Motivated by recent realizations of spin-1 NaRb mixtures in the experiments[Phys.Rev.Lett.114,255301(2015);Phys.Rev.Lett.128,223201(2022)],we investigate heteronuclear magnetism in the Mott-insulating regime.Different...Motivated by recent realizations of spin-1 NaRb mixtures in the experiments[Phys.Rev.Lett.114,255301(2015);Phys.Rev.Lett.128,223201(2022)],we investigate heteronuclear magnetism in the Mott-insulating regime.Different from the identical mixtures where the boson statistics only admits even parity states from angular momentum composition,for heteronuclear atoms in principle all angular momentum states are allowed,which can give rise to new magnetic phases.While various magnetic phases can be developed over these degenerate spaces,the concrete symmetry breaking phases depend on not only the degree of degeneracy but also the competitions from many-body interactions.We unveil these rich phases using the bosonic dynamical mean-field theory approach.These phases are characterized by various orders,including spontaneous magnetization order,spin magnitude order,singlet pairing order,and nematic order,which may coexist specially in the regime with odd parity.Finally we address the possible parameter regimes for observing these spin-ordered Mott phases.展开更多
Retaining the ultrathin structure of two-dimensional materials is very important for stabilizing their catalytic performances.However,aggregation and restacking are unavoidable,to some extent,due to the van der Waals ...Retaining the ultrathin structure of two-dimensional materials is very important for stabilizing their catalytic performances.However,aggregation and restacking are unavoidable,to some extent,due to the van der Waals interlayer interaction of two-dimensional materials.Here,we address this challenge by preparing an origami accordion structure of ultrathin twodimensional graphitized carbon nitride(oa-C_(3)N_(4))with rich vacancies.This novel structured oa-C_(3)N_(4) shows exceptional photocatalytic activity for the CO_(2) reduction reaction,which is 8.1 times that of the pristine C_(3)N_(4).The unique structure not only prevents restacking but also increases light harvesting and the density of vacancy defects,which leads to modification of the electronic structure,regulation of the CO_(2) adsorption energy,and a decrease in the energy barrier of the carbon dioxide to carboxylic acid intermediate reaction.This study provides a new avenue for the development of stable highperformance two-dimensional catalytic materials.展开更多
Three-dimensional(3D)degenerate Fermi gases in the presence of spin-orbit coupling,inducing various kinds of physical findings and phenomena,have attracted tremendous attention in these years.We investigate the 3D spi...Three-dimensional(3D)degenerate Fermi gases in the presence of spin-orbit coupling,inducing various kinds of physical findings and phenomena,have attracted tremendous attention in these years.We investigate the 3D spin-orbit coupled degenerate Fermi gases in theory and first present the analytic expression of their ground state.Our study provides an innovative perspective into understanding of the topological properties of 3D unconventional superconductors,and describes the topological phase transitions in trivial and topological phase areas.Further,such a system is provided with a richer set of Cooper pairings than traditional superconductors.The dual Cooper pairs with same spin directions emerge and exhibit peculiar behaviors,leading to topological phase transitions.Our study and discussion can be generalized to some other types of unconventional superconductors and areas of optical lattices.展开更多
Room temperature ferroelectric thin films are the key element of high-density nonvolatile memories in modern electronics. However, with the further miniaturization of the electronic devices beyond the Moore’s law, co...Room temperature ferroelectric thin films are the key element of high-density nonvolatile memories in modern electronics. However, with the further miniaturization of the electronic devices beyond the Moore’s law, conventional ferroelectrics suffer great challenge arising from the critical thickness effect, where the ferroelectricity is unstable if the film thickness is reduced to nanometer or single atomic layer limit. Two-dimensional(2D) materials, thanks to their stable layered structure, saturate interfacial chemistry, weak interlayer couplings, and the benefit of preparing stable ultra-thin film at 2D limit, are promising for exploring 2D ferroelectricity and related device applications. Therefore, it provides an effective approach to overcome the limitation in conventional ferroelectrics with the study of 2D ferroelectricity in van der Waals(vdW) materials. In this review article,we briefly introduce recent progresses on 2D ferroelectricity in layered vdW materials. We will highlight the study on atomically thin α-In2Se3, which is an emergent ferroelectric semiconductor with the coupled in-plane and out-of-plane ferroelectricity. Furthermore, two prototype ferroelectric devices based on ferroelectric α-In2Se3 will also be reviewed.展开更多
