Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reactio...Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reaction(HOR).Herein,we describe the synthesis of a Pt single electrocatalyst inside single-walled carbon nanotubes(SWCNTs)via a redox reaction.Characterizations via electron microscopy,X-ray photoelectron microscopy,and X-ray absorption spectroscopy show the single-atom nature of the Pt.The electrochemical behavior of the sample to hydrogen and oxygen was investigated using the advanced floating electrode technique,which minimizes mass transport limitations and gives a thorough insight into the activity of the electrocatalyst.The single-atom samples showed higher HOR activity than state-of-the-art 30%Pt/C while almost no oxygen reduction reaction activity in the proton exchange membrane fuel cell operating range.The selective activity toward HOR arose as the main fingerprint of the catalyst confinement in the SWCNTs.展开更多
Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further de...Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.展开更多
Single-atom catalysts(SACs)are gaining popularity in catalytic reactions due to their nearly 100%atomic utilization and defined active sites,which provide great convenience for studying the catalytic mechanism of cata...Single-atom catalysts(SACs)are gaining popularity in catalytic reactions due to their nearly 100%atomic utilization and defined active sites,which provide great convenience for studying the catalytic mechanism of catalysts.However,SACs still present challenges such as complex formation processes,low loading and easy agglomeration of catalysts.Herein,we systematically discuss the synthesis methods for SACs,including coprecipitation,impregnation,atomic layer deposition,pyrolysis and Anti-Ostwald ripening etc.Various techniques for characterizing single-atom catalysts(SACs)are described in detail.The utilization of individual atoms in various photocatalytic reactions and their mechanisms of action in different reactions are explained.The purpose of this review is to introduce single-atom synthesis methods,characterization techniques,specific catalytic action and their applications in the direction of photocatalysis,and to provide a reference for the industrialization of photocatalytic single-atoms,which is currently impossible,in the hope of promoting further development of photocatalytic single-atoms.展开更多
Single atom catalysts(SACs)have garnered significant attention in the field of catalysis over the past decade due to their exceptional atom utilization efficiency and distinct physical and chemical properties.For the ...Single atom catalysts(SACs)have garnered significant attention in the field of catalysis over the past decade due to their exceptional atom utilization efficiency and distinct physical and chemical properties.For the semiconductor-based electrical gas sensor,the core is the catalysis process of target gas molecules on the sensitive materials.In this context,the SACs offer great potential for highly sensitive and selective gas sensing,however,only some of the bubbles come to the surface.To facilitate practical applications,we present a comprehensive review of the preparation strategies for SACs,with a focus on overcoming the challenges of aggregation and low loading.Extensive research efforts have been devoted to investigating the gas sensing mechanism,exploring sensitive materials,optimizing device structures,and refining signal post-processing techniques.Finally,the challenges and future perspectives on the SACs based gas sensing are presented.展开更多
The photostability of a colloidal single photon emitter in near-infrared regime at room temperature is investigated.The fluorescence lifetime,blinking phenomenon,and anti-bunching effect of a single CdTeSe/ZnS quantum...The photostability of a colloidal single photon emitter in near-infrared regime at room temperature is investigated.The fluorescence lifetime,blinking phenomenon,and anti-bunching effect of a single CdTeSe/ZnS quantum dot with an emission wavelength of 800 nm at room temperature are studied.The second-order correlation function at zero delay time is much smaller than 0.1,which proves that the emission from single quantum dots at 800 nm is a highly pure single-photon source.The effects of the irradiation duration on the fluorescence from single quantum dots are analyzed.The experimental results can be explained by a recombination model including a multi-nonradiative recombination center model and a multi-charged model.展开更多
High-purity copper(Cu) with excellent thermal and electrical conductivity, is crucial in modern technological applications, including heat exchangers, integrated circuits, and superconducting magnets. The current puri...High-purity copper(Cu) with excellent thermal and electrical conductivity, is crucial in modern technological applications, including heat exchangers, integrated circuits, and superconducting magnets. The current purification process is mainly based on the zone/electrolytic refining or anion exchange, however, which excessively relies on specific integrated equipment with ultra-high vacuum or chemical solution environment, and is also bothered by external contaminants and energy consumption. Here we report a simple approach to purify the Cu foils from 99.9%(3N) to 99.99%(4N) by a temperature-gradient thermal annealing technique, accompanied by the kinetic evolution of single crystallization of Cu.The success of purification mainly relies on(i) the segregation of elements with low effective distribution coefficient driven by grain-boundary movements and(ii) the high-temperature evaporation of elements with high saturated vapor pressure.The purified Cu foils display higher flexibility(elongation of 70%) and electrical conductivity(104% IACS) than that of the original commercial rolled Cu foils(elongation of 10%, electrical conductivity of ~ 100% IACS). Our results provide an effective strategy to optimize the as-produced metal medium, and therefore will facilitate the potential applications of Cu foils in precision electronic products and high-frequency printed circuit boards.展开更多
