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 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
Water oxidation-a critical yet sluggish step in green hydrogen production-is a major bottleneck for electrolysis efficiency.Traditional catalysts often degrade quickly under the high current densities needed for indus...Water oxidation-a critical yet sluggish step in green hydrogen production-is a major bottleneck for electrolysis efficiency.Traditional catalysts often degrade quickly under the high current densities needed for industrial scale.展开更多
Harnessing solar energy for renewable fuel production through artificial photosynthesis offers an ideal solution to the current energy and environmental crises.Among various methods,photoelectrochemical(PEC)water spli...Harnessing solar energy for renewable fuel production through artificial photosynthesis offers an ideal solution to the current energy and environmental crises.Among various methods,photoelectrochemical(PEC)water splitting stands out as a promising approach for direct solar-driven hydrogen production.Enhancing the efficiency and stability of photoelectrodes is a key focus in PEC water-splitting research.Tantalum nitride(Ta_(3)N_(5)),with its suitable band gap and band-edge positions for PEC water splitting,has emerged as a highly promising photoanode material.This review begins by introducing the history and fundamental characteristics of Ta_(3)N_(5),emphasizing both its advantages and challenges.It then explores methods to improve light absorption efficiency,charge separation and transfer efficiency,surface reaction rate,and the stability of Ta_(3)N_(5) photoanodes.Additionally,the review discusses the progress of research on tandem PEC cells incorporating Ta_(3)N_(5) photoanodes.Finally,it looks ahead to future research directions for Ta_(3)N_(5) photoanodes.The strategic approach outlined in this review can also be applied to other photoelectrode materials,providing guidance for their development.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
Electrocatalytic water splitting(EWS)driven by renewable energy is vital for clean hydrogen(H2)production and reducing reliance on fossil fuels.While IrO_(2) and RuO_(2) are the leading electrocatalysts for the oxygen...Electrocatalytic water splitting(EWS)driven by renewable energy is vital for clean hydrogen(H2)production and reducing reliance on fossil fuels.While IrO_(2) and RuO_(2) are the leading electrocatalysts for the oxygen evolution reaction(OER)and Pt for the hydrogen evolution reaction(HER)in acidic environments,the need for efficient,stable,and affordable materials persists.Recently,transition-metal borides(TMBs),particularly metal diborides(MDbs),have gained attention due to their unique layered crystal structures with multicentered boron bonds,offering remarkable physicochemical properties.Their nearly 2D structures boost electrochemical performance by offering high conductivity and a large active surface area,making them well-suited for advanced energy storage and conversion technologies.This review provides a comprehensive overview of the critical factors for water splitting,the crystal and electronic structures of MDbs,and their synthetic strategies.Furthermore,it examines the relationship between catalytic performance and intermediate adsorption as elucidated by first-principle calculations.The review also highlights the latest experimental advancements in MDb-based electrocatalysts and addresses the current challenges and future directions for their development.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
The development of bifunctional electrocatalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)at high current density under industrial temperatures is crucial for large-scale industrial hydrog...The development of bifunctional electrocatalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)at high current density under industrial temperatures is crucial for large-scale industrial hydrogen production from water splitting.In this work,M-MnO_(2)@TNTA composite electrodes were prepared by depositing various metal ion-doped manganese oxide nanoparticles on the titania nanotube array(TNTA)by successive ionic layer adsorption reaction(SILAR)method,and their HER and OER electrocatalytic performances were investigated in 1 M KOH.Results show that the CoFe-MnO_(2)@TNTA composite electrode prepared by simultaneous doping of Co^(3+)and Fe^(3+)in MnO_(2) exhibits optimal catalytic performance.Compared with MnO_(2)@TNTA without ion doping,the overpotentials of CoFe-MnO_(2)@TNTA at 10 mA cm^(-2)(η_(10))for HER and OER are reduced by 571 and 665 mV.In addition,the electrode perfor-mance can be significantly enhanced by increasing the test temperature,and the porous array structure enables CoFe-MnO_(2)@TNTA to exhibit better performance at high current densities.At 50℃,which is the common industrial electrolytic water temperature,the η_(10) of CoFe-MnO_(2)@TNTA for HER is almost equal to that of the Pt/C electrode.The η_(100) of CoFe-MnO_(2)@TNTA for HER is reduced by 35 mV compared with the Pt/C electrode.Moreover,η_(200) of CoFe-MnO_(2)@TNTA for OER is significantly lowered by 111 and 184 mV compared with IrO_(2) and RuO_(2) electrodes.Utilizing CoFe-MnO_(2)@TNTA as both the cathode and anode for overall water splitting,the electrolysis voltage is merely 2.33 V under the current density of 200 mA cm^(-2),much lower than that of IrO_(2)(+)||Pt/C(-)(2.68 V).The present work may provide a valuable reference for the development of self-supporting bifunctional electrodes suitable for high-current-density water splitting at industrial temperatures.展开更多