High-fidelity two-qubit gates are essential for the realization of large-scale quantum computation and simulation.Tunable coupler design is used to reduce the problem of parasitic coupling and frequency crowding in ma...High-fidelity two-qubit gates are essential for the realization of large-scale quantum computation and simulation.Tunable coupler design is used to reduce the problem of parasitic coupling and frequency crowding in manyqubit systems and thus thought to be advantageous. Here we design an extensible 5-qubit system in which center transmon qubit can couple to every four near-neighboring qubits via a capacitive tunable coupler and experimentally demonstrate high-fidelity controlled-phase(CZ) gate by manipulating central qubit and one nearneighboring qubit. Speckle purity benchmarking and cross entropy benchmarking are used to assess the purity fidelity and the fidelity of the CZ gate. The average purity fidelity of the CZ gate is 99.69±0.04% and the average fidelity of the CZ gate is 99.65±0.04%, which means that the control error is about 0.04%. Our work is helpful for resolving many challenges in implementation of large-scale quantum systems.展开更多
Electrochemical transformation emerges as an important solution to sustainable energy conversion and chemical production.Conventional electrolytic systems usually operate under galvanostatic or potentiostatic conditio...Electrochemical transformation emerges as an important solution to sustainable energy conversion and chemical production.Conventional electrolytic systems usually operate under galvanostatic or potentiostatic conditions that sometimes result in unsatisfactory efficiencies or selectivities.Pulse electrolysis by pulsating and programming the potentials/currents can feature unique tunability to the electrodeelectrolyte interface properties that can give rise to drastically different electrochemical behaviors compared to the steady-state counterparts.Although invented almost 100 years ago,pulse electrolysis has received little attention over the period,but has recently attracted a revived focus toward the energyefficient electrolysis.This review will summarize the history and recent efforts of pulse electrolysis in three categories:water electrolysis,CO_(2)electrolysis and other electrolysis.In each section,the advantage of pulse electrolysis over steady-state electrolysis will be discussed in detail,giving a comprehensive overview of the pulse effect on the electrolytic systems.Finally,we will provide our vision of future directions in pulse electrolysis based on previous works.展开更多
The development of high-fidelity two-qubit quantum gates is essential for digital quantum computing.Here,we propose and realize an all-microwave parametric controlled-Z(CZ)gates by coupling strength modulation in a su...The development of high-fidelity two-qubit quantum gates is essential for digital quantum computing.Here,we propose and realize an all-microwave parametric controlled-Z(CZ)gates by coupling strength modulation in a superconducting Transmon qubit system with tunable couplers.After optimizing the design of the tunable coupler together with the control pulse numerically,we experimentally realized a 100 ns CZ gate with high fidelity of 99.38%±0.34%and the control error being 0.1%.We note that our CZ gates are not affected by pulse distortion and do not need pulse correction,providing a solution for the real-time pulse generation in a dynamic quantum feedback circuit.With the expectation of utilizing our all-microwave control scheme to reduce the number of control lines through frequency multiplexing in the future,our scheme draws a blueprint for the high-integrable quantum hardware design.展开更多
Achieving highly regioselective synthesis in organic chemistry is challenging due to the uncontrollable orientation between reacting partners.External electric fields(EEFs)can influence the reactivity and selectivity ...Achieving highly regioselective synthesis in organic chemistry is challenging due to the uncontrollable orientation between reacting partners.External electric fields(EEFs)can influence the reactivity and selectivity of the substrate by causing directional adsorption.However,scalable and efficient techniques for using EEFs as“smart catalysts”have been lacking,hindering their application.In this study,we present a novel method for modifying the regioselectivity of quinoxaline-2(1H)-ones by functionalizing their C7-position using the electric double layer(EDL)theory.This approach led to moderate to good yields of the corresponding C7-thiocyanation products.DFT calculations and control experiments demonstrated that EEFs could reverse the regioselectivity of quinoxaline-2(1H)-ones,allowing the C7-thiocyanation to proceed via a radical reaction mechanism.Additionally,the resulting 7-thiocyano-1-methylquinoxaline-2(1H)-ones exhibited promising AIE properties.Our work showcases a promising strategy for achieving highly regioselective functionalization by aligning the electric field with the desired reaction/bond axis.展开更多
