Metallic layered transition metal dichalcogenides(TMDs)nanomaterials based on Group 5 transition metals are attracting substantial interests as alternative catalysts for hydrogen evolution reaction(HER).However,contro...Metallic layered transition metal dichalcogenides(TMDs)nanomaterials based on Group 5 transition metals are attracting substantial interests as alternative catalysts for hydrogen evolution reaction(HER).However,controllable preparation of tantalum diselenide(TaSe2)remains challenging,which has hindered the exploration on its application in HER.Herein,we develop a facile method named surface-assisted chemical vapor transport(SACVT)for controllable synthesis of TaSe2 plates and nanobelts,by regulating the molar ratio of selenium to tantalum and reaction temperature.Unique quasi-arrays and self-supported structure help TaSe2 nanobelt own more active sites and higher ability of charge transfer,so it is superior to TaSe2 plate in electrocatalytic HER.Interestingly,they both exhibit the ability to optimize their morphologies upon cycling for dramatically improved and robust electrocatalytic performance.The selfoptimized structures can increase the effective active surface by exposing more active sites on the basal-planes and edges,shorten the interlayer electron-transfer pathways at a thinned domain,and accelerate the charge transfer,which mainly derive from high basal-plane activity and weak interaction between layers of metallic TaSe2.This work provides a reliable way for controllable synthesis of different TaSe2 structures,motivating further efforts to explore new high-efficiency catalysts in the large family of metallic TMDs for electrochemical energy conversion.展开更多
Today＇s production systems are demanded to exhibit an increased flexibility and mutability in order to deal with dynamically changing conditions, objectives and an increasing number of product variants within industr...Today＇s production systems are demanded to exhibit an increased flexibility and mutability in order to deal with dynamically changing conditions, objectives and an increasing number of product variants within industrial turbulent environments. Flexible automated systems are requested in order to improve dynamic production efficiency, e.g. robot-based hardware and PC-based controllers, but these usually induce a significantly higher production complexity, whereby the efforts for planning and programming, but also setups and reconfiguration, expand. In this paper a definition and some concepts of self-optimizing assembly systems are presented to describe possible ways to reduce the planning efforts in complex production systems. The concept of self-optimization in assembly systems will be derived from a theoretical approach and will be transferred to a specific application scenario---the automated assembly of a miniaturized solid state laser--where the challenges of unpredictable influences from e.g. component tolerances can be overcome by the help of self-optimization.展开更多
QoS-aware service composition is aimed to maximize the global QoS of a composite service when selecting candidate services.In a context sensitive service execution environment in pervasive computing,the context inform...QoS-aware service composition is aimed to maximize the global QoS of a composite service when selecting candidate services.In a context sensitive service execution environment in pervasive computing,the context information for service composition is not static:device,policy,and user constraints,and QoS requirements may change,new services may be deployed,old ones withdrawn,or existing ones change their QoS parameters.This results in the current service composition plan failing or its QoS degrading from the optimum.In this paper,a runtime self-optimizing service composition framework is proposed.An implementation of a prototype for this framework is presented,addressing the issues of reducing extra delay while increasing global QoS in service composition in a dynamic context environment.Three service re-plan algorithms are compared that can be used in dynamic context environment,i.e.,minimal-conflict hill-climbing repair genetic algorithm(MCHC-repair GA),an improved penalty-based GA,and our multi-population conflicts sorted repair genetic algorithm(MP-CS-repair GA),as well as three kinds of service composition mechanisms-with backup,without backup,and our context-aware service re-selection mechanisms.The results show that our MP-CS-repair GA and context-aware service re-selection method can reduce more extra delay while acquiring a higher global QoS for the composite service in a context sensitive environment.This context-aware service re-selection mechanism also shows some adaptability to different context change frequencies and user requirements for reducing computation cost in the self-optimizing process.展开更多
In this paper, a novel exact fixed-node quantum Monte Carlo (EFNQMC) algorithm was proposed, which is a self-optimizing and self-improving procedure. In contrast to the previous EFNQMC method, the importance function ...In this paper, a novel exact fixed-node quantum Monte Carlo (EFNQMC) algorithm was proposed, which is a self-optimizing and self-improving procedure. In contrast to the previous EFNQMC method, the importance function of this method is optimized synchronistically in the diffusion procedure, but not before beginning the EFNQMC computation. In order to optimize the importance function, the improved steepest descent technique is used, in which the step size is automatically adjustable. The procedure is quasi-Newton type and converges super linearly. The present method also uses a novel trial function, which has correct electron-electron and electron-nucleus cusp conditions. The novel EFNQMC algorithm and the novel trial function are employed to calculate the energies of 1 1A 1 state of CH 2, 1A g state of C 8 and the ground-states of H 2, LiH, Li 2 and H 2O.展开更多
