Single-atom catalysts,featuring some of the most unique activities,selectivity,and high metal utilization,have been extensively studied over the past decade.Given their high activity,selectivity,especially towards sma...Single-atom catalysts,featuring some of the most unique activities,selectivity,and high metal utilization,have been extensively studied over the past decade.Given their high activity,selectivity,especially towards small molecules or key intermediate conversions,they can be synergized together with other active species(typically other single atoms,atomic clusters,or nanoparticles)in either tandem or parallel or both,leading to much better performance in complex catalytic processes.Although there have been reports on effectively combining the multiple components into one single catalytic entity,the combination and synergy between single atoms and other active species have not been reviewed and examined in a systematic manner.Herein,in this overview,the key synergistic interactions,binary complementary effects,and the bifunctional functions of single atoms with other active species are defined and discussed in detail.The integration functions of their marriages are in-vestigated with particular emphasis on the homogeneous and heterogeneous combinations,spatial distribution,synthetic strategies,and the thus-derived outstanding catalytic performance,together with new light shined on the catalytic mechanisms by zooming in several case studies.The dynamic nature of each of the active species and in particular their interactions in such new catalytic entities in the heterogeneous electrocatalytic processes are visited,on the basis of the in situ/operando evidence.Last,we feature the current chal-lenges and future perspectives of these integrated catalytic entities that can offer guidance for advanced catalyst design by the rational combination and synergy of binary or multiple active species.展开更多
Electrocatalytic CO2 reduction to CO is a sustainable process for energy conversion.However,this process is still hindered by the diffusi limited mass transfer,low electrical conductivity and catalytic activity.Theref...Electrocatalytic CO2 reduction to CO is a sustainable process for energy conversion.However,this process is still hindered by the diffusi limited mass transfer,low electrical conductivity and catalytic activity.Therefore,new strategies for catalyst design should be adopted to solve these problems and improve the electrocatalytic performa nee for CO production.Herein,we report a multiscale carb on foam confining〔single iron atoms prepared with the assistant of S1O2 template.The pore-enriched environment at the macro-scale facilitates the diffusion of reacta nts and products.The graphe ne nano sheets at the nano-scale promote the charge tran sfer duri ng the reaction.The single iron atoms con fined in carb on matrix at the atomic-scale provide the active sites for electrocatalytic CO2 reductio n to CO.The optimized catalyst achieves a CO Faradaic efficiency of 94.9%at a moderate potential of-0.5 V vs.RHE.Furthermore,the performance can be maintained over 60 hours due to the stable single iron atoms coordi nated with four n itroge n atoms in the carb on matrix.This work provides a promising strategy to improve both the activity and stability of single atom catalysts for electrocatalytic CO2 reduction to CO.展开更多
Reducing the dimensions of metallic nanoparticles to isolated,single atom has attracted considerable attention in heterogeneous catalysis,because it significantly improves atomic utilization and often leads to distinc...Reducing the dimensions of metallic nanoparticles to isolated,single atom has attracted considerable attention in heterogeneous catalysis,because it significantly improves atomic utilization and often leads to distinct catalytic performance.Through extensive research,it has been recognized that the local coordination environment of single atoms has an important influence on their electronic structures and catalytic behaviors.In this review,we summarize a series of representative systems of single-atom catalysts,discussing their preparation,characterization,and structure-property relationship,with an emphasis on the correlation between the coordination spheres of isolated reactive centers and their intrinsic catalytic activities.We also share our perspectives on the current challenges and future research promises in the development of single-atom catalysis.With this article,we aim to highlight the possibility of finely tuning the catalytic performances by engineering the coordination spheres of single-atom sites and provide new insights into the further development for this emerging research field.展开更多