Modulation of the surface electron distribution is a challenging problem that determines the adsorption ability of catalytic process.Here,we address this challenge by bridging the inner and outer layers of the core–s...Modulation of the surface electron distribution is a challenging problem that determines the adsorption ability of catalytic process.Here,we address this challenge by bridging the inner and outer layers of the core–shell structure through the bridge Br atom.Carbon shell wrapped copper bromide nanorods(CuBr@C)are constructed for the first time by chemical vapour deposition with hexabromobenzene(HBB).HBB pyrolysis provides both bridge Br atom and C shells.The C shell protects the stability of the internal halide structure,while the bridge Br atom triggers the rearrangement of the surface electrons and exhibits excellent electrocatalytic activity.Impressively,the hydrogen evolution reaction(HER)activity of CuBr@C is significantly better than that of commercial N-doped carbon nanotubes,surpassing commercial Pt/C at over 200 mA·cm^(−2).Density functional theory(DFT)calculations reveal that bridge Br atoms inspire aggregation of delocalized electrons on C-shell surfaces,leading to optimization of hydrogen adsorption energy.展开更多
The Kibble-Zurek(KZ)mechanism has played a fundamental role in defect formation with universal scaling laws in nonequilibrium phase transitions.However,this theory may not accurately predict the scaling laws in inhomo...The Kibble-Zurek(KZ)mechanism has played a fundamental role in defect formation with universal scaling laws in nonequilibrium phase transitions.However,this theory may not accurately predict the scaling laws in inhomogeneous systems and slow quenching processes.Here,we present a generalized KZ mechanism for the defect formation in trapped ions with the freeze-out condition gt=b0τ(t),where g is a universal quenching velocity function and b0 is a constant.We derived a differential equationφ(x,t)to account for the frozen correlation length of a kink in an inhomogeneous system and demonstrated a smooth crossover from a fast quenching process to a slow quenching process,which agrees well with the experiments performed by Ulm et al.[Nat.Commun.4,2290(2013)]and Pyka et al.[Nat.Commun.4,2291(2013)].Furthermore,we confirmed our theoretical model using molecular dynamics simulation by solving the stochastic differential equation,showing excellent agreement with the results from the differential equation.Our theory provides a general theoretical framework for studying KZ physics in inhomogeneous systems,which has applications in other nonequilibrium platforms studied experimentally.展开更多
Information on the physicochemical properties of chemical species is an important prerequisite when performing tasks such as process design and product design.However,the lack of extensive data and high experimental c...Information on the physicochemical properties of chemical species is an important prerequisite when performing tasks such as process design and product design.However,the lack of extensive data and high experimental costs hinder the development of prediction techniques for these properties.Moreover,accuracy and predictive capabilities still limit the scope and applicability of most property estimation methods.This paper proposes a new Gaussian process-based modeling framework that aims to manage a discrete and high-dimensional input space related to molecular structure representation with the group-contribution approach.A warping function is used to map discrete input into a continuous domain in order to adjust the correlation between different compounds.Prior selection techniques,including prior elicitation and prior predictive checking,are also applied during the building procedure to provide the model with more information from previous research findings.The framework is assessed using datasets of varying sizes for 20 pure component properties.For 18 out of the 20 pure component properties,the new models are found to give improved accuracy and predictive power in comparison with other published models,with and without machine learning.展开更多
Aiming at the basic and key technical problems in prevention and control of sugarcane white leaf disease(SCWL),this study systematically overcame key technical bottleneck of prevention and control of new SCWL after 10...Aiming at the basic and key technical problems in prevention and control of sugarcane white leaf disease(SCWL),this study systematically overcame key technical bottleneck of prevention and control of new SCWL after 10 years of collaborative research,and achieved several innovative achievements.SCWL phytoplasmas newly recorded in China and the new subgroup of SCWL phytoplasmas(16SrXI-D)were discovered for the first time in Yunnan,and the whole genome analysis of the epidemic subgroup was completed.The main transmission source of SCWL pathogens has been identified as infected seed canes,and Tettigoniella viridis and Clovia conifer were newly discovered as vectors for virus transmission.The disease resistance of 25 main varieties was identified,and 10 control varieties were selected.The prevention and control strategy of"emphasizing early warning,strictly carrying out quarantine,blocking the vectors and controlling residual plants"was put forward,and a comprehensive prevention technique was established through integration of various techniques,and standardized technical regulations were formulated for demonstration application.The promotion and application of these achievements have realized scientific prevention and control of SCWL,effectively curbed the spread of SCWL,and ensured the safety of sugarcane producing areas in China,achieving great economic,social and ecological benefits and providing technical support for high-quality development,loss reduction and efficiency improvement of China's sugar industry.展开更多
