Terahertz imaging has become increasingly important across various fields and practical production applications.Achieving both high sensitivity and high speed remains a primary challenge for most current THz imaging t...Terahertz imaging has become increasingly important across various fields and practical production applications.Achieving both high sensitivity and high speed remains a primary challenge for most current THz imaging technologies.In this work,we present an imaging system based on Rydberg atomic vapor operating at frequencies exceeding 1 THz.By utilizing Cesium133 atoms coupled with THz waves,de-excitation radiation generated after atomic excitation to Rydberg states converts invisible THz waves into visible light,enabling the acquisition of spatial information and intensity distributions of THz fields.The system achieves a minimum detectable power of 330 fW∕s1∕2per(2.4×2.4)μm2,an imaging resolution of approximately 1.7 mm,and an imaging bandwidth of 8.6 MHz.Additionally,the theoretical imaging rate can exceed 1 MHz.The Rydberg-atom-based THz imaging system exhibits a simple structure and is amenable to miniaturization.This THz imaging method holds promise for advancing applications in THz nondestructive testing,biomedical imaging,and concealed object detection.展开更多
Asymmetric spin-orbit interaction(ASOI)has been widely employed in multifunctional applications through breaking the conjugate symmetry constraints of geometric phase metasurfaces.However,its implementation commonly s...Asymmetric spin-orbit interaction(ASOI)has been widely employed in multifunctional applications through breaking the conjugate symmetry constraints of geometric phase metasurfaces.However,its implementation commonly suffers from lower robustness and complex design due to the requirement of subwavelength structures with different dimensions.Here,we demonstrate that two independent phase profiles can be generated only by designing the rotation angles of two C3 catenary meta-atoms in one unit based on the generalized Pancharatnam-Berry(PB)phase and interaction between meta-atoms,realizing ASOI.As a proof of concept,a spin-decoupled metadevice is fabricated and characterized,whose measured efficiencies approach 61.9%/52.8%for left-ight-handed circular polarization light incidence at 10.6μm.This work may provide a methodology for multifunctional light field modulation,holography multiplexing,and linear and nonlinear optical responses manipulation.展开更多
Topological vacua,a family of degenerate ground states of the Yang–Mills fields with zero field strength but nontrivial topological structures,play a fundamental role in particle physics and quantum field theory.Howe...Topological vacua,a family of degenerate ground states of the Yang–Mills fields with zero field strength but nontrivial topological structures,play a fundamental role in particle physics and quantum field theory.However,they have not yet been experimentally observed.Here,we propose an experimental scheme to realize a real-space SU(2)artificial Yang–Mills topological vacua using a cloud of two-Λ-level cold atoms.展开更多
We developed a model of a quantum Otto engine using two coupled two-level atoms.Based on the platform,we show that frequency detuning and the coupling strength induced by dipole-dipole interactions can lead to decoher...We developed a model of a quantum Otto engine using two coupled two-level atoms.Based on the platform,we show that frequency detuning and the coupling strength induced by dipole-dipole interactions can lead to decoherence by disrupting coherent energy exchange.We focus on fundamental thermodynamic quantities,including heat absorption,release to heat baths,work done and efficiency.It is noteworthy that the interatomic coupling strength and frequency detuning do not merely affect the shape of the work and the efficiency but ultimately govern its quantitative magnitude.In the field of quantum thermodynamics,we have established an upper bound efficiency that is stricter than the Carnot limit.Moreover,our analysis confirms that quantum coherence enables the system to exceed the efficiency threshold of a classical Otto heat engine.The second law of thermodynamics holds all the while.Our results constitute a step forward in the design of conceptually new quantum thermodynamic devices which take advantage of uniquely quantum resources of quantum coherence.展开更多
Hydrofuroin(HDF),a key precursor of fuel,can be produced by electrocatalytic furfural(FF)hydrodimerization,offering a promising way to generate value-added products.However,this process is hindered by sluggish C-C cou...Hydrofuroin(HDF),a key precursor of fuel,can be produced by electrocatalytic furfural(FF)hydrodimerization,offering a promising way to generate value-added products.However,this process is hindered by sluggish C-C coupling and hydrogenation steps,resulting in low Faradaic efficiency(FE).Herein,atomically dispersed Ru sites anchored on lattice vacancies of La0.9NiO3(Ru-La0.9NiO3)electrocatalysts were demonstrated as an efficient electrocatalyst for FF hydrodimerization,where an intermediate spillover strategy significantly enhances the FE.Mechanistic investigations reveal that Ru single atoms serve as active sites for the initial hydrogenation to form the FF-CHOH*intermediate with almost 100%selectivity,thereby suppressing the side reaction of hydrogen evolution.Subsequently,the increased FF-CHOH*intermediate undergoes spillover to adjacent Ni sites,decreasing the energy barrier for the subsequent C-C coupling step to HDF(ΔG=0.63 eV).As a result,the Ru-La0.9NiO3catalyst displays a high FE of 74%and a production rate of 3.95 mmol cm-2h-1toward electrocatalytic FF hydrodimerization to HDF product.This work provides an efficient intermediate spillover approach,offering mechanistic insights into Ru-Ni synergism in Ru-La0.9NiO3and providing a sensible method for electrocatalytic hydrodimerization of furfural to produce high-value products.展开更多
The integration of multiple active sites has been demonstrated to significantly enhance the electrocatalytic performance of the hydrogen evolution reaction(HER).However,the precise construction of synergistic SAs/NCs ...The integration of multiple active sites has been demonstrated to significantly enhance the electrocatalytic performance of the hydrogen evolution reaction(HER).However,the precise construction of synergistic SAs/NCs sites and a thorough understanding of their reaction mechanisms remain challenging.Herein,a straightforward synthetic strategy is developed for the fabrication of Ru SAs and NCs supported on nitrogen-doped carbon spheres derived from m-aminophenol/formaldehyde resin(denoted as Ru1-n@AFCS),achieved by tuning the ratio of resorcinol to m-aminophenol during phenolic resin polymerization.The optimized Ru1-n@AFCS HER performance in alkaline media,requiring an overpotential of only 11.2 mV to achieve 10 mA cm-2 and displaying a mass activity of 5158.2 A g-1,which is 60 times higher than that of commercial 20%Pt/C(85.4 A g-1)at-0.025 V vs.RHE.When integrated into an anion-exchange-membrane water electrolyzer,the catalyst achieves a current density of 1 A cm-2 at 1.80 V with a remarkable noble metal mass activity of 55.2 A mg-Ru-1.Combined experimental and theoretical calculations reveal that the nitrogen-doped carbon support modulates electronic structure of Ru NCs,while adjacent isolated Ru SAs facilitate hydrogen transfer via strong hydroxyl adsorption,collectively forming a“dual-engine”catalytic center that significantly enhances alkaline HER performance.展开更多