Topological phase of matter is now a mainstream of research in condensed matter physics, of which the classification, synthesis, and detection of topological states have brought excitements over the recent decade whil...Topological phase of matter is now a mainstream of research in condensed matter physics, of which the classification, synthesis, and detection of topological states have brought excitements over the recent decade while remain incomplete with ongoing challenges in both theory and experiment. Here we propose to establish a universal non-equilibrium characterization of the equilibrium topological quantum phases classified by integers, and further propose the high-precision dynamical schemes to detect such states. The framework of the dynamical classification theory consists of basic theorems. First, we uncover that classifying a d-dimensional(dD) gapped topological phase of generic multibands can reduce to a(d-1)D invariant defined on so-called band inversion surfaces(BISs), rendering a bulk-surface duality which simplifies the topological characterization. Further, we show in quenching across phase boundary the(pseudo) spin dynamics to exhibit unique topological patterns on BISs, which are attributed to the post-quench bulk topology and manifest a dynamical bulk-surface correspondence. For this the topological phase is classified by a dynamical topological invariant measured from an emergent dynamical spintexture field on the BISs. Applications to quenching experiments on feasible models are proposed and studied, demonstrating the new experimental strategies to detect topological phases with high feasibility. This work opens a broad new direction to classify and detect topological phases by non-equilibrium quantum dynamics.展开更多
A fully relativistic distorted-wave program is developed based on the Grasp92 and Ratip packages to calculate electron impact excitation （EIE） cross sections. As a first application of the program, the EIE cross sec...A fully relativistic distorted-wave program is developed based on the Grasp92 and Ratip packages to calculate electron impact excitation （EIE） cross sections. As a first application of the program, the EIE cross sections of Be-like C^α＋ ions from the metastable 1s^22s2p^3 p to 1s^22p^2 ^3 p excitation and the inner-shell excitations are calculated systematically. Meanwhile, the correlation effects of target states are discussed. It is found that the correlation effects play an important role in the low energy EIE cross sections. An excellent agreement is found when the results are compared with previous calculations and recent measurements.展开更多
The large-scale synthesis of platinum-free electrocatalysts for the oxygen reduction reaction(ORR)remains a grand challenge.We report the large-scale production of stable and active ORR electrocatalysts based on iron,...The large-scale synthesis of platinum-free electrocatalysts for the oxygen reduction reaction(ORR)remains a grand challenge.We report the large-scale production of stable and active ORR electrocatalysts based on iron,an earth-abundant element.A core–shell zeolitic imidazolate framework–tannic acid coordination polymer composite(ZIF-8@K-TA)was utilized as the catalyst precursor,which was transformed into iron atoms dispersed in hollow porous nitrogen-doped carbon capsules(H-Fe-N_(x)-C)through ion exchange and pyrolysis.H-Fe-N_(x)-C fea-tures site-isolated single-atom iron centers coordinated to nitrogen in graphitic layers,high levels of nitrogen doping,and high permeability to incoming gases.Benefiting from these characteristics,H-Fe-N_(x)-C demonstrated efficient electrocatalytic activity(E_(1/2)=0.92 V,vs.RHE)and stability towards the ORR in both alkaline and acidic media.In ORR performance,it surpassed the majority of recently reported Fe-N-C catalysts and the standard Pt/C catalyst.In addition,H-Fe-N_(x)-C showed outstanding tolerance to methanol.展开更多
We report the 87Sr optical lattice clock developed at the National Time Service Center. We achieved a closed-loop operation of the optical lattice clock based on 87Sr atoms. The linewidth of the spin-polarized clock p...We report the 87Sr optical lattice clock developed at the National Time Service Center. We achieved a closed-loop operation of the optical lattice clock based on 87Sr atoms. The linewidth of the spin-polarized clock peak is 3.9 Hz with a clock laser pulse length of 300 ms, which corresponds to a Fourier-limited linewidth of 3 Hz. The fitting of the in-loop error signal data shows that the instability is approximately 5 × 10 15τ-1/2, affected primarily by the white noise. The fractional frequency difference averages down to 5.7 × 10 ^-17 for an averaging time of 3000 s.展开更多
Metal isolated single atomic sites catalysts have attracted intensive attention in recent years owing to their maximized atom utilization and unique structure.Despite the success of single atom catalyst synthesis,dire...Metal isolated single atomic sites catalysts have attracted intensive attention in recent years owing to their maximized atom utilization and unique structure.Despite the success of single atom catalyst synthesis,directly anchoring metal single atoms on three-dimensional(3D)macro support,which is promising to achieve the heterogenization of homogeneous catalysis,remains a challenge and a blank in this field.Herein,we successfully fabricate metal single atoms(Pd,Pt,Ru,Au)on porous carbon nitride/reduced graphene oxide(C3N4/rGO)foam as highly efficient catalysts with convenient recyclability.C3N4/rGO foam features two-dimensional microstructures with abundant N chelating sites for the stabilization of metal single atoms and vertically-aligned hierarchical mesostructure that benefits the mass diffusion.The obtained Pdi/C3N4/rGO monolith catalyst exhibits much enhanced activity over its nanoparticle counterpart for Suzuki-Miyaura reaction.Moreover,the Pdi/C3N4/rGO monolith catalyst can be readily assembled in a flow reactor to achieve the highly efficient continuous production of 4-nitro-1,1'-biphenyl through Suzuki-Miyaura coupling.展开更多
