Atomic spin gyroscopes are promising candidates for next-generation inertial navigation due to extremely high theoretical precision,relatively small size among atomic gyroscopes,and promising potential for miniaturiza...Atomic spin gyroscopes are promising candidates for next-generation inertial navigation due to extremely high theoretical precision,relatively small size among atomic gyroscopes,and promising potential for miniaturization.In particular,the spin-exchange relaxation-free(SERF)atomic gyroscope relies on optical pumping to polarize atoms,enabling rotation sensing through the Faraday optical rotation angle(FORA).However,fluctuations in atomic density introduce systematic errors in FORA measurements,limiting long-term stability.We present a data-driven decoupling method that isolates atomic density fluctuations from the FORA signal by modeling spatially resolved light absorption in the vapor cell.The model accounts for the spatial distribution of spin polarization in the pump-light interaction volume,density-dependent relaxation rates,wall-induced relaxation,and polarization diffusion,and is implemented within a finite-element framework.Compared to the conventional Lambert-Beer law,which assumes one-dimensional homogeneity,our approach captures the full threedimensional density and polarization distribution,significantly improving the accuracy of light absorption modeling.The resulting absorption-density maps are used to train a feedforward neural network,yielding a high-precision estimator for atomic density fluctuations.This estimator enables the construction of a decoupling equation that separates the density contribution from the FORA signal.Experimental validation shows that this method improves the bias instability atσ(100 s)of the gyroscope was improved by 73.1%compared to traditional platinum-resistance-based stabilization.The proposed framework is general and can be extended to other optical pumping-based sensors,such as optically pumped magnetometers.展开更多
Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the effica...Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.展开更多
The single-atom replacement strategy is a typical approach which just converts elements in lead compounds into their analogues with very small chemical changes.In this research,we implemented this strategy to modify t...The single-atom replacement strategy is a typical approach which just converts elements in lead compounds into their analogues with very small chemical changes.In this research,we implemented this strategy to modify the sulfonamide scaffold identified in our previous work,and resulting in the synthesis of 40 novel sulfonamide derivatives not previously reported in the literature.The insecticidal activities of these compounds against the Mythimna separata and Plutella xylostella were assessed.Our findings indicate that the pyridine sulfonamide structure significantly enhances insecticidal efficacy.Specifically,compound 7c exhibited LC 50 values of 0.157 and 0.256 mg/mL against the M.separata and P.xylostella,which significantly increased 97-and 41-fold compared to celangulin V,respectively.The experimental results revealed that pyridine sulfonamide analogues could serve as potential green insecticides.展开更多
Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibite...Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibited very high performance in peroxymonosulfate activation.The Fe single-atom filled an N vacancy on the triazine ring edge of C_(3)N_(4),as confirmed through X-ray absorption fine structure,density functional calculation and elec-tron paramagnetic resonance.The SAFe_(0.4)–C_(3)N_(4)/PMS system could completely remove phenol(20 mg/L)within 10 min and its first-order kinetic constant was 12.3 times that of the Fe_(3)O_(4)/PMS system.Under different ini-tial pH levels and in various anionic environments,SAFe_(0.4)–C_(3)N_(4) still demonstrated excellent catalytic activity,achieving a removal rate of over 90%for phenol within 12 min.In addition,SAFe_(0.4)–C_(3)N_(4) exhibited outstanding selectivity in reaction systems with different pollutants,showing excellent degradation effects on electron-rich pollutants only.Hydroxyl radicals(•OH),singlet oxygen(1O_(2))and high-valent iron oxide(Fe(Ⅳ)=O)were de-tected in the SAFe_(0.4)–C_(3)N_(4)/PMS system through free radical capture experiments.Further experiments on the quenching of active species and a methyl phenyl sulfoxide probe confirmed that 1O_(2) and Fe(Ⅳ)=O played dom-inant roles.Additionally,the change in the current response after adding PMS and phenol in succession proved that a direct electron transfer path between organic matter and the catalyst surface was unlikely to exist in the SAFe_(0.4)–C_(3)N_(4)/PMS/Phenol degradation system.This study provides a new demonstration of the catalytic mech-anism of single-atom catalysts.展开更多
The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulat...The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulate the electronic structure of MoS_(2),thereby obtaining a multifunctional catalyst that serves as an efficient sulfur host.The W/V dual single-atomdoped MoS_(2)grown on carbon nanofibers(CMWVS)demonstrates a strong adsorption ability for lithium polysulfides,suppressing the shuttle effects.Additionally,the doping process also results in the phase transition from 2H-MoS_(2)to 1T-MoS_(2)and generates sufficient edge sulfur atoms,promoting the charge/electron transfer and enriching the reaction sites.All these merits contribute to the superior conversion reaction kinetics,leading to the outstanding Li-S battery performance.When fabricated as cathodes by compositing with sulfur,the CMWVS/S cathode delivers a high capacity of 1481.7 mAh g^(-1)at 0.1 C(1 C=1672 mAh g^(-1))and maintains 816.3 m Ah g^(-1)after 1000 cycles at 1.0 C,indicating outstanding cycling stability.Even under a high sulfur loading of 7.9 mg cm^(-2)and lean electrolyte conditions(E/S ratio of 9.0μL mg^(-1)),the cathode achieves a high areal capacity of 8.2 m Ah cm^(-2),showing great promise for practical Li-S battery applications.This work broadens the scope of doping strategies in transition-metal dichalcogenides by tailoring their electronic structures,providing insightful direction for the rational development of high-efficiency electrocatalysts for advanced Li-S battery applications.展开更多