Ultrasonic-assisted micro-electro-discharge machining(EDM)has the potential to enhance processing responses such as material removal rate(MRR)and surface finish.To understand the reasons for this enhancement,the physi...Ultrasonic-assisted micro-electro-discharge machining(EDM)has the potential to enhance processing responses such as material removal rate(MRR)and surface finish.To understand the reasons for this enhancement,the physical mechanisms responsible for the individual discharges and the craters that they form need to be explored.This work examines features of craters formed by single discharges at various parameter values in both conventional and ultrasonic-assistedEDM of Ti6Al4V.High-speed imaging of the plasma channel is performed,and data on the individual discharges are captured in real-time.A 2D axisymmetric model using finite element software is established to model crater formation.On the basis of simulation and experimental results,a comparative study is then carried out to examine the effects of ultrasonic vibrational assistance on crater geometry.For every set ofEDM parameters,the crater diameter and depth from a single discharge are found to be higher in ultrasonic-assistedEDM than in conventionalEDM.The improved crater geometry and the reduced bulge formation at the crater edges are attributed to the increased melt pool velocity and temperature predicted by the model.展开更多
In paper[Chin.Phys.B 32070308(2023)],Xing et al.proposed a semi-quantum secret sharing protocol by using single particles.We study the security of the proposed protocol and find that it is not secure,that is,the three...In paper[Chin.Phys.B 32070308(2023)],Xing et al.proposed a semi-quantum secret sharing protocol by using single particles.We study the security of the proposed protocol and find that it is not secure,that is,the three dishonest agents,Bob,Charlie and Emily can collude to obtain Alice's secret without the help of David.展开更多
We demonstrated a scheme of phase-locked terahertz quantum cascade lasers(THz QCLs)array,with a single-mode pulse power of 108 mW at 13 K.The device utilizes a Talbot cavity to achieve phase locking among five ridge l...We demonstrated a scheme of phase-locked terahertz quantum cascade lasers(THz QCLs)array,with a single-mode pulse power of 108 mW at 13 K.The device utilizes a Talbot cavity to achieve phase locking among five ridge lasers with first-order buried distributed feedback(DFB)grating,resulting in nearly five times amplification of the single-mode power.Due to the optimum length of Talbot cavity depends on wavelength,the combination of Talbot cavity with the DFB grating leads to better power amplification than the combination with multimode Fabry-Perot(F-P)cavities.The Talbot cavity facet reflects light back to the ridge array direction and achieves self-imaging in the array,enabling phase-locked operation of ridges.We set the spacing between adjacent elements to be 220μm,much larger than the free-space wavelength,ensuring the operation of the fundamental supermode throughout the laser's dynamic range and obtaining a high-brightness far-field distribution.This scheme provides a new approach for enhancing the single-mode power of THz QCLs.展开更多
Single-atom(SA)catalysts with nearly 100%atom utilization have been widely employed in electrolysis for decades,due to the outperforming catalytic activity and selectivity.However,most of the reported SA catalysts are...Single-atom(SA)catalysts with nearly 100%atom utilization have been widely employed in electrolysis for decades,due to the outperforming catalytic activity and selectivity.However,most of the reported SA catalysts are fixed through the strong bonding between the dispersed single metallic atoms with nonmetallic atoms of the substrates,which greatly limits the controllable regulation of electrocatalytic activity of SA catalysts.In this work,Pt-Ni bonded Pt SA catalyst with adjustable electronic states was successfully constructed through a controllable electrochemical reduction on the coordination unsaturated amorphous Ni(OH)_(2)nanosheet arrays.Based on the X-ray absorption fine structure analysis and first-principles calculations,Pt SA was bonded with Ni sites of amorphous Ni(OH)_(2),rather than conventional O sites,resulting in negatively charged Pt^(δ-).In situ Raman spectroscopy revealed that the changed configuration and electronic states greatly enhanced absorbability for activated hydrogen atoms,which were the essential intermediate for alkaline hydrogen evolution reaction.The hydrogen spillover process was revealed from amorphous Ni(OH)_(2)that effectively cleave the H-O-H bond of H_(2)O and produce H atom to the Pt SA sites,leading to a low overpotential of 48 mV in alkaline electrolyte at-1000 mA cm^(-2)mg^(-1)_(Pt),evidently better than commercial Pt/C catalysts.This work provided new strategy for the control-lable modulation of the local structure of SA catalysts and the systematic regulation of the electronic states.展开更多
Nickel(Ni)-rich cathode materials have become promising candidates for the next-generation electrical vehicles due to their high specific capacity.However,the poor thermodynamic stability(including cyclic performance ...Nickel(Ni)-rich cathode materials have become promising candidates for the next-generation electrical vehicles due to their high specific capacity.However,the poor thermodynamic stability(including cyclic performance and safety performance or thermal stability)will restrain their wide commercial application.Herein,a single-crystal Ni-rich Li Ni_(0.83)Co_(0.12)Mn_(0.05)O_(2) cathode material is synthesized and modified by a dual-substitution strategy in which the high-valence doping element improves the structural stability by forming strong metal–oxygen binding forces,while the low-valence doping element eliminates high Li^(+)/Ni^(2+)mixing.As a result,this synergistic dual substitution can effectively suppress H2-H3 phase transition and generation of microcracks,thereby ultimately improving the thermodynamic stability of Ni-rich cathode material.Notably,the dual-doped Ni-rich cathode delivers an extremely high capacity retention of 81%after 250 cycles(vs.Li/Li+)in coin-type half cells and 87%after 1000 cycles(vs.graphite/Li^(+))in pouch-type full cells at a high temperature of 55℃.More impressively,the dual-doped sample exhibits excellent thermal stability,which demonstrates a higher thermal runaway temperature and a lower calorific value.The synergetic effects of this dual-substitution strategy pave a new pathway for addressing the critical challenges of Ni-rich cathode at high temperatures,which will significantly advance the high-energy-density and high-safety cathodes to the subsequent commercialization.展开更多
