Numerous reports have suggested that the performance of organic optoelectronic devices based on organicfieldeffect transistors(OFETs)is largely dependent on their interfaces.Self-assembled monolayers(SAMs)have been co...Numerous reports have suggested that the performance of organic optoelectronic devices based on organicfieldeffect transistors(OFETs)is largely dependent on their interfaces.Self-assembled monolayers(SAMs)have been commonly used to engineer the interfaces of high-performance devices,particularly due to their well-defined structures and simple operation process through simple chemical adsorption growth.In this review,the structures of OFETs and SAM-modified OFETs are described,while different SAMs have been characterized.Furthermore,recent advances in the interface engineering of OFETs are described,the applicability of SAMs in functional devices of OFETs is reviewed,and existing problems and future developments in thisfield have been identified.展开更多
Implant-associated infections caused by biomedical catheters severely threaten patients'health.The use of electrochemical control on NO release from benign nitrite equipped in the catheter can potentially resolve ...Implant-associated infections caused by biomedical catheters severely threaten patients'health.The use of electrochemical control on NO release from benign nitrite equipped in the catheter can potentially resolve this issue with excellent biocompatibility.Inspired by nitrite reductase,a Cu-BDC(BDC:benzene-1,4-dicarboxylic acid)catalyst with coordinated Cu(Ⅱ)sites was constructed as a heterogeneous electrocatalyst to control nitrite reduction to nitric oxide for catheter antibacteria.The combined results of in situ and ex situ tests unveil the key function of interconversion between Cu(Ⅱ)and Cu(Ⅰ)species in NO_(2)^(-)reduction to NO.After being incorporated into the actual catheter,the Cu-BDC catalyst exhibits high electrocatalytic activity toward NO_(2)^(-)reduction to NO and excellent antibacteria efficacy with a sterilizing rate of 99.9%,paving the way for the development of advanced metal-organic frameworks(MOFs)electrocatalysts for catheter antibacteria.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-vip doping system,showing its wide applicability.展开更多
The compatibility of the gate dielectrics with semiconductors is vital for constructing efficient conducting channel for high charge transport.However,it is still a highly challenging mission to clearly clarify the re...The compatibility of the gate dielectrics with semiconductors is vital for constructing efficient conducting channel for high charge transport.However,it is still a highly challenging mission to clearly clarify the relationship between the dielectric layers and the chemical structure of semiconductors,especially vacuum-deposited small molecules.Here,interfacial molecular screening of polyimide(Kapton)dielectric in organic field-effect transistors(OFETs)is comprehensively studied.It is found that the semiconducting small molecules with alkyl side chains prefer to form a high-quality charge transport layer on polyimide(PI)dielectrics compared with the molecules without alkyl side chains.On this basis,the fabricated transistors could reach the mobility of 1.2 cm^(2) V^(−1)s^(−1) the molecule with alkyl side chains on bare PI dielectric.What is more,the compatible semiconductor and dielectric would further produce a low activation energy(E_(A))of 3.01 meV towards efficient charge transport even at low temperature(e.g.,100 K,0.9 cm^(2) V^(−1)s^(−1)).Our research provides a guiding scheme for the construction of high-performance thin-film field-effect transistors based on PI dielectric layer at room and low temperatures.展开更多
Organic afterglow materials have drawn increasing attention for their great potential in practical applications.Until now,most of them just show the lifetimes in milliseconds or seconds,while the realization of long p...Organic afterglow materials have drawn increasing attention for their great potential in practical applications.Until now,most of them just show the lifetimes in milliseconds or seconds,while the realization of long persistent luminescence(LPL)lasting for minutes or even hours is difficult.In 2017,Adachi and Kabe successfully realize the LPL with a duration longer than 1 hour in a purely organic system,which can be even comparable to some excellent inorganic materials.However,partially for the unclear structure-property relationship,organic LPL materials are still rather scarce,especially for the stable ones in air or aqueous solution.In this review,we present the recent progress in organic LPL,mainly focusing on the material design strategy and internal mechanism.It is anticipated that the deep understanding can be beneficial for the further development of organic LPL materials with good stability in air and even aqueous phase.展开更多
Aggregation-induced emission(AIE) has drawn great attention worldwide for its unique optical phenomenon and huge potential applications. Since coined by Ben Zhong Tang et al. in 2001, AIE has been deeply investigated ...Aggregation-induced emission(AIE) has drawn great attention worldwide for its unique optical phenomenon and huge potential applications. Since coined by Ben Zhong Tang et al. in 2001, AIE has been deeply investigated and widely utilized in many important areas, such as organic light-emitting diode(OLED), sensor, and bio-imaging. Herein, we highlight some important progress of AIE in these eighteen years, including the exploration of internal mechanism and potential applications. Furthermore,some other interestingly emissive behaviors, originating but distinguishing from the AIE concept, are presented. It is anticipated an overall understanding about AIE could be easily caught from this short review for scientists, no matter whether they are involved in this exciting and rising research area or not.展开更多