The demand for clean and sustainable energy has encouraged the production of hydrogen from water electrolyzers.To overcome the obstacle to improving the efficiency of water electrolyzers,it is highly desired to fabric...The demand for clean and sustainable energy has encouraged the production of hydrogen from water electrolyzers.To overcome the obstacle to improving the efficiency of water electrolyzers,it is highly desired to fabricate active electrocatalysts for the sluggish oxygen evolution process.However,there is generally an intrinsic gap between the as-prepared and real electrocatalysts due to structure evolution under the oxidative reaction conditions.Here,we combine in-situ anionic leaching and atomic deposition to realize single-atom catalysts with self-optimized structures.The introduced F ions facilitate structural transformation from Co(OH)xF into CoOOH(F),which generates an amorphous edge surface to provide more anchoring sites for Ir single atoms.Meanwhile,the in-situ anionic leaching of F ions elevates the Co valence state of Ir_(1)/CoOOH(F)more significantly than the counterpart without F ions(Ir_(1)/CoOOH),leading to stronger adsorption of oxygenated intermediates.As revealed by electrochemical measurements,the increased Ir loading together with the favored adsorption of*OH intermediates improve the catalytic activity of Ir_(1)/CoOOH(F).Specifically,Ir_(1)/CoOOH(F)delivered a current density of 10 mA cm-2at an overpotential of 238 mV,being lower than 314 mV for Ir_(1)/CoOOH.The results demonstrated the facility of the in-situ optimization process to optimize catalyst structure for improved performance.展开更多
The copper disc casting machine is core equipment for producing copper anode plates in the copper metallurgy industry.The copper disc casting machine casting package motion curve(CPMC) is significant for precise casti...The copper disc casting machine is core equipment for producing copper anode plates in the copper metallurgy industry.The copper disc casting machine casting package motion curve(CPMC) is significant for precise casting and efficient production.However,the lack of exact casting modeling and real-time simulation information severely restricts dynamic CPMC optimization.To this end,a liquid copper droplet model describes the casting package copper flow pattern in the casting process.Furthermore,a CPMC optimization model is proposed for the first time.On top of this,a digital twin dual closed-loop self-optimization application framework(DT-DCS) is constructed for optimizing the copper disc casting process to achieve self-optimization of the CPMC and closed-loop feedback of manufacturing information during the casting process.Finally,a case study is carried out based on the proposed methods in the industrial field.展开更多
Cognitive optical network is the intermediate to combine artificial intelligence technology with network,and also the important network technology to promote network intelligence level constantly.In the paper,it analy...Cognitive optical network is the intermediate to combine artificial intelligence technology with network,and also the important network technology to promote network intelligence level constantly.In the paper,it analyzes the cognitive optical network structure with the application of artificial intelligence technology by starting from the basic conditions of cognitive network and cognitive optional network on the basis of fully understanding the connotation of cognitive network and cognitive optical network,and explores its self-governance functions,so as to better realize the self-optimization and self-configuration of network.展开更多
The pharmaceutical industry is now paying increased attention to continuous manufacturing.While the revolution to continuous and automated manufacturing is deepening in most of the top pharma companies in the world,th...The pharmaceutical industry is now paying increased attention to continuous manufacturing.While the revolution to continuous and automated manufacturing is deepening in most of the top pharma companies in the world,the advancement of automated pharmaceutical continuous manufacturing in China is relatively slow due to some key challenges including the lack of knowledge on the related technologies and shortage of qualified personnels.In this review,emphasis is given to two of the crucial technologies in automated pharmaceutical continuous manufacturing,i.e.,process analytical technology(PAT)and self-optimizing algorithm.Research work published in recent 5 years employing advanced PAT tools and self-optimization algorithms is introduced,which represents the great progress that has been made in automated pharmaceutical continuous manufacturing.展开更多
