The morphology effect of Zr-doped CeOwas studied in terms of their activities in the selective oxidation of styrene to styrene oxide using tert-butyl hydroperoxide as the oxidant. In the present work, Zrdoped CeOnanor...The morphology effect of Zr-doped CeOwas studied in terms of their activities in the selective oxidation of styrene to styrene oxide using tert-butyl hydroperoxide as the oxidant. In the present work, Zrdoped CeOnanorods exhibited the highest catalytic performance(yield of styrene oxide and TOF value)followed by nanoparticles and nanocubes. For the Zr-doped CeOnanorods, the apparent activation energy is 56.3 k J/mol, which is much lower than the values of catalysts supported on nanoparticles and nanocubes(73.3 and 93.4 k J/mol). The high resolution transmission electron microscopy results indicated that(100) and(110) crystal planes are predominantly exposed for Zr-doped CeOnanorods while(100)and(111) for nanocubes,(111) for nanoparticles. The remarkably increased catalytic activity of the Zrdoped CeOnanorods is mainly attributed to the higher percentage of Cespecies and more oxygen vacancies, which are associated with their exposed(100) and(110) crystal planes. Furthermore, recycling studies proved that the heterogeneous Zr-doped CeOnanorods did not lose its initial high catalytic activity after five successive recycles.展开更多
Polyoxymethylene dimethyl ethers are recognized as the prospective diesel additive to decrease the pollutant emission from the light-duty vehicles,which can be polymerize form the monomer of dimethoxymethane(DMM).The ...Polyoxymethylene dimethyl ethers are recognized as the prospective diesel additive to decrease the pollutant emission from the light-duty vehicles,which can be polymerize form the monomer of dimethoxymethane(DMM).The industrial synthesis of DMM is mainly involved two-step process:methanol is oxidized to form the formaldehyde in fixed bed reactor and then reacted with the generated formaldehyde through acetalization in continuous stirred-tank reactor.Due to huge energy consumption,this typical synthesis route of DMM needs to be upgraded and more green routes should be determined.In this review,four state-of-the-art one-step direct synthetic routes,including two upgrading routes(methanol direct oxidation and direct dehydrogenation)and two green routes(methanol diethyl ether direct oxidation and carbon oxides direct hydrogenation),have been summarized and compared.Combination with the reaction mechanism and catalytic performance on the different catalysts,the challenges and opportu nities for every synthetic route are proposed.The relationships between catalyst structu re and property in different synthesis strategy are also investigated and then the suggestions of the design of catalyst are given about future research directions that efforts should be made in.Hopefully,this review can bridge the gap between newly developed catalysts and synthesis technology to realize their commercial applications in the near future.展开更多
The high-purity distillation column system is strongly nonlinear and coupled,which makes it difficult to control.Active disturbance rejection control(ADRC)has been widely used in distillation systems,but it has limita...The high-purity distillation column system is strongly nonlinear and coupled,which makes it difficult to control.Active disturbance rejection control(ADRC)has been widely used in distillation systems,but it has limitations in controlling distillation systems with large time delays since ADRC employs ESO and feedback control law to estimate the total disturbance of the system without considering the large time delays.This paper designs a proportion integral-type active disturbance rejection generalized predictive control(PI-ADRGPC)algorithm to control the distillation column system with large time delay.It replaces the PD controller in ADRC with a proportion integral-type generalized predictive control(PI-GPC),thereby improving the performance of control systems with large time delays.Since the proposed controller has many parameters and is difficult to tune,this paper proposes to use the grey wolf optimization(GWO)to tune these parameters,whose structure can also be used by other intelligent optimization algorithms.The performance of GWO tuned PI-ADRGPC is compared with the control performance of GWO tuned ADRC method,multi-verse optimizer(MVO)tuned PI-ADRGPC and MVO tuned ADRC.The simulation results show that the proposed strategy can track reference well and has a good disturbance rejection performance.展开更多