The incorporation of noble metals has been proven to be an effective strategy for enhancing the catalytic performance of Cu-based catalysts.Nevertheless,precise control of the structure of noble metals to achieve outs...The incorporation of noble metals has been proven to be an effective strategy for enhancing the catalytic performance of Cu-based catalysts.Nevertheless,precise control of the structure of noble metals to achieve outstanding selective hydrogenation activity remains challenging.In this study,two catalysts with well-defined Pd configurations,including atomically dispersed Pd species(CuPd0.01/SiO2)and Pd clusters(CuPd0.05/SiO2),were constructed for the selective hydrogenation of furfural.Even at extremely low Pd loading(0.01 wt%),the single-atom Pd-incorporated catalyst achieved furfural conversion of80.2%under mild conditions(90℃,1 MPa H2),exceeding both CuPd0.05/SiO2(76.3%)and monometallic Cu/SiO2(56.3%).Kinetic analysis indicated that the apparent activation energy decreased to 140.2 kJ/mol compared to the unmodified catalyst(255.2 kJ/mol).Density functional theory calculations revealed that isolated Pd atoms induced electron redistribution at the Pd-Cu interface,facilitated H2dissociation,and promoted C=O activation.In contrast,the formation of Pd clusters caused a negative effect,which reduced the local electron density of adjacent Cu sites and decreased the number of effective active sites.These results establish a clear structure-performance relationship between Pd configuration and selective hydrogenation activity,providing insights for the rational design of highly efficient Cu-based hydrogenation catalysts for biomass-derived chemicals under mild conditions.展开更多
The conversion of solar energy into hydrogen represents a promising and sustainable approach to addressing the global energy crisis and mitigating environmental pollution.However,achieving the industrial benchmark of ...The conversion of solar energy into hydrogen represents a promising and sustainable approach to addressing the global energy crisis and mitigating environmental pollution.However,achieving the industrial benchmark of solar-to-hydrogen efficiency remains challenging due to the inherently insufficient spatial separation of charge carriers and sluggish interfacial kinetics.Engineering redox-active sites has emerged as an effective approach to enhance photocatalytic hydrogen evolution performance.Herein,a dual-mode copper-modified titanium dioxide photocatalyst(Cu/TiO2),comprising isolated Cu atoms and CuO nanoclusters,was successfully synthesized via a facile molten salt method.The optimized Cu/TiO2exhibited a remarkable hydrogen evolution rate of 37.6 mmol g-1h-1with methanol as a sacrificial agent,representing a 96-fold enhancement compared to pristine TiO2.Mechanistic studies revealed that isolated Cu atoms incorporated into the TiO2lattice substantially lower the free energy of hydrogen adsorption(*H),thereby promoting the proton reduction half-reaction.Simultaneously,the surface-dispersed CuO nanoclusters were found to reduce the overpotential for methanol oxidation,thereby accelerating the oxidation half-reaction and facilitating overall charge balance during photocatalysis.Furthermore,photocatalytic hydrogen production coupled with the oxidation of various organic molecules was evaluated under a low sacrificial agent concentration(0.1%)over the Cu/TiO2photocatalyst,offering a more sustainable and practically relevant assessment of catalyst performance for green energy applications.展开更多
Traditional strong metal-support interactions(SMSIs)induced by encapsulated reducible oxide overlayers on metal nanoparticles can suppress sintering but has a strong negative impact on the catalytic activity because o...Traditional strong metal-support interactions(SMSIs)induced by encapsulated reducible oxide overlayers on metal nanoparticles can suppress sintering but has a strong negative impact on the catalytic activity because of decreased availability of active sites.Herein,we design three SMSIs configurations on Pt-TiO2via crystal-phase engineering.These configurations comprised encapsulated Pt nanoparticle(NPs)with TiO2-xoverlayer on anatase,weakly embedded Pt clusters on P25,and deeply embedded Pt Ox-induced Pt single-atom(SA)structure on rutile.These configurations exhibited Pt species at multiple scales,ranging from NPs to SAs.Among them,Pt supported rutile TiO2sample(Pt-TiO2(R)-H)achieved extremely low CO selectivity(2.05%,200℃)and optimal H2production performance due to the enhanced SMSIs from Pt-Ti coordination in the deeply embedded Pt Oxregion.This Pt-Ti coordination facilitated the electron transfer from Pt to Ti and induced dual-function centers of electron-deficient Ptδ+-Pt2+pairs(0<δ<2,where Ptδ+represent Pt SAs)for methanol decomposition and electron-rich Ti3+-oxygen vacancies for water dissociation.Such unique configuration altered the MSR reaction pathway and the kinetic rates of each elementary step in these reaction pathways were systematically analyzed.This work proposes an SMSIs configuration induced by a deeply embedded structure,which mitigates the negative impact on catalytic activity from encapsulated overlayers,meanwhile providing a strategy for developing high-loading Pt SAs catalysts.展开更多
Photocatalytic conversion of carbon dioxide(CO2)to methanol is hindered by inefficient charge separation and complex multielectron pathways.To address these challenges,we report a synergistic catalyst design in whi...Photocatalytic conversion of carbon dioxide(CO2)to methanol is hindered by inefficient charge separation and complex multielectron pathways.To address these challenges,we report a synergistic catalyst design in which cobalt vacancies(VCo)are coupled with indium single atoms(In SAs).VCo sites were precisely constructed on Co3O4nanosheets using a chlorine cold plasma technique,acting as“atomic sockets”that confine In SAs and form a robust In-O-VCo coordination structure.The resulting In/Co3−xO4catalyst delivered a high methanol production rate of 466.7μmol/(g·h)with 92.3%selectivity under simulated solar irradiation,which was eight times greater than that of the vacancy-free catalyst.Mechanistic studies revealed a synergistic functional division:the VCo sites efficiently adsorbed and dissociated H2O to supply protons,whereas the In SAs polarized CO2and stabilized the critical*COOH intermediate.This synergy of strong electronic metal-support interactions improved charge separation and steered the reaction pathway toward methanol,offering a novel atomic-level strategy for designing highly selective CO2photoreduction catalysts.展开更多