“Union is strength”.In the realm of organic molecules,the macroscopic performance of molecular aggregates is not just the simple overlay of single molecules,and in many cases,new properties can be created by molecul...“Union is strength”.In the realm of organic molecules,the macroscopic performance of molecular aggregates is not just the simple overlay of single molecules,and in many cases,new properties can be created by molecular uniting with particular packing modes[1–4].As to the organic emissive materials,various changes can be rea-lized from single molecules to aggregates(Fig.1),in-cluding the emerged bright emission,the varied emission color,the different emission forms,and the arisen new excitation processes.展开更多
Researchers investigated the organic optoelectronic materials and facilitated their development in organic light-emitting diodes(OLEDs),chemo-and biosensors,organic solar cells,data storage,and anticounterfeiting devi...Researchers investigated the organic optoelectronic materials and facilitated their development in organic light-emitting diodes(OLEDs),chemo-and biosensors,organic solar cells,data storage,and anticounterfeiting devices.Atoms make up molecules through chemical bonds,and molecular aggregates are formed through weak intermolecular interactions.The opto-electronic performance of these materials depends on not only the properties of the well-designed molecules with specific function groups,but also their aggregate states.The molecular aggregates in the form of nanoparticles can be applied in biological imaging,and films can be applied to photovoltaic and photodeformable devices,in which,the alignment of optoelectronic molecules can be either an ordered crystalline or an amorphous state.Generally,the crystalline materials could be deeply investigated by single crystal/powder X-ray diffraction analysis,which could provide the accurate information about molecular conformations,interactions and packing characteristics.It afforded a convenient way to investigate the possible relationship between molecular aggregates and opto-electronic properties.Among various opto-electronic materials,organic room temperature phosphorescence(RTP)materials exhibit the extremely sensitive luminescence property to molecular aggregates,even the dynamic properties can be detected by the tiny change of molecular aggregates.Thus,we selected the organic RTP emission as the output information of molecular aggregates,and afforded typical examples to find the possible relation between RTP effect and molecular packing.Accordingly,molecular packing can be adjusted by the external force as light,mechanical force,temperature,electric field,and so on,as well as the molecular structures as the building blocks,and the systematic investigation in the dynamic and static aggregation structures is of great value to the design of various optoelectronic materials.This review discusses the relationship among molecular structures,aggregation behaviors and corresponding optoelectronic properties by a comprehensive summary of recent research in our group,and the concept of molecular uniting set identified characteristic(MUSIC)is afforded.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
Bright emission of organic luminogens at aggregated state has attracted increasing attention for their potential applications in opto-electronic devices and bio-/chemo-sensors.In this article,upon the introduction of ...Bright emission of organic luminogens at aggregated state has attracted increasing attention for their potential applications in opto-electronic devices and bio-/chemo-sensors.In this article,upon the introduction of different substituents(Br,Ph and TPh)to the large conjugated core of 9-methyl-9H-dibenzo[a,c]carbazole(DBC)moiety,the resultant luminogens demonstrated PL quantum yields in solid state ranging from 4.81%to 47.39%.Through the systematic investigation of molecular packing,together with theory calculation,the strong intermolecular electronic coupling in the dimers is proved as the main factor to the bright emission in the solid state.The results afforded a new avenue to investigate the intrinsic relationship among the molecular structures,packing modes and emission properties.展开更多
Molecular interactions are crucial in diverse fields of protein folding,material science,nanotechnology,and life origins.Although mounting experimental research controls luminescent behavior by adjusting molecular int...Molecular interactions are crucial in diverse fields of protein folding,material science,nanotechnology,and life origins.Although mounting experimental research controls luminescent behavior by adjusting molecular interactions in light-emitting materials,it remains elusive to correlate microscopic molecular interactions with macroscopic luminescent behavior directly.Here,we synthesized three red luminogens with subtle structural variation and investigated the influence of molecular interactions on their luminescent behavior in solution and aggregate states.Our results indicate that strongπ-πand D-A interactions in both dilute solution(between luminogen and solvent molecules)and aggregate(between luminogens)states cause the redshift in emission,while weak interactions(e.g.,Van der Waals,C–H…π,and C–H…F interactions)enhance the quantum yield.This work provides a thoughtful investigation into the complicated influence of various molecular interactions on luminescent behavior.展开更多
Biomass is a green and producible source of energy and chemicals.Hence,developing high-efficiency catalysts for biomass utilization and transformation is urgently demanded.Metal-organic framework(MOF)-based solid acid...Biomass is a green and producible source of energy and chemicals.Hence,developing high-efficiency catalysts for biomass utilization and transformation is urgently demanded.Metal-organic framework(MOF)-based solid acid materials have been considered as promising catalysts in biomass transformation.In this review,we first introduce the genre of Lewis acid and Brønsted acid sites commonly generated in MOFs or MOF-based composites.Then,the methods for the generation and adjustment of corresponding acid sites are overviewed.Next,the catalytic applications of MOF-based solid acid materials in various biomass transformation reactions are summarized and discussed.Furthermore,based on our personal insights,the challenges and outlook on the future development of MOF-based solid acid catalysts are provided.We hope that this review will provide an instructive roadmap for future research on MOFs and MOF-based composites for biomass transformation.展开更多