The author introduces the Hardy spaces associated with the Herz spaces and the Beurling algebras on homogeneous groups and establishes their atomic decomposition characterizations. As the applications of this decompos...The author introduces the Hardy spaces associated with the Herz spaces and the Beurling algebras on homogeneous groups and establishes their atomic decomposition characterizations. As the applications of this decomposition, the duals of these Hardy spaces and the boundedness of the central δ-Calderon-Zygmund operators on these Hardy spaces are studied.展开更多
Pt/CeO2 catalysts with unitary Pt species,nanoparticles,clusters or single atoms,often exhibit excellent activity and unique selectivity in many catalytic reactions benefiting from their small size,abundant unsaturate...Pt/CeO2 catalysts with unitary Pt species,nanoparticles,clusters or single atoms,often exhibit excellent activity and unique selectivity in many catalytic reactions benefiting from their small size,abundant unsaturated active sites,and unique electro nic structure.In recent years,a tre mendous number of related articles have provided great inspiration to future research and development of Pt/CeO2 catalysts.In this review,the state-of-the-art evolution of Pt nanoparticles to Pt single atoms on CeO2 is reviewed with the emphasis on synthetic strategies,advanced characterization techniques(allowing one to clarify the single atoms from clusters),the catalytic applications and mechanisms from the viewpoint of theoretical calculation.Finally,the critical outlooks and the challenges faced in developing the single-atom Pt/CeO2 catalysts are highlighted.展开更多
Despite of suitable band structures for harvesting solar light and driving water redox reactions,polymeric carbon nitride(PCN)has suffered from poor charge transfer ability and sluggish surface reaction kinetics,which...Despite of suitable band structures for harvesting solar light and driving water redox reactions,polymeric carbon nitride(PCN)has suffered from poor charge transfer ability and sluggish surface reaction kinetics,which limit its photocatalytic activity for water splitting.Herein,atomically dispersed Zn-coordinated three-dimensional(3D)sponge-like PCN(Zn-PCN)is synthesized through a novel intermediate coordination strategy.Advanced characterizations and theoretical calculations well evidence that Zn single atoms are coordinated and stabilized on PCN in the form of Zn-N_(6) configura-tion featured with an electron-deficient state.Such an electronic configuration has been demonstrated contributive to promoted electron excitation,accelerated charge separation and transfer as well as reduced water redox barriers.Further benefited from the abundant surface active sites derived from the 3D porous structure,Zn-PCN realizes visible-light photocatalysis for overall water splitting with H_(2) and O_(2) simultaneously evolved at a stoichiometric ratio of 2:1.This work brings new insights into the design of novel single-atom photocatalysts by deepening the understanding of electronic configurations and reactive sites favorable to excellent photocatalysis for water splitting and related solar energy conversion reactions.展开更多
Potassium-ion batteries(PIBs) hold great potential as an alternative to lithium-ion batteries due to the abundant reserves of potassium and similar redox potentials of K+/K and Li+/Li. Unfortunately, PIBs with carbona...Potassium-ion batteries(PIBs) hold great potential as an alternative to lithium-ion batteries due to the abundant reserves of potassium and similar redox potentials of K+/K and Li+/Li. Unfortunately, PIBs with carbonaceous electrodes present sluggish kinetics, resulting in unsatisfactory cycling stability and poor rate capability. Herein, we demonstrate that the synergistic effects of the enlarged interlayer spacing and enhanced capacitive behavior induced by the co-doping of nitrogen and sulfur atoms into a carbon structure(NSC) can improve its potassium storage capability. Based on the capacitive contribution calculations, electrochemical impedance spectroscopy, the galvanostatic intermittent titration technique, and density functional theory results, the NSC electrode is found to exhibit favorable electronic conductivity,enhanced capacitive adsorption behavior, and fast K+ ion diffusion kinetics. Additionally, a series of exsitu characterizations demonstrate that NSC exhibits superior structural stability during the(de)potassiation process. As a result, NSC displays a high reversible capacity of 302.8 mAh g-1 at 0.1 Ag-1 and a stable capacity of 105.2 m Ahg-1 even at 2 Ag-1 after 600 cycles. This work may offer new insight into the effects of the heteroatom doping of carbon materials on their potassium storage properties and facilitate their application in PIBs.展开更多
Quantum simulation is a powerful tool to study a variety of problems in physics, ranging from high-energy physics to condensed-matter physics. In this article, we review the recent theoretical and experimental progres...Quantum simulation is a powerful tool to study a variety of problems in physics, ranging from high-energy physics to condensed-matter physics. In this article, we review the recent theoretical and experimental progress in quantum simulation of Dirac equation with tunable parameters by using ultracold neutral atoms trapped in optical lattices or subject to light-induced synthetic gauge fields. The effective theories for the quasiparticles become relativistic under certain conditions in these systems, making them ideal platforms for studying the exotic relativistic effects. We focus on the realization of one, two, and three dimensional Dirac equations as well as the detection of some relativistic effects, including particularly the well-known Zitterbewegung effect and Klein tunneling. The realization of quantum anomalous Hall effects is also briefly discussed.展开更多