Hydrazine-assisted water electrolysis is a promising route for hydrogen production,and efficient bifunctional electrodes for the anodic hydrazine oxidation reaction(HzOR)and the cathodic hydrogen evolution reaction(HE...Hydrazine-assisted water electrolysis is a promising route for hydrogen production,and efficient bifunctional electrodes for the anodic hydrazine oxidation reaction(HzOR)and the cathodic hydrogen evolution reaction(HER)simplify the devices and enhance the technological advantage.However,suffering from the incompatible adsorption of different intermediates and the sluggish reaction kinetics,the design of effective and durable bi-functional electrodes still faces challenges.Herein,a Lewis acid(WOx)of powerful electron-accepting ability stabilized single-atom Ir catalyst(Ir-SA@WOx),intriguing strong metalsupport interaction(SMSI),is demonstrated to efficiently activate H2O and N2H4molecules.Ir-SA@WOxshows exceptional activity for both HER and HzOR(26.31 and 44.79 A mgIr-1at-100 mV),surpassing commercial Pt/C and Ir/C by factors of 41.8 and 27.6,respectively.A hydrazine-assisted water electrolyzer fabricated with Ir-SA@WOxachieves a current density of 100 mA cm-2at an ultra-low cell voltage of 0.313 V and electricity consumption of merely 0.75 kWh m-3H2,significantly lower than conventional water electrolysis systems(1.852 V,4.43 kWh m-3H2).In situ infrared absorption spectroscopy and theoretical calculations elucidate that the SMSI in Ir-SA@WOxreconstructs the electronic structure to facilitate the activation of the rigid water at the catalyst/electrolyte interface into free species,also optimizes H*adsorption and accelerates dehydrogenation kinetics of the potential-determining step of N2H3*-toN2H2*at Ir-sites,thereby realizing high activity for both HER and HzOR.This work illustrates the tailoring of electronic structures via the SMSI effect for catalytic-activity enhancement,guiding the design of advanced bi-functional catalysts for energy-efficient hydrogen production.展开更多
Mordenite(MOR)zeolites are key catalysts in dimethyl ether(DME)carbonylation,with their performance governed by the distribution of Brùnsted acid sites(BAS)associated with framework aluminum(Al).The 8-membered ri...Mordenite(MOR)zeolites are key catalysts in dimethyl ether(DME)carbonylation,with their performance governed by the distribution of Brùnsted acid sites(BAS)associated with framework aluminum(Al).The 8-membered ring(8-MR)channels host the desired active BAS,while BAS in the 12-membered ring(12-MR)channels promote coking,making precise Al siting critical.Traditional views posit Al siting is fixed post-crystallization,yet emerging evidence reveals dynamic Al relocation during the ripening stage of the crystallization.Despite this potential,mechanisms governing Al migration in MOR remain unclear,with most studies focusing on post-synthetic modifications that risk structural integrity.This study investigates the crystallization dynamics of MOR,using in situ solid-state nuclear magnetic resonance(NMR)to probe the real-time chemical environment of Al and employing advanced characterization techniques to track framework Al migration.During the ripening stage of crystallization,framework Al atoms migrate directionally from T1,T2,and T3 to the T4 site,which influences the catalytic performance of mordenite.Based on this,the crystallization duration can be adjusted to enhance catalytic efficiency and stability.This work advances fundamental understanding of zeolite crystallization and provides a roadmap for designing MOR catalysts with tailored active sites,bridging synthesis control to industrial application in coal-based ethanol production.展开更多
Iron-based single-atom(SA)catalysts offer a promising alternative to noble-metal catalysts for the oxygen reduction reaction(ORR),yet their limited intrinsic activity and durability hinder practical energy device appl...Iron-based single-atom(SA)catalysts offer a promising alternative to noble-metal catalysts for the oxygen reduction reaction(ORR),yet their limited intrinsic activity and durability hinder practical energy device applications.Herein,we introduce a novel TiN/TiC-supported Fe SA catalyst(TiNC/Fe-NC)with a hierarchical heterostructure that synergistically enhances Fe-Nx site activity and accessibility.The TiNC/Fe-NC catalyst achieves outstanding ORR performances,with half-wave potentials(E1/2)of 0.852 V in acidic media and 0.942 V in alkaline media.Theoretical simulations reveal that strong electronic interaction and efficient charge transfer between TiNC and Fe-Nx sites optimize the adsorption energetics of key ORR intermediates,driving the enhanced activity.Remarkably,TiNC effectively scavenges reactive oxygen radicals generated at the Fe centers,ensuring exceptional durability with a minimal 28 mV loss in E1/2 after 10,000 cycles at 80℃in acid media.In practical applications,TiNC/Fe-NC delivers peak power densities of 306 mW cm-2 in zinc-air battery and 732 mW cm-2 in proton exchange membrane fuel cells,with remarkable long-term stability.This work establishes TiNC/Fe-NC as a highperformance,durable catalyst for advanced energy storage and conversion technologies.展开更多
Single-atom catalysts(SACs)with a two-dimensional(2D)material as the support offer peculiar active sites at edges and in planes,which differ significantly in their chemical environments and consequently in their catal...Single-atom catalysts(SACs)with a two-dimensional(2D)material as the support offer peculiar active sites at edges and in planes,which differ significantly in their chemical environments and consequently in their catalytic performances in reactions.Herein,we report that Pt single atoms anchored at the edges of 2D MoS2nanosheets deliver dramatically high activity for CO2hydrogenation to CO,in contrast to Pt single atoms as well as their aggregations of 2D-rafts on the in-plane MoS2showing inferior activity.By a combination of experimental and theoretical studies,it was found that the activation of CO2was significantly facilitated on the Pt single atoms with the synergetic effect of its neighboring Mo at the edges,which readily dissociates into gaseous CO with a low energy barrier.Pt,which is isolated by the Scoordinated surroundings on the in-planes,is inert toward CO2adsorption and activation,thus leading to poor activity.This research reveals the close association between the catalytic performance of SACs with their chemical environments,and provides insights into the mechanism modulated by the synergetic effect between single-atom active sites and the support.展开更多
Enhancing the conduction and polarization properties of the emerging two-dimensional carbon material graphdiyne(GDY)represents a crucial step in broadening its application in microwave absorption.A novel strategy was ...Enhancing the conduction and polarization properties of the emerging two-dimensional carbon material graphdiyne(GDY)represents a crucial step in broadening its application in microwave absorption.A novel strategy was proposed to improve the microwave absorption performance of GDY through precise regulation of single-atom structures.Using three-dimensional spherical GDY as a substrate,Two Fe single-atom absorbers were successfully constructed:one anchored by Fe-N-GDY(FeN2C2)via sp-N/sp-C cooperative coordination,and the other anchored by Fe-GDY(FeC4)via sp-C coordination alone.Combined experimental characterization and theoretical calculations revealed that the FeN2C2configuration induces stronger charge transfer and dipole polarization.This effect synergistically optimizes both the dielectric loss and impedance matching of the material.Consequently,the optimal sample Fe-N-GDY achieved an effective absorption bandwidth of 5.98 GHz at a matched thickness of 2.0 mm,with a minimum reflection loss of−51.2 dB.The strategy was further extended to multiple 3d transition metals(Cr,Mn,Co,Ni,Cu,and Zn).Results indicate that GroupⅧelements(Fe,Co,Ni)exhibit superior performance in practical materials due to their electronic structures that favor balancing polarization and conduction losses.Radar cross section simulations confirm the exceptional attenuation capabilities of this series of absorbers in real-world scenarios.This work not only pioneers new applications for GDY in microwave absorption but also establishes a theoretical foundation for rationally designing atomically precise electromagnetic functional materials by revealing the“single-atom structure-property”correlation.展开更多