Highly efficient persistent organic room temperature phosphorescence(RTP) has attracted increasing attention because of promising applications in fields of chemical sensors, optoelectronic devices, information securit...Highly efficient persistent organic room temperature phosphorescence(RTP) has attracted increasing attention because of promising applications in fields of chemical sensors, optoelectronic devices, information security, and bioimaging, etc. Wherein,the crystal engineering of H-aggregation offers stabilization for long-lived triplet exciton for RTP, but the related research is rare because of the scarcity of ideal phosphorescent H-aggregate. Herein, we designed planar tricoordinate organoboron derivatives with molecular arrangement in ideal H-aggregation. The integration of Br atom can largely enhance RTP efficiency through increasing SOC effect, while the antiparallel molecular arrangement causes annihilation of triplet exciton. Thanks to good selfassembly property, their RTP can even be observed in PMMA matrix with doping ratio of merely 1 wt%. We further found that the cryogenic temperature contributes to stabilizing triplet exciton in H-aggregation, leading to red-shifted phosphorescence. By applying high hydrostatic pressure, the phosphorescence was largely enhanced and redshifted, demonstrating the crucial role of H-aggregation on RTP property. In phosphorescent tissue imaging of live mouse, nanoparticles of BrBA exhibited high contrast image via eliminating the interference of autofluorescence.展开更多
Enantioselective recognition and separation are the most important issues in the fields of chemistry,pharmacy,agrochemical,and food science.Here,we developed two optically active diamines showing aggregation-induced e...Enantioselective recognition and separation are the most important issues in the fields of chemistry,pharmacy,agrochemical,and food science.Here,we developed two optically active diamines showing aggregation-induced emission(AIE)that can discriminate 5 kinds of chiral acids with high enantioselectivity.Especially,a very high fluorescence intensity ratio(IL/ID)of 281 for(±)-Dibenzoyl-D/L-tartaric acid was obtained through the collection of fluorescence change after interaction with chiral AIE-active diamine.By virtue of AIE property and intermolecular acidbase interaction,enantioselective separation was facilely realized by simple filtration of the precipitates formed by chiral AIE luminogen(AIEgen)and one enantiomer in the racemic solution.The chiral HPLC data indicated that the precipitates of AIEgen/chiral acid possessed 82%L-analyte(the enantiomeric excess value was assessed to be 64%ee).Therefore,this method can serve as a simple,convenient,and low-cost tool for chiral detection and separation.展开更多
In recent years, the demand direction for electronic equipment has expanded into embedded and miniaturized devices. The heat radiation problem has become one of the most significant factors for hindering the developme...In recent years, the demand direction for electronic equipment has expanded into embedded and miniaturized devices. The heat radiation problem has become one of the most significant factors for hindering the development of electronic devices. Since heat radiation material is one of the important components in electronic devices, the demand for enhancing thermal conductivity is also increasingly urgent. Research on thermal conductive polymer composites has become a major direction for developing functional composites. This work reviewed the recent progress in the fabrication of thermal conductive polymer composites. Five different structures are presented, including the using of single fillers,hybrid fillers, double threshold percolation structure, segregated structure and other complex multiphase structures. Specifically, the preparation of high-performance thermal conductive polymer composites was introduced through the combination of various thermal conductive fillers.Finally, the development direction of high thermal conductive polymer composites was briefly explored.展开更多
Zinc-air batteries(ZABs)are widely studied because of their high theoretical energy density,high battery voltage,environmental protection,and low price.However,the slow kinetics of oxygen reduction reaction(ORR)and ox...Zinc-air batteries(ZABs)are widely studied because of their high theoretical energy density,high battery voltage,environmental protection,and low price.However,the slow kinetics of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)on the air electrode limits the further application of ZABs,so that how to develop a cheap,efficient,and stable catalyst with bifunctional catalytic activity is the key to solving the development of ZABs.Transition metal compounds are widely used as cathode materials for ZABs due to their low cost,high electrocatalytic activity,and stable structure.This review summarizes the research progress of transition metal compounds as bifunctional catalysts for ZABs.The development history,operation principle,and mechanism of ORR and OER reactions are introduced first.The application and development of transition metal compounds as bifunctional catalysts for ZABs in recent years are systematically introduced,including transition metal oxides(TMOs),transition metal nitrides(TMNs),transition metal sulfides(TMSs),transition metal carbides(TMCs),transition metal phosphates(TMPs),and others.In addition,the shortcomings of transition metal compounds as bifunctional catalysts for ZABs were summarized and reasonable design strategies and improvement measures were put forward,aiming at providing a reference for the design and construction of high-performance ZABs cathode materials.Finally,the challenges and future in this field are discussed and prospected.展开更多