The oxidation behavior of a novel Ni-based single-crystal 4774DD1 superalloy for industrial gas turbine applications was investigated by the isothermal oxidation at 980℃ and discontinuous oxidation weight gain method...The oxidation behavior of a novel Ni-based single-crystal 4774DD1 superalloy for industrial gas turbine applications was investigated by the isothermal oxidation at 980℃ and discontinuous oxidation weight gain methods.The phase constitution and morphology of surface oxides and the characteristics of the crosssection oxide film were analyzed by XRD,SEM and EDS.Results show that the oxidation kinetics of the 4774DD1 superalloy follows the cubic law,indicating its weak oxidation resistance at this temperature.As the oxidation time increases,the composition of the oxide film evolves as following:One layer consisting of a bottom Al_(2)O_(3)sublayer and an upper(Al_(2)O_(3)+NiO)mixture sublayer after oxidized for 25 h.Then,two layers composed of an outermost small NiO discontinuous grain layer and an internal layer for 75 h.This internal layer is consisted of the bottom Al_(2)O_(3)sublayer,an intermediate narrow CrTaO_(4)sublayer,and an upper(Al_(2)O_(3)+NiO)mixture sublayer.Also two layers comprising an outermost relative continuous NiO layer with large grain size and an internal layer as the oxidation time increases to 125 h.This internal layer is composed of the upper(Al_(2)O_(3)+NiO)mixture sublayer,an intermediate continuous(CrTaO_(4)+NiWO_(4))mixture sublayer,and a bottom Al_(2)O_(3)sublayer.Finally,three layers consisting of an outermost(NiAl2O_(4)+NiCr2O_(4))mixture layer,an intermediate(CrTaO_(4)+NiWO_(4))mixture layer,and a bottom Al_(2)O_(3)layer for 200 h.展开更多
Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and...Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of interaction.Herein,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery performance.The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic activity.Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.展开更多
The environmental contamination caused by antibiotics is increasingly conspicuous due to their widespread manufacture and misuse. Plasma has been employed in recent years for the remediation of antibiotic pollution in...The environmental contamination caused by antibiotics is increasingly conspicuous due to their widespread manufacture and misuse. Plasma has been employed in recent years for the remediation of antibiotic pollution in the environment. In this work, a falling-film dielectric barrier discharge was used to degrade the antibiotic tetracycline(TC) in water. The reactor combined the gas-liquid discharge and active gas bubbling to improve the TC degradation performance. The discharge characteristics, chemical species’ concentration, and degradation rates at different parameters were systematically studied. Under the optimized conditions(working gas was pure oxygen, liquid flow rate was 100 mL/min, gas flow rate was 1 L/min,voltage was 20 kV, single treatment), TC was removed beyond 70% in a single flow treatment with an energy efficiency of 145 mg/(kW·h). The reactor design facilitated gas and liquid flow in the plasma area to produce more ozone in bubbles after a single flow under pure oxygen conditions, affording fast TC degradation. Furthermore, long-term stationary experiment indicated that long-lived active species can sustain the degradation of TC. Compared with other plasma treatment systems, this work offers a fast and efficient degradation method, showing significant potential in practical industrial applications.展开更多
Plant morphogenesis relies on precise gene expression programs at the proper time and position which is orchestrated by transcription factors(TFs)in intricate regulatory networks in a cell-type specific manner.Here we...Plant morphogenesis relies on precise gene expression programs at the proper time and position which is orchestrated by transcription factors(TFs)in intricate regulatory networks in a cell-type specific manner.Here we introduced a comprehensive single-cell transcriptomic atlas of Arabidopsis seedlings.This atlas is the result of meticulous integration of 63 previously published scRNA-seq datasets,addressing batch effects and conserving biological variance.This integration spans a broad spectrum of tissues,including both below-and above-ground parts.Utilizing a rigorous approach for cell type annotation,we identified 47 distinct cell types or states,largely expanding our current view of plant cell compositions.We systematically constructed cell-type specific gene regulatory networks and uncovered key regulators that act in a coordinated manner to control cell-type specific gene expression.Taken together,our study not only offers extensive plant cell atlas exploration that serves as a valuable resource,but also provides molecular insights into gene-regulatory programs that varies from different cell types.展开更多
In dentistry, panoramic X-ray images are extensively used by dentists for tooth structure analysis and disease diagnosis. However, the manual analysis of these images is time-consuming and prone to misdiagnosis or ove...In dentistry, panoramic X-ray images are extensively used by dentists for tooth structure analysis and disease diagnosis. However, the manual analysis of these images is time-consuming and prone to misdiagnosis or overlooked. While deep learning techniques have been employed to segment teeth in panoramic X-ray images, accurate segmentation of individual teeth remains an underexplored area. In this study, we propose an end-to-end deep learning method that effectively addresses this challenge by employing an improved combinatorial loss function to separate the boundaries of adjacent teeth, enabling precise segmentation of individual teeth in panoramic X-ray images. We validate the feasibility of our approach using a challenging dataset. By training our segmentation network on 115 panoramic X-ray images, we achieve an intersection over union (IoU) of 86.56% for tooth segmentation and an accuracy of 65.52% in tooth counting on 87 test set images. Experimental results demonstrate the significant improvement of our proposed method in single tooth segmentation compared to existing methods.展开更多