Based on our work on single cesium atoms trapped in a large-magnetic-gradient vapour-cell magneto-optical trap （MOT）, the signal-to-noise ratio （SNR） is remarkably improved. Also a far-off-resonance optical dipole...Based on our work on single cesium atoms trapped in a large-magnetic-gradient vapour-cell magneto-optical trap （MOT）, the signal-to-noise ratio （SNR） is remarkably improved. Also a far-off-resonance optical dipole trap （FORT） formed by a strongly-focused 1064 nm single frequency Nd：YVO4 laser beam is introduced. One cesium atom is prepared in the MOT, and then it can transfer successfully between the MOT and the FORT which is overlapped with the MOT. Utilizing the effective transfer, the lifetime of single atoms trapped in the FORT is measured to be 6.9± 0.3 s. Thus we provide a system where the atomic qubit can be coherently manipulated.展开更多
Atomically dispersed catalysts have attracted attention in energy conversion applications because their efficiency and chemoselectivity for special catalysis are superior to those of traditional catalysts. However, th...Atomically dispersed catalysts have attracted attention in energy conversion applications because their efficiency and chemoselectivity for special catalysis are superior to those of traditional catalysts. However, they have limitations owing to the extremely low metal-loading content on supports, difficulty in the precise control of the metal location and amount as well as low stability at high temperatures. We prepared a highly doped single metal atom hybrid via a single-step thermal pyrolysis of glucose, dicyandiamide, and inorganic metal salts. High-angle annular dark field-scanning transmission electron microscopy （HAADF-STEM） and X-ray absorption fine structure spectroscopy （XAFS） revealed that nitrogen atoms doped into the graphene matrix were pivotal for metal atom stabilization by generating a metal-Nx coordination structure. Due to the strong anchoring effect of the graphene matrix, the metal loading content was over 4 wt.% in the isolated atomic hybrid （the Pt content was as high as 9.26 wt.% in the Pt-doped hybrid）. Furthermore, the single iron-doped hybrid （Fe@N-doped graphene） showed a remarkable electrocatalytic performance for the oxygen reduction reaction. The peak power density was - 199 mW·cm-2 at a current density of 310 mA·cm-2 and superior to that of a commercial Pt/C catalyst when it was used as a cathode catalyst in assembled zinc-air batteries. This work offered a feasible approach to design and fabricate highly doped single metal atoms （SMAs） catalysts for potential energy applications.展开更多
We report a transportable one-dimensional optical lattice clock based on 87Sr at the National Time Service Center.The transportable apparatus consists of a compact vacuum system and compact optical subsystems.The vacu...We report a transportable one-dimensional optical lattice clock based on 87Sr at the National Time Service Center.The transportable apparatus consists of a compact vacuum system and compact optical subsystems.The vacuum system with a size of 90 cm×20 cm×42 cm and the beam distributors are assembled on a double-layer optical breadboard.The modularized optical subsystems are integrated on independent optical breadboards.By using a 230 ms clock laser pulse,spin-polarized spectroscopy with a linewidth of 4.8 Hz is obtained which is close to the 3.9 Hz Fourier-limit linewidth.The time interleaved self-comparison frequency instability is determined to be 6.3 × 10^-17 at an averaging time of 2000 s.展开更多
基金JW and team thank the support of MOE,Singapore(MOE2018-T2-2-095),for research conducted at the National University of Singapore.
文摘Single-atom catalysts,featuring some of the most unique activities,selectivity,and high metal utilization,have been extensively studied over the past decade.Given their high activity,selectivity,especially towards small molecules or key intermediate conversions,they can be synergized together with other active species(typically other single atoms,atomic clusters,or nanoparticles)in either tandem or parallel or both,leading to much better performance in complex catalytic processes.Although there have been reports on effectively combining the multiple components into one single catalytic entity,the combination and synergy between single atoms and other active species have not been reviewed and examined in a systematic manner.Herein,in this overview,the key synergistic interactions,binary complementary effects,and the bifunctional functions of single atoms with other active species are defined and discussed in detail.The integration functions of their marriages are in-vestigated with particular emphasis on the homogeneous and heterogeneous combinations,spatial distribution,synthetic strategies,and the thus-derived outstanding catalytic performance,together with new light shined on the catalytic mechanisms by zooming in several case studies.The dynamic nature of each of the active species and in particular their interactions in such new catalytic entities in the heterogeneous electrocatalytic processes are visited,on the basis of the in situ/operando evidence.Last,we feature the current chal-lenges and future perspectives of these integrated catalytic entities that can offer guidance for advanced catalyst design by the rational combination and synergy of binary or multiple active species.