The laminated porous N-deficient g-C3N4(CN–H)is successfully synthesized by a facile two-step hydrothermal calcination method using oxalic acid-assisted melamine as the precursor.Compared with pristine g-C3N4(224μmo...The laminated porous N-deficient g-C3N4(CN–H)is successfully synthesized by a facile two-step hydrothermal calcination method using oxalic acid-assisted melamine as the precursor.Compared with pristine g-C3N4(224μmol g-1h-1),the CN–H shows superior photocatalytic hydrogen production activity(up to 728μmol g-1h-1),which is three times higher than the unmodified counterpart.To draw out the multifaceted influences of oxalic acid modification on the visible-light-induced photocatalytic activity,various techniques are utilized to investigate the formation mechanism,structural characteristics and photoelectrical properties of CN–H.The results indicate that the addition of a trace amount of oxalic acid to the precursor melamine results in a g-C3N4 structure possessing the advantage of both nitrogen defects and laminated porosity.These properties can enlarge specific surface areas of g-C3N4,enhance an efficient separating of photogenerated electron-hole pairs and extend the range of spectral response,all contributing to the enhancement of the visible-light-induced photocatalytic activity.展开更多
Silicon-vacancy(VSi)centers in silicon carbide(SiC)are expected to serve as solid qubits,which can be used in quantum computing and sensing.As a new controllable color center fabrication method,femtosecond(fs)laserwri...Silicon-vacancy(VSi)centers in silicon carbide(SiC)are expected to serve as solid qubits,which can be used in quantum computing and sensing.As a new controllable color center fabrication method,femtosecond(fs)laserwriting has been gradually applied in the preparation of VSi in SiC.In this study,4H-SiCwas directlywritten by an fs laser and characterized at 293 K by atomic force microscopy,confocal photoluminescence(PL),and Raman spectroscopy.PL signals of VSi were found and analyzed using 785 nm laser excitation by means of depth profiling and two-dimensional mapping.The influence of machining parameters on the VSi formation was analyzed,and the three-dimensional distribution of VSi defects in the fs laser writing of 4H-SiC was established.展开更多
Fast radio bursts(FRBs)are extragalactic radio transients with millisecond duration and brightness temperature.An FRB-associated X-ray burst(XRB)was recently found to arise from the Galactic magnetar SGR J1935+2154.Fo...Fast radio bursts(FRBs)are extragalactic radio transients with millisecond duration and brightness temperature.An FRB-associated X-ray burst(XRB)was recently found to arise from the Galactic magnetar SGR J1935+2154.Following the model of Dai,in which an FRB may originate from a magnetar encountering an asteroid,we focus on explaining the spectrum of the XRB associated with FRB 200428 from SGR J1935+2154.Collisions between asteroidal fragments and the magnetar surface produce a fireball,which further expands relativistically.Due to the velocity difference among some shells in the fireball,internal shocks would form far away from the magnetar,and further emit X-ray emission.We propose that the FRB-associated XRB can be produced by synchrotron emission from the internal shocks,and then constrain the physical parameters by the observed XRB spectrum.展开更多
To obtain the optimal Bayesian network(BN)structure,researchers often use the hybrid learning algorithm that combines the constraint-based(CB)method and the score-and-search(SS)method.This hybrid method has the proble...To obtain the optimal Bayesian network(BN)structure,researchers often use the hybrid learning algorithm that combines the constraint-based(CB)method and the score-and-search(SS)method.This hybrid method has the problemthat the search efficiency could be improved due to the ample search space.The search process quickly falls into the local optimal solution,unable to obtain the global optimal.Based on this,the Particle SwarmOptimization(PSO)algorithm based on the search space constraint process is proposed.In the first stage,the method uses dynamic adjustment factors to constrain the structure search space and enrich the diversity of the initial particles.In the second stage,the update mechanism is redefined,so that each step of the update process is consistent with the current structure which forms a one-to-one correspondence.At the same time,the“self-awakened”mechanism is added to prevent precocious particles frombeing part of the best.After the fitness value of the particle converges prematurely,the activation operation makes the particles jump out of the local optimal values to prevent the algorithmfromconverging too quickly into the local optimum.Finally,the standard network dataset was compared with other algorithms.The experimental results showed that the algorithmcould find the optimal solution at a small number of iterations and a more accurate network structure to verify the algorithm’s effectiveness.展开更多