The fine-structure constantαwas introduced into physics by Arnold Somerfeld more than a century ago(1915).This quantity is attributed with the significance of describing the interaction between electrically charged p...The fine-structure constantαwas introduced into physics by Arnold Somerfeld more than a century ago(1915).This quantity is attributed with the significance of describing the interaction between electrically charged particles and photons and its official value is α=7.2973525643(11)×10−3[1/α=137.035999177(21)]according to the National Institute of Standards and Technology,NIST,on October 18,2025.This constant is the ratio of the square of the electron charge e to twice the product of the vacuum permittivityε0,Planck’s constant h,and the speed of light in a vacuum c;α=e2/(2ε0hc).So,fine-structure constant is expressed using four physical constants,which give the specified dimensionless physical number.The physical meaning of this constant has never been fully explained,so various meanings and properties are still attributed to this constant today.Since this constant appears in many physical phenomena,and without any real insight into its physical background,many people refer to it as a mystical constant.In article here,the finestructure constant is physically derived using the structural constant of all atoms,which is in turn related to the ionization energy of each individual atom.This gives things a different and clear meaning,so there is no room for any mysticism now.Here we will provide a physically clear basis for interpreting the meaning of the fine-structure constant,this uses theoretical methods of the author of this article as well in experimental tests conducted by NIST,when testing the ionization potential of 110 atoms from Mendeleev’s periodic table of elements,starting from hydrogen,with ordinal number one,to Darmstadtium,with ordinal number 110.In short,the research mentioned here has confirmed the existence of the structural constant of all atoms in each atom with an accuracy greater than any other NIST physical quantity,which means that these other physical quantities in which the structural constant of all atoms appears should be corrected accordingly,as stated for each specific case in this article.展开更多
We propose to trap circular Rydberg atoms(CRAs)via a ponderomotive potential well formed by a superimposed vortex light beam.We analytically calculate the ponderomotive potential energy for a Bessel vortex light beam....We propose to trap circular Rydberg atoms(CRAs)via a ponderomotive potential well formed by a superimposed vortex light beam.We analytically calculate the ponderomotive potential energy for a Bessel vortex light beam.We work out a corrected version of the classical circular orbit approximation for a CRA which fits the exact result much better than the usual approximation.We reveal the three-dimensional characteristics of the potential well for some benchmark values of the CRA principal quantum number and beam parameters such as the frequency,the opening angle and topological charge of the vortex.We investigate how we can achieve similar trapping effects for different principal quantum numbers by varying beam parameters.The potential provides a lattice structure along the beam axis where one CRA could be trapped at each lattice site.展开更多
Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish ...Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni2P by concurrently introducing B-doped atoms and P vacancies in Ni2P (Vp-B-Ni2P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni2P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni2P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni2P-separators present outstanding rate ability of 777 m A h g-1at 5 C and high areal capacity of 8.03 mA h cm-2under E/S of 5μL mg-1and sulfur loading of 7.20 mg cm-2.This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.展开更多
The introduction of metal single atoms(SAs)into semiconductors can effectively optimize their electronic configuration and enhance their photocatalytic properties.Therefore,it is crucial to clarify the corresponding p...The introduction of metal single atoms(SAs)into semiconductors can effectively optimize their electronic configuration and enhance their photocatalytic properties.Therefore,it is crucial to clarify the corresponding principles and photocatalytic mechanisms for efficient and sustainable photocatalytic water remediation systems.Herein,a promising Fe single-atom photocatalyst(FeSA-CN)is obtained by anchoring Fe SAs in graphitic carbon nitride using a simple calcination strategy.Characterization and experimental results indicate that the modification of Fe SAs not only introduces a doping energy level,but also changes the valence band position,which expands the light absorption range,enhances the reduction ability of photogenerated electrons,and improves the separation and transfer of photogenerated charge carriers.Subsequently,contaminants adsorbed on the FeSA-CN surface trigger their oxidation removal by h+,and the H2O2generated via two-electron direct reductions is converted in situ into OH by self-Fenton reaction for the synergistic contaminant degradation.In summary,FeSA-CN offers a promising pathway for single-atom photocatalysts in water remediation because of outstanding contamination removal efficiency,adaptability,and stability.展开更多
基金National Key Research and Development Program of China(2022YFA1203504)National Natural Science Foundation of China(62588201,12274424)Guangdong Pearl River Talents Program(2021QN02Z104)。
摘要Terahertz imaging has become increasingly important across various fields and practical production applications.Achieving both high sensitivity and high speed remains a primary challenge for most current THz imaging technologies.In this work,we present an imaging system based on Rydberg atomic vapor operating at frequencies exceeding 1 THz.By utilizing Cesium133 atoms coupled with THz waves,de-excitation radiation generated after atomic excitation to Rydberg states converts invisible THz waves into visible light,enabling the acquisition of spatial information and intensity distributions of THz fields.The system achieves a minimum detectable power of 330 fW∕s1∕2per(2.4×2.4)μm2,an imaging resolution of approximately 1.7 mm,and an imaging bandwidth of 8.6 MHz.Additionally,the theoretical imaging rate can exceed 1 MHz.The Rydberg-atom-based THz imaging system exhibits a simple structure and is amenable to miniaturization.This THz imaging method holds promise for advancing applications in THz nondestructive testing,biomedical imaging,and concealed object detection.