We propose a novel cooling protocol within a triple-Laguerre-Gaussian cavity optomechanical system,which is designed to suppress the thermal vibrations of a rotating mirror to reach its quantum ground state.The system...We propose a novel cooling protocol within a triple-Laguerre-Gaussian cavity optomechanical system,which is designed to suppress the thermal vibrations of a rotating mirror to reach its quantum ground state.The system incorporates two auxiliary cavities and an atomic ensemble coupled to a Laguerre-Gaussian rotational cavity.By carefully selecting system parameters,the cooling process of the rotating mirror is significantly enhanced,while the heating process is effectively suppressed,enabling efficient ground-state cooling even in the unresolved sideband regime.Compared to previous works,our scheme reduces the stringent restrictions on auxiliary systems,making it more experimentally feasible under broader parameter conditions.These findings provide a robust approach for achieving ground-state cooling in mechanical resonators.展开更多
Rydberg-atom-based superheterodyne receivers integrate self-calibration,high sensitivity,a wide operational frequency range,and phase/frequency resolved detection capabilities,demonstrating broad application prospects...Rydberg-atom-based superheterodyne receivers integrate self-calibration,high sensitivity,a wide operational frequency range,and phase/frequency resolved detection capabilities,demonstrating broad application prospects as nextgeneration microwave receivers.Linear gain and linear dynamic range(LDR)are critical metrics for assessing receiver sensitivity and demodulation fidelity,respectively.We numerically solve the four-level master equation and then employ particle swarm optimization(PSO)algorithm to co-optimize linear gain and LDR in atomic superheterodyne receivers based on balanced homodyne detection.Further,we systematically account for dominant dephasing mechanisms in the simulation,encompassing spontaneous decay,transit dephasing,collision dephasing,laser linewidth dephasing,and Doppler averaging.Homodyne readout utilizes both the real and imaginary parts of polarizability for sensing.In the case of the photon shot noise limit,its signal-to-noise ratio(SNR)expression resembles that of direct optical-intensity readout.However,the inherent coherent subtraction operation in homodyne detection significantly suppresses common-mode noise,while appropriately increasing the reference beam power enhances the gain in practical experiments.Indeed,this co-optimization problem,characterized by a high-dimensional variable space,two objectives,and non-convexity,is well-suited for solution by PSO.In addition,probe and coupling detuning contribute equivalently to polarizability and compensate for each other owing to Doppler averaging,thereby reducing the optimization variable space by one.By adopting a product form of linear gain and LDR as the fitness function,the PSO achieves rapid convergence.Here,the effectiveness of the PSO results is verified via the total harmonic distortion(THD).The relative error-based LDR calculation method we proposed efficiently measures receiver response linearity with consuming fewer computational resources.This research is expected to offer valuable insights into enhancing the performance of Rydberg-atom-based superheterodyne receivers.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-N_(x) site activity and accessibility.The TiNC/Fe-NC catalyst achieves outstanding ORR performances,with half-wave potentials(E_(1/2))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-N_(x) 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 E_(1/2) 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
Atomic layer deposition(ALD)is extensively used to fabricate doped dielectrics due to its ability to deposit conformal films with atomic-scale thickness control.Al-doped TiO_(2)(ATO)is a promising high-k dielectric fo...Atomic layer deposition(ALD)is extensively used to fabricate doped dielectrics due to its ability to deposit conformal films with atomic-scale thickness control.Al-doped TiO_(2)(ATO)is a promising high-k dielectric for dynamic random access memory(DRAM)applications,offering a high dielectric constant with a remarkable leakage-lowering effect by Al acceptor doping.However,ATO fabrication via conventional supercycle-based ALD suffers from severe crystallinity loss during the growth of TiO_(2) upon Al doping owing to the dopant-induced lattice disorder.In addition,Al doping cannot reduce any inherent O vacancies(V_(O))of TiO_(2),although the original purpose of doping was to address the n-type nature caused by V_(O).To resolve these limitations,we propose a single-step,in-situ Ar/O_(2) post-doping plasma(PDP)process immediately after the Al dopant incorporation.Using the PDP process,simultaneous atomic-scale dopant migration-mediated crystallization and V_(O) annihilation were successfully initiated.Thus,the surface concentration of the dopant decreased,reducing the dopant-induced lattice distortion,while promoting the highly crystallized seed layer-like surface.Consequently,strong rutile-phase recovery was accompanied by enhanced lattice-matched growth.In addition,the PDP process significantly lowers the V_(O)-to-lattice oxygen ratio by facilitating the recombination between reactive O species and V_(O),increasing the corresponding 0.4 e V of conduction band offset(CBO).Despite the common trade-off between the dielectric constant and leakage,the Pt/PDP-ATO/Ru capacitor exhibited a simultaneous 30%increase in dielectric constant and up to a 1.6-order reduction in leakage current density.展开更多
Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g...Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g-C_(3)N_(4) heterojunctions to improve process cost-effectiveness.The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction demonstrated an effective removal of 93.6%thiamphenicol(TAP)within 45 min,with the rate constant(0.0584 min^(-1))that was 2.4 and 2.8 times that of Co_(3)O_(4) and g-C_(3)N_(4) alone,respectively.The formation of heterojunctions facilitated electron transfer,enriched the electron density on Co_(3)O_(4),and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates.The enhanced production of atomic hydrogen(H*)of Co_(3)O_(4)/g-C_(3)N_(4),which increased by 13.6-28.2 times,contributed more to pollutant removal(64.0%),much higher than that of Co_(3)O_(4)(37.3%)and g-C_(3)N_(4)(6.1%).The energy barrier for H_(2) formation on Co_(3)O_(4)/g-C_(3)N_(4)(0.75 eV)was higher than that on Co_(3)O_(4)(-1.84 eV),supporting that it could stabilize H*and inhibit the formation of H_(2).The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction exhibited stable performance with less impact by pH and co-existing ions,and posed effectiveness for the dechlorination of typical chlorinated antibiotics.This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.展开更多
Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)an...Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)and stability(longevity)remains challenging,as the interplay between metal atoms,supports,and reactants is poorly understood.展开更多