In order to improve the performance of organic luminescent materials,lots of studies have been carried out at the molecular level.However,these materials are mostly applied as solids or aggregates in practical applica...In order to improve the performance of organic luminescent materials,lots of studies have been carried out at the molecular level.However,these materials are mostly applied as solids or aggregates in practical applications,in which the relationship between aggregation structure and luminescent property should be paid more attention.Here,we obtained five phenothiazine 5,5-dioxide(O-PTZ)derivatives with distinct molecular conformations by rational design of chemical structures,and systematically studied their room-temperature phosphorescence(RTP)effect in solid state.It was found that O-PTZ dimers with quasi-equatorial(eq)conformation tended to show strongerπ-πinteraction than quasi-axial(ax)conformers in crystal state,which was more conducive to the generation of RTP.Based on this result,a multi-level structural model of organic solids was proposed to draw the relationship between aggregation structure and RTP effect,just like the research for the structureproperty relationship of proteins.Using this structural model as the guide,boosted RTP efficiency from 1%to 20%was successfully achieved in the corresponding host-guest doping system,showing its wide applicability.展开更多
The development of photo-responsive room temperature phosphorescence(RTP)materials has attracted more and more attention for their broad application pro-spects.Until now,it is still difficult to obtain the related ma-...The development of photo-responsive room temperature phosphorescence(RTP)materials has attracted more and more attention for their broad application pro-spects.Until now,it is still difficult to obtain the related ma-terials with both high efficiency and long lifetime.And the lacking of emission in blue and red regions also largely re-stricts their further applications.In this work,we reported a new strategy to maintain both high efficiency and long lifetime in RTP luminogens through the integration of phenothiazine to facilitate n-π*transition and polycyclic aromatic hydro-carbons(PAHs)dominated byπ-π*transition.When they were doped into polymer matrix,full color photo-induced RTP materials were obtained for the changedπ-conjugation of PAHs.Among them,PTri@PVP showed the best RTP per-formance with phosphorescence efficiency of 20.73%and lifetime up to 819 ms.Specifically,after turning off the ul-traviolet-visible(UV)irradiation upon this system,time-de-pendent phosphorescence afterglow from green to blue was exhibited,which was found to originate from two distinct molecular conformations and could be further regulated by thermal stimulus.Accordingly,multiple anti-counterfeiting applications,including screen printing,multi-color patterns and multi-dimensional information encryption,were suc-cessfully demonstrated.展开更多
We developed a new one step approach to synthesize g-C3N4 nano-sheets by direct thermal pyrolysis process of urea in NH3 atmosphere. For the first time, the influence of the preparation gas atmosphere on the compositi...We developed a new one step approach to synthesize g-C3N4 nano-sheets by direct thermal pyrolysis process of urea in NH3 atmosphere. For the first time, the influence of the preparation gas atmosphere on the composition, crystalline and polymerization degree, and the activity of the g-C3N4 synthesized from thermal condensation of urea was investigated. Impressively, the g-C3N4 nano-sheets obtained under NH3 gas atmosphere exhibited much superi- or photo-catalytic activities to the prepared g-C3N4 in air or N2, and the rate of the g-C3N4-NH3 was about 5 times higher than that on g-C3N4-N2 sample. The detailed characterization analysis revealed that NH3 thermal pyrolysis atmosphere contributed to the polymerization degree and the formation of the layer with a more regular structure due to the efficiently extending of the conjugated π-conjugative system, which was favorable to the transfer of the photo-induced charge carriers. Furthermore, we studied in depth the structure-performance relationship in the sys- tem, and it was found that the synergistic effect of the larger surface area, the adjusted band energy structure and the well crystallization may be conductive to the higher separation of the electron-hole pair, thus leading to the won- derful performance for the g-C3N4-NH3. Notably, the method has the merits of low cost, scalable production and environmental friendliness.展开更多
Organic luminogens with room temperature phosphorescence(RTP)have been paid great attention and developed rapidly for their wide application values.Until now,the internal mechanism and source of phosphorescence are st...Organic luminogens with room temperature phosphorescence(RTP)have been paid great attention and developed rapidly for their wide application values.Until now,the internal mechanism and source of phosphorescence are still obscure,especially for the relationship between molecular dimer and RTP emission.Hence,we designed and synthesized eight phenothiazine 5,5-dioxide derivatives to directly reveal how the monomer and dimer in packing affect the RTP behavior.Dimers with strongπ-πstacking(θ<20.66°;d<3.86A)lead to pure triplet excimer emission,while those with weakπ-πstacking(27.02°<θ<40.64°;3.84A<d<4.41A)contribute to dual RTP emissions of both monomer and triplet excimer.The valuable information of this work would promote the further development of this research field,as well as others in aggregate.展开更多