High gravimetric energy density, earth-abundance, and environmental friendliness of hydrogen sources have inspired the utilization of hydrogen fuel as a clean alternative to fossil fuels. Hydrogen evolution reaction ...High gravimetric energy density, earth-abundance, and environmental friendliness of hydrogen sources have inspired the utilization of hydrogen fuel as a clean alternative to fossil fuels. Hydrogen evolution reaction (HER), a half reaction of water splitting, is crucial to the low-cost production of pure H2 fuels but necessitates the use of electrocatalysts to expedite reaction kinetics. Owing to the availability of low-cost oxygen evolution reaction (OER) catalysts for the counter electrode in alkaline media and the lack of low-cost OER catalysts in acidic media, researchers have focused on developing HER catalysts in alkaline media with high activity and stability. Nickel is well-known as an HER catalyst and continuous efforts have been undertaken to improve Ni-based catalysts as alkaline electrolyzers: In this review, we summarize earlier studies of HER activity and mechanism on Ni surfaces, along with recent progress in the optimization of the Ni-based catalysts using various modern techniques. Recently developed Ni-based HER catalysts are categorized according to their chemical nature, and the advantages as well as limitations of each category are discussed. Among all Ni-based catalysts, Ni-based alloys and Ni-based hetero-structure exhibit the most promising electrocatalytic activity and stability owing to the fine-tuning of their surface adsorption properties via a synergistic nearby element or domain. Finally, selected applications of the developed Ni-based HER catalysts are highlighted, such as water splitting, the chloralkali process, and microbial electrolysis cell.展开更多
The palea and lemma are floral organ structures unique to grasses;these structures form the hull and directly affect grain size and quality. However, the molecular mechanisms controlling the development of the hull ar...The palea and lemma are floral organ structures unique to grasses;these structures form the hull and directly affect grain size and quality. However, the molecular mechanisms controlling the development of the hull are not well understood. In this study, we characterized the rice(Oryza sativa) abnormal flower and grain1(afg1) mutant, a new allele of OsMADS6. Similar to previously characterized osmads6 alleles, in the afg1 floret, the palea lost its marginal region and acquired the lemma identity. However, in contrast to other osmads6 alleles, the afg1 mutant showed altered grain size and grain quality, with decreased total starch and amylose contents, and increased protein and soluble sugar contents. The analysis of transcriptional activity suggested that AFG1 is a transcriptional activator and may affect grain size by regulating the expression levels of several genes related to cell expansion and proliferation in the afg1 mutant. These results revealed that AFG1 plays an important role in determining palea identity and affecting grain yield and quality in rice.展开更多
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0500000)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0301200)+1 种基金the National Natural Science Foundation of China(Grant Nos.12074431,12274384,and 12374252)the Excellent Youth Foundation of Hunan Scientific Committee(Grant No.2021JJ10044).
文摘Motivated by recent realizations of spin-1 NaRb mixtures in the experiments[Phys.Rev.Lett.114,255301(2015);Phys.Rev.Lett.128,223201(2022)],we investigate heteronuclear magnetism in the Mott-insulating regime.Different from the identical mixtures where the boson statistics only admits even parity states from angular momentum composition,for heteronuclear atoms in principle all angular momentum states are allowed,which can give rise to new magnetic phases.While various magnetic phases can be developed over these degenerate spaces,the concrete symmetry breaking phases depend on not only the degree of degeneracy but also the competitions from many-body interactions.We unveil these rich phases using the bosonic dynamical mean-field theory approach.These phases are characterized by various orders,including spontaneous magnetization order,spin magnitude order,singlet pairing order,and nematic order,which may coexist specially in the regime with odd parity.Finally we address the possible parameter regimes for observing these spin-ordered Mott phases.