Convolutional neural networks(CNNs) exhibit excellent performance in the areas of image recognition and object detection, which can enhance the intelligence level of spacecraft. However, in aerospace, energetic partic...Convolutional neural networks(CNNs) exhibit excellent performance in the areas of image recognition and object detection, which can enhance the intelligence level of spacecraft. However, in aerospace, energetic particles, such as heavy ions, protons, and alpha particles, can induce single event effects(SEEs) that lead CNNs to malfunction and can significantly impact the reliability of a CNN system. In this paper, the MNIST CNN system was constructed based on a 28 nm systemon-chip(SoC), and then an alpha particle irradiation experiment and fault injection were applied to evaluate the SEE of the CNN system. Various types of soft errors in the CNN system have been detected, and the SEE cross sections have been calculated. Furthermore, the mechanisms behind some soft errors have been explained. This research will provide technical support for the design of radiation-resistant artificial intelligence chips.展开更多
This study explores the application of single photon detection(SPD)technology in underwater wireless optical communication(UWOC)and analyzes the influence of different modulation modes and error correction coding type...This study explores the application of single photon detection(SPD)technology in underwater wireless optical communication(UWOC)and analyzes the influence of different modulation modes and error correction coding types on communication performance.The study investigates the impact of on-off keying(OOK)and 2-pulse-position modulation(2-PPM)on the bit error rate(BER)in single-channel intensity and polarization multiplexing.Furthermore,it compares the error correction performance of low-density parity check(LDPC)and Reed-Solomon(RS)codes across different error correction coding types.The effects of unscattered photon ratio and depolarization ratio on BER are also verified.Finally,a UWOC system based on SPD is constructed,achieving 14.58 Mbps with polarization OOK multiplexing modulation and 4.37 Mbps with polarization 2-PPM multiplexing modulation using LDPC code error correction.展开更多
We report the magnetotransport and thermal properties of RuAs_(2) single crystal.RuAs_(2) exhibits semiconductor behavior and localization effect.The crossover from normal state to diffusive transport in the weak loca...We report the magnetotransport and thermal properties of RuAs_(2) single crystal.RuAs_(2) exhibits semiconductor behavior and localization effect.The crossover from normal state to diffusive transport in the weak localization(WL)state and then to variable range hopping(VRH)transport in the strong localization state has been observed.The transitions can be reflected in the measurement of resistivity and Seebeck coefficient.Negative magnetoresistance(NMR)emerges with the appearance of localization effect and is gradually suppressed in high magnetic field.The temperature dependent phase coherence length extracted from the fittings of NMR also indicates the transition from WL to VRH.The measurement of Hall effect reveals an anomaly of temperature dependent carrier concentration caused by localization effect.Our findings show that RuAs_(2) is a suitable platform to study the localized state.展开更多
Quantum key distribution(QKD),rooted in quantum mechanics,offers information-theoretic security.However,practi-cal systems open security threats due to imperfections,notably bright-light blinding attacks targeting sin...Quantum key distribution(QKD),rooted in quantum mechanics,offers information-theoretic security.However,practi-cal systems open security threats due to imperfections,notably bright-light blinding attacks targeting single-photon detectors.Here,we propose a concise,robust defense strategy for protecting single-photon detectors in QKD systems against blinding attacks.Our strategy uses a dual approach:detecting the bias current of the avalanche photodiode(APD)to defend against con-tinuous-wave blinding attacks,and monitoring the avalanche amplitude to protect against pulsed blinding attacks.By integrat-ing these two branches,the proposed solution effectively identifies and mitigates a wide range of bright light injection attempts,significantly enhancing the resilience of QKD systems against various bright-light blinding attacks.This method forti-fies the safeguards of quantum communications and offers a crucial contribution to the field of quantum information security.展开更多
基金support from Horizon 2020 program within the ITN FlowcampDZ acknowledges funding from the Wohl Foundation for research for the promotion of UK-Israel research cooperationDZ acknowledges funding from Israel Ministry of Energy(grant#220-11-047).
文摘Utilizing supported single atoms as catalysts presents an opportunity to reduce the usage of critical raw materials such as platinum,which are essential for electrochemical reactions such as hydrogen oxidation reaction(HOR).Herein,we describe the synthesis of a Pt single electrocatalyst inside single-walled carbon nanotubes(SWCNTs)via a redox reaction.Characterizations via electron microscopy,X-ray photoelectron microscopy,and X-ray absorption spectroscopy show the single-atom nature of the Pt.The electrochemical behavior of the sample to hydrogen and oxygen was investigated using the advanced floating electrode technique,which minimizes mass transport limitations and gives a thorough insight into the activity of the electrocatalyst.The single-atom samples showed higher HOR activity than state-of-the-art 30%Pt/C while almost no oxygen reduction reaction activity in the proton exchange membrane fuel cell operating range.The selective activity toward HOR arose as the main fingerprint of the catalyst confinement in the SWCNTs.
基金support from the Shenzhen Science and Technology Program(No.KQTD20190929173914967,ZDSYS20220527171401003,and JCYJ20200109110416441).
文摘Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.
