A stimuli-responsive supramolecular polymer network(G-(CN)_(2)⊂BXDSP5)with aggregation-induced emission(AIE)properties has been efficiently constructed by host-guest interactions between pillar[5]arene derivative BXDS...A stimuli-responsive supramolecular polymer network(G-(CN)_(2)⊂BXDSP5)with aggregation-induced emission(AIE)properties has been efficiently constructed by host-guest interactions between pillar[5]arene derivative BXDSP5 and a homoditopic guest G-(CN)_(2),which shows not only excellent fluorescence properties due to the AIE effect but also desirable ion-sensing abilities in both solution and solid states,holding great potential in the applicable fluorescence detection for Fe^(3+).The resultant G-(CN)_(2)⊂BXDSP5 can be transformed into supramolecular polymer gel at high concentration via multiple noncovalent interactions,showing multi-stimuli-responsiveness in response to temperature change,mechanical force,and competitive agent.Meanwhile,the xerogel of supramolecular polymer material has been successfully used to remove Fe^(3+)from water with high adsorption efficiency.In addition,an ionresponsive film based on supramolecular polymer has also been developed,which can serve as a practical and convenient fluorescence test kit for detecting Fe^(3+).展开更多
The geometries and electronic structures of a series of electron donor-acceptor radical molecules have been studied theoretically.The computational results show that the introduction of substituents with strong electr...The geometries and electronic structures of a series of electron donor-acceptor radical molecules have been studied theoretically.The computational results show that the introduction of substituents with strong electron donating ability into tri-(2,4,6-trichlorophenyl)methyl(TTM)radicals enables the radical molecules to form the non-Aufbau electronic structure.The difficulty of forming the non-Aufbau electronic structure decreases with the enhancement of the electron donating ability of the substituent,but the expansion of the molecular conjugated system is not conducive to the formation.The hybridization of different fragments in molecular orbitals results in the disproportionation of orbital energy level and forms a staggered energy level structure.The electronic structure of radical molecules can be adjusted by substituents and molecular skeleton profoundly,which is a very effective means for molecular design.展开更多
Cubic-perovskite (SrTiO3) has a great potential to be utilized in a wide range of applications. However, currently very little is known about the shape and facet effects of SrTiO3 on their physicochemical properties...Cubic-perovskite (SrTiO3) has a great potential to be utilized in a wide range of applications. However, currently very little is known about the shape and facet effects of SrTiO3 on their physicochemical properties. This is largely owing to the difficulties in controlling the morphology of facets during synthesis. Herein, we describe a facile route for the facet- and size-controlled fabrication of single- crystalline SrTiO3 triangular prisms with highly exposed {101} side faces and {111} end faces. Theoretical and experimental studies of their photocatalytic performance have shown that triangular prisms exhibit superior photocatalytic activities than nanocubes with exposed (001) faces for the degradation of organic contaminants, which may be primarily attributed to the much higher surface energy of {101} facets (2.97 J/m^2) and {111} facets (2.80 J/m^2) than of that of {001} facets (0.98 J/m^2).展开更多
Covalent organic frameworks(COFs) are an emerging class of porous covalent organic structures whose backbones were composed of light elements(B,C,N,O,Si) and linked by robust covalent bonds to endow such material ...Covalent organic frameworks(COFs) are an emerging class of porous covalent organic structures whose backbones were composed of light elements(B,C,N,O,Si) and linked by robust covalent bonds to endow such material with desirable properties,i.e.,inherent porosity,well-defined pore aperture,ordered channel structure,large surface area,high stability,and multi-dimension.As expected,the abovementioned properties of COFs broaden the applications of this class of materials in various fields such as gas storage and separation,catalysis,optoelectronics,sensing,small molecules adsorption,and drug delivery.In this review,we outlined the synthesis of COFs and highlighted their applications ranging from the initial gas storage and separation to drug delivery.展开更多
A fluorescent supramolecular polymer network with an excellent triple-stimuli responsive property based on metal-ligand coordination and host-guest interactions has been constructed from a terpyridine-monofunctionaliz...A fluorescent supramolecular polymer network with an excellent triple-stimuli responsive property based on metal-ligand coordination and host-guest interactions has been constructed from a terpyridine-monofunctionalized leaning tower[6]arene,a tetraphenylethylene AIEgen,and a bridging coordination ion(Zn^2+).Addition of competitive binding agents,trifluoroacetic acid,and/or pillar[5]arene can break the metal coordination and/or host-guest inclusion complexation,and thermal heating can weaken the non-covalent interactions in the supramolecular polymer gel,all leading to the gel-to-sol transition.展开更多