In this paper, we first establish the global existence and asymptotic behavior of solutions by using the semigroup method and multiplicative techniques, then further prove the existence of a uniform attractor for a no...In this paper, we first establish the global existence and asymptotic behavior of solutions by using the semigroup method and multiplicative techniques, then further prove the existence of a uniform attractor for a non-autonomous thermoelastic system by using the method of uniform contractive functions. The main advantage of this method is that we need only to verify compactness condition with the same type of energy estimates as that for establishing absorbing sets. Moreover, we also investigate an alternative result of solutions to the semilinear thermoelastic systems by virtue of the semigroup method.展开更多
Objective To explore the association between induced abortion and tubal infertility in Chengdu, China.Methods A 1 : 2 case-control study was designed. Infertile women with bilateral tubal occlusion in the case group ...Objective To explore the association between induced abortion and tubal infertility in Chengdu, China.Methods A 1 : 2 case-control study was designed. Infertile women with bilateral tubal occlusion in the case group compared with two control groups: infertile control group with bilateral tubal patency and pregnant control group with currently pregnancy. Data were collected using questionnaires through face-to-face interviews, covering the subjects' demographic details and histories of gynecology and obstetrics. Adjusted odds ratio was calculated as a measure of the association using stepwise multiple logistic regression analysis.Results Induced abortion was not found to be associated with tubal infertility in the analysis including either the infertile controls or the pregnant controls, but other risk factors were found, such as history of acute pelvic inflammatory disease (PID), lower abdominal surgeries, dysmenorrhea and pregnancy.Conclusion It is contended that facing an increasing trend of infertile cases with tubal occlusion in China, it is emphasized that special attention should paid to the long term impact of reproductive tract infection, especially, asymptomatic ones, rather than induced abortion.展开更多
A Reduced Order Model(ROM)based analysis method for turbomachinery cascade coupled mode flutter is presented in this paper.The unsteady aerodynamic model is established by a system identification technique combined wi...A Reduced Order Model(ROM)based analysis method for turbomachinery cascade coupled mode flutter is presented in this paper.The unsteady aerodynamic model is established by a system identification technique combined with a set of Aerodynamic Influence Coefficients(AIC).Subsequently,the aerodynamic model is encoded into the state space and then coupled with the structural dynamic equations,resulting in a ROM of the cascade aeroelasticity.The cascade flutter can be determined by solving the eigenvalues of the ROM.Bending-torsional coupled mode flutter analysis for the Standard Configuration Eleven(SC11)cascade is used to validate the proposed method.展开更多
基金the financial support from NNSFC(Project 21373054,21303023,21173052)the Natural Science Foundation of Shanghai Science and Technology Committee(08DZ2270500)
文摘The morphology effect of Zr-doped CeOwas studied in terms of their activities in the selective oxidation of styrene to styrene oxide using tert-butyl hydroperoxide as the oxidant. In the present work, Zrdoped CeOnanorods exhibited the highest catalytic performance(yield of styrene oxide and TOF value)followed by nanoparticles and nanocubes. For the Zr-doped CeOnanorods, the apparent activation energy is 56.3 k J/mol, which is much lower than the values of catalysts supported on nanoparticles and nanocubes(73.3 and 93.4 k J/mol). The high resolution transmission electron microscopy results indicated that(100) and(110) crystal planes are predominantly exposed for Zr-doped CeOnanorods while(100)and(111) for nanocubes,(111) for nanoparticles. The remarkably increased catalytic activity of the Zrdoped CeOnanorods is mainly attributed to the higher percentage of Cespecies and more oxygen vacancies, which are associated with their exposed(100) and(110) crystal planes. Furthermore, recycling studies proved that the heterogeneous Zr-doped CeOnanorods did not lose its initial high catalytic activity after five successive recycles.