In addition to the electron transfer,the appropriate H-adsorption affinity of active centers on the metal cocatalyst surface is quite important for high hydrogen-production activity of cocatalyst-modified photo-cataly...In addition to the electron transfer,the appropriate H-adsorption affinity of active centers on the metal cocatalyst surface is quite important for high hydrogen-production activity of cocatalyst-modified photo-catalysts.The typical Cu and Ru metal cocatalysts clearly exhibit a weak Cu-H bond and a strong Ru-H bond,respectively,resulting in limited activity for photocatalytic H_(2)evolution.In this work,an ingenious strategy of self-optimized H-adsorption affinity in CuRu alloy cocatalyst is developed to simultaneously reinforce the Cu-H bond and weaken the Ru-H bond by the intrinsic electron transfer from Cu to Ru atom.The CuRu alloy nanoparticles(2-3 nm)were deposited on the TiO_(2)surface to prepare CuRu/TiO_(2)through a one-step photoreduction method.Photocatalytic tests exhibited that the highest H_(2)-production rate of CuRu/TiO_(2)photocatalyst reached up to 5.316 mmol h^(-1)g^(-1),which was 24.80,1.86,and 2.60 times higher than that of the TiO_(2),Cu/TiO_(2),and Ru/TiO_(2),respectively.Based on the characterization results and theoretical calculations,the CuRu alloy cocatalyst exhibits excellent self-optimized H-adsorption affinity via the spontaneous electron transfer from Cu to Ru atom,which can greatly accelerate the photocatalytic H_(2)-production rate of TiO_(2).This work provides a feasible idea for the self-optimized H-adsorption affinity of metal active sites in the photocatalytic H_(2)-generation field.展开更多
In this paper we proposed a novel exact fixed-node quantum Monte Carlo (EFNQMC) algorithm, which is a self-optimizing and self-improving procedure. In contrast to the previous EFNQMC method, the trial function is opti...In this paper we proposed a novel exact fixed-node quantum Monte Carlo (EFNQMC) algorithm, which is a self-optimizing and self-improving procedure. In contrast to the previous EFNQMC method, the trial function is optimized synchronistically in the diffusion procedure, but not before the beginning of EFNQMC computation. In order to optimize the trial function, the improved steepest descent technique is used, in which the step size is automatically adjustable. The procedure is quasi-Newton and converges super linearly. We also use a novel trial function, which has correct electron-electron and electron-nucleus cusp conditions. The novel EFNQMC algorithm and the novel trial function are employed to calculate the energies of 11 A1 state of CH2, 1Ag state of C8 and the ground-states of H2, LiH, Li2, H2O, respectively. The test results show that both the novel algorithm and the trial function proposed in the present paper are very excellent.展开更多
Aqueous zinc-ion batteries(AZIBs)have attracted widespread attention due to the advantages of high safety and environmental friendliness.Although V_(2)O_(3) is a promising cathode,the strong electrostatic interaction ...Aqueous zinc-ion batteries(AZIBs)have attracted widespread attention due to the advantages of high safety and environmental friendliness.Although V_(2)O_(3) is a promising cathode,the strong electrostatic interaction between Zn^(2+) and V_(2)O_(3) crystal,and the sluggish reaction kinetics still limit their application in AZIBs.Herein,the oxygen defects rich V_(2)O_(3) with conducive poly(3,4-ethylenedioxythiophene)(PEDOT)shell(V_(2)O_(3)-Od@PEDOT)was fabricated for AZIBs by combining the sulfur-assisted thermal reduction and in-situ polymerization method.The introduced oxygen vacancies of V_(2)O_(3)–Od@PEDOT weaken the electrostatic interaction between Zn^(2+) and the host material,improving the interfacial electron transport,while the PEDOT coating enhances the structural stability and conductivity of V_(2)O_(3),thus accelerating the reaction kinetics.Based on the advantages,V_(2)O_(3)–Od@PEDOT electrode delivers a reversible capacity of 495 mAh·g^(−1) at 0.1 A·g^(−1),good rate capability(189 mAh·g^(−1)at 8.0 A·g^(−1)),and an impressive cycling stability with 90.1%capacity retention over 1000 cycles at 8.0 A·g^(−1).The strategy may provide a path for exploiting the other materials for high performance AZIBs.展开更多
With the irreversible trend of the convergence and cooperation among heterogeneous networks, there emerge some important issues for network evolution. One of them is to reconfigure network elements such as cellular ba...With the irreversible trend of the convergence and cooperation among heterogeneous networks, there emerge some important issues for network evolution. One of them is to reconfigure network elements such as cellular base stations （BSs） or access points （APs） of wireless local area networks （WLANs） according to the real-time network environment, in order to maximize the cooperation gain of different networks. In this paper, we consider cognitive pilot channel （CPC） as an assistant to enable cooperation among heterogeneous networks. Based on the widely used reinforcement learning algorithm, this paper has proposed the heterogeneous network self-optimization algorithm （HNSA） to solve the adaptation problem in reconfigurable systems. In the algorithm, distributed agents perform reinforcement learning, and make decisions cooperatively with the help of CPC in order to reduce the system blocking rate and improve network revenue. Finally our simulation proves the anticipated goal is achieved.展开更多
Despite acknowledgment of structural reconstruction of materials following oxygen evolution reaction (OER) reaction, the role of support during the reconstruction process has been ignored. Given this, we directly in s...Despite acknowledgment of structural reconstruction of materials following oxygen evolution reaction (OER) reaction, the role of support during the reconstruction process has been ignored. Given this, we directly in situ transform the residual iron present in raw single-walled carbon nanotubes (SWCNT) into Fe_(2)O_(3) and thus build Fe_(2)O_(3)-CNT as the model system. Intriguingly, an anomalous self-optimization occurred on SWCNT and the derived components show satisfactory electrochemical performance. Soft X-ray absorption spectroscopy (sXAS) analysis and theory calculation correspondingly indicate that self-optimization yields stronger interaction between SWCNT and Fe_(2)O_(3) nanoparticles, where the electrons migrate from Fe_(2)O_(3) to optimized SWCNT. Such polarization will generate a positive charge center and thus boost the OER activity. This finding directly observes the self-optimization of support effect, providing a new perspective for OER and related electrochemical reactions.展开更多
