions. Additionally, agitation is conducive to higher diffusion rates of the generated hydrogen and co-produced oxygen, hindering their ability to re-couple to water on Pt loaded to TiO2 powder. In order to create agitation without consuming any electricity, a novel technique utilizing Rayleigh convection was applied, and its ability to enhance photocatalytic water splitting rates was evaluated. Higher Rayleigh convective flow rates resulted in higher photocatalytic water splitting rates. Utilization of Rayleigh convection approximately doubled the photocatalytic water splitting rates, despite relatively low convective flow velocities (obtained through simple thermo-hydrodynamic simulations). The rate enhancement achieved through Rayleigh convection is a result of its ability to disperse the ultrafine Pt/TiO2 particles throughout the whole medium, leading to volumetric reactions.
基金supported by the National Key R&D Program of China[Grant No.2023YFA1406304(J J)]the National Natural Science Foundation of China[Grant No.12174362(J J)]+2 种基金the Innovation Program for Quantum Science and Technology[Grant No.2021ZD0302803(D L F)]the New Cornerstone Science Foundation(D L F)Beamline 03U of the Shanghai Synchrotron Radiation Facility,which is supported by ME2 project under contract No.11227902 from the National Natural Science Foundation of China。
文摘Altermagnets represent a newly discovered class of magnetically ordered materials.Among all the candidates,CrSb stands out due to its largest spin splitting energy and highest Néel temperature exceeding 700 K,making it promising for room-temperature spintronic applications.Here we have successfully grown high quality CrSb(100)thin film on GaAs(110)substrate by molecular beam epitaxy.Using angle-resolved photoemission spectroscopy,we successfully obtained the three-dimensional electronic structure of the thin film.Moreover,we observed the emergence of the altermagnetic splitting bands corresponding to the calculated results along the low symmetry pathsT-QandP-D.The bands near the Fermi level are only spin splitting bands along theP-Ddirection,with splitting energy reaching as high as 910 meV.This finding provides insights into the magnetic properties of CrSb thin films and paves the way for further studies on their electronic structure and potential applications in spintronics.
基金supported by grants managed by l’Agence Nationale de la Recherche under the Investissements d’Avenir programs Grant Nos. ANR-18-EURE-0014, ANR-10-LABX-0039-PALM, and ANR-22-CE30-0044supported by grants from Japan Society for the Promotion of Science (JSPS) KAKENHI (Grant No. 23K20038)+2 种基金JSPS Core-to-Core program (Grant No. JPJSCCA20230003)carried out within the framework of the EUROfusion Consortium, funded by the European Union via the Euratom Research and Training Programme (Grant Agreement No. 101052200-EUROfusion)operated within the framework of the Enabling Research Project No. AWP24-ENR-IFE.02.CEA-01 “Magnetized ICF”
文摘We report the observation of Zeeman splitting in multiple spectral lines emitted by a laser-produced,magnetized plasma(1–3×10^(18)cm^(-3),1–15 eV)in the context of a laboratory astrophysics experiment under a controlled magneticfield up to 20T.Nitrogen lines(NII)in the visible range were used to diagnose the magneticfield and plasma conditions.This was performed by coupling our data with(563–574 nm)the Stark–Zeeman line-shape code PPPB.The excellent agreement between experiment and simulations paves the way for a non-intrusive experimental platform to get time-resolved measurements of the local magneticfield in laboratory plasmas.
基金supported by the National Natural Science Foundation of China(Grant Nos.T2394475,T2394470,T2394471,and 12174129)the China Postdoctoral Science Foundation(Grant No.2023M741269).
文摘Altermagnets,a class of unconventional antiferromagnets with non-relativistic spin-splitting,offer promising potential for antiferromagnetic spintronic devices.While many altermagnets are limited by either low magnetic transition temperatures or weak spin splitting,the recently discovered metal CrSb,with high N′eel temperature(T_(N)=710 K)and significant spin-splitting due to its unique spin space group,provides a robust platform for remarkable tunneling magnetoresistance(TMR)in collinear all-antiferromagnetic tunnel junctions(AATJs).This study systematically investigates the spin-polarized Fermi surface of CrSb and spin-dependent electron transport in CrSb-based AATJs.The CrSb/β-InSe/CrSb junction with a three-monolayer InSe barrier exhibits a TMR ratio of approximately 290%,with energy-dependent analysis revealing TMR ratios that may exceed 850%when considering the shift of the Fermi energy.We also demonstrate the angle-dependent TMR of CrSb-based AATJs by adjusting N′eel vector orientations.Our findings might provide strong theoretical support for CrSb as a versatile building block for all-antiferromagnetic memory devices.