基金We gratefully acknowledge the financial support from the Ministry of Science and Technology of China(Nos.2016YFA0204100 and 2016YFA0200200)the National Natural Science Foundation of China(Nos.21573220 and 21802124)+2 种基金the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(No.QYZDB-SSW-JSC020)the DNL Cooperation Fund,CAS(No.DNL180201)We thank staff at the BL14W1 beamline of the Shanghai Synchrotron Radiation Facilities(SSRF)for assistance with the X-ray absorption spectroscopy measurements.
文摘Electrocatalytic CO2 reduction to CO is a sustainable process for energy conversion.However,this process is still hindered by the diffusi limited mass transfer,low electrical conductivity and catalytic activity.Therefore,new strategies for catalyst design should be adopted to solve these problems and improve the electrocatalytic performa nee for CO production.Herein,we report a multiscale carb on foam confining〔single iron atoms prepared with the assistant of S1O2 template.The pore-enriched environment at the macro-scale facilitates the diffusion of reacta nts and products.The graphe ne nano sheets at the nano-scale promote the charge tran sfer duri ng the reaction.The single iron atoms con fined in carb on matrix at the atomic-scale provide the active sites for electrocatalytic CO2 reductio n to CO.The optimized catalyst achieves a CO Faradaic efficiency of 94.9%at a moderate potential of-0.5 V vs.RHE.Furthermore,the performance can be maintained over 60 hours due to the stable single iron atoms coordi nated with four n itroge n atoms in the carb on matrix.This work provides a promising strategy to improve both the activity and stability of single atom catalysts for electrocatalytic CO2 reduction to CO.
基金This work is supported by NSFC(21773242,21935010)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB20000000)+1 种基金National Key Research and Development Program of China(2018YFA0208600)King Abdullah University of Science and Technology.J.Dong acknowledges financial support from Youth Innovation Promotion Association of Chinese Academy of Sciences(2018017).
文摘Reducing the dimensions of metallic nanoparticles to isolated,single atom has attracted considerable attention in heterogeneous catalysis,because it significantly improves atomic utilization and often leads to distinct catalytic performance.Through extensive research,it has been recognized that the local coordination environment of single atoms has an important influence on their electronic structures and catalytic behaviors.In this review,we summarize a series of representative systems of single-atom catalysts,discussing their preparation,characterization,and structure-property relationship,with an emphasis on the correlation between the coordination spheres of isolated reactive centers and their intrinsic catalytic activities.We also share our perspectives on the current challenges and future research promises in the development of single-atom catalysis.With this article,we aim to highlight the possibility of finely tuning the catalytic performances by engineering the coordination spheres of single-atom sites and provide new insights into the further development for this emerging research field.
基金supported by the National Key Research and Development Program of China (2016YFA0301604)National Natural Science Foundation of China (11574008 and 11761161003)the Thousand-Young-Talent Program of China
文摘Topological phase of matter is now a mainstream of research in condensed matter physics, of which the classification, synthesis, and detection of topological states have brought excitements over the recent decade while remain incomplete with ongoing challenges in both theory and experiment. Here we propose to establish a universal non-equilibrium characterization of the equilibrium topological quantum phases classified by integers, and further propose the high-precision dynamical schemes to detect such states. The framework of the dynamical classification theory consists of basic theorems. First, we uncover that classifying a d-dimensional(dD) gapped topological phase of generic multibands can reduce to a(d-1)D invariant defined on so-called band inversion surfaces(BISs), rendering a bulk-surface duality which simplifies the topological characterization. Further, we show in quenching across phase boundary the(pseudo) spin dynamics to exhibit unique topological patterns on BISs, which are attributed to the post-quench bulk topology and manifest a dynamical bulk-surface correspondence. For this the topological phase is classified by a dynamical topological invariant measured from an emergent dynamical spintexture field on the BISs. Applications to quenching experiments on feasible models are proposed and studied, demonstrating the new experimental strategies to detect topological phases with high feasibility. This work opens a broad new direction to classify and detect topological phases by non-equilibrium quantum dynamics.