The so-called close-coupled gas atomization process involves melting a metal and using a high-pressure gas jet positioned close to the melt stream to rapidly break it into fine,spherical powder particles.This techniqu...The so-called close-coupled gas atomization process involves melting a metal and using a high-pressure gas jet positioned close to the melt stream to rapidly break it into fine,spherical powder particles.This technique,adapted for blast furnace slag granulation using a circular seam nozzle,typically aims to produce solid slag particles sized 30–140μm,thereby allowing the utilization of slag as a resource.This study explores the atomization dynamics of liquid blast furnace slag,focusing on the effects of atomization pressure.Primary atomization is simulated using a combination of the Volume of Fluid(VOF)method and the Shear Stress Transport k-ωturbulence model,while secondary atomization is analyzed through the Discrete Phase Model(DPM).The results reveal that primary atomization progresses in three stages:the slag column transforms into an umbrella-shaped liquid film,whose leading edge fragments into particles while forming a cavity-like structure,which is eventually torn into ligaments.This primary deformation is driven by the interplay of airflow velocity in the recirculation zone and the guide tube outlet pressure(Fp).Increasing the atomization pressure amplifies airflow velocity,recirculation zone size,expansion and shock waves,though the guide tube outlet pressure variations remain irregular.Notably,at 4.5 MPa,the primary deformation is most pronounced.Secondary atomization yields finer slag particles as a result of more vigorous primary atomization.For this pressure,the smallest average particle size and the highest yield of particles within the target range(30–140μm)are achieved.展开更多
Aberration-corrected annular dark-field scanning transmission electron microscopy(ADF-STEM)is a powerful tool for structural and chemical analysis of materials.Conventional analyses of ADF-STEM images rely on human la...Aberration-corrected annular dark-field scanning transmission electron microscopy(ADF-STEM)is a powerful tool for structural and chemical analysis of materials.Conventional analyses of ADF-STEM images rely on human labeling,making them labor-intensive and prone to subjective error.Here,we introduce a deep-learning-based workflow combining a pix2pix network for image denoising and either a mathematical algorithm local intensity threshold segmentation(LITS)or another deep learning network UNet for chemical identification.After denoising,the processed images exhibit a five-fold improvement in signal-to-noise ratio and a 20%increase in accuracy of atomic localization.Then,we take atomic-resolution images of Y–Ce dual-atom catalysts(DACs)and Fe-doped ReSe_(2) nanosheets as examples to validate the performance.Pix2pix is applied to identify atomic sites in Y–Ce DACs with a location recall of 0.88 and a location precision of 0.99.LITS is used to further differentiate Y and Ce sites by the intensity of atomic sites.Furthermore,pix2pix and UNet workflow with better automaticity is applied to identification of Fe-doped ReSe_(2) nanosheets.Three types of atomic sites(Re,the substitution of Fe for Re,and the adatom of Fe on Re)are distinguished with the identification recall of more than 0.90 and the precision of higher than 0.93.These results suggest that this strategy facilitates high-quality and automated chemical identification of atomic-resolution images.展开更多
Translator’s Note:Shou Chin Wang(Wang Shoujing)was one of the few Chinese physicists who made significant contributions to the early development of quantum mechanics.One of his representative works is the study on th...Translator’s Note:Shou Chin Wang(Wang Shoujing)was one of the few Chinese physicists who made significant contributions to the early development of quantum mechanics.One of his representative works is the study on the van der Waals potential based on quantum mechanics.Specifically,using the second-order perturbation theory in quantum mechanics,he derived a long-range attractive potential of the form−1/R6 between two widely separated atoms.Since individual atoms are non-polar,meaning their average dipole moments are zero,this interaction arises from fluctuations in the instantaneous electric dipole moments of the two atoms.展开更多
Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and c...Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and competition against the hydrogen evolution reaction hinder its practical implementation.To address these,the design of highly active catalysts is critical.Single-atom catalysts(SACs)have shown great potential because of their maximized atom utilization,but their limited stability and low metal loading restrict their performances.On the other hand,dual-atom catalysts(DACs)are atomic catalysts with two metal atoms nearby and offer enhanced electrocatalytic performances by aligning with the N≡N bond to enhance N2 reduction efficiency,potentially overcoming the limitations of SAC.This review discusses recent advances in SACs and more importantly DACs for ENRR,highlighting their advantages,limitations,and the need for advanced characterization techniques to better understand catalyst behavior.The review concludes by underscoring the importance of research to optimize these catalysts for efficient and sustainable nitrogen fixation.展开更多
Here we present a highly efficient protocol utilizing nickel-hydride hydrogen atom transfer catalysis for the regio-and enantioselective hydrofluorination of internal alkenes.This method efficiently assembles a wide a...Here we present a highly efficient protocol utilizing nickel-hydride hydrogen atom transfer catalysis for the regio-and enantioselective hydrofluorination of internal alkenes.This method efficiently assembles a wide array of enantioenrichedβ-fluoro amides with excellent regio-and enantioselectivity from internal unactivated alkenes.Mechanistic investigations suggest that this transformation proceeds via a NiHhydrogen atom transfer to alkene,followed by a stereoselective fluorine atom transfer process.The weak coordination effect of the tethered amide group is identified as a crucial factor governing the observed regio-and enantioselectivity.展开更多
Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their p...Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their potential for achieving ultra-highκ,with BAs serving as a particularly representative example due to its unique combination of large bandgap and high thermal conductivity.In this paper,the efects of atomic mass modifcation on phonon bandgap andκare systematically investigated using a BAs model,accounting for both three-and four-phonon scattering processes.A 20%increase inκcan be obtained by substituting B,achieved through widening the phonon bandgap,which suppresses phonon scattering.Notably,the AAOO four-phonon scattering channel is more suppressed than the AAO three-phonon channel,leading to an increased phonon lifetime(τ).For As,κcan also be enhanced by 5%when replaced by lighter atoms,such as^(69)As,primarily due to the increased phonon group velocity(υ).We systematically clarify how atomic-mass-induced bandgap variations afectτ,υ,and thereforeκin wide-bandgap systems.Our work provides a specifc scheme for further improving the ultra-highκof materials with large bandgaps,which possesses great guiding signifcance.展开更多
A research team led by Prof.YANG Kai at the Institute of Physics(IOP),Chinese Academy of Sciences,in collaboration with Prof.FERNÁNDEZ-ROSSIER Joaquín from International Iberian Nanotechnology Laboratory,has...A research team led by Prof.YANG Kai at the Institute of Physics(IOP),Chinese Academy of Sciences,in collaboration with Prof.FERNÁNDEZ-ROSSIER Joaquín from International Iberian Nanotechnology Laboratory,has demonstrated all-electrical control of quantum interference in individual atomic spins on a surface,opening new possibilities for fast and robust quantum-state manipulation at the atomic scale.展开更多
Regulating the electronic structure and oxygencontaining intermediates adsorption behavior on Fe-based catalysts is of great significance to cope with the sluggish oxygen reduction reaction(ORR)kinetics,but it still r...Regulating the electronic structure and oxygencontaining intermediates adsorption behavior on Fe-based catalysts is of great significance to cope with the sluggish oxygen reduction reaction(ORR)kinetics,but it still remains a great challenge.In this work,Fe atom clusters(Fe_(AC))modified by high-density Cu single atoms(Cu_(SA))in a N,S-doped porous carbon substrate(Fe_(AC)/Cu_(SA)@NCS)is reported for enhanced ORR electrocatalysis.Fe_(AC)/Cu_(SA)@NCS exhibits excellent ORR performance with a half-wave potential(E_(1/2))of 0.911 V,a high four-electron process selectivity and excellent stability.The ORR performance is also verified in the Fe_(AC)/Cu_(SA)@NCS-based Zn-air battery,which shows a high peak power density of 192.67 mW cm^(-2),a higher specific capacity of 808.3 mAh g^(-1)and impressive charge-discharge cycle stability.Moreover,density functional theory calculations show that Cu single atoms synergistically modulate the electronic structure Fe active atoms in Fe atomic clusters,reducing the energy barrier of the rate-determining step(i.e.,*OH desorption)on Fe_(AC)/Cu_(SA)@NCS.This work provides an effective way to regulate the electronic structure of Fe-based catalysts and optimize their electrocatalytic activity based on the introduction of a second metal source.展开更多
Heteroatom doping is a promising strategy for designing cost-effective and stable electrocatalysts toward the oxygen evolution reaction(OER),but the enhancement mechanism remains unclear.Herein,atomic Ir-O-Cu and Ir-O...Heteroatom doping is a promising strategy for designing cost-effective and stable electrocatalysts toward the oxygen evolution reaction(OER),but the enhancement mechanism remains unclear.Herein,atomic Ir-O-Cu and Ir-O-Ir motifs are engineered into CuO nanowires via cation exchange and dehydration to elucidate the OER mechanism.Systematic characterizations confirm the atomic dispersion of Ir within the CuO lattice and the electron transfer from Ir to CuO while preserving the host structure.The asprepared single-atom Ir-doped CuO(IrSA-CuO),featuring predominant Cu-O-Ir motifs and coexisting IrO-Ir motifs,achieves a low OER overpotential of 204 mV at 10 mA cm^(-2)in 1 M KOH,coupled with a 69-fold higher mass activity than commercial IrO_(2).Furthermore,the Ir_(SA)-CuO maintains long-term stability for 300 h at 200 mA cm^(-2)with minimal overpotential alteration and an additional 120 h at500 mA cm^(-2)with overpotential increased by 15 mV.In situ Raman spectroscopy reveals that the Ir-O-Ir motifs suppress Cu^(Ⅱ) oxidation to Cu^(Ⅲ) by delaying the onset potential,enhancing the structural stability during OER.Density functional theory calculations demonstrate the Cu-O-Ir motifs lower the adsorption energy of bridged ^(*)O via asymmetric bonding,accelerating ^(*)OOH formation in the ratedetermining step.This work presents a heteroatom engineering strategy to balance electrocatalytic activity and durability,providing a blueprint for industrial electrocatalyst design.展开更多
基金supported by the Beijing Natural Science Foundation(Grant No.3252013)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0300402)+1 种基金the National Natural Science Foundation of China(Grant No.61673041)Key Area Research and Development Program of Guangdong Province(Grant No.2021B0101410005)。
文摘Atomic spin gyroscopes are promising candidates for next-generation inertial navigation due to extremely high theoretical precision,relatively small size among atomic gyroscopes,and promising potential for miniaturization.In particular,the spin-exchange relaxation-free(SERF)atomic gyroscope relies on optical pumping to polarize atoms,enabling rotation sensing through the Faraday optical rotation angle(FORA).However,fluctuations in atomic density introduce systematic errors in FORA measurements,limiting long-term stability.We present a data-driven decoupling method that isolates atomic density fluctuations from the FORA signal by modeling spatially resolved light absorption in the vapor cell.The model accounts for the spatial distribution of spin polarization in the pump-light interaction volume,density-dependent relaxation rates,wall-induced relaxation,and polarization diffusion,and is implemented within a finite-element framework.Compared to the conventional Lambert-Beer law,which assumes one-dimensional homogeneity,our approach captures the full threedimensional density and polarization distribution,significantly improving the accuracy of light absorption modeling.The resulting absorption-density maps are used to train a feedforward neural network,yielding a high-precision estimator for atomic density fluctuations.This estimator enables the construction of a decoupling equation that separates the density contribution from the FORA signal.Experimental validation shows that this method improves the bias instability atσ(100 s)of the gyroscope was improved by 73.1%compared to traditional platinum-resistance-based stabilization.The proposed framework is general and can be extended to other optical pumping-based sensors,such as optically pumped magnetometers.