基金Jilin Province Science and Technology Development Program,Grant/Award Number:20190201233JCProject for Self-innovation Capability Construction of Jilin Province Development and Reform Commission,Grant/Award Number:2021C026+3 种基金Program for JLU Science and Technology Innovative Research Team,Grant/Award Numbers:JLUSTIRT,2017TD-09National Natural Science Foundation of China,Grant/Award Numbers:12034002,51872116Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province,Grant/Award Number:JC2018004Excellent Young Foundation of Harbin Normal University,Grant/Award Number:XKYQ201304。
文摘Retaining the ultrathin structure of two-dimensional materials is very important for stabilizing their catalytic performances.However,aggregation and restacking are unavoidable,to some extent,due to the van der Waals interlayer interaction of two-dimensional materials.Here,we address this challenge by preparing an origami accordion structure of ultrathin twodimensional graphitized carbon nitride(oa-C_(3)N_(4))with rich vacancies.This novel structured oa-C_(3)N_(4) shows exceptional photocatalytic activity for the CO_(2) reduction reaction,which is 8.1 times that of the pristine C_(3)N_(4).The unique structure not only prevents restacking but also increases light harvesting and the density of vacancy defects,which leads to modification of the electronic structure,regulation of the CO_(2) adsorption energy,and a decrease in the energy barrier of the carbon dioxide to carboxylic acid intermediate reaction.This study provides a new avenue for the development of stable highperformance two-dimensional catalytic materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.61805162,11774328,and 12274005)the National Key Research and Development Program of China(Grant No.2021YFA1401900)。
文摘Three-dimensional(3D)degenerate Fermi gases in the presence of spin-orbit coupling,inducing various kinds of physical findings and phenomena,have attracted tremendous attention in these years.We investigate the 3D spin-orbit coupled degenerate Fermi gases in theory and first present the analytic expression of their ground state.Our study provides an innovative perspective into understanding of the topological properties of 3D unconventional superconductors,and describes the topological phase transitions in trivial and topological phase areas.Further,such a system is provided with a richer set of Cooper pairings than traditional superconductors.The dual Cooper pairs with same spin directions emerge and exhibit peculiar behaviors,leading to topological phase transitions.Our study and discussion can be generalized to some other types of unconventional superconductors and areas of optical lattices.
基金supported by the National Key Research and Development Program of China (Grant Nos. 2017YFA0 205004, 2018YFA03066004, and 2016YFA0301700)the National Natural Science Foundation of China (Grant Nos. 11674295 and 11774328)+3 种基金the Fundamental Research Funds for the Central Universities (Grant No. WK2340000082)Anhui Initiative in Quantum Information Technologies (Grant No. AHY170000)the USTC start-up fundingthe China Government Youth 1000-Plan Talent Program
文摘Room temperature ferroelectric thin films are the key element of high-density nonvolatile memories in modern electronics. However, with the further miniaturization of the electronic devices beyond the Moore’s law, conventional ferroelectrics suffer great challenge arising from the critical thickness effect, where the ferroelectricity is unstable if the film thickness is reduced to nanometer or single atomic layer limit. Two-dimensional(2D) materials, thanks to their stable layered structure, saturate interfacial chemistry, weak interlayer couplings, and the benefit of preparing stable ultra-thin film at 2D limit, are promising for exploring 2D ferroelectricity and related device applications. Therefore, it provides an effective approach to overcome the limitation in conventional ferroelectrics with the study of 2D ferroelectricity in van der Waals(vdW) materials. In this review article,we briefly introduce recent progresses on 2D ferroelectricity in layered vdW materials. We will highlight the study on atomically thin α-In2Se3, which is an emergent ferroelectric semiconductor with the coupled in-plane and out-of-plane ferroelectricity. Furthermore, two prototype ferroelectric devices based on ferroelectric α-In2Se3 will also be reviewed.
基金the National Key R&D Program of China(Grant No.2017YFA0304300)the Chinese Academy of Sciences+6 种基金Anhui Initiative in Quantum Information TechnologiesTechnology Committee of Shanghai Municipalitythe National Natural Science Foundation of China(Grants Nos.11905217,11774326,and 11905294)the Shanghai Municipal Science and Technology Major Project(Grant No.2019SHZDZX01)the Natural Science Foundation of Shanghai(Grant No.19ZR1462700)the Key-Area Research and Development Program of Guangdong Provice(Grant No.2020B0303030001)the Youth Talent Lifting Project(Grant No.2020-JCJQ-QT-030)。
文摘High-fidelity two-qubit gates are essential for the realization of large-scale quantum computation and simulation.Tunable coupler design is used to reduce the problem of parasitic coupling and frequency crowding in manyqubit systems and thus thought to be advantageous. Here we design an extensible 5-qubit system in which center transmon qubit can couple to every four near-neighboring qubits via a capacitive tunable coupler and experimentally demonstrate high-fidelity controlled-phase(CZ) gate by manipulating central qubit and one nearneighboring qubit. Speckle purity benchmarking and cross entropy benchmarking are used to assess the purity fidelity and the fidelity of the CZ gate. The average purity fidelity of the CZ gate is 99.69±0.04% and the average fidelity of the CZ gate is 99.65±0.04%, which means that the control error is about 0.04%. Our work is helpful for resolving many challenges in implementation of large-scale quantum systems.