基金The King Mongkut’s Institute of Technology Ladkrabang(KMITL),Thailandthe Franco-Thai scholarship program。
文摘The chemical looping reforming of methane through the nonstoichiometric ceria redox cycle(CeO2/CeO2-δ) has been experimentally investigated in a directly irradiated solar reactor to convert both solar energy and methane to syngas in the temperature range 900–1050 °C. Experiments were carried out with different ceria shapes via two-step redox cycling composed of endothermic partial reduction of ceria with methane and complete exothermic re-oxidation of reduced ceria with H2 O/CO2 at the same operating temperature, thereby demonstrating the capability to operate the cycle isothermally. A parametric study considering different ceria macrostructure variants(ceria packed powder, ceria packed powder mixed with inert Al2 O3 particles, and ceria reticulated porous foam) and operating parameters(methane flow-rate, reduction temperature, or sintering temperature) was conducted in order to unravel their impact on the bed-averaged oxygen non-stoichiometry(δ), syngas yield, methane conversion, and solar reactor performance. The ceria cycling stability was also experimentally investigated to demonstrate repeatable syngas production by alternating the flow between CH4 and H2 O(or CO2). A decrease in sintering temperature of the ceria foam was beneficial for increasing syngas selectivity, methane conversion,and reactor performance. Increasing both CH4 concentration and reduction temperature enhanced δ with the maximum value up to 0.41 but concomitantly favored CH4 cracking reaction. The ceria reticulated porous foam showed better performance in terms of effective heat transfer, due to volumetric absorption of concentrated solar radiation and uniform heating with lower solar power consumption, thereby promoting the solar-to-fuel energy conversion efficiency that reached up to 5.60%. The energy upgrade factor achieved during cycle was up to 1.19. Stable patterns in the δ and syngas yield for consecutive cycles with the ceria foam validated material performance stability.
基金supported by the National Natural Science Foundation of China(Grant Nos.12174129,T2394475,and T2394470)。
文摘Altermagnets,a new type of collinear antiferromagnet,exhibiting non-degenerate electron and magnon dispersion in momentum space have attracted intensive research attention.We theoretically analyze the origin and feature of chiral magnon splitting in representative altermagnets including tetragonal RuO_(2),hexagonal MnTe,and orthorhombic LaMnO_(3).The magnon spin transport properties including spin Seebeck and spin Nernst coefcients have been investigated.Through these materials,we demonstrate the diference of chiral splitting in d-wave and g-wave antiferromagnet on magnon transport.RuO2with planar magnon splitting exhibits signifcant magnon spin Nernst and magnon spin Seebeck anisotropy in(110)and(001)planes,whereas MnTe,due to its bulk-like magnon splitting,is incapable of producing magnon spin Nernst efect.Our work may provide in-depth understanding on the mechanisms of nonrelativistic magnon splitting and thermal spin transport in altermagnets.
基金supported by the Science Center of the National Science Foundation of China(Grant No.52088101)the National Key Research and Development Program of China(Grant Nos.2023YFA1406400,2021YFA1400300,and 2023YFA1607403)the National Natural Science Foundation of China(Grant Nos.T2394472 and T2394470).
文摘The two-dimensional electron gas(2DEG)formed at the interface between two oxide insulators provides new opportunities for electronics and spintronics.The broken inversion symmetry at the heterointerface results in a Rashba spin-orbit coupling(RSOC)effect that enables the conversion between spin and charge currents.However,conducting oxide interfaces that simultaneously exhibit strong RSOC and high carrier mobility-a combination query for achieving high spin-to-charge inter-conversion efficiencies-remain scarce.Herein,we report a correlated 2DEG with giant Rashba splitting and high electron mobility in(111)-oriented EuTiO_(3)/KTaO_(3)(ETO/KTO)heterostructures under light illumination.Upon light modulation,a unique carrier-dependent giant anomalous Hall effect,the signature of spin-polarized 2DEG,emerges with a sign crossover at a carrier density of approximately 5.0×10^(13)cm^(-2),highlighting dramatic changes in the band topology of KTO(111)interface.Furthermore,at 2 K,the carrier mobility is enhanced from 103 cm^(2)·V^(-1)·s^(-1)to 1800 cm^(2)·V^(-1)·s^(-1),a remarkable enhancement of approximately 20 times.Accompanying with a giant Rashba coefficient αR up to 360meV·˚A,this high mobility ferromagnetic 5d oxide 2DEG is predicted to achieve a giant spin-to-charge conversion efficiency ofλ~10 nm,showing great potential for designing low-power spin-orbitronic devices.
基金financial support by the National Natural Science Foundation of China (21605015)the Development Project of Science and Technology of Jilin Province (20170101176JC)+3 种基金the Fundamental Research Funds for the Central Universities (2412017BJ003)the Recruitment Program of Global Youth Experts, the Jilin Provincial Department of Educationthe start-up funds from Northeast Normal Universitythe service support from Analysis and Testing Center of Northeast Normal University
文摘Generally,the catalytic overpotentials of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)are unavoidable because of the low charge transfer.In this work,two strategies of alloying of Co with Ni and enclosing of electrocatalysts with carbonaceous materials were both used to accelerate the catalytic efficiency of cobalt selenide for water splitting.The nitrogen-doped carbon(NC)layer improves the reaction kinetics by efficient charge transfer.The alloying of metal into composited electrocatalysts can modify the electronic properties of host materials,thereby tuning the adsorption behavior of intermediate and improving the electrocatalytic activity.As expected,Nyquist plots reveal that the charge-transfer resistance(Rct)of nickel cobalt selenide encapsulated into nitrogen-doped carbon layer(CoNiSe/NC-3,Co:Ni=1:1)are just 5 and 9 for HER and OER,respectively,which are much lower than those of CoSe/NC-1(Co:Ni=1:0)(81 and 138)and CoNiSe/NC-3 without NC(CoNiSe-3)(54 and 25).With the high charge transfer and porous structure,CoNiSe/NC-3 shows good performance for both HER and OER.When current density reaches 10 m A cm-2,only 100 and 270 mV overpotentials are required for HER and OER,respectively.With the potential of 1.65 V,full water splitting also can be catalyzed by Co Ni Se/NC-3 with current density of 20 m A cm-2,suggesting that CoNiSe/NC-3 could be used as replacement for noble metal electrocatalysts.