基金financially supported by the National Natural Science Foundation of China (22172044 and 22208048)Heilongjiang Provincial Natural Science Foundation of China (YQ2022B005 and YQ2022B001)+4 种基金the Young Elite Scientists Sponsorship Program by CAST (No.YESS20210262)the China Postdoctoral Science Foundation-Funded Project (No.2021M690571)the Heilongjiang Postdoctoral Fund (No.LBH-Z21096)the Provincial Natural Science Foundation Joint Guidance Project (No.LH2020F001)the Fundamental Research Funds for the Central Universities (No.2572023CT10)。
文摘Single-atom catalysts(SACs)are gaining popularity in catalytic reactions due to their nearly 100%atomic utilization and defined active sites,which provide great convenience for studying the catalytic mechanism of catalysts.However,SACs still present challenges such as complex formation processes,low loading and easy agglomeration of catalysts.Herein,we systematically discuss the synthesis methods for SACs,including coprecipitation,impregnation,atomic layer deposition,pyrolysis and Anti-Ostwald ripening etc.Various techniques for characterizing single-atom catalysts(SACs)are described in detail.The utilization of individual atoms in various photocatalytic reactions and their mechanisms of action in different reactions are explained.The purpose of this review is to introduce single-atom synthesis methods,characterization techniques,specific catalytic action and their applications in the direction of photocatalysis,and to provide a reference for the industrialization of photocatalytic single-atoms,which is currently impossible,in the hope of promoting further development of photocatalytic single-atoms.
基金supported by the National Key Research and Development Program of China(2022YFB3204700)the National Natural Science Foundation of China(52122513)+2 种基金the Natural Science Foundation of Heilongjiang Province(YQ2021E022)the Natural Science Foundation of Chongqing(2023NSCQ-MSX2286)the Fundamental Research Funds for the Central Universities(HIT.BRET.2021010)。
文摘Single atom catalysts(SACs)have garnered significant attention in the field of catalysis over the past decade due to their exceptional atom utilization efficiency and distinct physical and chemical properties.For the semiconductor-based electrical gas sensor,the core is the catalysis process of target gas molecules on the sensitive materials.In this context,the SACs offer great potential for highly sensitive and selective gas sensing,however,only some of the bubbles come to the surface.To facilitate practical applications,we present a comprehensive review of the preparation strategies for SACs,with a focus on overcoming the challenges of aggregation and low loading.Extensive research efforts have been devoted to investigating the gas sensing mechanism,exploring sensitive materials,optimizing device structures,and refining signal post-processing techniques.Finally,the challenges and future perspectives on the SACs based gas sensing are presented.
基金Project supported by the National Natural Science Foundation of China(Grant No.92165202)the Innovation Program for Quantum Science and Technology,China(Grant No.2021ZD0300701)the Strategic Priority Research Program(A)of Chinese Academy of Sciences(Grant No.XDA18040300).
文摘The photostability of a colloidal single photon emitter in near-infrared regime at room temperature is investigated.The fluorescence lifetime,blinking phenomenon,and anti-bunching effect of a single CdTeSe/ZnS quantum dot with an emission wavelength of 800 nm at room temperature are studied.The second-order correlation function at zero delay time is much smaller than 0.1,which proves that the emission from single quantum dots at 800 nm is a highly pure single-photon source.The effects of the irradiation duration on the fluorescence from single quantum dots are analyzed.The experimental results can be explained by a recombination model including a multi-nonradiative recombination center model and a multi-charged model.
基金Project supported by the Basic and Applied Basic Research Foundation of Guangdong Province,China(Grant Nos.2019A1515110302 and 2022A1515140003)the Key Research and Development Program of Guangdong Province,China(Grant Nos.2020B010189001,2021B0301030002,2019B010931001,and 2018B030327001)+5 种基金the National Natural Science Foundation of China(Grant Nos.52172035,52025023,52322205,51991342,52021006,51991344,52100115,11888101,92163206,12104018,and 12274456)the National Key Research and Development Program of China(Grant Nos.2021YFB3200303,2022YFA1405600,2018YFA0703700,2021YFA1400201,and 2021YFA1400502)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB33000000)the Pearl River Talent Recruitment Program of Guangdong Province,China(Grant No.2019ZT08C321)China Postdoctoral Science Foundation(Grant Nos.2020T130022 and 2020M680178)the Science and Technology Plan Project of Liaoning Province,China(Grant No.2021JH2/10100012).
文摘High-purity copper(Cu) with excellent thermal and electrical conductivity, is crucial in modern technological applications, including heat exchangers, integrated circuits, and superconducting magnets. The current purification process is mainly based on the zone/electrolytic refining or anion exchange, however, which excessively relies on specific integrated equipment with ultra-high vacuum or chemical solution environment, and is also bothered by external contaminants and energy consumption. Here we report a simple approach to purify the Cu foils from 99.9%(3N) to 99.99%(4N) by a temperature-gradient thermal annealing technique, accompanied by the kinetic evolution of single crystallization of Cu.The success of purification mainly relies on(i) the segregation of elements with low effective distribution coefficient driven by grain-boundary movements and(ii) the high-temperature evaporation of elements with high saturated vapor pressure.The purified Cu foils display higher flexibility(elongation of 70%) and electrical conductivity(104% IACS) than that of the original commercial rolled Cu foils(elongation of 10%, electrical conductivity of ~ 100% IACS). Our results provide an effective strategy to optimize the as-produced metal medium, and therefore will facilitate the potential applications of Cu foils in precision electronic products and high-frequency printed circuit boards.
基金support from the Department of Science and Technology (DST),Government of India (Grant No.ECR/DST/2017/000918)the Indian Institute of Technology Ropar for providing financial support under an ISIRD grant (F.No.9-282/2017IITRPR/705).