基金Research Special Project for First-class Disciplines in Inner Mongolia Autonomous Region(YLXKZX-NGD-017)Natural Science Foundation of Inner Mongolia Autonomous Region(2024QN06018)+1 种基金Inner Mongolia Autonomous Region High Level Talent Introduction and Research Support Program(DC2400002157)Doctoral Research Start Up Fund of Inner Mongolia University of Technology(BS2024001)。
摘要Asymmetric spin-orbit interaction(ASOI)has been widely employed in multifunctional applications through breaking the conjugate symmetry constraints of geometric phase metasurfaces.However,its implementation commonly suffers from lower robustness and complex design due to the requirement of subwavelength structures with different dimensions.Here,we demonstrate that two independent phase profiles can be generated only by designing the rotation angles of two C3 catenary meta-atoms in one unit based on the generalized Pancharatnam-Berry(PB)phase and interaction between meta-atoms,realizing ASOI.As a proof of concept,a spin-decoupled metadevice is fabricated and characterized,whose measured efficiencies approach 61.9%/52.8%for left-ight-handed circular polarization light incidence at 10.6μm.This work may provide a methodology for multifunctional light field modulation,holography multiplexing,and linear and nonlinear optical responses manipulation.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFA1405300)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0301705)Guangdong Provincial Quantum Science Strategic Initiative(Grant No.GDZX2304-002)。
摘要Topological vacua,a family of degenerate ground states of the Yang–Mills fields with zero field strength but nontrivial topological structures,play a fundamental role in particle physics and quantum field theory.However,they have not yet been experimentally observed.Here,we propose an experimental scheme to realize a real-space SU(2)artificial Yang–Mills topological vacua using a cloud of two-Λ-level cold atoms.
基金supported by University-Industry Collaborative Education Program(Project No.220506627183928).
摘要We developed a model of a quantum Otto engine using two coupled two-level atoms.Based on the platform,we show that frequency detuning and the coupling strength induced by dipole-dipole interactions can lead to decoherence by disrupting coherent energy exchange.We focus on fundamental thermodynamic quantities,including heat absorption,release to heat baths,work done and efficiency.It is noteworthy that the interatomic coupling strength and frequency detuning do not merely affect the shape of the work and the efficiency but ultimately govern its quantitative magnitude.In the field of quantum thermodynamics,we have established an upper bound efficiency that is stricter than the Carnot limit.Moreover,our analysis confirms that quantum coherence enables the system to exceed the efficiency threshold of a classical Otto heat engine.The second law of thermodynamics holds all the while.Our results constitute a step forward in the design of conceptually new quantum thermodynamic devices which take advantage of uniquely quantum resources of quantum coherence.
基金supported by the National Natural Science Foundation of China (No. 22469016)the Central Government Guides Local Science and Technology Development Funds of Inner Mongolia (2023ZY0007)+2 种基金the Fundamental Research Funds for the Provincial Universities of Zhejiang (ZX2025000270)the Natural Science Foundation of Zhejiang Province, the Ningbo Yongjiang Talent Programmethe projects on enhancing basic research capabilities of postgraduate students in universities in Inner Mongolia (ZTY2024033)
摘要Hydrofuroin(HDF),a key precursor of fuel,can be produced by electrocatalytic furfural(FF)hydrodimerization,offering a promising way to generate value-added products.However,this process is hindered by sluggish C-C coupling and hydrogenation steps,resulting in low Faradaic efficiency(FE).Herein,atomically dispersed Ru sites anchored on lattice vacancies of La0.9NiO3(Ru-La0.9NiO3)electrocatalysts were demonstrated as an efficient electrocatalyst for FF hydrodimerization,where an intermediate spillover strategy significantly enhances the FE.Mechanistic investigations reveal that Ru single atoms serve as active sites for the initial hydrogenation to form the FF-CHOH*intermediate with almost 100%selectivity,thereby suppressing the side reaction of hydrogen evolution.Subsequently,the increased FF-CHOH*intermediate undergoes spillover to adjacent Ni sites,decreasing the energy barrier for the subsequent C-C coupling step to HDF(ΔG=0.63 eV).As a result,the Ru-La0.9NiO3catalyst displays a high FE of 74%and a production rate of 3.95 mmol cm-2h-1toward electrocatalytic FF hydrodimerization to HDF product.This work provides an efficient intermediate spillover approach,offering mechanistic insights into Ru-Ni synergism in Ru-La0.9NiO3and providing a sensible method for electrocatalytic hydrodimerization of furfural to produce high-value products.
摘要The integration of multiple active sites has been demonstrated to significantly enhance the electrocatalytic performance of the hydrogen evolution reaction(HER).However,the precise construction of synergistic SAs/NCs sites and a thorough understanding of their reaction mechanisms remain challenging.Herein,a straightforward synthetic strategy is developed for the fabrication of Ru SAs and NCs supported on nitrogen-doped carbon spheres derived from m-aminophenol/formaldehyde resin(denoted as Ru1-n@AFCS),achieved by tuning the ratio of resorcinol to m-aminophenol during phenolic resin polymerization.The optimized Ru1-n@AFCS HER performance in alkaline media,requiring an overpotential of only 11.2 mV to achieve 10 mA cm-2 and displaying a mass activity of 5158.2 A g-1,which is 60 times higher than that of commercial 20%Pt/C(85.4 A g-1)at-0.025 V vs.RHE.When integrated into an anion-exchange-membrane water electrolyzer,the catalyst achieves a current density of 1 A cm-2 at 1.80 V with a remarkable noble metal mass activity of 55.2 A mg-Ru-1.Combined experimental and theoretical calculations reveal that the nitrogen-doped carbon support modulates electronic structure of Ru NCs,while adjacent isolated Ru SAs facilitate hydrogen transfer via strong hydroxyl adsorption,collectively forming a“dual-engine”catalytic center that significantly enhances alkaline HER performance.