Broadly,the oxygen evolution reaction(OER)has been deeply understood as a significant part of energy conversion and storage.Nevertheless,the anions in the OER catalysts have been neglected for various reasons such as ...Broadly,the oxygen evolution reaction(OER)has been deeply understood as a significant part of energy conversion and storage.Nevertheless,the anions in the OER catalysts have been neglected for various reasons such as inactive sites,dissolution,and oxidation,amongst others.Herein,we applied a model catalyst s-Ni(OH)2 to track the anionic behavior in the catalyst during the electrochemical process to fill this gap.The advanced operando synchrotron radiation Fourier transform infrared(SR-FTIR)spectroscopy,synchrotron radiation photoelectron spectroscopy(SRPES)depth detection and differential X-ray absorption fine structure(D-XAFS)spectrum jointly point out that some oxidized sulfur species(SO_(4)^(2-))will selfoptimize new Ni–S bonds during OER process.Such amazing anionic self-optimization(ASO)behavior has never been observed in the OER process.Subsequently,the optimization-derived component shows a significantly improved electrocatalytic performance(activity,stability,etc.)compared to reference catalyst Ni(OH)_(2).Theoretical calculation further suggests that the ASO process indeed derives a thermodynamically stable structure of the OER catalyst,and then gives its superb catalytic performance by optimizing the thermodynamic and kinetic processes in the OER,respectively.This work demonstrates the vital role of anions in the electrochemical process,which will open up new perspectives for understanding OER and provide some new ideas in related fields(especially catalysis and chemistry).展开更多
Currently, the power electronics-based devices, includinglarge-scale non-synchronized generators and reactivepower compensators, are widely used in power grids. This helpsintroduce the coupling interactions between th...Currently, the power electronics-based devices, includinglarge-scale non-synchronized generators and reactivepower compensators, are widely used in power grids. This helpsintroduce the coupling interactions between the devices andthe power grid, resulting in a new sub-synchronous oscillationphenomenon. It is a critical element for the stability operation ofthe power grid and its devices. In this paper, the sub-synchronousoscillation phenomenon of the power grid connected with largescalewind power generation is analyzed in detail. Then, inorder to damp the sub-synchronous oscillation, a coordinateddamping optimization control strategy for wind power generatorsand their reactive power compensators is proposed. The proposedcoordinated control strategy tracks the sub-synchronousoscillation current signal to correct the corresponding controlsignal, which increases the damping of power electronics. Theresponse characteristics of the proposed control strategy areanalyzed, and a self-optimization parameter tuning method basedon sensitivity analysis is proposed. The simulation results validatethe effectiveness and the availability of the proposed controlstrategy.展开更多
基金supported by the Beijing Natural Science Foundation(2172027)the Tsinghua University Initiative Scientific Research Program+3 种基金the National Natural Science Foundation of China(21802154)the Fund of Key Laboratory of Advanced Materials of Ministry of Education(2018AML05)the Foundation of Director of the Technical Institute of Physics and Chemistry of CASthe Youth Innovation Promotion Association of the CAS(2019026)
文摘Metallic layered transition metal dichalcogenides(TMDs)nanomaterials based on Group 5 transition metals are attracting substantial interests as alternative catalysts for hydrogen evolution reaction(HER).However,controllable preparation of tantalum diselenide(TaSe2)remains challenging,which has hindered the exploration on its application in HER.Herein,we develop a facile method named surface-assisted chemical vapor transport(SACVT)for controllable synthesis of TaSe2 plates and nanobelts,by regulating the molar ratio of selenium to tantalum and reaction temperature.Unique quasi-arrays and self-supported structure help TaSe2 nanobelt own more active sites and higher ability of charge transfer,so it is superior to TaSe2 plate in electrocatalytic HER.Interestingly,they both exhibit the ability to optimize their morphologies upon cycling for dramatically improved and robust electrocatalytic performance.The selfoptimized structures can increase the effective active surface by exposing more active sites on the basal-planes and edges,shorten the interlayer electron-transfer pathways at a thinned domain,and accelerate the charge transfer,which mainly derive from high basal-plane activity and weak interaction between layers of metallic TaSe2.This work provides a reliable way for controllable synthesis of different TaSe2 structures,motivating further efforts to explore new high-efficiency catalysts in the large family of metallic TMDs for electrochemical energy conversion.