基金supported by the National Key R&D Program of China (2021YFA1502802)the National Natural Science Foundation of China (U21B2092, 22202213, 22402210, 22502215, 22502214, 22572200, and 22579171)+3 种基金the International Partnership Program of Chinese Academy of Sciences (172GJHZ2022028MI)the Shenyang Bureau of Science and Technology (24-213-3-25)the Natural Science Foundation of Liaoning Province (2025BS0153)Zhongke Technology Achievement Transfer and Transformation Center of Henan Province 2025119
文摘Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.
基金supported by the National Natural Science Foundation of China[Grant No.21977083].
文摘The single-atom replacement strategy is a typical approach which just converts elements in lead compounds into their analogues with very small chemical changes.In this research,we implemented this strategy to modify the sulfonamide scaffold identified in our previous work,and resulting in the synthesis of 40 novel sulfonamide derivatives not previously reported in the literature.The insecticidal activities of these compounds against the Mythimna separata and Plutella xylostella were assessed.Our findings indicate that the pyridine sulfonamide structure significantly enhances insecticidal efficacy.Specifically,compound 7c exhibited LC 50 values of 0.157 and 0.256 mg/mL against the M.separata and P.xylostella,which significantly increased 97-and 41-fold compared to celangulin V,respectively.The experimental results revealed that pyridine sulfonamide analogues could serve as potential green insecticides.
基金supported by the National Natural Science Foundation of China(Nos.22406081,22276086,22306086)the Natural Science Foundation of Jiangxi Province(No.20232BAB213029),all of which are greatly acknowledged by the authors.
文摘Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibited very high performance in peroxymonosulfate activation.The Fe single-atom filled an N vacancy on the triazine ring edge of C_(3)N_(4),as confirmed through X-ray absorption fine structure,density functional calculation and elec-tron paramagnetic resonance.The SAFe_(0.4)–C_(3)N_(4)/PMS system could completely remove phenol(20 mg/L)within 10 min and its first-order kinetic constant was 12.3 times that of the Fe_(3)O_(4)/PMS system.Under different ini-tial pH levels and in various anionic environments,SAFe_(0.4)–C_(3)N_(4) still demonstrated excellent catalytic activity,achieving a removal rate of over 90%for phenol within 12 min.In addition,SAFe_(0.4)–C_(3)N_(4) exhibited outstanding selectivity in reaction systems with different pollutants,showing excellent degradation effects on electron-rich pollutants only.Hydroxyl radicals(•OH),singlet oxygen(1O_(2))and high-valent iron oxide(Fe(Ⅳ)=O)were de-tected in the SAFe_(0.4)–C_(3)N_(4)/PMS system through free radical capture experiments.Further experiments on the quenching of active species and a methyl phenyl sulfoxide probe confirmed that 1O_(2) and Fe(Ⅳ)=O played dom-inant roles.Additionally,the change in the current response after adding PMS and phenol in succession proved that a direct electron transfer path between organic matter and the catalyst surface was unlikely to exist in the SAFe_(0.4)–C_(3)N_(4)/PMS/Phenol degradation system.This study provides a new demonstration of the catalytic mech-anism of single-atom catalysts.
基金supported by the National Natural Science Foundation of China(52402166)the Science and Technology Development Fund+2 种基金Macao SAR(0065/2023/AFJ,0116/2022/A3)the Australian Research Council(DE220100154)the Natural Science Foundation of Guangdong Province(2025A1515011120)。
文摘The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulate the electronic structure of MoS_(2),thereby obtaining a multifunctional catalyst that serves as an efficient sulfur host.The W/V dual single-atomdoped MoS_(2)grown on carbon nanofibers(CMWVS)demonstrates a strong adsorption ability for lithium polysulfides,suppressing the shuttle effects.Additionally,the doping process also results in the phase transition from 2H-MoS_(2)to 1T-MoS_(2)and generates sufficient edge sulfur atoms,promoting the charge/electron transfer and enriching the reaction sites.All these merits contribute to the superior conversion reaction kinetics,leading to the outstanding Li-S battery performance.When fabricated as cathodes by compositing with sulfur,the CMWVS/S cathode delivers a high capacity of 1481.7 mAh g^(-1)at 0.1 C(1 C=1672 mAh g^(-1))and maintains 816.3 m Ah g^(-1)after 1000 cycles at 1.0 C,indicating outstanding cycling stability.Even under a high sulfur loading of 7.9 mg cm^(-2)and lean electrolyte conditions(E/S ratio of 9.0μL mg^(-1)),the cathode achieves a high areal capacity of 8.2 m Ah cm^(-2),showing great promise for practical Li-S battery applications.This work broadens the scope of doping strategies in transition-metal dichalcogenides by tailoring their electronic structures,providing insightful direction for the rational development of high-efficiency electrocatalysts for advanced Li-S battery applications.