Designing the coordination environment of heteroatoms around metal sites and optimizing the electronic structure of diatomic metal sites remain significant challenges in achieving efficient CO_(2)overall splitting.Her...Designing the coordination environment of heteroatoms around metal sites and optimizing the electronic structure of diatomic metal sites remain significant challenges in achieving efficient CO_(2)overall splitting.Herein,we report four configurations(Cu/Ni-N_(4)C_(2),Cu/Ni-N_(2)C_(4),Cu/Ni-N_(2)C_(3)and Cu/Ni-N_(2)C_(2))constructed by precise regulation of the coordination environment around bimetallic atoms.Cu/Ni-N_(2)C_(2)showed high performance in electrochemical CO_(2)reduction(ECR)and water oxidation evolution reaction(OER).In the electrochemical CO_(2)overall splitting reaction,it achieved a Faraday efficiency of CO(FECO)of98.0%at a low cell voltage of-2.9 V,significantly higher than widely reported values.Moreover,the FE_(CO)is above 90%over-2.7 to-4.1 V of cell voltages.Cu/Ni-N_(2)C_(2)achieved long-term ECR stability of 110 h at-100 mA cm^(-2).Mechanism studies revealed that the change of coordination environment around the diatomic pairs moves the d-band center of the Ni atom closer to the Fermi level,thereby modulating the adsorption capacity of the catalysts to the reaction intermediates^(*)COOH and^(*)O.This work presents valuable insights into the rational design of diatomic catalysts and elucidates the intricate structureperformance relationship in advancing electrochemical CO_(2)overall splitting technology and energyconversion applications.展开更多
Noble metal-loaded layered hydroxides exhibit high efficiency in electrocatalyzing water splitting.However,their widespread use as bifunctional electrocatalysts is hindered by low metal loading,inefficient yield,and c...Noble metal-loaded layered hydroxides exhibit high efficiency in electrocatalyzing water splitting.However,their widespread use as bifunctional electrocatalysts is hindered by low metal loading,inefficient yield,and complex synthesis processes.In this work,platinum atoms were anchored onto nickel-iron layered double hydroxide/carbon nanotube(LDH/CNT)hybrid electrocatalysts by using a straightforward milling technique with K_(2)Pt Cl_(6)·6H_(2)O as the Pt source.By adjusting the Pt-to-Fe ratio to 1/2 and 1/10,excellent electrocatalysts—Pt_(1/6)-Ni_(2/3)Fe_(1/3)-LDH/CNT and Pt_(1/30)-Ni_(2/3)Fe_(1/3)-LDH/CNT—were achieved with superior performance in hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),outperforming the corresponding commercial Pt/C(20 wt%)and Ru O_(2)electrocatalysts.The enhanced electrochemical performance is attributed to the modification of Pt's electronic structure,which exhibits electron-rich states for HER and electrondeficient states for OER,significantly boosting Pt's electrochemical activity.Furthermore,the simple milling technology for controlling Pt loading offers a promising approach for scaling up the production of electrocatalysts.展开更多
Photocatalytic H_(2)production from water splitting is a promising candidate for solving the increasing energy crisis and environmental issues.Herein we report a novel g-C_(3)N_(4)/Ag In_(x)S_(y)S-scheme heterojunctio...Photocatalytic H_(2)production from water splitting is a promising candidate for solving the increasing energy crisis and environmental issues.Herein we report a novel g-C_(3)N_(4)/Ag In_(x)S_(y)S-scheme heterojunction photocatalyst for water splitting into stoichiometric H_(2)and H_(2)O_(2)under visible light.The catalyst was prepared by depositing 3D bimetallic sulfide(Ag In_(x)S_(y))nanotubes onto 2D g-C_(3)N_(4)nanosheets.Owing to the special 3D-on-2D configuration,the photogenerated carriers could be rapidly transferred and effectively separated through the abundant interfacial heterostructures to avoid recombination,and therefore excellent performance for visible light-driven water splitting could be obtained,with a 24-h H_(2)evolution rate up to 237μmol g^(-1)h^(-1).Furthermore,suitable band alignment enables simultaneous H_(2)and H_(2)O_(2)production in a 1:1 stoichiometric ratio.H_(2)and H_(2)O_(2)were evolved on the conduction band of g-C_(3)N_(4)and on the valance band of Ag In_(x)S_(y),respectively.The novel 3D-on-2D configuration for heterojunction construction proposed in this work provided alternative research ideas toward photocatalytic reaction.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 stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-...The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.展开更多
Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the ...Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the world’s shortage of fossil energy.However,efficient seawater splitting is hindered by slow kinetics caused by the ultra-low conductivity and the presence of bacteria,microorganisms,and stray ions in seawater.Additionally,producing hydrogen on an industrial scale is challenging due to the high production cost.The present review addresses these challenges from the catalyst point of view,namely,that designing catalysts with high catalytic activity and stability can directly affect the rate and effect of seawater splitting.From the ion transfer perspective,designing membranes can block harmful ions,improving the stability of seawater splitting.From the energy point of view,mixed seawater systems and self-powered systems also provide new and low-energy research systems for seawater splitting.Finally,ideas and directions for further research on direct seawater splitting in the future are pointed out,with the aim of achieving low-cost and high-efficiency hydrogen production.展开更多
The development of stable and efficient non-noble metal cocatalysts has arisen as a promising yet challenging endeavor in the context of photocatalytic overall water splitting.In this study,NiCo alloy cocatalysts were...The development of stable and efficient non-noble metal cocatalysts has arisen as a promising yet challenging endeavor in the context of photocatalytic overall water splitting.In this study,NiCo alloy cocatalysts were synthesized with nickel/cobalt metal organic framework(NiCo-MOF)as source of nickel and cobalt.Systematic characterization results demonstrate the successful deposition of alloy cocatalysts onto the surface of SrTiO_(3).The prepared SrTiO_(3)loaded NiCo-alloy can generate hydrogen and oxygen in a stoichiometric ratio for photocatalytic overall water splitting,achieving an apparent quantum yield of 11.9%at 350±10 nm.Theoretical calculations indicate that the introduction of cobalt has a beneficial regulatory effect on the hydrogen evolution sites of Ni,reducing the free energy of H adsorption.The synergistic catalytic effect of bimetallic catalysts contributes to enhancing photocatalytic activity and stability.This study offers constructive insights for the development of high-efficiency and cost-effective cocatalyst systems.展开更多
The reasonable design of material morphology and eco-friendly electrocatalysts are essential to highly efficient water splitting.It is proposed that a promising strategy effectively regulates the electronic structure ...The reasonable design of material morphology and eco-friendly electrocatalysts are essential to highly efficient water splitting.It is proposed that a promising strategy effectively regulates the electronic structure of the d-orbitals of CoP using cerium doping in this paper,thus significantly improving the intrinsic property and conductivity of CoP for water splitting.As a result,the as-synthesize porous Ce-doped CoP micro-polyhedron composite derived from Ce-ZIF-67 as bifunctional electrocatalytic materials exhibits excellent electrocatalytic performance in both the oxygen evolution reaction(OER)and the hydrogen evolution reaction(HER),overpotentials of about 152 mV for HER at 10 mA cm^(-2)and about 352 mV for OER at 50 mA cm^(-2),and especially it shows outstanding long-term stability.Besides,an alkaline electrolyzer,using Ce0.04Co0.96P electrocatalyst as both the anode and cathode,delivers a cell voltage value of1.55 V at the current density of 10 mA cm^(-2).The calculation results of the density functional theory(DFT)demonstrate that the introduction of an appropriate amount of Ce into CoP can enhance the conductivity,and can induce the electronic modulation to regulate the selective adsorption of reaction intermediates on catalytic surface and the formation of O*intermediates(CoOOH),which exhibits an excellent electrocatalytic performance.This study provides novel insights into the design of an extraordinary performance water-splitting of the multicomponent electrocatalysts.展开更多
Green hydrogen is crucial for advancing renewable energy technologies and protecting the environment.This study introduces a controllable method for bimetallic nickel-cobalt phosphide on reduced graphene oxide on nick...Green hydrogen is crucial for advancing renewable energy technologies and protecting the environment.This study introduces a controllable method for bimetallic nickel-cobalt phosphide on reduced graphene oxide on nickel foam(NiCo_(3)P.C/NF).The material demonstrated low overpotentials of 58 and 180 mV at10 mA cm^(-2)for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in 1.0 M KOH.It achieved excellent electrochemical water-splitting performance with operating voltages of 1.54 and 2.6 V at 10 and 500 mA cm^(-2),respectively.The overall water-splitting performance of NiCo_(3).C/NF was extremely stable after 75 h of operation at 53 mA cm^(-2),retaining 98%efficiency,better than the sample Pt-C+RuO_(2),and outperforming previous reports.Density functional theory(DFT)results revealed a synergistic NiCo_(3)P.C interaction that yields nearly zero Gibbs free energy change(-0.100 eV)and upshift d-band center,the real active site at the Ni in HER,and the lowest overpotentials 0.26 V at the P active sites for OER.Furthermore,electronic charge distribution shows the maximum charge distribution between the NiCo_(3)P phase and graphene sheet heterojunction,enhancing the electrocatalyst conductivity.This combined approach offers an innovative strategy to design sustainable electrocatalysts for water s plitting.展开更多