The brightness of fluorescent agents directly determines the imaging performance as required.Among various fluorophores,small organic species are promising given its exact purity/composition and excellent processibili...The brightness of fluorescent agents directly determines the imaging performance as required.Among various fluorophores,small organic species are promising given its exact purity/composition and excellent processibility.However,chromophores with planar geometry may suffer from the undesirable aggregation-caused quenching(ACQ)phenomenon.Encouragingly,luminogens showing aggregation-induced emission(AIE)features are preferable as the aggregates which are the most common used state.In this review,we mainly focus on the strategies employed for boosting the brightness of AIE-active luminogens(AIEgens).From molecule to mor-phology levels,approaches that regulate electronic transition processes of the molecule or the packing extent of aggregates in order to confine molecular motion,reduceπ-πstacking,disrupt fluorophore-water interactions,etc.,are presented.In the end,the current challenges and perspectives are briefly discussed.We anticipate that this review will stimulate new insights and more efforts for the advancement of ultrabright AIEgens.展开更多
The research of photo-responsive materials,with changed absorption and emission under light stimulus,has drawn more and more attention due to their wide applications.However,most of them suffered from the notorious ag...The research of photo-responsive materials,with changed absorption and emission under light stimulus,has drawn more and more attention due to their wide applications.However,most of them suffered from the notorious aggregation-caused quenching(ACQ)effect,which often led to the unconspicuous luminescent change in photo-responsive process.To solve this problem,the strategy of combining aggregation-induced emission(AIE)and photochromic properties was utilized,which largely enriched the phenomenon and application of photo-responsive materials.This short review summarized the recent progress of photo-responsive AIE materials with changed UV absorbance or PL phenomenon under UV-irradiation,including the types of molecular structures,internal mechanisms and the practical applications.Also,some outlooks were given on the further exploration of this field at the end of this paper.展开更多
The lipid droplet(LD)is a dynamic organelle responsible for lipid storage and metabolism that plays important roles in maintaining lipid homeostasis.However,limited strategies are available for tracking the LD content...The lipid droplet(LD)is a dynamic organelle responsible for lipid storage and metabolism that plays important roles in maintaining lipid homeostasis.However,limited strategies are available for tracking the LD content exchange.In this contribution,we report a novel fluorescent probe,TPEAmAl,for real-time LD content dynamics tracking.TPE-AmAl is LD-specific,but emits faintly due to its intramolecular motion.Upon photoactivation,it undergoes a photocyclodehydrogenation reaction and shows a large fluorescence increment.Thus,it can be used for highlighting selected LDs with high spatial resolution.By measuring the fluorescence changes in the distal region,the lipid content exchange efficiency can be estimated.In our experiment,LD content exchange rate differences between nascent and mature LDs as well as cells with normal and deficient LD budding machinery are observed.This probe expands the fluorescence-based toolbox for LD content dynamics studies.展开更多
The investigation of n-type doping holds a significant interest for the application of thermoelectrics.Herein,the doping of an indandione-terminated compound Q-4F with a singlet open-shell ground state was studied usi...The investigation of n-type doping holds a significant interest for the application of thermoelectrics.Herein,the doping of an indandione-terminated compound Q-4F with a singlet open-shell ground state was studied using two n-dopants N-DMBI and LCV.Both of these two dopants can effectively dope Q-4F due to the large offset between the singly occupied molecular orbital(SOMO)of dopants and the lowest unoccupied molecular orbital(LUMO)of Q-4F.N-DMBI has a higher doping ability than LCV as demonstrated by the UV-vis-NIR and EPR measurements.However,in comparison to N-DMBI doped Q-4F,LCV doped system exhibits much higher electrical conductivity and power factor due to its unperturbed molecular packing and favorable morphology after doping.The optimal conductivity of LCV doped Q-4F is 7.16×10^(-2)±0.16 S·cm^(-1) and the highest power factor reaches 12.3±0.85μW·m–1·K^(-2).These results demonstrate that the modulation of n-dopants is a powerful strategy to balance the doping efficiency and microstructure toward a maximum thermoelectric performance.展开更多
基金support from National Key Research and Development Program(2021YFA0717900)National Natural Science Foundation of China(62004138,52273190,52121002).
文摘Numerous reports have suggested that the performance of organic optoelectronic devices based on organicfieldeffect transistors(OFETs)is largely dependent on their interfaces.Self-assembled monolayers(SAMs)have been commonly used to engineer the interfaces of high-performance devices,particularly due to their well-defined structures and simple operation process through simple chemical adsorption growth.In this review,the structures of OFETs and SAM-modified OFETs are described,while different SAMs have been characterized.Furthermore,recent advances in the interface engineering of OFETs are described,the applicability of SAMs in functional devices of OFETs is reviewed,and existing problems and future developments in thisfield have been identified.