文摘Today＇s production systems are demanded to exhibit an increased flexibility and mutability in order to deal with dynamically changing conditions, objectives and an increasing number of product variants within industrial turbulent environments. Flexible automated systems are requested in order to improve dynamic production efficiency, e.g. robot-based hardware and PC-based controllers, but these usually induce a significantly higher production complexity, whereby the efforts for planning and programming, but also setups and reconfiguration, expand. In this paper a definition and some concepts of self-optimizing assembly systems are presented to describe possible ways to reduce the planning efforts in complex production systems. The concept of self-optimization in assembly systems will be derived from a theoretical approach and will be transferred to a specific application scenario---the automated assembly of a miniaturized solid state laser--where the challenges of unpredictable influences from e.g. component tolerances can be overcome by the help of self-optimization.
文摘QoS-aware service composition is aimed to maximize the global QoS of a composite service when selecting candidate services.In a context sensitive service execution environment in pervasive computing,the context information for service composition is not static:device,policy,and user constraints,and QoS requirements may change,new services may be deployed,old ones withdrawn,or existing ones change their QoS parameters.This results in the current service composition plan failing or its QoS degrading from the optimum.In this paper,a runtime self-optimizing service composition framework is proposed.An implementation of a prototype for this framework is presented,addressing the issues of reducing extra delay while increasing global QoS in service composition in a dynamic context environment.Three service re-plan algorithms are compared that can be used in dynamic context environment,i.e.,minimal-conflict hill-climbing repair genetic algorithm(MCHC-repair GA),an improved penalty-based GA,and our multi-population conflicts sorted repair genetic algorithm(MP-CS-repair GA),as well as three kinds of service composition mechanisms-with backup,without backup,and our context-aware service re-selection mechanisms.The results show that our MP-CS-repair GA and context-aware service re-selection method can reduce more extra delay while acquiring a higher global QoS for the composite service in a context sensitive environment.This context-aware service re-selection mechanism also shows some adaptability to different context change frequencies and user requirements for reducing computation cost in the self-optimizing process.
基金theNationalNaturalScienceFoundationofChina (No .2 0 1730 14 )andScienceFoundationofHunanProvince
文摘In this paper, a novel exact fixed-node quantum Monte Carlo (EFNQMC) algorithm was proposed, which is a self-optimizing and self-improving procedure. In contrast to the previous EFNQMC method, the importance function of this method is optimized synchronistically in the diffusion procedure, but not before beginning the EFNQMC computation. In order to optimize the importance function, the improved steepest descent technique is used, in which the step size is automatically adjustable. The procedure is quasi-Newton type and converges super linearly. The present method also uses a novel trial function, which has correct electron-electron and electron-nucleus cusp conditions. The novel EFNQMC algorithm and the novel trial function are employed to calculate the energies of 1 1A 1 state of CH 2, 1A g state of C 8 and the ground-states of H 2, LiH, Li 2 and H 2O.