文摘Ultrasonic-assisted micro-electro-discharge machining(EDM)has the potential to enhance processing responses such as material removal rate(MRR)and surface finish.To understand the reasons for this enhancement,the physical mechanisms responsible for the individual discharges and the craters that they form need to be explored.This work examines features of craters formed by single discharges at various parameter values in both conventional and ultrasonic-assistedEDM of Ti6Al4V.High-speed imaging of the plasma channel is performed,and data on the individual discharges are captured in real-time.A 2D axisymmetric model using finite element software is established to model crater formation.On the basis of simulation and experimental results,a comparative study is then carried out to examine the effects of ultrasonic vibrational assistance on crater geometry.For every set ofEDM parameters,the crater diameter and depth from a single discharge are found to be higher in ultrasonic-assistedEDM than in conventionalEDM.The improved crater geometry and the reduced bulge formation at the crater edges are attributed to the increased melt pool velocity and temperature predicted by the model.
基金Project supported by the Offline Course Program of“Experiment of College Physics”in the 2022-year Anhui Provincial Quality Engineering Program (Grant No.2022xxkc134)the Program for Academic Leader Reserve Candidates in Tongling University (Grant Nos.2020tlxyxs43 and 2014tlxyxs30)+1 种基金the Talent Scientific Research Foundation of Tongling University (Grant No.2015tlxyrc01)the 2014 year Program for Excellent Youth Talents in University of Anhui Province。
文摘In paper[Chin.Phys.B 32070308(2023)],Xing et al.proposed a semi-quantum secret sharing protocol by using single particles.We study the security of the proposed protocol and find that it is not secure,that is,the three dishonest agents,Bob,Charlie and Emily can collude to obtain Alice's secret without the help of David.
基金funded by National Natural Science Foundation of China, grant numbers 62335006, 62274014, 62235016, 61734006, 61835011, 61991430funded by Key Program of the Chinese Academy of Sciences, grant numbers XDB43000000, QYZDJSSW-JSC027Beijing Municipal Science & Technology Commission, grant number Z221100002722018
文摘We demonstrated a scheme of phase-locked terahertz quantum cascade lasers(THz QCLs)array,with a single-mode pulse power of 108 mW at 13 K.The device utilizes a Talbot cavity to achieve phase locking among five ridge lasers with first-order buried distributed feedback(DFB)grating,resulting in nearly five times amplification of the single-mode power.Due to the optimum length of Talbot cavity depends on wavelength,the combination of Talbot cavity with the DFB grating leads to better power amplification than the combination with multimode Fabry-Perot(F-P)cavities.The Talbot cavity facet reflects light back to the ridge array direction and achieves self-imaging in the array,enabling phase-locked operation of ridges.We set the spacing between adjacent elements to be 220μm,much larger than the free-space wavelength,ensuring the operation of the fundamental supermode throughout the laser's dynamic range and obtaining a high-brightness far-field distribution.This scheme provides a new approach for enhancing the single-mode power of THz QCLs.
基金supported by National Natural Science Foundation of China(52373221,U1910208,52250119)the National Key R&D Program of China(2020YFA0710403)the Scientific Research Fund of Hunan Provincial Education Department(NO.23B0114).
文摘Single-atom(SA)catalysts with nearly 100%atom utilization have been widely employed in electrolysis for decades,due to the outperforming catalytic activity and selectivity.However,most of the reported SA catalysts are fixed through the strong bonding between the dispersed single metallic atoms with nonmetallic atoms of the substrates,which greatly limits the controllable regulation of electrocatalytic activity of SA catalysts.In this work,Pt-Ni bonded Pt SA catalyst with adjustable electronic states was successfully constructed through a controllable electrochemical reduction on the coordination unsaturated amorphous Ni(OH)_(2)nanosheet arrays.Based on the X-ray absorption fine structure analysis and first-principles calculations,Pt SA was bonded with Ni sites of amorphous Ni(OH)_(2),rather than conventional O sites,resulting in negatively charged Pt^(δ-).In situ Raman spectroscopy revealed that the changed configuration and electronic states greatly enhanced absorbability for activated hydrogen atoms,which were the essential intermediate for alkaline hydrogen evolution reaction.The hydrogen spillover process was revealed from amorphous Ni(OH)_(2)that effectively cleave the H-O-H bond of H_(2)O and produce H atom to the Pt SA sites,leading to a low overpotential of 48 mV in alkaline electrolyte at-1000 mA cm^(-2)mg^(-1)_(Pt),evidently better than commercial Pt/C catalysts.This work provided new strategy for the control-lable modulation of the local structure of SA catalysts and the systematic regulation of the electronic states.
基金financially supported by the Natural Science Foundation of Jiangsu Province,China (BK20210887)the Jiangsu Provincial Double Innovation Program,China (JSSCB20210984)+1 种基金the Natural Science Fund for Colleges and Universities of Jiangsu Province,China (21KJB450003)the Jiangsu University of Science and Technology Doctoral Research Start-up Fund,China (120200012)。
文摘Nickel(Ni)-rich cathode materials have become promising candidates for the next-generation electrical vehicles due to their high specific capacity.However,the poor thermodynamic stability(including cyclic performance and safety performance or thermal stability)will restrain their wide commercial application.Herein,a single-crystal Ni-rich Li Ni_(0.83)Co_(0.12)Mn_(0.05)O_(2) cathode material is synthesized and modified by a dual-substitution strategy in which the high-valence doping element improves the structural stability by forming strong metal–oxygen binding forces,while the low-valence doping element eliminates high Li^(+)/Ni^(2+)mixing.As a result,this synergistic dual substitution can effectively suppress H2-H3 phase transition and generation of microcracks,thereby ultimately improving the thermodynamic stability of Ni-rich cathode material.Notably,the dual-doped Ni-rich cathode delivers an extremely high capacity retention of 81%after 250 cycles(vs.Li/Li+)in coin-type half cells and 87%after 1000 cycles(vs.graphite/Li^(+))in pouch-type full cells at a high temperature of 55℃.More impressively,the dual-doped sample exhibits excellent thermal stability,which demonstrates a higher thermal runaway temperature and a lower calorific value.The synergetic effects of this dual-substitution strategy pave a new pathway for addressing the critical challenges of Ni-rich cathode at high temperatures,which will significantly advance the high-energy-density and high-safety cathodes to the subsequent commercialization.