基金supported by the International S&T Cooperation Projects of China(2015DFR10510)the National Natural Science Foundation of China(61440048+1 种基金61562018)the Scientific Research Program of the Higher Education Institutions of Hainan Province(HNKY2014-04)
文摘Polyoxymethylene dimethyl ethers are recognized as the prospective diesel additive to decrease the pollutant emission from the light-duty vehicles,which can be polymerize form the monomer of dimethoxymethane(DMM).The industrial synthesis of DMM is mainly involved two-step process:methanol is oxidized to form the formaldehyde in fixed bed reactor and then reacted with the generated formaldehyde through acetalization in continuous stirred-tank reactor.Due to huge energy consumption,this typical synthesis route of DMM needs to be upgraded and more green routes should be determined.In this review,four state-of-the-art one-step direct synthetic routes,including two upgrading routes(methanol direct oxidation and direct dehydrogenation)and two green routes(methanol diethyl ether direct oxidation and carbon oxides direct hydrogenation),have been summarized and compared.Combination with the reaction mechanism and catalytic performance on the different catalysts,the challenges and opportu nities for every synthetic route are proposed.The relationships between catalyst structu re and property in different synthesis strategy are also investigated and then the suggestions of the design of catalyst are given about future research directions that efforts should be made in.Hopefully,this review can bridge the gap between newly developed catalysts and synthesis technology to realize their commercial applications in the near future.
基金funded by the National Natural Science Foundation of China(61973175,62073177 and 61973172)South African National Research Foundation(132797)+2 种基金South African National Research Foundation Incentive(114911)Eskom Tertiary Education Support Programme Grant of South AfricaTianjin Research Innovation Project for Postgraduate Students(2021YJSB018,2020YJSB003)。
文摘The high-purity distillation column system is strongly nonlinear and coupled,which makes it difficult to control.Active disturbance rejection control(ADRC)has been widely used in distillation systems,but it has limitations in controlling distillation systems with large time delays since ADRC employs ESO and feedback control law to estimate the total disturbance of the system without considering the large time delays.This paper designs a proportion integral-type active disturbance rejection generalized predictive control(PI-ADRGPC)algorithm to control the distillation column system with large time delay.It replaces the PD controller in ADRC with a proportion integral-type generalized predictive control(PI-GPC),thereby improving the performance of control systems with large time delays.Since the proposed controller has many parameters and is difficult to tune,this paper proposes to use the grey wolf optimization(GWO)to tune these parameters,whose structure can also be used by other intelligent optimization algorithms.The performance of GWO tuned PI-ADRGPC is compared with the control performance of GWO tuned ADRC method,multi-verse optimizer(MVO)tuned PI-ADRGPC and MVO tuned ADRC.The simulation results show that the proposed strategy can track reference well and has a good disturbance rejection performance.
基金financial support by the National Natural Science Foundation of China (Project 21373054)the Natural Science Foundation of Shanghai Science and Technology Committee (08DZ2270500)
文摘The laminated porous N-deficient g-C3N4(CN–H)is successfully synthesized by a facile two-step hydrothermal calcination method using oxalic acid-assisted melamine as the precursor.Compared with pristine g-C3N4(224μmol g-1h-1),the CN–H shows superior photocatalytic hydrogen production activity(up to 728μmol g-1h-1),which is three times higher than the unmodified counterpart.To draw out the multifaceted influences of oxalic acid modification on the visible-light-induced photocatalytic activity,various techniques are utilized to investigate the formation mechanism,structural characteristics and photoelectrical properties of CN–H.The results indicate that the addition of a trace amount of oxalic acid to the precursor melamine results in a g-C3N4 structure possessing the advantage of both nitrogen defects and laminated porosity.These properties can enlarge specific surface areas of g-C3N4,enhance an efficient separating of photogenerated electron-hole pairs and extend the range of spectral response,all contributing to the enhancement of the visible-light-induced photocatalytic activity.