基金the financial support from National Postdoctoral Science Foundation of China(Nos.2021M702436 and BX2021211)Haihe Laboratory of Sustainable Chemical Transformations+1 种基金National Natural Science Foundation of China(Nos.22101202 and 22071173)Tianjin Science and Technology Programme(Nos.20JCJQJC00050 and 22ZYJDSS00060)。
文摘Implant-associated infections caused by biomedical catheters severely threaten patients'health.The use of electrochemical control on NO release from benign nitrite equipped in the catheter can potentially resolve this issue with excellent biocompatibility.Inspired by nitrite reductase,a Cu-BDC(BDC:benzene-1,4-dicarboxylic acid)catalyst with coordinated Cu(Ⅱ)sites was constructed as a heterogeneous electrocatalyst to control nitrite reduction to nitric oxide for catheter antibacteria.The combined results of in situ and ex situ tests unveil the key function of interconversion between Cu(Ⅱ)and Cu(Ⅰ)species in NO_(2)^(-)reduction to NO.After being incorporated into the actual catheter,the Cu-BDC catalyst exhibits high electrocatalytic activity toward NO_(2)^(-)reduction to NO and excellent antibacteria efficacy with a sterilizing rate of 99.9%,paving the way for the development of advanced metal-organic frameworks(MOFs)electrocatalysts for catheter antibacteria.
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-vip doping system,showing its wide applicability.
基金financial support from National Key Research and Development Program(Nos.2021YFA0717900,2022YFE0124200)National Natural Science Foundation of China(Nos.62004138,52273190,61905121,U2241221)Haihe Laboratory of Sustainable Chemical Transformations.
文摘The compatibility of the gate dielectrics with semiconductors is vital for constructing efficient conducting channel for high charge transport.However,it is still a highly challenging mission to clearly clarify the relationship between the dielectric layers and the chemical structure of semiconductors,especially vacuum-deposited small molecules.Here,interfacial molecular screening of polyimide(Kapton)dielectric in organic field-effect transistors(OFETs)is comprehensively studied.It is found that the semiconducting small molecules with alkyl side chains prefer to form a high-quality charge transport layer on polyimide(PI)dielectrics compared with the molecules without alkyl side chains.On this basis,the fabricated transistors could reach the mobility of 1.2 cm^(2) V^(−1)s^(−1) the molecule with alkyl side chains on bare PI dielectric.What is more,the compatible semiconductor and dielectric would further produce a low activation energy(E_(A))of 3.01 meV towards efficient charge transport even at low temperature(e.g.,100 K,0.9 cm^(2) V^(−1)s^(−1)).Our research provides a guiding scheme for the construction of high-performance thin-film field-effect transistors based on PI dielectric layer at room and low temperatures.
基金the National Natural Science Foundation of China(No.52273191,22235006)the Chinese Chemical Society Young Talent Lifting Project,the Natural Science Foundation of Tianjin City(No.22JCYBJC00760)+1 种基金the starting Grants of Tianjin University and Tianjin Government,the Open Fund of the State Key Laboratory of Luminescent Materials and Devices(South China University of Technology)(No.2024-skllmd-04)Independent Innovation Fund of Tianjin University(No.2023XPD-0014),for financial support.
文摘Organic afterglow materials have drawn increasing attention for their great potential in practical applications.Until now,most of them just show the lifetimes in milliseconds or seconds,while the realization of long persistent luminescence(LPL)lasting for minutes or even hours is difficult.In 2017,Adachi and Kabe successfully realize the LPL with a duration longer than 1 hour in a purely organic system,which can be even comparable to some excellent inorganic materials.However,partially for the unclear structure-property relationship,organic LPL materials are still rather scarce,especially for the stable ones in air or aqueous solution.In this review,we present the recent progress in organic LPL,mainly focusing on the material design strategy and internal mechanism.It is anticipated that the deep understanding can be beneficial for the further development of organic LPL materials with good stability in air and even aqueous phase.
基金supported by the Starting Grants of Tianjin University and Tianjin Government
文摘Aggregation-induced emission(AIE) has drawn great attention worldwide for its unique optical phenomenon and huge potential applications. Since coined by Ben Zhong Tang et al. in 2001, AIE has been deeply investigated and widely utilized in many important areas, such as organic light-emitting diode(OLED), sensor, and bio-imaging. Herein, we highlight some important progress of AIE in these eighteen years, including the exploration of internal mechanism and potential applications. Furthermore,some other interestingly emissive behaviors, originating but distinguishing from the AIE concept, are presented. It is anticipated an overall understanding about AIE could be easily caught from this short review for scientists, no matter whether they are involved in this exciting and rising research area or not.
基金the National Natural Science Foundation of China (51673151)Natural Science Foundation of Hubei Province (2017CFA002)the Fundamental Research Funds for the Central Universities (2042017kf0247 and 2042018kf0014) for financial support
文摘“Union is strength”.In the realm of organic molecules,the macroscopic performance of molecular aggregates is not just the simple overlay of single molecules,and in many cases,new properties can be created by molecular uniting with particular packing modes[1–4].As to the organic emissive materials,various changes can be rea-lized from single molecules to aggregates(Fig.1),in-cluding the emerged bright emission,the varied emission color,the different emission forms,and the arisen new excitation processes.