The quest for sustainable energy solutions has intensified the need for efficient water electrolysis techniques,pivotal for hydrogen production.However,developing effective bifunctional electrocatalysts capable of dri...The quest for sustainable energy solutions has intensified the need for efficient water electrolysis techniques,pivotal for hydrogen production.However,developing effective bifunctional electrocatalysts capable of driving the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)remains a formidable challenge.Addressing this,we introduce a novel built-in electric field(BEF)strategy to synthesize NiCoP–Co nanoarrays directly on Ti_(3)C_(2)T_(x) MXene substrates(NiCoP–Co/MXene).This approach leverages a significant work function difference(ΔΦ),propelling these nanoarrays as adept bifunctional electrocatalysts for comprehensive water splitting.MXene,in this process,plays a dual role.It acts as a conductive support,enhancing the catalyst’s overall conductivity,and facilitates an effective charge transport pathway,ensuring efficient charge transfer.Our study reveals that the BEF induces an electric field at the interface,prompting charge transfer from Co to NiCoP.This transfer modulates asymmetric charge distributions,which intricately control intermediates’adsorption and desorption dynamics.Such regulation is crucial for enhancing the reaction kinetics of both HER and OER.Furthermore,under oxidative conditions,the NiCoP–Co/MXene catalyst undergoes a structural metamorphosis into Ni(Co)oxides/hydroxides/MXene,increasing OER performance.This research demonstrates the BEF’s role in fine-tuning interfacial charge redistribution and underscores its potential in crafting more sophisticated electrocatalytic designs.The insights gained here could pave the way for the next generation of electrocatalysis,with far-reaching implications for energy conversion and storage technologies.展开更多
Exploring the intrinsic reasons for the dynamic reconstruction of catalysts during electrocatalytic reactions and their impact on activity enhancement still face severe challenges. Herein, the bifunctional catalyst Ru...Exploring the intrinsic reasons for the dynamic reconstruction of catalysts during electrocatalytic reactions and their impact on activity enhancement still face severe challenges. Herein, the bifunctional catalyst Ru/V-Co O/CP with doping strategy and heterostructure was synthesized for overall water splitting.The Ru/V-Co O exhibits excellent activity for HER and OER with low overpotentials of 49, 147 m V at a current density of 10 m A/cm^(2) in 1.0 mol/L KOH, respectively. The assembled electrolytic cell just needs voltages of 1.47 and 1.71 V to achieve 10 and 350 m A/cm^(2)current density under the same conditions and delivers an outstanding stability for over 100 h, which is far superior to the commercial Ru O_(2)||Pt/C cell. Experimental and theoretical results indicate that the doping of V species and the formation of heterostructures lead to charge redistribution. More importantly, the leaching of V species induces electron transfer form Co to O and then Ru through the Co-O-Ru electron bridge, optimizes the adsorption strength of the key intermediate, thereby reducing the free energy barrier of the rate-determining step and improving catalytic activity. This work proposes an effective strategy of using cation dissolution to induce electron transfer through the electron bridge and thus regulate the electronic structure of catalysts,providing new ideas for the design and development of efficient and stable electrocatalysts.展开更多
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.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.
文摘Water oxidation-a critical yet sluggish step in green hydrogen production-is a major bottleneck for electrolysis efficiency.Traditional catalysts often degrade quickly under the high current densities needed for industrial scale.
文摘Harnessing solar energy for renewable fuel production through artificial photosynthesis offers an ideal solution to the current energy and environmental crises.Among various methods,photoelectrochemical(PEC)water splitting stands out as a promising approach for direct solar-driven hydrogen production.Enhancing the efficiency and stability of photoelectrodes is a key focus in PEC water-splitting research.Tantalum nitride(Ta_(3)N_(5)),with its suitable band gap and band-edge positions for PEC water splitting,has emerged as a highly promising photoanode material.This review begins by introducing the history and fundamental characteristics of Ta_(3)N_(5),emphasizing both its advantages and challenges.It then explores methods to improve light absorption efficiency,charge separation and transfer efficiency,surface reaction rate,and the stability of Ta_(3)N_(5) photoanodes.Additionally,the review discusses the progress of research on tandem PEC cells incorporating Ta_(3)N_(5) photoanodes.Finally,it looks ahead to future research directions for Ta_(3)N_(5) photoanodes.The strategic approach outlined in this review can also be applied to other photoelectrode materials,providing guidance for their development.