基金This work was supported by the National Natural Science Foundation of China(No.51575389,51761135106)the National Key Research and Development Program of China(2016YFB1102203)+1 种基金the State Key Laboratory of Precision Measuring Technology and Instruments(Pilt1705)the‘111’Project by the State Administration of Foreign Experts Affairs and the Ministry of Education of China(Grant No.B07014)。
文摘Silicon-vacancy(VSi)centers in silicon carbide(SiC)are expected to serve as solid qubits,which can be used in quantum computing and sensing.As a new controllable color center fabrication method,femtosecond(fs)laserwriting has been gradually applied in the preparation of VSi in SiC.In this study,4H-SiCwas directlywritten by an fs laser and characterized at 293 K by atomic force microscopy,confocal photoluminescence(PL),and Raman spectroscopy.PL signals of VSi were found and analyzed using 785 nm laser excitation by means of depth profiling and two-dimensional mapping.The influence of machining parameters on the VSi formation was analyzed,and the three-dimensional distribution of VSi defects in the fs laser writing of 4H-SiC was established.
基金supported by the National Key Research and Development Program of China(Grant Nos.2017YFA0402600,2018YFA0404204)the National SKA Program of China(Grant No.2020SKA0120300)+9 种基金the National Natural Science Foundation of China(NSFC,Grant Nos.11833003,U2038105)supported by the National Natural Science Foundation of China(NSFC,Grant No.12003028)support from the National Natural Science Foundation of China(NSFC,Grant No.U1838113)the National Natural Science Foundation of China(NSFC,Grant Nos.11833003 and U2038105)the Program for Innovative Talents,Entrepreneur in JiangsuYunnan University(Grant No.C176220100087)support by Fundamental Research Funds for the Central Universities(14380046)the National Key Research and Development Programs of China(2018YFA0404204)the science research grants from the China Manned Space Project with NO.CMS-CSST-2021-B11the Program for Innovative Talents,Entrepreneur in Jiangsu。
文摘Fast radio bursts(FRBs)are extragalactic radio transients with millisecond duration and brightness temperature.An FRB-associated X-ray burst(XRB)was recently found to arise from the Galactic magnetar SGR J1935+2154.Following the model of Dai,in which an FRB may originate from a magnetar encountering an asteroid,we focus on explaining the spectrum of the XRB associated with FRB 200428 from SGR J1935+2154.Collisions between asteroidal fragments and the magnetar surface produce a fireball,which further expands relativistically.Due to the velocity difference among some shells in the fireball,internal shocks would form far away from the magnetar,and further emit X-ray emission.We propose that the FRB-associated XRB can be produced by synchrotron emission from the internal shocks,and then constrain the physical parameters by the observed XRB spectrum.
基金funded by the National Natural Science Foundation of China(62262016)in part by the Hainan Provincial Natural Science Foundation Innovation Research Team Project(620CXTD434)+1 种基金in part by the High-Level Talent Project Hainan Natural Science Foundation(620RC557)in part by the Hainan Provincial Key R&D Plan(ZDYF2021GXJS199).
文摘To obtain the optimal Bayesian network(BN)structure,researchers often use the hybrid learning algorithm that combines the constraint-based(CB)method and the score-and-search(SS)method.This hybrid method has the problemthat the search efficiency could be improved due to the ample search space.The search process quickly falls into the local optimal solution,unable to obtain the global optimal.Based on this,the Particle SwarmOptimization(PSO)algorithm based on the search space constraint process is proposed.In the first stage,the method uses dynamic adjustment factors to constrain the structure search space and enrich the diversity of the initial particles.In the second stage,the update mechanism is redefined,so that each step of the update process is consistent with the current structure which forms a one-to-one correspondence.At the same time,the“self-awakened”mechanism is added to prevent precocious particles frombeing part of the best.After the fitness value of the particle converges prematurely,the activation operation makes the particles jump out of the local optimal values to prevent the algorithmfromconverging too quickly into the local optimum.Finally,the standard network dataset was compared with other algorithms.The experimental results showed that the algorithmcould find the optimal solution at a small number of iterations and a more accurate network structure to verify the algorithm’s effectiveness.