基金supported by National Key Research and Development Program of China(2021YFA1500500,2019YFA0405600,2017YFA0204904,2019YFA0405602,and 2017YFA0403402)the National Science Fund for Distinguished Young Scholars(21925204)+8 种基金the National Natural Science Foundation of China(21972132,U1732149,U19A2015,U1732272,21673214,92045301,and 21902149)the Fundamental Research Funds for the Central Universities(20720220010)the Provincial Key Research and Development Program of Anhui(202004a05020074)the Anhui Natural Science Foundation for Young Scholars(2208085QB52)K.C.Wong Education(GJTD2020-15)the Hefei Municipal Natural Science Foundation(2021018)the DNL Cooperation Fund,CAS(DNL202003)Users with Excellence Program of Hefei Science Center CAS(2020HSCUE001)USTC Research Funds of the Double First-Class Initiative(YD2340002002)。
文摘The demand for clean and sustainable energy has encouraged the production of hydrogen from water electrolyzers.To overcome the obstacle to improving the efficiency of water electrolyzers,it is highly desired to fabricate active electrocatalysts for the sluggish oxygen evolution process.However,there is generally an intrinsic gap between the as-prepared and real electrocatalysts due to structure evolution under the oxidative reaction conditions.Here,we combine in-situ anionic leaching and atomic deposition to realize single-atom catalysts with self-optimized structures.The introduced F ions facilitate structural transformation from Co(OH)xF into CoOOH(F),which generates an amorphous edge surface to provide more anchoring sites for Ir single atoms.Meanwhile,the in-situ anionic leaching of F ions elevates the Co valence state of Ir_(1)/CoOOH(F)more significantly than the counterpart without F ions(Ir_(1)/CoOOH),leading to stronger adsorption of oxygenated intermediates.As revealed by electrochemical measurements,the increased Ir loading together with the favored adsorption of*OH intermediates improve the catalytic activity of Ir_(1)/CoOOH(F).Specifically,Ir_(1)/CoOOH(F)delivered a current density of 10 mA cm-2at an overpotential of 238 mV,being lower than 314 mV for Ir_(1)/CoOOH.The results demonstrated the facility of the in-situ optimization process to optimize catalyst structure for improved performance.
基金supported in part by the National Major Scientific Research Equipment of China (61927803)the National Natural Science Foundation of China Basic Science Center Project (61988101)+1 种基金Science and Technology Innovation Program of Hunan Province (2021RC4054)the China Postdoctoral Science Foundation (2021M691681)。
文摘The copper disc casting machine is core equipment for producing copper anode plates in the copper metallurgy industry.The copper disc casting machine casting package motion curve(CPMC) is significant for precise casting and efficient production.However,the lack of exact casting modeling and real-time simulation information severely restricts dynamic CPMC optimization.To this end,a liquid copper droplet model describes the casting package copper flow pattern in the casting process.Furthermore,a CPMC optimization model is proposed for the first time.On top of this,a digital twin dual closed-loop self-optimization application framework(DT-DCS) is constructed for optimizing the copper disc casting process to achieve self-optimization of the CPMC and closed-loop feedback of manufacturing information during the casting process.Finally,a case study is carried out based on the proposed methods in the industrial field.
文摘Cognitive optical network is the intermediate to combine artificial intelligence technology with network,and also the important network technology to promote network intelligence level constantly.In the paper,it analyzes the cognitive optical network structure with the application of artificial intelligence technology by starting from the basic conditions of cognitive network and cognitive optional network on the basis of fully understanding the connotation of cognitive network and cognitive optical network,and explores its self-governance functions,so as to better realize the self-optimization and self-configuration of network.
基金supported by the National Natural Science Foundation of China(Nos.21808059,21878088,and 21476077)Key Project of the Shanghai Science and Technology Committee(No.18DZ1112703)。
文摘The pharmaceutical industry is now paying increased attention to continuous manufacturing.While the revolution to continuous and automated manufacturing is deepening in most of the top pharma companies in the world,the advancement of automated pharmaceutical continuous manufacturing in China is relatively slow due to some key challenges including the lack of knowledge on the related technologies and shortage of qualified personnels.In this review,emphasis is given to two of the crucial technologies in automated pharmaceutical continuous manufacturing,i.e.,process analytical technology(PAT)and self-optimizing algorithm.Research work published in recent 5 years employing advanced PAT tools and self-optimization algorithms is introduced,which represents the great progress that has been made in automated pharmaceutical continuous manufacturing.
基金supported by the National Natural Science Foun-dation of China(Nos.22178275 and U22A20147)the Natural Science Foundation of Hubei Province of China(No.2022CFA001).