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financial support from the Scientific and Technological Research Council of Türkiye(223M182).
文摘Electrocatalytic water splitting(EWS)driven by renewable energy is vital for clean hydrogen(H2)production and reducing reliance on fossil fuels.While IrO_(2) and RuO_(2) are the leading electrocatalysts for the oxygen evolution reaction(OER)and Pt for the hydrogen evolution reaction(HER)in acidic environments,the need for efficient,stable,and affordable materials persists.Recently,transition-metal borides(TMBs),particularly metal diborides(MDbs),have gained attention due to their unique layered crystal structures with multicentered boron bonds,offering remarkable physicochemical properties.Their nearly 2D structures boost electrochemical performance by offering high conductivity and a large active surface area,making them well-suited for advanced energy storage and conversion technologies.This review provides a comprehensive overview of the critical factors for water splitting,the crystal and electronic structures of MDbs,and their synthetic strategies.Furthermore,it examines the relationship between catalytic performance and intermediate adsorption as elucidated by first-principle calculations.The review also highlights the latest experimental advancements in MDb-based electrocatalysts and addresses the current challenges and future directions for their development.
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financially supported by the National Natural Science Foundation of China(No.51972095).
文摘The development of bifunctional electrocatalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)at high current density under industrial temperatures is crucial for large-scale industrial hydrogen production from water splitting.In this work,M-MnO_(2)@TNTA composite electrodes were prepared by depositing various metal ion-doped manganese oxide nanoparticles on the titania nanotube array(TNTA)by successive ionic layer adsorption reaction(SILAR)method,and their HER and OER electrocatalytic performances were investigated in 1 M KOH.Results show that the CoFe-MnO_(2)@TNTA composite electrode prepared by simultaneous doping of Co^(3+)and Fe^(3+)in MnO_(2) exhibits optimal catalytic performance.Compared with MnO_(2)@TNTA without ion doping,the overpotentials of CoFe-MnO_(2)@TNTA at 10 mA cm^(-2)(η_(10))for HER and OER are reduced by 571 and 665 mV.In addition,the electrode perfor-mance can be significantly enhanced by increasing the test temperature,and the porous array structure enables CoFe-MnO_(2)@TNTA to exhibit better performance at high current densities.At 50℃,which is the common industrial electrolytic water temperature,the η_(10) of CoFe-MnO_(2)@TNTA for HER is almost equal to that of the Pt/C electrode.The η_(100) of CoFe-MnO_(2)@TNTA for HER is reduced by 35 mV compared with the Pt/C electrode.Moreover,η_(200) of CoFe-MnO_(2)@TNTA for OER is significantly lowered by 111 and 184 mV compared with IrO_(2) and RuO_(2) electrodes.Utilizing CoFe-MnO_(2)@TNTA as both the cathode and anode for overall water splitting,the electrolysis voltage is merely 2.33 V under the current density of 200 mA cm^(-2),much lower than that of IrO_(2)(+)||Pt/C(-)(2.68 V).The present work may provide a valuable reference for the development of self-supporting bifunctional electrodes suitable for high-current-density water splitting at industrial temperatures.
基金supported by Shanxi Provincial Key Research and Development Project(No.20201102002)。
文摘Designing the coordination environment of heteroatoms around metal sites and optimizing the electronic structure of diatomic metal sites remain significant challenges in achieving efficient CO_(2)overall splitting.Herein,we report four configurations(Cu/Ni-N_(4)C_(2),Cu/Ni-N_(2)C_(4),Cu/Ni-N_(2)C_(3)and Cu/Ni-N_(2)C_(2))constructed by precise regulation of the coordination environment around bimetallic atoms.Cu/Ni-N_(2)C_(2)showed high performance in electrochemical CO_(2)reduction(ECR)and water oxidation evolution reaction(OER).In the electrochemical CO_(2)overall splitting reaction,it achieved a Faraday efficiency of CO(FECO)of98.0%at a low cell voltage of-2.9 V,significantly higher than widely reported values.Moreover,the FE_(CO)is above 90%over-2.7 to-4.1 V of cell voltages.Cu/Ni-N_(2)C_(2)achieved long-term ECR stability of 110 h at-100 mA cm^(-2).Mechanism studies revealed that the change of coordination environment around the diatomic pairs moves the d-band center of the Ni atom closer to the Fermi level,thereby modulating the adsorption capacity of the catalysts to the reaction intermediates^(*)COOH and^(*)O.This work presents valuable insights into the rational design of diatomic catalysts and elucidates the intricate structureperformance relationship in advancing electrochemical CO_(2)overall splitting technology and energyconversion applications.