基金Project supported by the National Natural Science Foundation of China(Grant No.62471180)。
文摘We propose a novel cooling protocol within a triple-Laguerre-Gaussian cavity optomechanical system,which is designed to suppress the thermal vibrations of a rotating mirror to reach its quantum ground state.The system incorporates two auxiliary cavities and an atomic ensemble coupled to a Laguerre-Gaussian rotational cavity.By carefully selecting system parameters,the cooling process of the rotating mirror is significantly enhanced,while the heating process is effectively suppressed,enabling efficient ground-state cooling even in the unresolved sideband regime.Compared to previous works,our scheme reduces the stringent restrictions on auxiliary systems,making it more experimentally feasible under broader parameter conditions.These findings provide a robust approach for achieving ground-state cooling in mechanical resonators.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.62331024 and 62571549)the National Key Research and Development Program of China(Grant No.2022YFB2802804)。
文摘Rydberg-atom-based superheterodyne receivers integrate self-calibration,high sensitivity,a wide operational frequency range,and phase/frequency resolved detection capabilities,demonstrating broad application prospects as nextgeneration microwave receivers.Linear gain and linear dynamic range(LDR)are critical metrics for assessing receiver sensitivity and demodulation fidelity,respectively.We numerically solve the four-level master equation and then employ particle swarm optimization(PSO)algorithm to co-optimize linear gain and LDR in atomic superheterodyne receivers based on balanced homodyne detection.Further,we systematically account for dominant dephasing mechanisms in the simulation,encompassing spontaneous decay,transit dephasing,collision dephasing,laser linewidth dephasing,and Doppler averaging.Homodyne readout utilizes both the real and imaginary parts of polarizability for sensing.In the case of the photon shot noise limit,its signal-to-noise ratio(SNR)expression resembles that of direct optical-intensity readout.However,the inherent coherent subtraction operation in homodyne detection significantly suppresses common-mode noise,while appropriately increasing the reference beam power enhances the gain in practical experiments.Indeed,this co-optimization problem,characterized by a high-dimensional variable space,two objectives,and non-convexity,is well-suited for solution by PSO.In addition,probe and coupling detuning contribute equivalently to polarizability and compensate for each other owing to Doppler averaging,thereby reducing the optimization variable space by one.By adopting a product form of linear gain and LDR as the fitness function,the PSO achieves rapid convergence.Here,the effectiveness of the PSO results is verified via the total harmonic distortion(THD).The relative error-based LDR calculation method we proposed efficiently measures receiver response linearity with consuming fewer computational resources.This research is expected to offer valuable insights into enhancing the performance of Rydberg-atom-based superheterodyne receivers.
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)。
文摘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-N_(x) site activity and accessibility.The TiNC/Fe-NC catalyst achieves outstanding ORR performances,with half-wave potentials(E_(1/2))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-N_(x) 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 E_(1/2) 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supported by the Samsung Electronics Co.,Ltd.(ISO230414-05954-01)Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(NRF2021R1A6A1A03039981)+2 种基金the Korea Institute for Advancement of Technology(KIAT)Grant,funded by the Korea Government(MOTIE)(P0023703,HRD Program for Industrial Innovation)The computations were performed at the Korea Institute of Science and Technology Information(KISTI)National Supercomputing Center(KSC-2024-CRE-0316)the UNIST Supercomputing Center。
文摘Atomic layer deposition(ALD)is extensively used to fabricate doped dielectrics due to its ability to deposit conformal films with atomic-scale thickness control.Al-doped TiO_(2)(ATO)is a promising high-k dielectric for dynamic random access memory(DRAM)applications,offering a high dielectric constant with a remarkable leakage-lowering effect by Al acceptor doping.However,ATO fabrication via conventional supercycle-based ALD suffers from severe crystallinity loss during the growth of TiO_(2) upon Al doping owing to the dopant-induced lattice disorder.In addition,Al doping cannot reduce any inherent O vacancies(V_(O))of TiO_(2),although the original purpose of doping was to address the n-type nature caused by V_(O).To resolve these limitations,we propose a single-step,in-situ Ar/O_(2) post-doping plasma(PDP)process immediately after the Al dopant incorporation.Using the PDP process,simultaneous atomic-scale dopant migration-mediated crystallization and V_(O) annihilation were successfully initiated.Thus,the surface concentration of the dopant decreased,reducing the dopant-induced lattice distortion,while promoting the highly crystallized seed layer-like surface.Consequently,strong rutile-phase recovery was accompanied by enhanced lattice-matched growth.In addition,the PDP process significantly lowers the V_(O)-to-lattice oxygen ratio by facilitating the recombination between reactive O species and V_(O),increasing the corresponding 0.4 e V of conduction band offset(CBO).Despite the common trade-off between the dielectric constant and leakage,the Pt/PDP-ATO/Ru capacitor exhibited a simultaneous 30%increase in dielectric constant and up to a 1.6-order reduction in leakage current density.
基金supported by Natural Science Foundation of China(Nos.U23B20165 and 52170085)National Key R&D Program International Cooperation Project(No.2023YFE0108100)+1 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Fundamental Research Funds for the Central Universities,Nankai University.