文摘In addition to the electron transfer,the appropriate H-adsorption affinity of active centers on the metal cocatalyst surface is quite important for high hydrogen-production activity of cocatalyst-modified photo-catalysts.The typical Cu and Ru metal cocatalysts clearly exhibit a weak Cu-H bond and a strong Ru-H bond,respectively,resulting in limited activity for photocatalytic H_(2)evolution.In this work,an ingenious strategy of self-optimized H-adsorption affinity in CuRu alloy cocatalyst is developed to simultaneously reinforce the Cu-H bond and weaken the Ru-H bond by the intrinsic electron transfer from Cu to Ru atom.The CuRu alloy nanoparticles(2-3 nm)were deposited on the TiO_(2)surface to prepare CuRu/TiO_(2)through a one-step photoreduction method.Photocatalytic tests exhibited that the highest H_(2)-production rate of CuRu/TiO_(2)photocatalyst reached up to 5.316 mmol h^(-1)g^(-1),which was 24.80,1.86,and 2.60 times higher than that of the TiO_(2),Cu/TiO_(2),and Ru/TiO_(2),respectively.Based on the characterization results and theoretical calculations,the CuRu alloy cocatalyst exhibits excellent self-optimized H-adsorption affinity via the spontaneous electron transfer from Cu to Ru atom,which can greatly accelerate the photocatalytic H_(2)-production rate of TiO_(2).This work provides a feasible idea for the self-optimized H-adsorption affinity of metal active sites in the photocatalytic H_(2)-generation field.
文摘In this paper we proposed a novel exact fixed-node quantum Monte Carlo (EFNQMC) algorithm, which is a self-optimizing and self-improving procedure. In contrast to the previous EFNQMC method, the trial function is optimized synchronistically in the diffusion procedure, but not before the beginning of EFNQMC computation. In order to optimize the trial function, the improved steepest descent technique is used, in which the step size is automatically adjustable. The procedure is quasi-Newton and converges super linearly. We also use a novel trial function, which has correct electron-electron and electron-nucleus cusp conditions. The novel EFNQMC algorithm and the novel trial function are employed to calculate the energies of 11 A1 state of CH2, 1Ag state of C8 and the ground-states of H2, LiH, Li2, H2O, respectively. The test results show that both the novel algorithm and the trial function proposed in the present paper are very excellent.
基金This study was financially supported by the National Natural Science Foundation of China(No.22165028)the Nature Science Foundation of Gansu Province(No.20JR10RA108).
文摘Aqueous zinc-ion batteries(AZIBs)have attracted widespread attention due to the advantages of high safety and environmental friendliness.Although V_(2)O_(3) is a promising cathode,the strong electrostatic interaction between Zn^(2+) and V_(2)O_(3) crystal,and the sluggish reaction kinetics still limit their application in AZIBs.Herein,the oxygen defects rich V_(2)O_(3) with conducive poly(3,4-ethylenedioxythiophene)(PEDOT)shell(V_(2)O_(3)-Od@PEDOT)was fabricated for AZIBs by combining the sulfur-assisted thermal reduction and in-situ polymerization method.The introduced oxygen vacancies of V_(2)O_(3)–Od@PEDOT weaken the electrostatic interaction between Zn^(2+) and the host material,improving the interfacial electron transport,while the PEDOT coating enhances the structural stability and conductivity of V_(2)O_(3),thus accelerating the reaction kinetics.Based on the advantages,V_(2)O_(3)–Od@PEDOT electrode delivers a reversible capacity of 495 mAh·g^(−1) at 0.1 A·g^(−1),good rate capability(189 mAh·g^(−1)at 8.0 A·g^(−1)),and an impressive cycling stability with 90.1%capacity retention over 1000 cycles at 8.0 A·g^(−1).The strategy may provide a path for exploiting the other materials for high performance AZIBs.
基金Supported by the E3 Project within Community’s Seventh Framework Program (Grant No. FP7-ICT-2007-216248)the National Natural ScienceFoundation of China (Grant Nos. 60832009, 60632030)the National Basic Research Program of China (Grant No. 2009CB320406)
文摘With the irreversible trend of the convergence and cooperation among heterogeneous networks, there emerge some important issues for network evolution. One of them is to reconfigure network elements such as cellular base stations （BSs） or access points （APs） of wireless local area networks （WLANs） according to the real-time network environment, in order to maximize the cooperation gain of different networks. In this paper, we consider cognitive pilot channel （CPC） as an assistant to enable cooperation among heterogeneous networks. Based on the widely used reinforcement learning algorithm, this paper has proposed the heterogeneous network self-optimization algorithm （HNSA） to solve the adaptation problem in reconfigurable systems. In the algorithm, distributed agents perform reinforcement learning, and make decisions cooperatively with the help of CPC in order to reduce the system blocking rate and improve network revenue. Finally our simulation proves the anticipated goal is achieved.
