Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pos...Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pose ongoing challenges.Herein,we systematically explore the synergistic catalytic effect of incorporating Au with boron clusters for accelerating NRR kinetics.An in-situ abinitio strategy is employed to construct B-doped Au nanoparticles(2-6 nm in diameter)loaded on BO_(x) substrates(AuBO_(x)),in which B not only modulates the surface electronic structure of Au but also forms strong coupling interactions to stabilize the nanoparticles.The electrochemical results show that Au-BO_(x) possesses excellent NRR activity(NH_(3) yield of 48.52μg h^(-1)mg_(cat)^(-1),Faraday efficiency of 56.18%),and exhibits high stability and reproducibility throughout the electrocatalytic NRR process.Theoretical calculations reveal that the introduction of B induces the formation of both Au dangling bond and Au-B coupling bond.which considerably facilitates the hydrogenation of~*N_(2)^(-)~*NH_(3).The present work provides a new avenue for the preparation of metal-boron materials achieved by one-step reduction and doping process,utilizing boron clusters as reducing and stabilizing agents.展开更多
In this paper,a comparative study for kernel-PCA based linear parameter varying(LPV)model approximation of sufficiently nonlinear and reasonably practical systems is carried out.Linear matrix inequalities(LMIs)to be s...In this paper,a comparative study for kernel-PCA based linear parameter varying(LPV)model approximation of sufficiently nonlinear and reasonably practical systems is carried out.Linear matrix inequalities(LMIs)to be solved in LPV controller design process increase exponentially with the increase in a number of scheduling variables.Fifteen kernel functions are used to obtain the approximate LPV model of highly coupled nonlinear systems.An error to norm ratio of original and approximate LPV models is introduced as a measure of accuracy of the approximate LPV model.Simulation examples conclude the effectiveness of kernel-PCA for LPV model approximation as with the identification of accurate approximate LPV model,computation complexity involved in LPV controller design is decreased exponentially.展开更多
The rational design and synthesis of multimetallic nanostructures(NSs)with rich defects are of significant importance for their diverse applications,including their promising usage as high-efficiency catalysts for alc...The rational design and synthesis of multimetallic nanostructures(NSs)with rich defects are of significant importance for their diverse applications,including their promising usage as high-efficiency catalysts for alcohol oxidation reaction as a fuel source.Here,we report the synthesis of defect-rich,candied haws-shaped AuPtNi NSs using presynthesized gold(Au)nanowires as templates.The ternary AuPtNi NSs possess rich defects such as twins,stacking faults,and atomic steps.Impressively,the AuPtNi NSs exhibited excellent mass and specific activities toward methanol and ethanol oxidation reactions under acidic conditions.Our current work paves the way for the rational design and controlled synthesis of defect-rich multimetallic NSs to boost their performances in catalytic reactions.展开更多
基金supported by the National Natural Science Foundation of China(22075133,62288102,22375091,21971114,and 21701086)the Jiangsu Provincial Funds(BX2022013)。
文摘Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pose ongoing challenges.Herein,we systematically explore the synergistic catalytic effect of incorporating Au with boron clusters for accelerating NRR kinetics.An in-situ abinitio strategy is employed to construct B-doped Au nanoparticles(2-6 nm in diameter)loaded on BO_(x) substrates(AuBO_(x)),in which B not only modulates the surface electronic structure of Au but also forms strong coupling interactions to stabilize the nanoparticles.The electrochemical results show that Au-BO_(x) possesses excellent NRR activity(NH_(3) yield of 48.52μg h^(-1)mg_(cat)^(-1),Faraday efficiency of 56.18%),and exhibits high stability and reproducibility throughout the electrocatalytic NRR process.Theoretical calculations reveal that the introduction of B induces the formation of both Au dangling bond and Au-B coupling bond.which considerably facilitates the hydrogenation of~*N_(2)^(-)~*NH_(3).The present work provides a new avenue for the preparation of metal-boron materials achieved by one-step reduction and doping process,utilizing boron clusters as reducing and stabilizing agents.
文摘In this paper,a comparative study for kernel-PCA based linear parameter varying(LPV)model approximation of sufficiently nonlinear and reasonably practical systems is carried out.Linear matrix inequalities(LMIs)to be solved in LPV controller design process increase exponentially with the increase in a number of scheduling variables.Fifteen kernel functions are used to obtain the approximate LPV model of highly coupled nonlinear systems.An error to norm ratio of original and approximate LPV models is introduced as a measure of accuracy of the approximate LPV model.Simulation examples conclude the effectiveness of kernel-PCA for LPV model approximation as with the identification of accurate approximate LPV model,computation complexity involved in LPV controller design is decreased exponentially.
基金X.C.and Z.Z.contributed equally to this work.This work was supported financially by MOE under AcRF Tier 2(grant nos.MOE2015-T2-2-057,MOE2016-T2-2-103,and MOE2017-T2-1-162)AcRF Tier 1(grant nos.2016-T1-002-051,2017-T1-001-150,and 2017-T1-002-119)+4 种基金NTU under Start-Up Grant(no.M4081296.070.500000)Agency for Science,Technology and Research(A*STAR)under its AME IRG(Project No.A1783c0009)in Singapore.L.G.acknowledges the Key Research Program of Frontier Sciences,CAS(grant no.QYZDB-SSW-JSC035)National Natural Science Foundation of China(grant nos.51672307 and 51421002)We are thankful to the Facility for Analysis,Characterization,Testing and Simulation,Nanyang Technological University,Singapore,for the use of their electron microscopy(and/or X-ray)facilities.We would also like to thank 1W1B beamline of Beijing Synchrotron Radiation Facility(BSRF)for supporting this project.H.Z.thanks the support from ITC via the Hong Kong Branch of National Precious Metals Material Engineering Research Center and the Start-Up Grant from the City University of Hong Kong.This study used resources of the Advanced Photon Source,an Office of the Science User Facility,operated by the U.S.Department of Energy(DOE)Office of Science by Argonne National Laboratory and was supported by the U.S.DOE under contract no.DE-AC02-06CH11357the Canadian Light Source and its funding partners.This research also used 7-BM of the National Synchrotron Light Source II,U.S.DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no.DE-SC0012704.
文摘The rational design and synthesis of multimetallic nanostructures(NSs)with rich defects are of significant importance for their diverse applications,including their promising usage as high-efficiency catalysts for alcohol oxidation reaction as a fuel source.Here,we report the synthesis of defect-rich,candied haws-shaped AuPtNi NSs using presynthesized gold(Au)nanowires as templates.The ternary AuPtNi NSs possess rich defects such as twins,stacking faults,and atomic steps.Impressively,the AuPtNi NSs exhibited excellent mass and specific activities toward methanol and ethanol oxidation reactions under acidic conditions.Our current work paves the way for the rational design and controlled synthesis of defect-rich multimetallic NSs to boost their performances in catalytic reactions.