Dual-active sites(DASs)catalysts have positive potential applications in broad fields because of their specific active sites and synergistic catalytic effects.Therefore,the controllable synthesis and finely regulating...Dual-active sites(DASs)catalysts have positive potential applications in broad fields because of their specific active sites and synergistic catalytic effects.Therefore,the controllable synthesis and finely regulating the activity of such catalysts has become a hot research area for now.In this work,we developed a pyrolysis-etching-hydrogen activation strategy to prepare the DASs catalysts involving single-atom Cu and B on N-doped porous carbon material(Cu_(1)-B/NPC).Numerous systematic characterization and density functional theoretical(DFT)calculation results showed that the Cu and B existed as Cu-N4 porphyrinlike unit and B-N_(3)unit in the obtained catalyst.DFT calculations further revealed that single-atom Cu and B sites were linked by bridging N atoms to form the Cu_(1)-B-N6 dual-sites.The Cu_(1)-B/NPC catalyst was more effective than the single-active site catalysts with B-N_(3)sites in NPC(B/NPC)and Cu-N4 porphyrin-like sites in NPC(Cu_(1)/NPC),respectively,for the dehydrogenative coupling of dimethylphenylsilane(DiMPSH)with various alcohols,performing the great activity(>99%)and selectivity(>99%).The catalytic performances of the Cu_(1)-B/NPC catalyst remained nearly unchanged after five cycles,also indicating its outstanding recyclability.DFT calculations showed that the Cu_(1)-B-N6 dual-sites exhibited the lowest energy profile on the potential energy surface than that of sole B-N_(3)and Cu-N4 porphyrin-like sites.Furthermore,the rate-limiting step of dehydrogenation of DiMPSH on Cu_(1)-B-N6 dual-sites also showed a much lower activation energy than the other two single sites.Benefitting from the superiority of the Cu_(1)-B-N6 dual-sites,the Cu_(1)-B/NPC catalyst can also be used for CO_(2)electroreduction to produce syngas.Thus,DASs catalysts are promising to achieve multifunctional catalytic properties and have aroused positive attention in the field of catalysis.展开更多
Multifunctional drug delivery systems(DDSs)have shown great prospects in overcoming the heterogeneous barrier of delivery drugs to the complex tumor microenvironment(TME).In this study,multifunctional AS/Ge-pNAB micro...Multifunctional drug delivery systems(DDSs)have shown great prospects in overcoming the heterogeneous barrier of delivery drugs to the complex tumor microenvironment(TME).In this study,multifunctional AS/Ge-pNAB microgels with dual-active targeting,triple environment responsiveness,and fluorescence imaging capability were prepared through a straightforward procedure.This was aimed to improve the antitumor therapeutic application of gambogic acid(GA)based on the biological characteristics of TME.The microgels have a uniform double-layer structure with aptamer in the outer layer which helps in recognizing receptors on the tumor cells.The GA loaded nano-herb exhibited environment-responsive drug release profiles under acidic pH,reductant and high temperature.The nano-herb significantly improved the accumulation of GA in tumor sites through the synergistic combination of the enhanced permeability and retention effect and dual-ligand mediated internalization.Then,it accelerated intracellular drug release and killed tumor cells.Therefore,the nano-herb had specific therapeutic effects on the tumor in vitro and in vivo as they remarkably inhibited tumor growth while depicting optimal biosafety and lower levels of off-target toxicity.Overall,these findings demonstrate the great potential of the multifunctional AS/Ge-pNAB microgels for precisely targeted GA delivery and open a new avenue for the facile preparation of multifunctional DDSs.展开更多
The rational control of the active site of metal-organic frameworks(MOFs)derived nanomaterials is essential to build efficient bifunctional oxygen reduction/evolution reaction(ORR/OER)catalysts.Accordingly,through des...The rational control of the active site of metal-organic frameworks(MOFs)derived nanomaterials is essential to build efficient bifunctional oxygen reduction/evolution reaction(ORR/OER)catalysts.Accordingly,through designing and constructing a Co_(3)O_(4)-Co heterostructure embedded in Co,N co-doped carbon polyhedra derived(Co_(3)O_(4)-Co@NC)from the in-situ compositions of ZIF-67 and cobalt nanocrystals synthesized by the strategy of in-situ NaBH4 reduction,the dual-active site(Co_(3)O_(4)-Co and Co-N_(x))is synchronously realized in a MOFs derived nanomaterials.The formed Co_(3)O_(4)-Co@NC shows excellent bifunctional electrocatalytic activity with ultra-small potential gap(ΔE=E_(j=10)(OER)–E_(1/2)(ORR))of 0.72 V,which surpasses the commercial Pt/C and RuO_(2) catalysts.The theory calculation results reveal that the excellent bifunctional electrocatalytic activity can be attributed to the charge redistribution of Co of Co-N_(x) induced by the synergistic effects of well-tuned active sites of Co_(3)O_(4)-Co nanoparticle and Co-N_(x),thus optimizing the rate-determining step of the desorption of O_(2)^(*)intermediate in ORR and OH^(*)intermediate in OER.The rechargeable Zn-air batteries with our bifunctional catalysts exhibit superior performance as well as high cycling stability.This simple-effective optimization strategy offers prospects for tuning the active site of MOF derived bifunctional catalyst in electrochemical energy devices.展开更多