基金supports from the National Key R&D program of China(2019YFC1604602)supports from the National Key Basic Research Program of China(2019YFC1906700)the National Natural Science Foundation of China(21876049,51878643)。
文摘Electrochemical transformation emerges as an important solution to sustainable energy conversion and chemical production.Conventional electrolytic systems usually operate under galvanostatic or potentiostatic conditions that sometimes result in unsatisfactory efficiencies or selectivities.Pulse electrolysis by pulsating and programming the potentials/currents can feature unique tunability to the electrodeelectrolyte interface properties that can give rise to drastically different electrochemical behaviors compared to the steady-state counterparts.Although invented almost 100 years ago,pulse electrolysis has received little attention over the period,but has recently attracted a revived focus toward the energyefficient electrolysis.This review will summarize the history and recent efforts of pulse electrolysis in three categories:water electrolysis,CO_(2)electrolysis and other electrolysis.In each section,the advantage of pulse electrolysis over steady-state electrolysis will be discussed in detail,giving a comprehensive overview of the pulse effect on the electrolytic systems.Finally,we will provide our vision of future directions in pulse electrolysis based on previous works.
基金the USTC Center for Micro-and Nanoscale Research and Fabrication for supporting the sample fabricationQuantum CTek Co.,Ltd.for supporting the fabrication and the maintenance of room-temperature electronics+7 种基金supported by the National Key R&D Program of China(Grant No.2017YFA0304300)the Chinese Academy of Sciencesthe Anhui Initiative in Quantum Information Technologiesthe Technology Committee of Shanghai Municipalitythe National Natural Science Foundation of China(Grants No.11905217 and 11905294)the Natural Science Foundation of Shanghai(Grant No.19ZR1462700)he Key-Area Research and Development Program of Guangdong Province(Grant No.2020B0303030001)the China Postdoctoral Science Foundation。
文摘The development of high-fidelity two-qubit quantum gates is essential for digital quantum computing.Here,we propose and realize an all-microwave parametric controlled-Z(CZ)gates by coupling strength modulation in a superconducting Transmon qubit system with tunable couplers.After optimizing the design of the tunable coupler together with the control pulse numerically,we experimentally realized a 100 ns CZ gate with high fidelity of 99.38%±0.34%and the control error being 0.1%.We note that our CZ gates are not affected by pulse distortion and do not need pulse correction,providing a solution for the real-time pulse generation in a dynamic quantum feedback circuit.With the expectation of utilizing our all-microwave control scheme to reduce the number of control lines through frequency multiplexing in the future,our scheme draws a blueprint for the high-integrable quantum hardware design.
基金financially supported by the National Natural Science Foundation of China (22275054,52103314,21975072,and 51902106)Chenguang Plan of Shanghai Education Development Foundation (21CGA38)the Program of Shanghai Academic/Technology Research Leader (23XD1401000)。
基金supported by the National Natural Science Foundation of China(21172200,21302172)the Basic Research Training Project of Zhengzhou University(JC2020053021)supported by the National Research Foundation of Korea(CRI Project No.2018R1A3B1052702 for Jong Seung Kim)。
文摘Achieving highly regioselective synthesis in organic chemistry is challenging due to the uncontrollable orientation between reacting partners.External electric fields(EEFs)can influence the reactivity and selectivity of the substrate by causing directional adsorption.However,scalable and efficient techniques for using EEFs as“smart catalysts”have been lacking,hindering their application.In this study,we present a novel method for modifying the regioselectivity of quinoxaline-2(1H)-ones by functionalizing their C7-position using the electric double layer(EDL)theory.This approach led to moderate to good yields of the corresponding C7-thiocyanation products.DFT calculations and control experiments demonstrated that EEFs could reverse the regioselectivity of quinoxaline-2(1H)-ones,allowing the C7-thiocyanation to proceed via a radical reaction mechanism.Additionally,the resulting 7-thiocyano-1-methylquinoxaline-2(1H)-ones exhibited promising AIE properties.Our work showcases a promising strategy for achieving highly regioselective functionalization by aligning the electric field with the desired reaction/bond axis.