基金Wearegrateful to the National Natural Science Foundationof China(Nos.21734007,51973162,21875174)Excellent Youth Foundation of Hubei Scientific Committee(2020CFA084).
文摘Researchers investigated the organic optoelectronic materials and facilitated their development in organic light-emitting diodes(OLEDs),chemo-and biosensors,organic solar cells,data storage,and anticounterfeiting devices.Atoms make up molecules through chemical bonds,and molecular aggregates are formed through weak intermolecular interactions.The opto-electronic performance of these materials depends on not only the properties of the well-designed molecules with specific function groups,but also their aggregate states.The molecular aggregates in the form of nanoparticles can be applied in biological imaging,and films can be applied to photovoltaic and photodeformable devices,in which,the alignment of optoelectronic molecules can be either an ordered crystalline or an amorphous state.Generally,the crystalline materials could be deeply investigated by single crystal/powder X-ray diffraction analysis,which could provide the accurate information about molecular conformations,interactions and packing characteristics.It afforded a convenient way to investigate the possible relationship between molecular aggregates and opto-electronic properties.Among various opto-electronic materials,organic room temperature phosphorescence(RTP)materials exhibit the extremely sensitive luminescence property to molecular aggregates,even the dynamic properties can be detected by the tiny change of molecular aggregates.Thus,we selected the organic RTP emission as the output information of molecular aggregates,and afforded typical examples to find the possible relation between RTP effect and molecular packing.Accordingly,molecular packing can be adjusted by the external force as light,mechanical force,temperature,electric field,and so on,as well as the molecular structures as the building blocks,and the systematic investigation in the dynamic and static aggregation structures is of great value to the design of various optoelectronic materials.This review discusses the relationship among molecular structures,aggregation behaviors and corresponding optoelectronic properties by a comprehensive summary of recent research in our group,and the concept of molecular uniting set identified characteristic(MUSIC)is afforded.
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(51673151,51973162,21875174,21734007)the Natural Science Foundation of Hubei Province(2017CFA002)。
文摘Bright emission of organic luminogens at aggregated state has attracted increasing attention for their potential applications in opto-electronic devices and bio-/chemo-sensors.In this article,upon the introduction of different substituents(Br,Ph and TPh)to the large conjugated core of 9-methyl-9H-dibenzo[a,c]carbazole(DBC)moiety,the resultant luminogens demonstrated PL quantum yields in solid state ranging from 4.81%to 47.39%.Through the systematic investigation of molecular packing,together with theory calculation,the strong intermolecular electronic coupling in the dimers is proved as the main factor to the bright emission in the solid state.The results afforded a new avenue to investigate the intrinsic relationship among the molecular structures,packing modes and emission properties.
基金supported by the National Natural Science Foundation of China(21788102,52003228)the Innovation and Technology Commission(ITC-CNERC14SC01)+1 种基金the Research Grants Council of Hong Kong(16307020,C6009-17G,C6014-20W,and N-HKUST609/19)the Natural Science Foundation of Guangdong Province(2019B121205012)。
文摘Molecular interactions are crucial in diverse fields of protein folding,material science,nanotechnology,and life origins.Although mounting experimental research controls luminescent behavior by adjusting molecular interactions in light-emitting materials,it remains elusive to correlate microscopic molecular interactions with macroscopic luminescent behavior directly.Here,we synthesized three red luminogens with subtle structural variation and investigated the influence of molecular interactions on their luminescent behavior in solution and aggregate states.Our results indicate that strongπ-πand D-A interactions in both dilute solution(between luminogen and solvent molecules)and aggregate(between luminogens)states cause the redshift in emission,while weak interactions(e.g.,Van der Waals,C–H…π,and C–H…F interactions)enhance the quantum yield.This work provides a thoughtful investigation into the complicated influence of various molecular interactions on luminescent behavior.
基金funded by the National Natural Sci-ence Foundation of China(No.21905195)Natural Science Foundation of Tianjin City(No.20JCYBJC00800)PEIYANG Young Scholars Program of Tianjin University(No.2020XRX-0023).
文摘Biomass is a green and producible source of energy and chemicals.Hence,developing high-efficiency catalysts for biomass utilization and transformation is urgently demanded.Metal-organic framework(MOF)-based solid acid materials have been considered as promising catalysts in biomass transformation.In this review,we first introduce the genre of Lewis acid and Brønsted acid sites commonly generated in MOFs or MOF-based composites.Then,the methods for the generation and adjustment of corresponding acid sites are overviewed.Next,the catalytic applications of MOF-based solid acid materials in various biomass transformation reactions are summarized and discussed.Furthermore,based on our personal insights,the challenges and outlook on the future development of MOF-based solid acid catalysts are provided.We hope that this review will provide an instructive roadmap for future research on MOFs and MOF-based composites for biomass transformation.