The presence of renewable energy resources in LV distribution networks may lead to a distribution transformer,also known as a Smart Transformer(ST),experiencing the bidirectional power flow.Therefore,the ST must have ...The presence of renewable energy resources in LV distribution networks may lead to a distribution transformer,also known as a Smart Transformer(ST),experiencing the bidirectional power flow.Therefore,the ST must have the capability to operate in both directions.However,the reverse power is less as compared to the forward power,thus the design of ST with the same capacity in both directions increases the hardware cost and decreases the system efficiency.This paper proposes a Hybrid-modular-ST(H-ST),composed of a mixed use of single active bridge-based series resonant converter and dual active bridge instead of complete use of uni-or bi-directional converter adopted in the conventional solid-state-transformer.Based on the proposed H-ST,the impacts of power imbalance among cascaded modules in reverse operation mode are analyzed and then an effective solution based on reactive power compensation combined with the characteristics of the proposed architecture is adopted.The simulation and experimental results clearly validate the effectiveness and feasibility of the theoretical analyses.展开更多
The design of high-performance catalysts is the key to the efficient utilization of hydrogen energy.In this work,a PdCu nanoalloy was successfully anchored on TiO_(2)encapsulated with carbon to construct a catalyst.Ou...The design of high-performance catalysts is the key to the efficient utilization of hydrogen energy.In this work,a PdCu nanoalloy was successfully anchored on TiO_(2)encapsulated with carbon to construct a catalyst.Outstanding kinetics of the hydrolysis of ammonia borane(turnover frequency of 279 mol·min^(-1·)mol_(Pd)^(-1))ranking the third place among Pd-based catalysts was achieved in the absence of alkali.Both experimental research and theoretical calculations reveal a lower activation energy of the B-H bond on the PdCu nanoalloy catalyst than that on pristine Pd and a lower activation energy of the O-H bond than that on pristine Cu.The redistribution of d electron and the shift of the d-band center play a critical role in increasing the electron density of Pd and improving the catalytic performances of Pd_(0.1)Cu_(0.9)/TiO_(2)-porous carbon(Pd_(0.1)Cu_(0.9)/T-PC).This work provides novel insights into highly dual-active alloys and sheds light on the mechanism of dual-active sites in promoting borohydride hydrolysis.展开更多
The electric vehicle(EV)charging station is a critical part of the infrastructure for the wide adoption of EVs.Realtime simulation of an EV station plays an essential role in testing its operation under different oper...The electric vehicle(EV)charging station is a critical part of the infrastructure for the wide adoption of EVs.Realtime simulation of an EV station plays an essential role in testing its operation under different operating modes.However,the large numbers of high-frequency power electronic switches contained in EV chargers pose great challenges for real-time simulation.This paper proposes a compact electromagnetic transient program(C-EMTP)algorithm for FPGA-based real-time simulation of an EV station with multiple high-frequency chargers.The C-EMTP algorithm transforms the traditional EMTP algorithm into two parallel sub-tasks only consisting of simple matrix operations,to fully utilize the high parallelism of FPGA.The simulation time step can be greatly reduced compared with that of the traditional EMTP algorithm,and so the simulation accuracy for high-frequency power electronics is improved.The EV chargers can be decoupled with each other and simulated in parallel.A CPU-FPGA-based realtime simulation platform is developed and the proposed simulation of the EV station is implemented.The control strategy is simulated in a CPU with 100μs time-step,while the EV station circuit topology is simulated in a single FPGA with a 250 ns time-step.In the case studies,the EV station consists of a two-level rectifier and five dual-active bridge(DAB)EV chargers.It is tested under different scenarios,and the real-time simulation results are validated using PSCAD/EMTDC.展开更多
基金supported by the National Natural Science Foundation of China(Nos.51902003,22002085,21771003,21501004)the University Synergy Innovation Program of Anhui Province(No.GXXT-2021-020)+4 种基金the Anhui Province Natural Science Foundation(Nos.2108085QB71 and 2008085QB53)the Natural Science Research Project of Anhui Province Education Department(No.KJ2019A0581)the Open Project of Key Laboratory of Metallurgical Emission Reduction&Resources Recycling of Ministry of Education(No.JKF21-03)the Open Foundation of Anhui Laboratory of Clean Catalytic Engineering(No.LCCE-01)the Open Research Funds of Jiangxi Province Engineering Research Center of Ecological Chemical Industry(STKF2109).