基金supported by the fund of State Key Laboratory of Long-life High Temperature Materials(Grant No.DTCC28EE200787)the Natural Science Basic Research Plan in Shaanxi Province of China(Grant No.2022JQ-553)+3 种基金the China Postdoctoral Science Foundation(Grant No.2021M692555)the Excellent Youth Foundation of Shaanxi Province of China(Grant No.2021JC-08)the Beilin district of Xi’an Science and Technology Project(Grant No.GX2123)the support from the Youth Innovation Team of Shaanxi Universities。
文摘The oxidation behavior of a novel Ni-based single-crystal 4774DD1 superalloy for industrial gas turbine applications was investigated by the isothermal oxidation at 980℃ and discontinuous oxidation weight gain methods.The phase constitution and morphology of surface oxides and the characteristics of the crosssection oxide film were analyzed by XRD,SEM and EDS.Results show that the oxidation kinetics of the 4774DD1 superalloy follows the cubic law,indicating its weak oxidation resistance at this temperature.As the oxidation time increases,the composition of the oxide film evolves as following:One layer consisting of a bottom Al_(2)O_(3)sublayer and an upper(Al_(2)O_(3)+NiO)mixture sublayer after oxidized for 25 h.Then,two layers composed of an outermost small NiO discontinuous grain layer and an internal layer for 75 h.This internal layer is consisted of the bottom Al_(2)O_(3)sublayer,an intermediate narrow CrTaO_(4)sublayer,and an upper(Al_(2)O_(3)+NiO)mixture sublayer.Also two layers comprising an outermost relative continuous NiO layer with large grain size and an internal layer as the oxidation time increases to 125 h.This internal layer is composed of the upper(Al_(2)O_(3)+NiO)mixture sublayer,an intermediate continuous(CrTaO_(4)+NiWO_(4))mixture sublayer,and a bottom Al_(2)O_(3)sublayer.Finally,three layers consisting of an outermost(NiAl2O_(4)+NiCr2O_(4))mixture layer,an intermediate(CrTaO_(4)+NiWO_(4))mixture layer,and a bottom Al_(2)O_(3)layer for 200 h.
基金supported by the National Natural Science Foundation of China(51872115,12234018 and 52101256)Beijing Synchrotron Radiation Facility(BSRF,4B9A)。
文摘Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of interaction.Herein,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery performance.The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic activity.Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.
基金supported by the National Science Fund for Distinguished Young Scholars(No.51925703)National Natural Science Foundation of China(Nos.52022096 and 52261145695)。
文摘The environmental contamination caused by antibiotics is increasingly conspicuous due to their widespread manufacture and misuse. Plasma has been employed in recent years for the remediation of antibiotic pollution in the environment. In this work, a falling-film dielectric barrier discharge was used to degrade the antibiotic tetracycline(TC) in water. The reactor combined the gas-liquid discharge and active gas bubbling to improve the TC degradation performance. The discharge characteristics, chemical species’ concentration, and degradation rates at different parameters were systematically studied. Under the optimized conditions(working gas was pure oxygen, liquid flow rate was 100 mL/min, gas flow rate was 1 L/min,voltage was 20 kV, single treatment), TC was removed beyond 70% in a single flow treatment with an energy efficiency of 145 mg/(kW·h). The reactor design facilitated gas and liquid flow in the plasma area to produce more ozone in bubbles after a single flow under pure oxygen conditions, affording fast TC degradation. Furthermore, long-term stationary experiment indicated that long-lived active species can sustain the degradation of TC. Compared with other plasma treatment systems, this work offers a fast and efficient degradation method, showing significant potential in practical industrial applications.
基金supported by the National Natural Science Foundation of China (No.32070656)the Nanjing University Deng Feng Scholars Program+1 种基金the Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions,China Postdoctoral Science Foundation funded project (No.2022M711563)Jiangsu Funding Program for Excellent Postdoctoral Talent (No.2022ZB50)
文摘Plant morphogenesis relies on precise gene expression programs at the proper time and position which is orchestrated by transcription factors(TFs)in intricate regulatory networks in a cell-type specific manner.Here we introduced a comprehensive single-cell transcriptomic atlas of Arabidopsis seedlings.This atlas is the result of meticulous integration of 63 previously published scRNA-seq datasets,addressing batch effects and conserving biological variance.This integration spans a broad spectrum of tissues,including both below-and above-ground parts.Utilizing a rigorous approach for cell type annotation,we identified 47 distinct cell types or states,largely expanding our current view of plant cell compositions.We systematically constructed cell-type specific gene regulatory networks and uncovered key regulators that act in a coordinated manner to control cell-type specific gene expression.Taken together,our study not only offers extensive plant cell atlas exploration that serves as a valuable resource,but also provides molecular insights into gene-regulatory programs that varies from different cell types.