基金Supported by the National Natural Science Foundation of China under Grant Nos 10376026 and 10434100, the Foundation for the Excellent Youth Scholars of the Ministry of Education of China.
文摘A fully relativistic distorted-wave program is developed based on the Grasp92 and Ratip packages to calculate electron impact excitation （EIE） cross sections. As a first application of the program, the EIE cross sections of Be-like C^α＋ ions from the metastable 1s^22s2p^3 p to 1s^22p^2 ^3 p excitation and the inner-shell excitations are calculated systematically. Meanwhile, the correlation effects of target states are discussed. It is found that the correlation effects play an important role in the low energy EIE cross sections. An excellent agreement is found when the results are compared with previous calculations and recent measurements.
基金Foundation(B?0027)(SM),National Science Foundation of China(Grants 22006036)North China Electric Power University(XM2112307)(HY and XW)+1 种基金GINW is supported by a James Cook Research Fellowship from New Zealand Government funding,administered by the Royal Society Te Aparangisupport from the XAS beamline scientists of the Australian Synchrotron and the 14 W station of the Shanghai Synchrotron Radiation Facility(SSRF).
文摘The large-scale synthesis of platinum-free electrocatalysts for the oxygen reduction reaction(ORR)remains a grand challenge.We report the large-scale production of stable and active ORR electrocatalysts based on iron,an earth-abundant element.A core–shell zeolitic imidazolate framework–tannic acid coordination polymer composite(ZIF-8@K-TA)was utilized as the catalyst precursor,which was transformed into iron atoms dispersed in hollow porous nitrogen-doped carbon capsules(H-Fe-N_(x)-C)through ion exchange and pyrolysis.H-Fe-N_(x)-C fea-tures site-isolated single-atom iron centers coordinated to nitrogen in graphitic layers,high levels of nitrogen doping,and high permeability to incoming gases.Benefiting from these characteristics,H-Fe-N_(x)-C demonstrated efficient electrocatalytic activity(E_(1/2)=0.92 V,vs.RHE)and stability towards the ORR in both alkaline and acidic media.In ORR performance,it surpassed the majority of recently reported Fe-N-C catalysts and the standard Pt/C catalyst.In addition,H-Fe-N_(x)-C showed outstanding tolerance to methanol.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11474282 and 61775220)the Key Research Project of Frontier Science of the Chinese Academy of Sciences(Grant No.QYZDB-SSW-JSC004)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB21030700)
文摘We report the 87Sr optical lattice clock developed at the National Time Service Center. We achieved a closed-loop operation of the optical lattice clock based on 87Sr atoms. The linewidth of the spin-polarized clock peak is 3.9 Hz with a clock laser pulse length of 300 ms, which corresponds to a Fourier-limited linewidth of 3 Hz. The fitting of the in-loop error signal data shows that the instability is approximately 5 × 10 15τ-1/2, affected primarily by the white noise. The fractional frequency difference averages down to 5.7 × 10 ^-17 for an averaging time of 3000 s.
基金This work was supported by the National Key R&D Program of China(No.2018YFA0702003)the National Natural Science Foundation of China(No.21890383,21971137)Beijing Municipal Science&Technology Commission(No.Z191100007219003)。
文摘Metal isolated single atomic sites catalysts have attracted intensive attention in recent years owing to their maximized atom utilization and unique structure.Despite the success of single atom catalyst synthesis,directly anchoring metal single atoms on three-dimensional(3D)macro support,which is promising to achieve the heterogenization of homogeneous catalysis,remains a challenge and a blank in this field.Herein,we successfully fabricate metal single atoms(Pd,Pt,Ru,Au)on porous carbon nitride/reduced graphene oxide(C3N4/rGO)foam as highly efficient catalysts with convenient recyclability.C3N4/rGO foam features two-dimensional microstructures with abundant N chelating sites for the stabilization of metal single atoms and vertically-aligned hierarchical mesostructure that benefits the mass diffusion.The obtained Pdi/C3N4/rGO monolith catalyst exhibits much enhanced activity over its nanoparticle counterpart for Suzuki-Miyaura reaction.Moreover,the Pdi/C3N4/rGO monolith catalyst can be readily assembled in a flow reactor to achieve the highly efficient continuous production of 4-nitro-1,1'-biphenyl through Suzuki-Miyaura coupling.
基金Project (19871071) supported by National Natural Science Foundation of China
文摘The author introduces the Hardy spaces associated with the Herz spaces and the Beurling algebras on homogeneous groups and establishes their atomic decomposition characterizations. As the applications of this decomposition, the duals of these Hardy spaces and the boundedness of the central δ-Calderon-Zygmund operators on these Hardy spaces are studied.