文摘Dual-active sites(DASs)catalysts have positive potential applications in broad fields because of their specific active sites and synergistic catalytic effects.Therefore,the controllable synthesis and finely regulating the activity of such catalysts has become a hot research area for now.In this work,we developed a pyrolysis-etching-hydrogen activation strategy to prepare the DASs catalysts involving single-atom Cu and B on N-doped porous carbon material(Cu_(1)-B/NPC).Numerous systematic characterization and density functional theoretical(DFT)calculation results showed that the Cu and B existed as Cu-N4 porphyrinlike unit and B-N_(3)unit in the obtained catalyst.DFT calculations further revealed that single-atom Cu and B sites were linked by bridging N atoms to form the Cu_(1)-B-N6 dual-sites.The Cu_(1)-B/NPC catalyst was more effective than the single-active site catalysts with B-N_(3)sites in NPC(B/NPC)and Cu-N4 porphyrin-like sites in NPC(Cu_(1)/NPC),respectively,for the dehydrogenative coupling of dimethylphenylsilane(DiMPSH)with various alcohols,performing the great activity(>99%)and selectivity(>99%).The catalytic performances of the Cu_(1)-B/NPC catalyst remained nearly unchanged after five cycles,also indicating its outstanding recyclability.DFT calculations showed that the Cu_(1)-B-N6 dual-sites exhibited the lowest energy profile on the potential energy surface than that of sole B-N_(3)and Cu-N4 porphyrin-like sites.Furthermore,the rate-limiting step of dehydrogenation of DiMPSH on Cu_(1)-B-N6 dual-sites also showed a much lower activation energy than the other two single sites.Benefitting from the superiority of the Cu_(1)-B-N6 dual-sites,the Cu_(1)-B/NPC catalyst can also be used for CO_(2)electroreduction to produce syngas.Thus,DASs catalysts are promising to achieve multifunctional catalytic properties and have aroused positive attention in the field of catalysis.
基金financially supported by the National Natural Science Foundation of China(Nos.21907076 and 31901908)Natural Science Foundation of Tianjin(No.22JCQNJC01570)Scientific Project of Tianjin Municipal Education Commission(No.2022KJ026).
文摘Multifunctional drug delivery systems(DDSs)have shown great prospects in overcoming the heterogeneous barrier of delivery drugs to the complex tumor microenvironment(TME).In this study,multifunctional AS/Ge-pNAB microgels with dual-active targeting,triple environment responsiveness,and fluorescence imaging capability were prepared through a straightforward procedure.This was aimed to improve the antitumor therapeutic application of gambogic acid(GA)based on the biological characteristics of TME.The microgels have a uniform double-layer structure with aptamer in the outer layer which helps in recognizing receptors on the tumor cells.The GA loaded nano-herb exhibited environment-responsive drug release profiles under acidic pH,reductant and high temperature.The nano-herb significantly improved the accumulation of GA in tumor sites through the synergistic combination of the enhanced permeability and retention effect and dual-ligand mediated internalization.Then,it accelerated intracellular drug release and killed tumor cells.Therefore,the nano-herb had specific therapeutic effects on the tumor in vitro and in vivo as they remarkably inhibited tumor growth while depicting optimal biosafety and lower levels of off-target toxicity.Overall,these findings demonstrate the great potential of the multifunctional AS/Ge-pNAB microgels for precisely targeted GA delivery and open a new avenue for the facile preparation of multifunctional DDSs.
基金The authors acknowledge support from the National Natural Science Foundation of China(No.21875039)Minjiang Professorship(XRC-1677)+1 种基金Fujian province’s high level innovative and entrepreneurial talents(No.50012709)the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(No.SKLPEE-201814),Fuzhou University.