基金supported by the National Natural Science Foundation of China(21905198)the Starting Grants of Tianjin University,Tianjin Government.
文摘Highly efficient persistent organic room temperature phosphorescence(RTP) has attracted increasing attention because of promising applications in fields of chemical sensors, optoelectronic devices, information security, and bioimaging, etc. Wherein,the crystal engineering of H-aggregation offers stabilization for long-lived triplet exciton for RTP, but the related research is rare because of the scarcity of ideal phosphorescent H-aggregate. Herein, we designed planar tricoordinate organoboron derivatives with molecular arrangement in ideal H-aggregation. The integration of Br atom can largely enhance RTP efficiency through increasing SOC effect, while the antiparallel molecular arrangement causes annihilation of triplet exciton. Thanks to good selfassembly property, their RTP can even be observed in PMMA matrix with doping ratio of merely 1 wt%. We further found that the cryogenic temperature contributes to stabilizing triplet exciton in H-aggregation, leading to red-shifted phosphorescence. By applying high hydrostatic pressure, the phosphorescence was largely enhanced and redshifted, demonstrating the crucial role of H-aggregation on RTP property. In phosphorescent tissue imaging of live mouse, nanoparticles of BrBA exhibited high contrast image via eliminating the interference of autofluorescence.
基金National Natural Science Foundation of China,Grant/Award Numbers:52173152,21805002Guangdong Basic and Applied Basic Research Foundation,Grant/Award Number:2020A1515110476+4 种基金Fund of the Rising Stars of Shaanxi Province,Grant/Award Number:2021KJXX-48Natural Science Basic Research Plan in Shaanxi Province of China,Grant/Award Numbers:2019JQ-302,2021JQ-801Research Foundation of Education Department of Shaanxi Province,Grant/Award Number:20JS005Young Talent fund of University Association for Science and Technology in Shaanxi,China,Grant/Award Numbers:20190610,20210606Scientific and Technological Innovation Team of Shaanxi Province,Grant/Award Number:2022TD-36。
文摘Enantioselective recognition and separation are the most important issues in the fields of chemistry,pharmacy,agrochemical,and food science.Here,we developed two optically active diamines showing aggregation-induced emission(AIE)that can discriminate 5 kinds of chiral acids with high enantioselectivity.Especially,a very high fluorescence intensity ratio(IL/ID)of 281 for(±)-Dibenzoyl-D/L-tartaric acid was obtained through the collection of fluorescence change after interaction with chiral AIE-active diamine.By virtue of AIE property and intermolecular acidbase interaction,enantioselective separation was facilely realized by simple filtration of the precipitates formed by chiral AIE luminogen(AIEgen)and one enantiomer in the racemic solution.The chiral HPLC data indicated that the precipitates of AIEgen/chiral acid possessed 82%L-analyte(the enantiomeric excess value was assessed to be 64%ee).Therefore,this method can serve as a simple,convenient,and low-cost tool for chiral detection and separation.
基金financially supported by Graduate Innovation Fund of Wuhan Institute of Technology,Natural Science Foundation of Hubei Province (No.2022CFB630)Open Fund of Key Laboratory of Green Preparation and Application for Functional Materials,Ministry of Education (Hubei University) (No.202105)。
文摘In recent years, the demand direction for electronic equipment has expanded into embedded and miniaturized devices. The heat radiation problem has become one of the most significant factors for hindering the development of electronic devices. Since heat radiation material is one of the important components in electronic devices, the demand for enhancing thermal conductivity is also increasingly urgent. Research on thermal conductive polymer composites has become a major direction for developing functional composites. This work reviewed the recent progress in the fabrication of thermal conductive polymer composites. Five different structures are presented, including the using of single fillers,hybrid fillers, double threshold percolation structure, segregated structure and other complex multiphase structures. Specifically, the preparation of high-performance thermal conductive polymer composites was introduced through the combination of various thermal conductive fillers.Finally, the development direction of high thermal conductive polymer composites was briefly explored.
基金the German Research Foundation(DFG:LE 2249/15-1)the Sino-German Center for Research Promotion(GZ1579)Y.R.and C.F.X.would like to appreciate the support from the China Scholarship Council(Nos.202207030010 and 20210637004).
文摘Zinc-air batteries(ZABs)are widely studied because of their high theoretical energy density,high battery voltage,environmental protection,and low price.However,the slow kinetics of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)on the air electrode limits the further application of ZABs,so that how to develop a cheap,efficient,and stable catalyst with bifunctional catalytic activity is the key to solving the development of ZABs.Transition metal compounds are widely used as cathode materials for ZABs due to their low cost,high electrocatalytic activity,and stable structure.This review summarizes the research progress of transition metal compounds as bifunctional catalysts for ZABs.The development history,operation principle,and mechanism of ORR and OER reactions are introduced first.The application and development of transition metal compounds as bifunctional catalysts for ZABs in recent years are systematically introduced,including transition metal oxides(TMOs),transition metal nitrides(TMNs),transition metal sulfides(TMSs),transition metal carbides(TMCs),transition metal phosphates(TMPs),and others.In addition,the shortcomings of transition metal compounds as bifunctional catalysts for ZABs were summarized and reasonable design strategies and improvement measures were put forward,aiming at providing a reference for the design and construction of high-performance ZABs cathode materials.Finally,the challenges and future in this field are discussed and prospected.