基金This work was financially supported in part by the National Key R&D Program of China(Nos.2017YFA0303500 and 2020YFA0405800)National Natural Science Foundation of China(NSFC)(Nos.U1932201,U2032113,and 22075264)+3 种基金CAS Collaborative Innovation Program of Hefei Science Center(Nos.2019HSC-CIP002 and 2020HSC-CIP002)the USTC Start-Up Fund,and CAS Interdisciplinary Innovation TeamL.S.acknowledges the support from Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Nankai University(111 projects,B_(12)015).
文摘Despite acknowledgment of structural reconstruction of materials following oxygen evolution reaction (OER) reaction, the role of support during the reconstruction process has been ignored. Given this, we directly in situ transform the residual iron present in raw single-walled carbon nanotubes (SWCNT) into Fe_(2)O_(3) and thus build Fe_(2)O_(3)-CNT as the model system. Intriguingly, an anomalous self-optimization occurred on SWCNT and the derived components show satisfactory electrochemical performance. Soft X-ray absorption spectroscopy (sXAS) analysis and theory calculation correspondingly indicate that self-optimization yields stronger interaction between SWCNT and Fe_(2)O_(3) nanoparticles, where the electrons migrate from Fe_(2)O_(3) to optimized SWCNT. Such polarization will generate a positive charge center and thus boost the OER activity. This finding directly observes the self-optimization of support effect, providing a new perspective for OER and related electrochemical reactions.
基金supported in part by the National Key R&D Program of China(2017YFA0303500)the National Natural Science Foundation of China(U1932201,21727801,and 51902303)+4 种基金the National Natural Science Foundation of China-Ministry of Foreign Affairs and International Cooperation of Italy(51861135202)CAS International Partnership Program(211134KYSB20190063)Key Research Program of Frontier Sciences(QYZDB-SSW-SLH018)the University of Science and Technology of China start-up fundCAS Interdisciplinary Innovation Team。
文摘Broadly,the oxygen evolution reaction(OER)has been deeply understood as a significant part of energy conversion and storage.Nevertheless,the anions in the OER catalysts have been neglected for various reasons such as inactive sites,dissolution,and oxidation,amongst others.Herein,we applied a model catalyst s-Ni(OH)2 to track the anionic behavior in the catalyst during the electrochemical process to fill this gap.The advanced operando synchrotron radiation Fourier transform infrared(SR-FTIR)spectroscopy,synchrotron radiation photoelectron spectroscopy(SRPES)depth detection and differential X-ray absorption fine structure(D-XAFS)spectrum jointly point out that some oxidized sulfur species(SO_(4)^(2-))will selfoptimize new Ni–S bonds during OER process.Such amazing anionic self-optimization(ASO)behavior has never been observed in the OER process.Subsequently,the optimization-derived component shows a significantly improved electrocatalytic performance(activity,stability,etc.)compared to reference catalyst Ni(OH)_(2).Theoretical calculation further suggests that the ASO process indeed derives a thermodynamically stable structure of the OER catalyst,and then gives its superb catalytic performance by optimizing the thermodynamic and kinetic processes in the OER,respectively.This work demonstrates the vital role of anions in the electrochemical process,which will open up new perspectives for understanding OER and provide some new ideas in related fields(especially catalysis and chemistry).
基金the NationalNatural Science Foundation of China under Grant No.51577174.
文摘Currently, the power electronics-based devices, includinglarge-scale non-synchronized generators and reactivepower compensators, are widely used in power grids. This helpsintroduce the coupling interactions between the devices andthe power grid, resulting in a new sub-synchronous oscillationphenomenon. It is a critical element for the stability operation ofthe power grid and its devices. In this paper, the sub-synchronousoscillation phenomenon of the power grid connected with largescalewind power generation is analyzed in detail. Then, inorder to damp the sub-synchronous oscillation, a coordinateddamping optimization control strategy for wind power generatorsand their reactive power compensators is proposed. The proposedcoordinated control strategy tracks the sub-synchronousoscillation current signal to correct the corresponding controlsignal, which increases the damping of power electronics. Theresponse characteristics of the proposed control strategy areanalyzed, and a self-optimization parameter tuning method basedon sensitivity analysis is proposed. The simulation results validatethe effectiveness and the availability of the proposed controlstrategy.