文摘The rational control of the active site of metal-organic frameworks(MOFs)derived nanomaterials is essential to build efficient bifunctional oxygen reduction/evolution reaction(ORR/OER)catalysts.Accordingly,through designing and constructing a Co_(3)O_(4)-Co heterostructure embedded in Co,N co-doped carbon polyhedra derived(Co_(3)O_(4)-Co@NC)from the in-situ compositions of ZIF-67 and cobalt nanocrystals synthesized by the strategy of in-situ NaBH4 reduction,the dual-active site(Co_(3)O_(4)-Co and Co-N_(x))is synchronously realized in a MOFs derived nanomaterials.The formed Co_(3)O_(4)-Co@NC shows excellent bifunctional electrocatalytic activity with ultra-small potential gap(ΔE=E_(j=10)(OER)–E_(1/2)(ORR))of 0.72 V,which surpasses the commercial Pt/C and RuO_(2) catalysts.The theory calculation results reveal that the excellent bifunctional electrocatalytic activity can be attributed to the charge redistribution of Co of Co-N_(x) induced by the synergistic effects of well-tuned active sites of Co_(3)O_(4)-Co nanoparticle and Co-N_(x),thus optimizing the rate-determining step of the desorption of O_(2)^(*)intermediate in ORR and OH^(*)intermediate in OER.The rechargeable Zn-air batteries with our bifunctional catalysts exhibit superior performance as well as high cycling stability.This simple-effective optimization strategy offers prospects for tuning the active site of MOF derived bifunctional catalyst in electrochemical energy devices.
基金supported in part by National Key Research&Development Project of China(2017YFE0134300)in part by Shanghai 2022 Science and Technology Innovation Action Plan-Star Cultivation(Sailing Program)(22YF1415700)in part by the National Natural Science Foundation of China under Grant 52307215.
文摘The presence of renewable energy resources in LV distribution networks may lead to a distribution transformer,also known as a Smart Transformer(ST),experiencing the bidirectional power flow.Therefore,the ST must have the capability to operate in both directions.However,the reverse power is less as compared to the forward power,thus the design of ST with the same capacity in both directions increases the hardware cost and decreases the system efficiency.This paper proposes a Hybrid-modular-ST(H-ST),composed of a mixed use of single active bridge-based series resonant converter and dual active bridge instead of complete use of uni-or bi-directional converter adopted in the conventional solid-state-transformer.Based on the proposed H-ST,the impacts of power imbalance among cascaded modules in reverse operation mode are analyzed and then an effective solution based on reactive power compensation combined with the characteristics of the proposed architecture is adopted.The simulation and experimental results clearly validate the effectiveness and feasibility of the theoretical analyses.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.22279118,22279117,52071135,51871090,and U1804135)the Fundamental Research Funds for the Universities of Henan Province(No.NSFRF220201).
文摘The design of high-performance catalysts is the key to the efficient utilization of hydrogen energy.In this work,a PdCu nanoalloy was successfully anchored on TiO_(2)encapsulated with carbon to construct a catalyst.Outstanding kinetics of the hydrolysis of ammonia borane(turnover frequency of 279 mol·min^(-1·)mol_(Pd)^(-1))ranking the third place among Pd-based catalysts was achieved in the absence of alkali.Both experimental research and theoretical calculations reveal a lower activation energy of the B-H bond on the PdCu nanoalloy catalyst than that on pristine Pd and a lower activation energy of the O-H bond than that on pristine Cu.The redistribution of d electron and the shift of the d-band center play a critical role in increasing the electron density of Pd and improving the catalytic performances of Pd_(0.1)Cu_(0.9)/TiO_(2)-porous carbon(Pd_(0.1)Cu_(0.9)/T-PC).This work provides novel insights into highly dual-active alloys and sheds light on the mechanism of dual-active sites in promoting borohydride hydrolysis.
基金supported by China Postdoctoral Science Foundation(BX20200221,2020 M671122)National Key Research and Development Program of China(2019YFE012784)National Natural Science Foundation of China(51877133).
文摘The electric vehicle(EV)charging station is a critical part of the infrastructure for the wide adoption of EVs.Realtime simulation of an EV station plays an essential role in testing its operation under different operating modes.However,the large numbers of high-frequency power electronic switches contained in EV chargers pose great challenges for real-time simulation.This paper proposes a compact electromagnetic transient program(C-EMTP)algorithm for FPGA-based real-time simulation of an EV station with multiple high-frequency chargers.The C-EMTP algorithm transforms the traditional EMTP algorithm into two parallel sub-tasks only consisting of simple matrix operations,to fully utilize the high parallelism of FPGA.The simulation time step can be greatly reduced compared with that of the traditional EMTP algorithm,and so the simulation accuracy for high-frequency power electronics is improved.The EV chargers can be decoupled with each other and simulated in parallel.A CPU-FPGA-based realtime simulation platform is developed and the proposed simulation of the EV station is implemented.The control strategy is simulated in a CPU with 100μs time-step,while the EV station circuit topology is simulated in a single FPGA with a 250 ns time-step.In the case studies,the EV station consists of a two-level rectifier and five dual-active bridge(DAB)EV chargers.It is tested under different scenarios,and the real-time simulation results are validated using PSCAD/EMTDC.