基金supported by the Natural Science Foundation of Henan(242300421230)the Young Teacher Fundamental Research Cultivation Program of Zhengzhou University(JC23557030)the National Natural Science Foundation of China(U21A20281 and 22208322)。
文摘Noble metal-loaded layered hydroxides exhibit high efficiency in electrocatalyzing water splitting.However,their widespread use as bifunctional electrocatalysts is hindered by low metal loading,inefficient yield,and complex synthesis processes.In this work,platinum atoms were anchored onto nickel-iron layered double hydroxide/carbon nanotube(LDH/CNT)hybrid electrocatalysts by using a straightforward milling technique with K_(2)Pt Cl_(6)·6H_(2)O as the Pt source.By adjusting the Pt-to-Fe ratio to 1/2 and 1/10,excellent electrocatalysts—Pt_(1/6)-Ni_(2/3)Fe_(1/3)-LDH/CNT and Pt_(1/30)-Ni_(2/3)Fe_(1/3)-LDH/CNT—were achieved with superior performance in hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),outperforming the corresponding commercial Pt/C(20 wt%)and Ru O_(2)electrocatalysts.The enhanced electrochemical performance is attributed to the modification of Pt's electronic structure,which exhibits electron-rich states for HER and electrondeficient states for OER,significantly boosting Pt's electrochemical activity.Furthermore,the simple milling technology for controlling Pt loading offers a promising approach for scaling up the production of electrocatalysts.
基金financially supported by the National Natural Science Foundation of China(Nos.52362012,42077162,51978323)Natural Science Foundation of Jiangxi Province(No.2022ACB203014)+4 种基金Major Discipline Academic and Technical Leaders Training Program of Jiangxi Province(Nos.20213BCJ22018,20232BCJ22048)Natural Science Project of the Educational Department in Jiangxi Province(No.GJJ2201121)Natural Science Foundation of Nanchang Hangkong University(No.EA202202256)Educational Reform Project of Jiangxi Province(No.JXYJG-2022-135)Nanchang Hangkong University Educational Reform Project(Nos.sz2214,sz2213,JY22017,KCPY1806)。
文摘Photocatalytic H_(2)production from water splitting is a promising candidate for solving the increasing energy crisis and environmental issues.Herein we report a novel g-C_(3)N_(4)/Ag In_(x)S_(y)S-scheme heterojunction photocatalyst for water splitting into stoichiometric H_(2)and H_(2)O_(2)under visible light.The catalyst was prepared by depositing 3D bimetallic sulfide(Ag In_(x)S_(y))nanotubes onto 2D g-C_(3)N_(4)nanosheets.Owing to the special 3D-on-2D configuration,the photogenerated carriers could be rapidly transferred and effectively separated through the abundant interfacial heterostructures to avoid recombination,and therefore excellent performance for visible light-driven water splitting could be obtained,with a 24-h H_(2)evolution rate up to 237μmol g^(-1)h^(-1).Furthermore,suitable band alignment enables simultaneous H_(2)and H_(2)O_(2)production in a 1:1 stoichiometric ratio.H_(2)and H_(2)O_(2)were evolved on the conduction band of g-C_(3)N_(4)and on the valance band of Ag In_(x)S_(y),respectively.The novel 3D-on-2D configuration for heterojunction construction proposed in this work provided alternative research ideas toward photocatalytic reaction.
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sponsored by the National Natural Science Foundation of China(Nos.5210125 and 52375422)the Science Research Project of Hebei Education Department(No.BJK2023058)the Natural Science Foundation of Hebei Province(Nos.E2020208069,B2020208083 and E202320801).
文摘The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.
基金support by National Key Research and Development Program of China(2022YFB3803502)National Natural Science Foundation of China(52103076)+5 种基金Science and Technology Commission of Shanghai Municipality(23ZR1400300)special fund of Beijing Key Laboratory of Indoor Air Quality Evaluat ion and Control(NO.BZ0344KF21-02)State Key Laboratory of Electrical Insulation and Power Equipment(EIPE22203)JLF is a member of LSRE-LCM–Laboratory of Separation and Reaction Engineering-Laboratory of Catalysis and Materials,supported by national funds through FCT/MCTES(PIDDAC):LSRE-LCM,UIDB/50020/2020(DOI:10.54499/UIDB/50020/2020)UIDP/50020/2020(DOI:10.54499/UIDP/50020/2020)ALiCE,LA/P/0045/2020(DOI:10.54499/LA/P/0045/2020).