基金Project supported by the National Natural Science Foundation of China(21906063,21876061,21805112)Key Technology R&D Program of Shandong Province(2019GSF109042)。
文摘Pt/CeO2 catalysts with unitary Pt species,nanoparticles,clusters or single atoms,often exhibit excellent activity and unique selectivity in many catalytic reactions benefiting from their small size,abundant unsaturated active sites,and unique electro nic structure.In recent years,a tre mendous number of related articles have provided great inspiration to future research and development of Pt/CeO2 catalysts.In this review,the state-of-the-art evolution of Pt nanoparticles to Pt single atoms on CeO2 is reviewed with the emphasis on synthetic strategies,advanced characterization techniques(allowing one to clarify the single atoms from clusters),the catalytic applications and mechanisms from the viewpoint of theoretical calculation.Finally,the critical outlooks and the challenges faced in developing the single-atom Pt/CeO2 catalysts are highlighted.
基金This work was supported by the National Key Research and Development Program of China(2018YFB1502003)the National Natural Science Foundation of China(52225606,21875183,52172248)+2 种基金the“Fundamental Research Funds for the Central Universities”the Natural Science Basic Research Program of Shaanxi Province(2019JCW-10)“The Youth Innovation Team of Shaanxi Universities”.
文摘Despite of suitable band structures for harvesting solar light and driving water redox reactions,polymeric carbon nitride(PCN)has suffered from poor charge transfer ability and sluggish surface reaction kinetics,which limit its photocatalytic activity for water splitting.Herein,atomically dispersed Zn-coordinated three-dimensional(3D)sponge-like PCN(Zn-PCN)is synthesized through a novel intermediate coordination strategy.Advanced characterizations and theoretical calculations well evidence that Zn single atoms are coordinated and stabilized on PCN in the form of Zn-N_(6) configura-tion featured with an electron-deficient state.Such an electronic configuration has been demonstrated contributive to promoted electron excitation,accelerated charge separation and transfer as well as reduced water redox barriers.Further benefited from the abundant surface active sites derived from the 3D porous structure,Zn-PCN realizes visible-light photocatalysis for overall water splitting with H_(2) and O_(2) simultaneously evolved at a stoichiometric ratio of 2:1.This work brings new insights into the design of novel single-atom photocatalysts by deepening the understanding of electronic configurations and reactive sites favorable to excellent photocatalysis for water splitting and related solar energy conversion reactions.
基金supported by the National Natural Science Foundation of China (51932011, 51972346, 51802356, and 51872334)Innovation-Driven Project of Central South University (2020CX024)the Fundamental Research Funds for the Central Universities of Central South University (2020zzts075)。
文摘Potassium-ion batteries(PIBs) hold great potential as an alternative to lithium-ion batteries due to the abundant reserves of potassium and similar redox potentials of K+/K and Li+/Li. Unfortunately, PIBs with carbonaceous electrodes present sluggish kinetics, resulting in unsatisfactory cycling stability and poor rate capability. Herein, we demonstrate that the synergistic effects of the enlarged interlayer spacing and enhanced capacitive behavior induced by the co-doping of nitrogen and sulfur atoms into a carbon structure(NSC) can improve its potassium storage capability. Based on the capacitive contribution calculations, electrochemical impedance spectroscopy, the galvanostatic intermittent titration technique, and density functional theory results, the NSC electrode is found to exhibit favorable electronic conductivity,enhanced capacitive adsorption behavior, and fast K+ ion diffusion kinetics. Additionally, a series of exsitu characterizations demonstrate that NSC exhibits superior structural stability during the(de)potassiation process. As a result, NSC displays a high reversible capacity of 302.8 mAh g-1 at 0.1 Ag-1 and a stable capacity of 105.2 m Ahg-1 even at 2 Ag-1 after 600 cycles. This work may offer new insight into the effects of the heteroatom doping of carbon materials on their potassium storage properties and facilitate their application in PIBs.
文摘Quantum simulation is a powerful tool to study a variety of problems in physics, ranging from high-energy physics to condensed-matter physics. In this article, we review the recent theoretical and experimental progress in quantum simulation of Dirac equation with tunable parameters by using ultracold neutral atoms trapped in optical lattices or subject to light-induced synthetic gauge fields. The effective theories for the quasiparticles become relativistic under certain conditions in these systems, making them ideal platforms for studying the exotic relativistic effects. We focus on the realization of one, two, and three dimensional Dirac equations as well as the detection of some relativistic effects, including particularly the well-known Zitterbewegung effect and Klein tunneling. The realization of quantum anomalous Hall effects is also briefly discussed.