文摘In dentistry, panoramic X-ray images are extensively used by dentists for tooth structure analysis and disease diagnosis. However, the manual analysis of these images is time-consuming and prone to misdiagnosis or overlooked. While deep learning techniques have been employed to segment teeth in panoramic X-ray images, accurate segmentation of individual teeth remains an underexplored area. In this study, we propose an end-to-end deep learning method that effectively addresses this challenge by employing an improved combinatorial loss function to separate the boundaries of adjacent teeth, enabling precise segmentation of individual teeth in panoramic X-ray images. We validate the feasibility of our approach using a challenging dataset. By training our segmentation network on 115 panoramic X-ray images, we achieve an intersection over union (IoU) of 86.56% for tooth segmentation and an accuracy of 65.52% in tooth counting on 87 test set images. Experimental results demonstrate the significant improvement of our proposed method in single tooth segmentation compared to existing methods.
基金Project supported by the National Natural Science Foundation of China(Grant No.12305303)the Natural Science Foundation of Hunan Province of China(Grant Nos.2023JJ40520,2021JJ40444,and 2019JJ30019)+3 种基金the Research Foundation of Education Bureau of Hunan Province of China(Grant No.20A430)the Science and Technology Innovation Program of Hunan Province(Grant No.2020RC3054)the Natural Science Basic Research Plan in the Shaanxi Province of China(Grant No.2023-JC-QN-0015)the Doctoral Research Fund of University of South China。
文摘Convolutional neural networks(CNNs) exhibit excellent performance in the areas of image recognition and object detection, which can enhance the intelligence level of spacecraft. However, in aerospace, energetic particles, such as heavy ions, protons, and alpha particles, can induce single event effects(SEEs) that lead CNNs to malfunction and can significantly impact the reliability of a CNN system. In this paper, the MNIST CNN system was constructed based on a 28 nm systemon-chip(SoC), and then an alpha particle irradiation experiment and fault injection were applied to evaluate the SEE of the CNN system. Various types of soft errors in the CNN system have been detected, and the SEE cross sections have been calculated. Furthermore, the mechanisms behind some soft errors have been explained. This research will provide technical support for the design of radiation-resistant artificial intelligence chips.
基金supported in part by the National Natural Science Foundation of China(Nos.62071441 and 61701464)in part by the Fundamental Research Funds for the Central Universities(No.202151006).
文摘This study explores the application of single photon detection(SPD)technology in underwater wireless optical communication(UWOC)and analyzes the influence of different modulation modes and error correction coding types on communication performance.The study investigates the impact of on-off keying(OOK)and 2-pulse-position modulation(2-PPM)on the bit error rate(BER)in single-channel intensity and polarization multiplexing.Furthermore,it compares the error correction performance of low-density parity check(LDPC)and Reed-Solomon(RS)codes across different error correction coding types.The effects of unscattered photon ratio and depolarization ratio on BER are also verified.Finally,a UWOC system based on SPD is constructed,achieving 14.58 Mbps with polarization OOK multiplexing modulation and 4.37 Mbps with polarization 2-PPM multiplexing modulation using LDPC code error correction.
基金Project supported by the National Key Research and Development Program of China (Grant Nos.2023YFA1406500 and 2019YFA0308602)the National Natural Science Foundation of China (Grant Nos.12104011,12274388,12074425,52102333,12104010,12204004,and 11874422)the Natural Science Foundation of Anhui Province (Grant Nos.2108085QA22 and 2108085MA16)。
文摘We report the magnetotransport and thermal properties of RuAs_(2) single crystal.RuAs_(2) exhibits semiconductor behavior and localization effect.The crossover from normal state to diffusive transport in the weak localization(WL)state and then to variable range hopping(VRH)transport in the strong localization state has been observed.The transitions can be reflected in the measurement of resistivity and Seebeck coefficient.Negative magnetoresistance(NMR)emerges with the appearance of localization effect and is gradually suppressed in high magnetic field.The temperature dependent phase coherence length extracted from the fittings of NMR also indicates the transition from WL to VRH.The measurement of Hall effect reveals an anomaly of temperature dependent carrier concentration caused by localization effect.Our findings show that RuAs_(2) is a suitable platform to study the localized state.
基金This work was supported by the Major Scientific and Technological Special Project of Anhui Province(202103a13010004)the Major Scientific and Technological Special Project of Hefei City(2021DX007)+1 种基金the Key R&D Plan of Shandong Province(2020CXGC010105)the China Postdoctoral Science Foundation(2021M700315).
文摘Quantum key distribution(QKD),rooted in quantum mechanics,offers information-theoretic security.However,practi-cal systems open security threats due to imperfections,notably bright-light blinding attacks targeting single-photon detectors.Here,we propose a concise,robust defense strategy for protecting single-photon detectors in QKD systems against blinding attacks.Our strategy uses a dual approach:detecting the bias current of the avalanche photodiode(APD)to defend against con-tinuous-wave blinding attacks,and monitoring the avalanche amplitude to protect against pulsed blinding attacks.By integrat-ing these two branches,the proposed solution effectively identifies and mitigates a wide range of bright light injection attempts,significantly enhancing the resilience of QKD systems against various bright-light blinding attacks.This method forti-fies the safeguards of quantum communications and offers a crucial contribution to the field of quantum information security.