基金supported by Innovation Program for Quantum Science and Technology (2021ZD0300200)Shanghai Municipal Science and Technology Major Project (2019SHZDZX01)+13 种基金Special funds from Jinan Science and Technology Bureau and Jinan High Tech Zone Management Committeethe Chinese Academy of Sciences (CAS)Anhui Initiative in Quantum Information TechnologiesTechnology Committee of Shanghai MunicipalityNatural Science Foundation of Shandong Province (ZR202209080019)Key-Area Research and Development Program of Guangdong Provice (2020B0303030001)supported in part by the Japanese MEXT Quantum Leap Flagship Program (MEXT Q-LEAP,JPMXS0118069605)the support from the Youth Talent Lifting Project (2020-JCJQ-QT-030)the National Natural Science Foundation of China (12274464,and 11905294)China Postdoctoral Science Foundationthe Open Research Fund from State Key Laboratory of High Performance Computing of China (201901-01)supported by Shanghai Rising-Star Program (23QA1410000)the Youth Innovation Promotion Association of CAS (2022460)the support from THE XPLORER PRIZE。
基金the National Natural Science Foundation of China(Nos.51872116 and 12034002)Jilin Province Science and Technology Development Program(No.20210301009GX)+3 种基金Project for Self-innovation Capability Construction of Jilin Province Development and Reform Commission(No.2021C026)the Program for JLU Science and Technology Innovative Research Team(JLUSTIRT,No.2017TD-09)Jilin Province Science and Technology Development Program(No.20190201233JC)the Fundamental Research Funds for the Central Universities.
文摘Modulation of the surface electron distribution is a challenging problem that determines the adsorption ability of catalytic process.Here,we address this challenge by bridging the inner and outer layers of the core–shell structure through the bridge Br atom.Carbon shell wrapped copper bromide nanorods(CuBr@C)are constructed for the first time by chemical vapour deposition with hexabromobenzene(HBB).HBB pyrolysis provides both bridge Br atom and C shells.The C shell protects the stability of the internal halide structure,while the bridge Br atom triggers the rearrangement of the surface electrons and exhibits excellent electrocatalytic activity.Impressively,the hydrogen evolution reaction(HER)activity of CuBr@C is significantly better than that of commercial N-doped carbon nanotubes,surpassing commercial Pt/C at over 200 mA·cm^(−2).Density functional theory(DFT)calculations reveal that bridge Br atoms inspire aggregation of delocalized electrons on C-shell surfaces,leading to optimization of hydrogen adsorption energy.
基金supported by the National Natural Science Foundation of China(Grant Nos.11904099,and 11774328)Natural Science Foundation of Hunan Province of China(Grant No.2021JJ30210)Innovation Program for Quantum Science and Technology(Grant Nos.2021ZD0301600,2021ZD0301200,and 2021ZD0301500)。
文摘The Kibble-Zurek(KZ)mechanism has played a fundamental role in defect formation with universal scaling laws in nonequilibrium phase transitions.However,this theory may not accurately predict the scaling laws in inhomogeneous systems and slow quenching processes.Here,we present a generalized KZ mechanism for the defect formation in trapped ions with the freeze-out condition gt=b0τ(t),where g is a universal quenching velocity function and b0 is a constant.We derived a differential equationφ(x,t)to account for the frozen correlation length of a kink in an inhomogeneous system and demonstrated a smooth crossover from a fast quenching process to a slow quenching process,which agrees well with the experiments performed by Ulm et al.[Nat.Commun.4,2290(2013)]and Pyka et al.[Nat.Commun.4,2291(2013)].Furthermore,we confirmed our theoretical model using molecular dynamics simulation by solving the stochastic differential equation,showing excellent agreement with the results from the differential equation.Our theory provides a general theoretical framework for studying KZ physics in inhomogeneous systems,which has applications in other nonequilibrium platforms studied experimentally.
基金support from the National Natural Science Foundation of China(22150410338 and 61973268)is gratefully acknowledged.