文摘Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g-C_(3)N_(4) heterojunctions to improve process cost-effectiveness.The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction demonstrated an effective removal of 93.6%thiamphenicol(TAP)within 45 min,with the rate constant(0.0584 min^(-1))that was 2.4 and 2.8 times that of Co_(3)O_(4) and g-C_(3)N_(4) alone,respectively.The formation of heterojunctions facilitated electron transfer,enriched the electron density on Co_(3)O_(4),and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates.The enhanced production of atomic hydrogen(H*)of Co_(3)O_(4)/g-C_(3)N_(4),which increased by 13.6-28.2 times,contributed more to pollutant removal(64.0%),much higher than that of Co_(3)O_(4)(37.3%)and g-C_(3)N_(4)(6.1%).The energy barrier for H_(2) formation on Co_(3)O_(4)/g-C_(3)N_(4)(0.75 eV)was higher than that on Co_(3)O_(4)(-1.84 eV),supporting that it could stabilize H*and inhibit the formation of H_(2).The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction exhibited stable performance with less impact by pH and co-existing ions,and posed effectiveness for the dechlorination of typical chlorinated antibiotics.This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.
文摘Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)and stability(longevity)remains challenging,as the interplay between metal atoms,supports,and reactants is poorly understood.
基金the Tangshan University Doctor Innovation Fund(Project Number:1402306).
文摘The so-called close-coupled gas atomization process involves melting a metal and using a high-pressure gas jet positioned close to the melt stream to rapidly break it into fine,spherical powder particles.This technique,adapted for blast furnace slag granulation using a circular seam nozzle,typically aims to produce solid slag particles sized 30–140μm,thereby allowing the utilization of slag as a resource.This study explores the atomization dynamics of liquid blast furnace slag,focusing on the effects of atomization pressure.Primary atomization is simulated using a combination of the Volume of Fluid(VOF)method and the Shear Stress Transport k-ωturbulence model,while secondary atomization is analyzed through the Discrete Phase Model(DPM).The results reveal that primary atomization progresses in three stages:the slag column transforms into an umbrella-shaped liquid film,whose leading edge fragments into particles while forming a cavity-like structure,which is eventually torn into ligaments.This primary deformation is driven by the interplay of airflow velocity in the recirculation zone and the guide tube outlet pressure(Fp).Increasing the atomization pressure amplifies airflow velocity,recirculation zone size,expansion and shock waves,though the guide tube outlet pressure variations remain irregular.Notably,at 4.5 MPa,the primary deformation is most pronounced.Secondary atomization yields finer slag particles as a result of more vigorous primary atomization.For this pressure,the smallest average particle size and the highest yield of particles within the target range(30–140μm)are achieved.
基金supported by the National Key Research and Development Program of China(2022YFA1505700)National Natural Science Foundation of China(22475214 and 22205232)+2 种基金Talent Plan of Shanghai Branch,Chinese Academy of Sciences(CASSHB-QNPD-2023-020)Natural Science Foundation of Fujian Province(2023J06044)the Self-deployment Project Research Program of Haixi Institutes,Chinese Academy of Sciences(CXZX-2022-JQ06 and CXZX-2022-GH03)。
文摘Aberration-corrected annular dark-field scanning transmission electron microscopy(ADF-STEM)is a powerful tool for structural and chemical analysis of materials.Conventional analyses of ADF-STEM images rely on human labeling,making them labor-intensive and prone to subjective error.Here,we introduce a deep-learning-based workflow combining a pix2pix network for image denoising and either a mathematical algorithm local intensity threshold segmentation(LITS)or another deep learning network UNet for chemical identification.After denoising,the processed images exhibit a five-fold improvement in signal-to-noise ratio and a 20%increase in accuracy of atomic localization.Then,we take atomic-resolution images of Y–Ce dual-atom catalysts(DACs)and Fe-doped ReSe_(2) nanosheets as examples to validate the performance.Pix2pix is applied to identify atomic sites in Y–Ce DACs with a location recall of 0.88 and a location precision of 0.99.LITS is used to further differentiate Y and Ce sites by the intensity of atomic sites.Furthermore,pix2pix and UNet workflow with better automaticity is applied to identification of Fe-doped ReSe_(2) nanosheets.Three types of atomic sites(Re,the substitution of Fe for Re,and the adatom of Fe on Re)are distinguished with the identification recall of more than 0.90 and the precision of higher than 0.93.These results suggest that this strategy facilitates high-quality and automated chemical identification of atomic-resolution images.
文摘Translator’s Note:Shou Chin Wang(Wang Shoujing)was one of the few Chinese physicists who made significant contributions to the early development of quantum mechanics.One of his representative works is the study on the van der Waals potential based on quantum mechanics.Specifically,using the second-order perturbation theory in quantum mechanics,he derived a long-range attractive potential of the form−1/R6 between two widely separated atoms.Since individual atoms are non-polar,meaning their average dipole moments are zero,this interaction arises from fluctuations in the instantaneous electric dipole moments of the two atoms.
基金supported by the National Research Foundation of Korea(2022R1C1C2005786,RS-2023-00256106,RS-2023-00207831,RS-2024-00346153).
文摘Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and competition against the hydrogen evolution reaction hinder its practical implementation.To address these,the design of highly active catalysts is critical.Single-atom catalysts(SACs)have shown great potential because of their maximized atom utilization,but their limited stability and low metal loading restrict their performances.On the other hand,dual-atom catalysts(DACs)are atomic catalysts with two metal atoms nearby and offer enhanced electrocatalytic performances by aligning with the N≡N bond to enhance N2 reduction efficiency,potentially overcoming the limitations of SAC.This review discusses recent advances in SACs and more importantly DACs for ENRR,highlighting their advantages,limitations,and the need for advanced characterization techniques to better understand catalyst behavior.The review concludes by underscoring the importance of research to optimize these catalysts for efficient and sustainable nitrogen fixation.
基金This research was made possible as a result of a generous grant from the Fundamental Research Funds for the Central Universities(Nos.2232024Y-01,2232024A-03)the National Science Fund for Excellent Young Scholars(No.22122101).