基金supported by the National Natural Science Foundation of China(52122317,22175120)the Developmental Fund for Science and Technology of Shenzhen government(JCYJ20220531101201003,RCYX20200714114525101,JCYJ20190808153415062,JCYJ20190808142403590)the Natural Science Foundation for Distinguished Young Scholars of Guangdong Province(2020B1515020011).
文摘The brightness of fluorescent agents directly determines the imaging performance as required.Among various fluorophores,small organic species are promising given its exact purity/composition and excellent processibility.However,chromophores with planar geometry may suffer from the undesirable aggregation-caused quenching(ACQ)phenomenon.Encouragingly,luminogens showing aggregation-induced emission(AIE)features are preferable as the aggregates which are the most common used state.In this review,we mainly focus on the strategies employed for boosting the brightness of AIE-active luminogens(AIEgens).From molecule to mor-phology levels,approaches that regulate electronic transition processes of the molecule or the packing extent of aggregates in order to confine molecular motion,reduceπ-πstacking,disrupt fluorophore-water interactions,etc.,are presented.In the end,the current challenges and perspectives are briefly discussed.We anticipate that this review will stimulate new insights and more efforts for the advancement of ultrabright AIEgens.
基金This work was supported by the National Natural Science Foundation of China(No.21905197)the Starting Grants of Tianjin University and Tianjin Government,China.
文摘The research of photo-responsive materials,with changed absorption and emission under light stimulus,has drawn more and more attention due to their wide applications.However,most of them suffered from the notorious aggregation-caused quenching(ACQ)effect,which often led to the unconspicuous luminescent change in photo-responsive process.To solve this problem,the strategy of combining aggregation-induced emission(AIE)and photochromic properties was utilized,which largely enriched the phenomenon and application of photo-responsive materials.This short review summarized the recent progress of photo-responsive AIE materials with changed UV absorbance or PL phenomenon under UV-irradiation,including the types of molecular structures,internal mechanisms and the practical applications.Also,some outlooks were given on the further exploration of this field at the end of this paper.
基金the National Natural Science Foundation of China(no.22005050)for its financial supportE.W.acknowledges the financial support from National Natural Science Foundation of China(no.52073082)+2 种基金Hubei Provincial Natural Science Foundation of China(no.2017CFB489)J.W.acknowledges financial support from GuangDong Basic and Applied Basic Research Foundation Regional Joint Fund(grant no.2020A1515110328)B.Z.T and S.C.acknowledge the Collaborative Research Fund(CRF)of the University Grants Committee(C6014-20W)for their financial support.
文摘The lipid droplet(LD)is a dynamic organelle responsible for lipid storage and metabolism that plays important roles in maintaining lipid homeostasis.However,limited strategies are available for tracking the LD content exchange.In this contribution,we report a novel fluorescent probe,TPEAmAl,for real-time LD content dynamics tracking.TPE-AmAl is LD-specific,but emits faintly due to its intramolecular motion.Upon photoactivation,it undergoes a photocyclodehydrogenation reaction and shows a large fluorescence increment.Thus,it can be used for highlighting selected LDs with high spatial resolution.By measuring the fluorescence changes in the distal region,the lipid content exchange efficiency can be estimated.In our experiment,LD content exchange rate differences between nascent and mature LDs as well as cells with normal and deficient LD budding machinery are observed.This probe expands the fluorescence-based toolbox for LD content dynamics studies.
基金supported by the National Key R&D Program of China(2021YFA0717900)the National Natural Science Foundation of China(Nos.22222506,52073209,and 52121002)and the Fundamental Research Funds for the Central Universities.
文摘The investigation of n-type doping holds a significant interest for the application of thermoelectrics.Herein,the doping of an indandione-terminated compound Q-4F with a singlet open-shell ground state was studied using two n-dopants N-DMBI and LCV.Both of these two dopants can effectively dope Q-4F due to the large offset between the singly occupied molecular orbital(SOMO)of dopants and the lowest unoccupied molecular orbital(LUMO)of Q-4F.N-DMBI has a higher doping ability than LCV as demonstrated by the UV-vis-NIR and EPR measurements.However,in comparison to N-DMBI doped Q-4F,LCV doped system exhibits much higher electrical conductivity and power factor due to its unperturbed molecular packing and favorable morphology after doping.The optimal conductivity of LCV doped Q-4F is 7.16×10^(-2)±0.16 S·cm^(-1) and the highest power factor reaches 12.3±0.85μW·m–1·K^(-2).These results demonstrate that the modulation of n-dopants is a powerful strategy to balance the doping efficiency and microstructure toward a maximum thermoelectric performance.