文摘Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the world’s shortage of fossil energy.However,efficient seawater splitting is hindered by slow kinetics caused by the ultra-low conductivity and the presence of bacteria,microorganisms,and stray ions in seawater.Additionally,producing hydrogen on an industrial scale is challenging due to the high production cost.The present review addresses these challenges from the catalyst point of view,namely,that designing catalysts with high catalytic activity and stability can directly affect the rate and effect of seawater splitting.From the ion transfer perspective,designing membranes can block harmful ions,improving the stability of seawater splitting.From the energy point of view,mixed seawater systems and self-powered systems also provide new and low-energy research systems for seawater splitting.Finally,ideas and directions for further research on direct seawater splitting in the future are pointed out,with the aim of achieving low-cost and high-efficiency hydrogen production.
基金supported by the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China(No.52488201)the National Natural Science Foundation of China(No.52376209)+1 种基金the China Postdoctoral Science Foundation(Nos.2020T130503 and 2020M673386)China Fundamental Research Funds for the Central Universities.
文摘The development of stable and efficient non-noble metal cocatalysts has arisen as a promising yet challenging endeavor in the context of photocatalytic overall water splitting.In this study,NiCo alloy cocatalysts were synthesized with nickel/cobalt metal organic framework(NiCo-MOF)as source of nickel and cobalt.Systematic characterization results demonstrate the successful deposition of alloy cocatalysts onto the surface of SrTiO_(3).The prepared SrTiO_(3)loaded NiCo-alloy can generate hydrogen and oxygen in a stoichiometric ratio for photocatalytic overall water splitting,achieving an apparent quantum yield of 11.9%at 350±10 nm.Theoretical calculations indicate that the introduction of cobalt has a beneficial regulatory effect on the hydrogen evolution sites of Ni,reducing the free energy of H adsorption.The synergistic catalytic effect of bimetallic catalysts contributes to enhancing photocatalytic activity and stability.This study offers constructive insights for the development of high-efficiency and cost-effective cocatalyst systems.
基金supported by the National Natural Science Foundation of China(No.12162023&52268042)Key R&D Program of Gansu Province-International Cooperation Project(No.20YF8WA064)Natural Science Foundation of Gansu Province(No.22JR5RA253).
文摘The reasonable design of material morphology and eco-friendly electrocatalysts are essential to highly efficient water splitting.It is proposed that a promising strategy effectively regulates the electronic structure of the d-orbitals of CoP using cerium doping in this paper,thus significantly improving the intrinsic property and conductivity of CoP for water splitting.As a result,the as-synthesize porous Ce-doped CoP micro-polyhedron composite derived from Ce-ZIF-67 as bifunctional electrocatalytic materials exhibits excellent electrocatalytic performance in both the oxygen evolution reaction(OER)and the hydrogen evolution reaction(HER),overpotentials of about 152 mV for HER at 10 mA cm^(-2)and about 352 mV for OER at 50 mA cm^(-2),and especially it shows outstanding long-term stability.Besides,an alkaline electrolyzer,using Ce0.04Co0.96P electrocatalyst as both the anode and cathode,delivers a cell voltage value of1.55 V at the current density of 10 mA cm^(-2).The calculation results of the density functional theory(DFT)demonstrate that the introduction of an appropriate amount of Ce into CoP can enhance the conductivity,and can induce the electronic modulation to regulate the selective adsorption of reaction intermediates on catalytic surface and the formation of O*intermediates(CoOOH),which exhibits an excellent electrocatalytic performance.This study provides novel insights into the design of an extraordinary performance water-splitting of the multicomponent electrocatalysts.