文摘Here we present a highly efficient protocol utilizing nickel-hydride hydrogen atom transfer catalysis for the regio-and enantioselective hydrofluorination of internal alkenes.This method efficiently assembles a wide array of enantioenrichedβ-fluoro amides with excellent regio-and enantioselectivity from internal unactivated alkenes.Mechanistic investigations suggest that this transformation proceeds via a NiHhydrogen atom transfer to alkene,followed by a stereoselective fluorine atom transfer process.The weak coordination effect of the tethered amide group is identified as a crucial factor governing the observed regio-and enantioselectivity.
基金supported by the National Key Research and Development Program of China(Grant No.2023YFA1407001)the Department of Science and Technology of Jiangsu Province(Grant No.BK20220032)+1 种基金support from the Guang Dong Basic and Applied Basic Research Foundation(Grant No.2023A1515010365)support from the Postgraduate Research and Practice Innovation Program of Jiangsu Province under Grant No.KYCX25_1934。
文摘Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their potential for achieving ultra-highκ,with BAs serving as a particularly representative example due to its unique combination of large bandgap and high thermal conductivity.In this paper,the efects of atomic mass modifcation on phonon bandgap andκare systematically investigated using a BAs model,accounting for both three-and four-phonon scattering processes.A 20%increase inκcan be obtained by substituting B,achieved through widening the phonon bandgap,which suppresses phonon scattering.Notably,the AAOO four-phonon scattering channel is more suppressed than the AAO three-phonon channel,leading to an increased phonon lifetime(τ).For As,κcan also be enhanced by 5%when replaced by lighter atoms,such as^(69)As,primarily due to the increased phonon group velocity(υ).We systematically clarify how atomic-mass-induced bandgap variations afectτ,υ,and thereforeκin wide-bandgap systems.Our work provides a specifc scheme for further improving the ultra-highκof materials with large bandgaps,which possesses great guiding signifcance.
基金supported by the National Natural Science Foundation of Chinathe Beijing Natural Science Foundationthe National Key R&D Program of China,and the Chinese Academy of Sciences.
文摘A research team led by Prof.YANG Kai at the Institute of Physics(IOP),Chinese Academy of Sciences,in collaboration with Prof.FERNÁNDEZ-ROSSIER Joaquín from International Iberian Nanotechnology Laboratory,has demonstrated all-electrical control of quantum interference in individual atomic spins on a surface,opening new possibilities for fast and robust quantum-state manipulation at the atomic scale.
基金financially supported by the National Natural Science Foundation of China(No.22278042)the National Natural Science Foundation of Jiangsu Province(No.BK20240567)+2 种基金the Introduction and Cultivation of Leading Innovative Talents Foundation of Changzhou,Jiangsu Province(No.CQ20220093)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(No.24KJD530001)the Open Project Program of Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science(No.M2024-7),MOE
文摘Regulating the electronic structure and oxygencontaining intermediates adsorption behavior on Fe-based catalysts is of great significance to cope with the sluggish oxygen reduction reaction(ORR)kinetics,but it still remains a great challenge.In this work,Fe atom clusters(Fe_(AC))modified by high-density Cu single atoms(Cu_(SA))in a N,S-doped porous carbon substrate(Fe_(AC)/Cu_(SA)@NCS)is reported for enhanced ORR electrocatalysis.Fe_(AC)/Cu_(SA)@NCS exhibits excellent ORR performance with a half-wave potential(E_(1/2))of 0.911 V,a high four-electron process selectivity and excellent stability.The ORR performance is also verified in the Fe_(AC)/Cu_(SA)@NCS-based Zn-air battery,which shows a high peak power density of 192.67 mW cm^(-2),a higher specific capacity of 808.3 mAh g^(-1)and impressive charge-discharge cycle stability.Moreover,density functional theory calculations show that Cu single atoms synergistically modulate the electronic structure Fe active atoms in Fe atomic clusters,reducing the energy barrier of the rate-determining step(i.e.,*OH desorption)on Fe_(AC)/Cu_(SA)@NCS.This work provides an effective way to regulate the electronic structure of Fe-based catalysts and optimize their electrocatalytic activity based on the introduction of a second metal source.
基金supported by the Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China(No.2021ZR124)。
文摘Heteroatom doping is a promising strategy for designing cost-effective and stable electrocatalysts toward the oxygen evolution reaction(OER),but the enhancement mechanism remains unclear.Herein,atomic Ir-O-Cu and Ir-O-Ir motifs are engineered into CuO nanowires via cation exchange and dehydration to elucidate the OER mechanism.Systematic characterizations confirm the atomic dispersion of Ir within the CuO lattice and the electron transfer from Ir to CuO while preserving the host structure.The asprepared single-atom Ir-doped CuO(IrSA-CuO),featuring predominant Cu-O-Ir motifs and coexisting IrO-Ir motifs,achieves a low OER overpotential of 204 mV at 10 mA cm^(-2)in 1 M KOH,coupled with a 69-fold higher mass activity than commercial IrO_(2).Furthermore,the Ir_(SA)-CuO maintains long-term stability for 300 h at 200 mA cm^(-2)with minimal overpotential alteration and an additional 120 h at500 mA cm^(-2)with overpotential increased by 15 mV.In situ Raman spectroscopy reveals that the Ir-O-Ir motifs suppress Cu^(Ⅱ) oxidation to Cu^(Ⅲ) by delaying the onset potential,enhancing the structural stability during OER.Density functional theory calculations demonstrate the Cu-O-Ir motifs lower the adsorption energy of bridged ^(*)O via asymmetric bonding,accelerating ^(*)OOH formation in the ratedetermining step.This work presents a heteroatom engineering strategy to balance electrocatalytic activity and durability,providing a blueprint for industrial electrocatalyst design.