基金National Natural Science Foundation of China,Grant/Award Numbers:52273191,22235006Natural Science Foundation of Tianjin City,Grant/Award Number:22JCYBJC00760+3 种基金Open Project Program of Wuhan National Laboratory for Optoelectronics,Grant/Award Number:2020WNLOKF013starting Grants of Tianjin University and Tianjin GovernmentIndependent Innovation Fund of Tianjin University,Grant/Award Number:2023XPD-0014Guangzhou AIE Higher Research Institute。
文摘In order to improve the performance of organic luminescent materials,lots of studies have been carried out at the molecular level.However,these materials are mostly applied as solids or aggregates in practical applications,in which the relationship between aggregation structure and luminescent property should be paid more attention.Here,we obtained five phenothiazine 5,5-dioxide(O-PTZ)derivatives with distinct molecular conformations by rational design of chemical structures,and systematically studied their room-temperature phosphorescence(RTP)effect in solid state.It was found that O-PTZ dimers with quasi-equatorial(eq)conformation tended to show strongerπ-πinteraction than quasi-axial(ax)conformers in crystal state,which was more conducive to the generation of RTP.Based on this result,a multi-level structural model of organic solids was proposed to draw the relationship between aggregation structure and RTP effect,just like the research for the structureproperty relationship of proteins.Using this structural model as the guide,boosted RTP efficiency from 1%to 20%was successfully achieved in the corresponding host-guest doping system,showing its wide applicability.
基金supported by the National Natural Science Foundation of China(52273191,22235006)the Natural Science Foundation of Tianjin City(22JCYBJC00760)+1 种基金the Starting Grants of Tianjin University and Tianjin Governmentthe Independent Innovation Fund of Tianjin University(2023XPD-0014)。
文摘The development of photo-responsive room temperature phosphorescence(RTP)materials has attracted more and more attention for their broad application pro-spects.Until now,it is still difficult to obtain the related ma-terials with both high efficiency and long lifetime.And the lacking of emission in blue and red regions also largely re-stricts their further applications.In this work,we reported a new strategy to maintain both high efficiency and long lifetime in RTP luminogens through the integration of phenothiazine to facilitate n-π*transition and polycyclic aromatic hydro-carbons(PAHs)dominated byπ-π*transition.When they were doped into polymer matrix,full color photo-induced RTP materials were obtained for the changedπ-conjugation of PAHs.Among them,PTri@PVP showed the best RTP per-formance with phosphorescence efficiency of 20.73%and lifetime up to 819 ms.Specifically,after turning off the ul-traviolet-visible(UV)irradiation upon this system,time-de-pendent phosphorescence afterglow from green to blue was exhibited,which was found to originate from two distinct molecular conformations and could be further regulated by thermal stimulus.Accordingly,multiple anti-counterfeiting applications,including screen printing,multi-color patterns and multi-dimensional information encryption,were suc-cessfully demonstrated.
文摘We developed a new one step approach to synthesize g-C3N4 nano-sheets by direct thermal pyrolysis process of urea in NH3 atmosphere. For the first time, the influence of the preparation gas atmosphere on the composition, crystalline and polymerization degree, and the activity of the g-C3N4 synthesized from thermal condensation of urea was investigated. Impressively, the g-C3N4 nano-sheets obtained under NH3 gas atmosphere exhibited much superi- or photo-catalytic activities to the prepared g-C3N4 in air or N2, and the rate of the g-C3N4-NH3 was about 5 times higher than that on g-C3N4-N2 sample. The detailed characterization analysis revealed that NH3 thermal pyrolysis atmosphere contributed to the polymerization degree and the formation of the layer with a more regular structure due to the efficiently extending of the conjugated π-conjugative system, which was favorable to the transfer of the photo-induced charge carriers. Furthermore, we studied in depth the structure-performance relationship in the sys- tem, and it was found that the synergistic effect of the larger surface area, the adjusted band energy structure and the well crystallization may be conductive to the higher separation of the electron-hole pair, thus leading to the won- derful performance for the g-C3N4-NH3. Notably, the method has the merits of low cost, scalable production and environmental friendliness.