基金financially supported by the National Natural Science Foundation of China(22108259)the key research and development project of Henan Province(241111230600)the financial support of the Natural Science Foundation of Henan Province(252300423737)。
摘要The incorporation of noble metals has been proven to be an effective strategy for enhancing the catalytic performance of Cu-based catalysts.Nevertheless,precise control of the structure of noble metals to achieve outstanding selective hydrogenation activity remains challenging.In this study,two catalysts with well-defined Pd configurations,including atomically dispersed Pd species(CuPd0.01/SiO2)and Pd clusters(CuPd0.05/SiO2),were constructed for the selective hydrogenation of furfural.Even at extremely low Pd loading(0.01 wt%),the single-atom Pd-incorporated catalyst achieved furfural conversion of80.2%under mild conditions(90℃,1 MPa H2),exceeding both CuPd0.05/SiO2(76.3%)and monometallic Cu/SiO2(56.3%).Kinetic analysis indicated that the apparent activation energy decreased to 140.2 kJ/mol compared to the unmodified catalyst(255.2 kJ/mol).Density functional theory calculations revealed that isolated Pd atoms induced electron redistribution at the Pd-Cu interface,facilitated H2dissociation,and promoted C=O activation.In contrast,the formation of Pd clusters caused a negative effect,which reduced the local electron density of adjacent Cu sites and decreased the number of effective active sites.These results establish a clear structure-performance relationship between Pd configuration and selective hydrogenation activity,providing insights for the rational design of highly efficient Cu-based hydrogenation catalysts for biomass-derived chemicals under mild conditions.
摘要The conversion of solar energy into hydrogen represents a promising and sustainable approach to addressing the global energy crisis and mitigating environmental pollution.However,achieving the industrial benchmark of solar-to-hydrogen efficiency remains challenging due to the inherently insufficient spatial separation of charge carriers and sluggish interfacial kinetics.Engineering redox-active sites has emerged as an effective approach to enhance photocatalytic hydrogen evolution performance.Herein,a dual-mode copper-modified titanium dioxide photocatalyst(Cu/TiO2),comprising isolated Cu atoms and CuO nanoclusters,was successfully synthesized via a facile molten salt method.The optimized Cu/TiO2exhibited a remarkable hydrogen evolution rate of 37.6 mmol g-1h-1with methanol as a sacrificial agent,representing a 96-fold enhancement compared to pristine TiO2.Mechanistic studies revealed that isolated Cu atoms incorporated into the TiO2lattice substantially lower the free energy of hydrogen adsorption(*H),thereby promoting the proton reduction half-reaction.Simultaneously,the surface-dispersed CuO nanoclusters were found to reduce the overpotential for methanol oxidation,thereby accelerating the oxidation half-reaction and facilitating overall charge balance during photocatalysis.Furthermore,photocatalytic hydrogen production coupled with the oxidation of various organic molecules was evaluated under a low sacrificial agent concentration(0.1%)over the Cu/TiO2photocatalyst,offering a more sustainable and practically relevant assessment of catalyst performance for green energy applications.
基金supported by the Postgraduate Research&Practice Innovation Program of Jiangsu Province(grant number KYCX233695)for providing financial support for this work。
摘要Traditional strong metal-support interactions(SMSIs)induced by encapsulated reducible oxide overlayers on metal nanoparticles can suppress sintering but has a strong negative impact on the catalytic activity because of decreased availability of active sites.Herein,we design three SMSIs configurations on Pt-TiO2via crystal-phase engineering.These configurations comprised encapsulated Pt nanoparticle(NPs)with TiO2-xoverlayer on anatase,weakly embedded Pt clusters on P25,and deeply embedded Pt Ox-induced Pt single-atom(SA)structure on rutile.These configurations exhibited Pt species at multiple scales,ranging from NPs to SAs.Among them,Pt supported rutile TiO2sample(Pt-TiO2(R)-H)achieved extremely low CO selectivity(2.05%,200℃)and optimal H2production performance due to the enhanced SMSIs from Pt-Ti coordination in the deeply embedded Pt Oxregion.This Pt-Ti coordination facilitated the electron transfer from Pt to Ti and induced dual-function centers of electron-deficient Ptδ+-Pt2+pairs(0<δ<2,where Ptδ+represent Pt SAs)for methanol decomposition and electron-rich Ti3+-oxygen vacancies for water dissociation.Such unique configuration altered the MSR reaction pathway and the kinetic rates of each elementary step in these reaction pathways were systematically analyzed.This work proposes an SMSIs configuration induced by a deeply embedded structure,which mitigates the negative impact on catalytic activity from encapsulated overlayers,meanwhile providing a strategy for developing high-loading Pt SAs catalysts.
基金supported by National Key Research and Development Program(No.2022YFA1504800)National Natural Science Foundation of China(No.22278316).
摘要Photocatalytic conversion of carbon dioxide(CO2)to methanol is hindered by inefficient charge separation and complex multielectron pathways.To address these challenges,we report a synergistic catalyst design in which cobalt vacancies(VCo)are coupled with indium single atoms(In SAs).VCo sites were precisely constructed on Co3O4nanosheets using a chlorine cold plasma technique,acting as“atomic sockets”that confine In SAs and form a robust In-O-VCo coordination structure.The resulting In/Co3−xO4catalyst delivered a high methanol production rate of 466.7μmol/(g·h)with 92.3%selectivity under simulated solar irradiation,which was eight times greater than that of the vacancy-free catalyst.Mechanistic studies revealed a synergistic functional division:the VCo sites efficiently adsorbed and dissociated H2O to supply protons,whereas the In SAs polarized CO2and stabilized the critical*COOH intermediate.This synergy of strong electronic metal-support interactions improved charge separation and steered the reaction pathway toward methanol,offering a novel atomic-level strategy for designing highly selective CO2photoreduction catalysts.