文摘Information on the physicochemical properties of chemical species is an important prerequisite when performing tasks such as process design and product design.However,the lack of extensive data and high experimental costs hinder the development of prediction techniques for these properties.Moreover,accuracy and predictive capabilities still limit the scope and applicability of most property estimation methods.This paper proposes a new Gaussian process-based modeling framework that aims to manage a discrete and high-dimensional input space related to molecular structure representation with the group-contribution approach.A warping function is used to map discrete input into a continuous domain in order to adjust the correlation between different compounds.Prior selection techniques,including prior elicitation and prior predictive checking,are also applied during the building procedure to provide the model with more information from previous research findings.The framework is assessed using datasets of varying sizes for 20 pure component properties.For 18 out of the 20 pure component properties,the new models are found to give improved accuracy and predictive power in comparison with other published models,with and without machine learning.
基金Supported by National Natural Science Foundation of China(31760504)China Agriculture Research System of MOF and MARA(CARS-17)Special Fund for the Construction of Modern Agricultural Industrial Technology System in Yunnan Province.
文摘Aiming at the basic and key technical problems in prevention and control of sugarcane white leaf disease(SCWL),this study systematically overcame key technical bottleneck of prevention and control of new SCWL after 10 years of collaborative research,and achieved several innovative achievements.SCWL phytoplasmas newly recorded in China and the new subgroup of SCWL phytoplasmas(16SrXI-D)were discovered for the first time in Yunnan,and the whole genome analysis of the epidemic subgroup was completed.The main transmission source of SCWL pathogens has been identified as infected seed canes,and Tettigoniella viridis and Clovia conifer were newly discovered as vectors for virus transmission.The disease resistance of 25 main varieties was identified,and 10 control varieties were selected.The prevention and control strategy of"emphasizing early warning,strictly carrying out quarantine,blocking the vectors and controlling residual plants"was put forward,and a comprehensive prevention technique was established through integration of various techniques,and standardized technical regulations were formulated for demonstration application.The promotion and application of these achievements have realized scientific prevention and control of SCWL,effectively curbed the spread of SCWL,and ensured the safety of sugarcane producing areas in China,achieving great economic,social and ecological benefits and providing technical support for high-quality development,loss reduction and efficiency improvement of China's sugar industry.
文摘High gravimetric energy density, earth-abundance, and environmental friendliness of hydrogen sources have inspired the utilization of hydrogen fuel as a clean alternative to fossil fuels. Hydrogen evolution reaction (HER), a half reaction of water splitting, is crucial to the low-cost production of pure H2 fuels but necessitates the use of electrocatalysts to expedite reaction kinetics. Owing to the availability of low-cost oxygen evolution reaction (OER) catalysts for the counter electrode in alkaline media and the lack of low-cost OER catalysts in acidic media, researchers have focused on developing HER catalysts in alkaline media with high activity and stability. Nickel is well-known as an HER catalyst and continuous efforts have been undertaken to improve Ni-based catalysts as alkaline electrolyzers: In this review, we summarize earlier studies of HER activity and mechanism on Ni surfaces, along with recent progress in the optimization of the Ni-based catalysts using various modern techniques. Recently developed Ni-based HER catalysts are categorized according to their chemical nature, and the advantages as well as limitations of each category are discussed. Among all Ni-based catalysts, Ni-based alloys and Ni-based hetero-structure exhibit the most promising electrocatalytic activity and stability owing to the fine-tuning of their surface adsorption properties via a synergistic nearby element or domain. Finally, selected applications of the developed Ni-based HER catalysts are highlighted, such as water splitting, the chloralkali process, and microbial electrolysis cell.
基金supported by the Zhejiang Natural Science Foundation(LY18C130007)the National Natural Science Foundation of China(91735304)+1 种基金the Central Public-interest Scientific Institution Basal Research Fund of China National Rice Research Institute(2017RG001-4)the National Science and Technology Major Project(2016ZX08009003-003-008)。
文摘The palea and lemma are floral organ structures unique to grasses;these structures form the hull and directly affect grain size and quality. However, the molecular mechanisms controlling the development of the hull are not well understood. In this study, we characterized the rice(Oryza sativa) abnormal flower and grain1(afg1) mutant, a new allele of OsMADS6. Similar to previously characterized osmads6 alleles, in the afg1 floret, the palea lost its marginal region and acquired the lemma identity. However, in contrast to other osmads6 alleles, the afg1 mutant showed altered grain size and grain quality, with decreased total starch and amylose contents, and increased protein and soluble sugar contents. The analysis of transcriptional activity suggested that AFG1 is a transcriptional activator and may affect grain size by regulating the expression levels of several genes related to cell expansion and proliferation in the afg1 mutant. These results revealed that AFG1 plays an important role in determining palea identity and affecting grain yield and quality in rice.