基金supported by the National Natural Science Foundation of China (Grant Nos 60578018 and 10434080)the project for excellent research team from the National Natural Science Foundation of China (Grant No 60821004)+4 种基金the Program for New Century Excellent Talents of the Education Ministry of China (Grant No NCET-07-0524)the State Basic Key Research Program of China (Grant No 2006CB921102)the Specialized Research Fund for the Doctoral Program of Higher Education of China(Grant No 20070108003)the Natural Science Foundation of Shanxi Province,China (Grant No 2007011003)the Scientific Research Funds for Returned Scholars Abroad of Shanxi Province,China
文摘Based on our work on single cesium atoms trapped in a large-magnetic-gradient vapour-cell magneto-optical trap （MOT）, the signal-to-noise ratio （SNR） is remarkably improved. Also a far-off-resonance optical dipole trap （FORT） formed by a strongly-focused 1064 nm single frequency Nd：YVO4 laser beam is introduced. One cesium atom is prepared in the MOT, and then it can transfer successfully between the MOT and the FORT which is overlapped with the MOT. Utilizing the effective transfer, the lifetime of single atoms trapped in the FORT is measured to be 6.9± 0.3 s. Thus we provide a system where the atomic qubit can be coherently manipulated.
基金This work is financially supported partly by Ministry of Science and Technology （MOST） （Nos. 2017YFA0303500 and 2014CB848900）, the National Natural Science Foundation of China （NSFC） （Nos. U1532112, 11574280 and 11605201 ）, CAS Interdisciplinary Innovation Team and CAS Key Research Program of Frontier Sciences （No. QYZDB-SSW-SLH018）. L. S. acknowledges the recruitment program of global experts, the CAS Hundred Talent Program and Key Laboratory of Advanced Energy Materials Chemistry （Ministry of Education） Nankai University. We thank the Shanghai Synchrotron Radiation Facility （14W1, SSRF）, the Beijing Synchrotron Radiation Facility （1W1B and soft-X-ray endstation, BSRF）, the Hefei Synchrotron Radiation Facility （Photoemission, MCD and Catalysis/ Surface Science Endstations, NSRL）, and the USTC Center for Micro and Nanoscale Research and Fabrication for helps in characterizations.
文摘Atomically dispersed catalysts have attracted attention in energy conversion applications because their efficiency and chemoselectivity for special catalysis are superior to those of traditional catalysts. However, they have limitations owing to the extremely low metal-loading content on supports, difficulty in the precise control of the metal location and amount as well as low stability at high temperatures. We prepared a highly doped single metal atom hybrid via a single-step thermal pyrolysis of glucose, dicyandiamide, and inorganic metal salts. High-angle annular dark field-scanning transmission electron microscopy （HAADF-STEM） and X-ray absorption fine structure spectroscopy （XAFS） revealed that nitrogen atoms doped into the graphene matrix were pivotal for metal atom stabilization by generating a metal-Nx coordination structure. Due to the strong anchoring effect of the graphene matrix, the metal loading content was over 4 wt.% in the isolated atomic hybrid （the Pt content was as high as 9.26 wt.% in the Pt-doped hybrid）. Furthermore, the single iron-doped hybrid （Fe@N-doped graphene） showed a remarkable electrocatalytic performance for the oxygen reduction reaction. The peak power density was - 199 mW·cm-2 at a current density of 310 mA·cm-2 and superior to that of a commercial Pt/C catalyst when it was used as a cathode catalyst in assembled zinc-air batteries. This work offered a feasible approach to design and fabricate highly doped single metal atoms （SMAs） catalysts for potential energy applications.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.61775220 and 11803042)the Key Research Project of Frontier Science of the Chinese Academy of Sciences(Grant No.QYZDB-SSW-JSC004)the strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB21030100).
文摘We report a transportable one-dimensional optical lattice clock based on 87Sr at the National Time Service Center.The transportable apparatus consists of a compact vacuum system and compact optical subsystems.The vacuum system with a size of 90 cm×20 cm×42 cm and the beam distributors are assembled on a double-layer optical breadboard.The modularized optical subsystems are integrated on independent optical breadboards.By using a 230 ms clock laser pulse,spin-polarized spectroscopy with a linewidth of 4.8 Hz is obtained which is close to the 3.9 Hz Fourier-limit linewidth.The time interleaved self-comparison frequency instability is determined to be 6.3 × 10^-17 at an averaging time of 2000 s.