基金supported by the Regional Leading Research Center Program(2019R1A5A8080326)funding from the Basic Science Research Program(2021R1F1A1048758,2022R1I1A1A01053248)+1 种基金the Regional Innovation Strategy(RIS)(2023RIS-008)through the National Research Foundation of Korea(NRF),funded by the Ministry of Educationsupported by the National Supercomputing Center,which provided supercomputing resources and technical support(TS-2024-RE-0039)。
文摘Green hydrogen is crucial for advancing renewable energy technologies and protecting the environment.This study introduces a controllable method for bimetallic nickel-cobalt phosphide on reduced graphene oxide on nickel foam(NiCo_(3)P.C/NF).The material demonstrated low overpotentials of 58 and 180 mV at10 mA cm^(-2)for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in 1.0 M KOH.It achieved excellent electrochemical water-splitting performance with operating voltages of 1.54 and 2.6 V at 10 and 500 mA cm^(-2),respectively.The overall water-splitting performance of NiCo_(3).C/NF was extremely stable after 75 h of operation at 53 mA cm^(-2),retaining 98%efficiency,better than the sample Pt-C+RuO_(2),and outperforming previous reports.Density functional theory(DFT)results revealed a synergistic NiCo_(3)P.C interaction that yields nearly zero Gibbs free energy change(-0.100 eV)and upshift d-band center,the real active site at the Ni in HER,and the lowest overpotentials 0.26 V at the P active sites for OER.Furthermore,electronic charge distribution shows the maximum charge distribution between the NiCo_(3)P phase and graphene sheet heterojunction,enhancing the electrocatalyst conductivity.This combined approach offers an innovative strategy to design sustainable electrocatalysts for water s plitting.
基金supported by Guangdong Basic and Applied Basic Research Foundation(Nos.2021A1515010261 and 2023A1515140153)Guangdong Special Innovative Projects of General Universities(No.2022KTSCX136)+1 种基金the Major and Special Project in the Field of Intelligent Manufacturing of the Universities in Guangdong Province(No.2020ZDZX2067)the Innovative Team Project of the Universities in Guangdong Province(No.2023KCXTD035).
文摘The quest for sustainable energy solutions has intensified the need for efficient water electrolysis techniques,pivotal for hydrogen production.However,developing effective bifunctional electrocatalysts capable of driving the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)remains a formidable challenge.Addressing this,we introduce a novel built-in electric field(BEF)strategy to synthesize NiCoP–Co nanoarrays directly on Ti_(3)C_(2)T_(x) MXene substrates(NiCoP–Co/MXene).This approach leverages a significant work function difference(ΔΦ),propelling these nanoarrays as adept bifunctional electrocatalysts for comprehensive water splitting.MXene,in this process,plays a dual role.It acts as a conductive support,enhancing the catalyst’s overall conductivity,and facilitates an effective charge transport pathway,ensuring efficient charge transfer.Our study reveals that the BEF induces an electric field at the interface,prompting charge transfer from Co to NiCoP.This transfer modulates asymmetric charge distributions,which intricately control intermediates’adsorption and desorption dynamics.Such regulation is crucial for enhancing the reaction kinetics of both HER and OER.Furthermore,under oxidative conditions,the NiCoP–Co/MXene catalyst undergoes a structural metamorphosis into Ni(Co)oxides/hydroxides/MXene,increasing OER performance.This research demonstrates the BEF’s role in fine-tuning interfacial charge redistribution and underscores its potential in crafting more sophisticated electrocatalytic designs.The insights gained here could pave the way for the next generation of electrocatalysis,with far-reaching implications for energy conversion and storage technologies.
基金supported by National Natural Science Foundation of China (No. 22006120)the Fundamental Research Funds for the Central Universities (No. SWU-XDJH202314)+1 种基金the Program for Innovation Team Building at Institutions of Higher Education in Chongqing (No. CXTDX201601011)Chongqing Municipal Natural Science Foundation (No. cstc2018jcyj AX0625)。
文摘Exploring the intrinsic reasons for the dynamic reconstruction of catalysts during electrocatalytic reactions and their impact on activity enhancement still face severe challenges. Herein, the bifunctional catalyst Ru/V-Co O/CP with doping strategy and heterostructure was synthesized for overall water splitting.The Ru/V-Co O exhibits excellent activity for HER and OER with low overpotentials of 49, 147 m V at a current density of 10 m A/cm^(2) in 1.0 mol/L KOH, respectively. The assembled electrolytic cell just needs voltages of 1.47 and 1.71 V to achieve 10 and 350 m A/cm^(2)current density under the same conditions and delivers an outstanding stability for over 100 h, which is far superior to the commercial Ru O_(2)||Pt/C cell. Experimental and theoretical results indicate that the doping of V species and the formation of heterostructures lead to charge redistribution. More importantly, the leaching of V species induces electron transfer form Co to O and then Ru through the Co-O-Ru electron bridge, optimizes the adsorption strength of the key intermediate, thereby reducing the free energy barrier of the rate-determining step and improving catalytic activity. This work proposes an effective strategy of using cation dissolution to induce electron transfer through the electron bridge and thus regulate the electronic structure of catalysts,providing new ideas for the design and development of efficient and stable electrocatalysts.