基金financially supported by National Natural Science Foundation of China(22279069,22478211 and 22372017)。
摘要Hydrazine-assisted water electrolysis is a promising route for hydrogen production,and efficient bifunctional electrodes for the anodic hydrazine oxidation reaction(HzOR)and the cathodic hydrogen evolution reaction(HER)simplify the devices and enhance the technological advantage.However,suffering from the incompatible adsorption of different intermediates and the sluggish reaction kinetics,the design of effective and durable bi-functional electrodes still faces challenges.Herein,a Lewis acid(WOx)of powerful electron-accepting ability stabilized single-atom Ir catalyst(Ir-SA@WOx),intriguing strong metalsupport interaction(SMSI),is demonstrated to efficiently activate H2O and N2H4molecules.Ir-SA@WOxshows exceptional activity for both HER and HzOR(26.31 and 44.79 A mgIr-1at-100 mV),surpassing commercial Pt/C and Ir/C by factors of 41.8 and 27.6,respectively.A hydrazine-assisted water electrolyzer fabricated with Ir-SA@WOxachieves a current density of 100 mA cm-2at an ultra-low cell voltage of 0.313 V and electricity consumption of merely 0.75 kWh m-3H2,significantly lower than conventional water electrolysis systems(1.852 V,4.43 kWh m-3H2).In situ infrared absorption spectroscopy and theoretical calculations elucidate that the SMSI in Ir-SA@WOxreconstructs the electronic structure to facilitate the activation of the rigid water at the catalyst/electrolyte interface into free species,also optimizes H*adsorption and accelerates dehydrogenation kinetics of the potential-determining step of N2H3*-toN2H2*at Ir-sites,thereby realizing high activity for both HER and HzOR.This work illustrates the tailoring of electronic structures via the SMSI effect for catalytic-activity enhancement,guiding the design of advanced bi-functional catalysts for energy-efficient hydrogen production.
基金supported by the National Key Research and Development Program of China(2024YFE0207000)the National Natural Science Foundation of China(22288101,22241801,22022202,22032005)+2 种基金the Dalian Outstanding Young Scientist Foundation(2021RJ01)the Liaoning International Joint Laboratory Project(2024JH2/102100005)the Liaoning Binhai Laboratory(LBLD-2025-03)。
摘要Mordenite(MOR)zeolites are key catalysts in dimethyl ether(DME)carbonylation,with their performance governed by the distribution of Brùnsted acid sites(BAS)associated with framework aluminum(Al).The 8-membered ring(8-MR)channels host the desired active BAS,while BAS in the 12-membered ring(12-MR)channels promote coking,making precise Al siting critical.Traditional views posit Al siting is fixed post-crystallization,yet emerging evidence reveals dynamic Al relocation during the ripening stage of the crystallization.Despite this potential,mechanisms governing Al migration in MOR remain unclear,with most studies focusing on post-synthetic modifications that risk structural integrity.This study investigates the crystallization dynamics of MOR,using in situ solid-state nuclear magnetic resonance(NMR)to probe the real-time chemical environment of Al and employing advanced characterization techniques to track framework Al migration.During the ripening stage of crystallization,framework Al atoms migrate directionally from T1,T2,and T3 to the T4 site,which influences the catalytic performance of mordenite.Based on this,the crystallization duration can be adjusted to enhance catalytic efficiency and stability.This work advances fundamental understanding of zeolite crystallization and provides a roadmap for designing MOR catalysts with tailored active sites,bridging synthesis control to industrial application in coal-based ethanol production.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSITRS2024-00345635 and RS-2021-NR060090)the Research Grant Council of the Hong Kong SAR(PolyU15302824)。
摘要Iron-based single-atom(SA)catalysts offer a promising alternative to noble-metal catalysts for the oxygen reduction reaction(ORR),yet their limited intrinsic activity and durability hinder practical energy device applications.Herein,we introduce a novel TiN/TiC-supported Fe SA catalyst(TiNC/Fe-NC)with a hierarchical heterostructure that synergistically enhances Fe-Nx site activity and accessibility.The TiNC/Fe-NC catalyst achieves outstanding ORR performances,with half-wave potentials(E1/2)of 0.852 V in acidic media and 0.942 V in alkaline media.Theoretical simulations reveal that strong electronic interaction and efficient charge transfer between TiNC and Fe-Nx sites optimize the adsorption energetics of key ORR intermediates,driving the enhanced activity.Remarkably,TiNC effectively scavenges reactive oxygen radicals generated at the Fe centers,ensuring exceptional durability with a minimal 28 mV loss in E1/2 after 10,000 cycles at 80℃in acid media.In practical applications,TiNC/Fe-NC delivers peak power densities of 306 mW cm-2 in zinc-air battery and 732 mW cm-2 in proton exchange membrane fuel cells,with remarkable long-term stability.This work establishes TiNC/Fe-NC as a highperformance,durable catalyst for advanced energy storage and conversion technologies.
基金financial supports from the Natural Science Foundation of Jiangsu Province(BK20231075)the National Natural Science Foundation of China(22208021)+6 种基金the Fundamental Research Funds for the Central Universities(QNTD202506)the National Key Research and Development Program(2025YFE0117000)the Science and Technology Project of Jiangsu Provincial Department of Science and Technology(BE2023852)the Science and Technology Project of Jiangsu Provincial Department of Science and Technology(BE2022613)the Key Research Project of the Science and Technology Department of Xinjiang,Development and Industrial Validation of a New Low-Energy Carbon Capture Solventthe CO2 Phase Change Absorption Catalytic Desorption Coupled System Design and Molecular Mechanism Research(2023KYJD1004)the Zhejiang Province Science and Technology Plan Project(2023C03156)。
摘要Single-atom catalysts(SACs)with a two-dimensional(2D)material as the support offer peculiar active sites at edges and in planes,which differ significantly in their chemical environments and consequently in their catalytic performances in reactions.Herein,we report that Pt single atoms anchored at the edges of 2D MoS2nanosheets deliver dramatically high activity for CO2hydrogenation to CO,in contrast to Pt single atoms as well as their aggregations of 2D-rafts on the in-plane MoS2showing inferior activity.By a combination of experimental and theoretical studies,it was found that the activation of CO2was significantly facilitated on the Pt single atoms with the synergetic effect of its neighboring Mo at the edges,which readily dissociates into gaseous CO with a low energy barrier.Pt,which is isolated by the Scoordinated surroundings on the in-planes,is inert toward CO2adsorption and activation,thus leading to poor activity.This research reveals the close association between the catalytic performance of SACs with their chemical environments,and provides insights into the mechanism modulated by the synergetic effect between single-atom active sites and the support.