基金We are grateful to the National Natural Science Foundation of China(No.51903188)the Natural Science Foundation of Tianjin City(No.19JCQNJC04500)+2 种基金the Open Project Program of Wuhan National Laboratory for Optoelectronics(No.2020WNLOKF013)the starting Grants of Tianjin University and Tianjin GovernmentIndependent Innovation Fund of Tianjin University for financial support.
文摘Organic luminogens with room temperature phosphorescence(RTP)have been paid great attention and developed rapidly for their wide application values.Until now,the internal mechanism and source of phosphorescence are still obscure,especially for the relationship between molecular dimer and RTP emission.Hence,we designed and synthesized eight phenothiazine 5,5-dioxide derivatives to directly reveal how the monomer and dimer in packing affect the RTP behavior.Dimers with strongπ-πstacking(θ<20.66°;d<3.86A)lead to pure triplet excimer emission,while those with weakπ-πstacking(27.02°<θ<40.64°;3.84A<d<4.41A)contribute to dual RTP emissions of both monomer and triplet excimer.The valuable information of this work would promote the further development of this research field,as well as others in aggregate.
基金Supported by the National Natural Science Foundation of China(No.1127106611671075)a grant from Shanghai Municipal Eduction Commission(No.13ZZ048)
文摘In this paper, we first establish the global existence and asymptotic behavior of solutions by using the semigroup method and multiplicative techniques, then further prove the existence of a uniform attractor for a non-autonomous thermoelastic system by using the method of uniform contractive functions. The main advantage of this method is that we need only to verify compactness condition with the same type of energy estimates as that for establishing absorbing sets. Moreover, we also investigate an alternative result of solutions to the semilinear thermoelastic systems by virtue of the semigroup method.
基金supported by the Special Programme of Research, Development, and Research Training in Human Reproduction, World Health Organization (Project 96809)
文摘Objective To explore the association between induced abortion and tubal infertility in Chengdu, China.Methods A 1 : 2 case-control study was designed. Infertile women with bilateral tubal occlusion in the case group compared with two control groups: infertile control group with bilateral tubal patency and pregnant control group with currently pregnancy. Data were collected using questionnaires through face-to-face interviews, covering the subjects' demographic details and histories of gynecology and obstetrics. Adjusted odds ratio was calculated as a measure of the association using stepwise multiple logistic regression analysis.Results Induced abortion was not found to be associated with tubal infertility in the analysis including either the infertile controls or the pregnant controls, but other risk factors were found, such as history of acute pelvic inflammatory disease (PID), lower abdominal surgeries, dysmenorrhea and pregnancy.Conclusion It is contended that facing an increasing trend of infertile cases with tubal occlusion in China, it is emphasized that special attention should paid to the long term impact of reproductive tract infection, especially, asymptomatic ones, rather than induced abortion.
基金supported by the National Science and Technology Major Project, China (No. 2017-II-0009-0023)the Aeronautical Science Foundation of China(No. 2020Z039053004)the Fundamental Research Funds for the Central Universities, China (No. 3102019OQD701)
文摘A Reduced Order Model(ROM)based analysis method for turbomachinery cascade coupled mode flutter is presented in this paper.The unsteady aerodynamic model is established by a system identification technique combined with a set of Aerodynamic Influence Coefficients(AIC).Subsequently,the aerodynamic model is encoded into the state space and then coupled with the structural dynamic equations,resulting in a ROM of the cascade aeroelasticity.The cascade flutter can be determined by solving the eigenvalues of the ROM.Bending-torsional coupled mode flutter analysis for the Standard Configuration Eleven(SC11)cascade is used to validate the proposed method.