基金financial support from the National Natural Science Foundation of China(No.22375166,22101229)Natural Science Basic Research Program of Shaanxi(No.2024JC-JCQN-44)+1 种基金the Key Research and Development Program of Shaanxi Province(2024GX-YBXM-379)Innovation Capability Support Program of Shaanxi Science and Technology Innovation Team Project(No.2025RS-CXTD-024).
摘要Enhancing the conduction and polarization properties of the emerging two-dimensional carbon material graphdiyne(GDY)represents a crucial step in broadening its application in microwave absorption.A novel strategy was proposed to improve the microwave absorption performance of GDY through precise regulation of single-atom structures.Using three-dimensional spherical GDY as a substrate,Two Fe single-atom absorbers were successfully constructed:one anchored by Fe-N-GDY(FeN2C2)via sp-N/sp-C cooperative coordination,and the other anchored by Fe-GDY(FeC4)via sp-C coordination alone.Combined experimental characterization and theoretical calculations revealed that the FeN2C2configuration induces stronger charge transfer and dipole polarization.This effect synergistically optimizes both the dielectric loss and impedance matching of the material.Consequently,the optimal sample Fe-N-GDY achieved an effective absorption bandwidth of 5.98 GHz at a matched thickness of 2.0 mm,with a minimum reflection loss of−51.2 dB.The strategy was further extended to multiple 3d transition metals(Cr,Mn,Co,Ni,Cu,and Zn).Results indicate that GroupⅧelements(Fe,Co,Ni)exhibit superior performance in practical materials due to their electronic structures that favor balancing polarization and conduction losses.Radar cross section simulations confirm the exceptional attenuation capabilities of this series of absorbers in real-world scenarios.This work not only pioneers new applications for GDY in microwave absorption but also establishes a theoretical foundation for rationally designing atomically precise electromagnetic functional materials by revealing the“single-atom structure-property”correlation.
摘要The fine-structure constantαwas introduced into physics by Arnold Somerfeld more than a century ago(1915).This quantity is attributed with the significance of describing the interaction between electrically charged particles and photons and its official value is α=7.2973525643(11)×10−3[1/α=137.035999177(21)]according to the National Institute of Standards and Technology,NIST,on October 18,2025.This constant is the ratio of the square of the electron charge e to twice the product of the vacuum permittivityε0,Planck’s constant h,and the speed of light in a vacuum c;α=e2/(2ε0hc).So,fine-structure constant is expressed using four physical constants,which give the specified dimensionless physical number.The physical meaning of this constant has never been fully explained,so various meanings and properties are still attributed to this constant today.Since this constant appears in many physical phenomena,and without any real insight into its physical background,many people refer to it as a mystical constant.In article here,the finestructure constant is physically derived using the structural constant of all atoms,which is in turn related to the ionization energy of each individual atom.This gives things a different and clear meaning,so there is no room for any mysticism now.Here we will provide a physically clear basis for interpreting the meaning of the fine-structure constant,this uses theoretical methods of the author of this article as well in experimental tests conducted by NIST,when testing the ionization potential of 110 atoms from Mendeleev’s periodic table of elements,starting from hydrogen,with ordinal number one,to Darmstadtium,with ordinal number 110.In short,the research mentioned here has confirmed the existence of the structural constant of all atoms in each atom with an accuracy greater than any other NIST physical quantity,which means that these other physical quantities in which the structural constant of all atoms appears should be corrected accordingly,as stated for each specific case in this article.
基金supported in part by Grants Nos.NSFC-12035008,NSFC-12247151,and NSFC-12447117。
摘要We propose to trap circular Rydberg atoms(CRAs)via a ponderomotive potential well formed by a superimposed vortex light beam.We analytically calculate the ponderomotive potential energy for a Bessel vortex light beam.We work out a corrected version of the classical circular orbit approximation for a CRA which fits the exact result much better than the usual approximation.We reveal the three-dimensional characteristics of the potential well for some benchmark values of the CRA principal quantum number and beam parameters such as the frequency,the opening angle and topological charge of the vortex.We investigate how we can achieve similar trapping effects for different principal quantum numbers by varying beam parameters.The potential provides a lattice structure along the beam axis where one CRA could be trapped at each lattice site.
基金Institute of Technology Research Fund Program for Young Scholars21C Innovation Laboratory Contemporary Amperex Technology Co.,Limited,Ninde, 352100, China (21C–OP-202314)。
摘要Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni2P by concurrently introducing B-doped atoms and P vacancies in Ni2P (Vp-B-Ni2P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni2P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni2P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni2P-separators present outstanding rate ability of 777 m A h g-1at 5 C and high areal capacity of 8.03 mA h cm-2under E/S of 5μL mg-1and sulfur loading of 7.20 mg cm-2.This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.
基金financially supported by the National Natural Science Foundation of China(Nos.52100032 and 52350005)the Basic and Applied Basic Research Project of Guangzhou(Nos.2024A04J3679 and 2024A03J0088)+2 种基金the Introduced Innovative Research and Development Team Project under the“The Pearl River Talent Recruitment Program”of Guangdong Province(No.2019ZT08L387)the Opening Project of Shanxi Province Key Laboratory of Chemical Process Intensification,North University of China(No.2023-HOCE10)the National College Students’Innovation and Entrepreneurship Training Program(No.202211078135)
摘要The introduction of metal single atoms(SAs)into semiconductors can effectively optimize their electronic configuration and enhance their photocatalytic properties.Therefore,it is crucial to clarify the corresponding principles and photocatalytic mechanisms for efficient and sustainable photocatalytic water remediation systems.Herein,a promising Fe single-atom photocatalyst(FeSA-CN)is obtained by anchoring Fe SAs in graphitic carbon nitride using a simple calcination strategy.Characterization and experimental results indicate that the modification of Fe SAs not only introduces a doping energy level,but also changes the valence band position,which expands the light absorption range,enhances the reduction ability of photogenerated electrons,and improves the separation and transfer of photogenerated charge carriers.Subsequently,contaminants adsorbed on the FeSA-CN surface trigger their oxidation removal by h+,and the H2O2generated via two-electron direct reductions is converted in situ into OH by self-Fenton reaction for the synergistic contaminant degradation.In summary,FeSA-CN offers a promising pathway for single-atom photocatalysts in water remediation because of outstanding contamination removal efficiency,adaptability,and stability.