High-entropy-oxides(HEOs),a new class of solids that contain five or more elemental species,have attracted increasing interests owing to their unique structures and fascinating physicochemical properties.However,it is...High-entropy-oxides(HEOs),a new class of solids that contain five or more elemental species,have attracted increasing interests owing to their unique structures and fascinating physicochemical properties.However,it is a huge challenge to construct various nanostructured,especially low-dimensional nanostructured HEOs under the high temperature synthetic conditions.Herein,a facile strategy using glucose-urea deep eutectic solvent(DES)as both a solvent and the carbon source of structure-directed template is proposed for the synthesis of various HEOs with two-dimentional(2D)nanonets and one-dimentional(1D)nanowires,including rock-salt(Co,Cu,Mg,Ni,Zn)O,spinel(Co,Cr,Fe,Mn,Ni)_(3)O_(4),and perovskite La(Co,Cr,Fe,Mn,Ni)O_(3).The as-prepared HEOs possessed five or more uniformly dispersed metal elements,large specific surface areas(more than 25 m^(2)·g^(−1)),and a pure single-phase structure.In addition,high cooling rate(cooling in air or liq-N_(2)-quenching)was indispensable to obtain a single-phase rock-salt(Co,Cu,Mg,Ni,Zn)O because of phase separation caused by copper.By taking advantage of unique features of HEOs,rock-salt(Co,Cu,Mg,Ni,Zn)O can function as a promising candidate for lithium-ion batteries(LIBs)anode material,which achieved excellent cycling stability.This work provides a feasible synthetic strategy for low-dimensional hierarchical HEOs,which creates new opportunities for the stable HEOs being highly active functional materials.展开更多
In recent years, cancer has become the number two cause of death around the world, and scientists have exploited various treatment maps. Calixarenes, with diversified features, have been widely applied into drug deliv...In recent years, cancer has become the number two cause of death around the world, and scientists have exploited various treatment maps. Calixarenes, with diversified features, have been widely applied into drug delivery systems, which can respond to multi-stimuli and exhibit excellent performance. In this mini-review, we summarize the recent advances on controlled drug delivery systems based on calixarenes, in the form of inclusion complexes, amphiphilic self-assembly nanocarriers including micelles, hydrogels, vesicles and liposomes, and supramolecular nanovalves on mesoporous silica nanomaterials.展开更多
We construct a fuorescent supramolecular system(TPE-Q_(4)⊂DSP5)of excellent tolerance to a wide range of pH by the facile selfassembly of a new pillar[5]arene bearing disulfonated arms(DSP5)with an AIE-active tetraphe...We construct a fuorescent supramolecular system(TPE-Q_(4)⊂DSP5)of excellent tolerance to a wide range of pH by the facile selfassembly of a new pillar[5]arene bearing disulfonated arms(DSP5)with an AIE-active tetraphenylethene-based tetratopic guest bearing four quaternary ammonium binding sites(TPE-Q_(4)),which exhibits strong blue emission even in dilute aqueous solutions along with much higher quantum yield and longer fuorescence lifetime than TPE-Q_(4) itself.Tis appreciable property can be attributed to the supramolecular assembly-induced emission(SAIE)mechanism endowed by the host-guest inclusion complexation based on synthetic macrocycles.Remarkably,the enhanced fuorescence of the supramolecular assembly is quenched efciently and exclusively by ferric ions in water with a high Stern–Volmer formula constant of 1.3×10^(5) mol^(−1),demonstrating the excellent cation selectivity and visualized responsiveness in ion sensing and detection.展开更多
An electrochemical sensor(carboxylatopillar[5]arene-coated nitrogen-doped carbon dots,namely CCDs)based on carboxylatopillar[5]arene(CP[5])functionalized nitrogen-doped carbon dots(N-CDs)has been developed in a facile...An electrochemical sensor(carboxylatopillar[5]arene-coated nitrogen-doped carbon dots,namely CCDs)based on carboxylatopillar[5]arene(CP[5])functionalized nitrogen-doped carbon dots(N-CDs)has been developed in a facile and economic manner.To improve the performance of this electrochemical sensor in pesticide detection,the optimal solution pH(pH 7)and loading amount of CCDs on the electrode(0.50 mg/mL)have been determined.By virtue of the good conductivity of N-CDs and the molecular recognition property of CP[5],CCDs modified glassy carbon electrode,namely CCDs/GCE,shows excellent anti-interference capability,selectivity,stability,and reproducibility in the sensitive detection of paraquat.The peak currents are proportional to the paraquat concentration(from 0.1μmol/L to 10μmol/L)with a detection limit of 6.4 nmol/L(S/N=3),indicating a great potential in pesticide detection.In comparison with the electrochemical sensors that require expensive metal nanoparticles and complex preparation processes,CCDs/GCE exhibits excellent detection capability of paraquat with lower cost and simpler preparation processes.展开更多
A biopolymer-inorganic hybrid system(MSN@PBLGF) is designed and fabricated from mesoporous silica nanoparticles(MSNs) and folic acid(FA)-terminated temperature-sensitive synthetic polypeptide,i.e.,poly(γ-benzyl-L-glu...A biopolymer-inorganic hybrid system(MSN@PBLGF) is designed and fabricated from mesoporous silica nanoparticles(MSNs) and folic acid(FA)-terminated temperature-sensitive synthetic polypeptide,i.e.,poly(γ-benzyl-L-glutamate)(PBLG) derivative,through a thiol-disulfide exchange reaction,where MSNs with high drug loading capacity serve as drug nanocarriers and the biocompatible PBLG biopolymer brushes installed on MSN surface through disulfide bonds endow the system with tumor-specific recognition ability and GSH/temperature dual-stimuli responsiveness.Controlled drug release experiments indicate that DOX can be tightly hosted in the system with limited premature release,but efficiently released in response to an increased concentration of GSH and/or an elevated temperature.Intracellular experiments demonstrate that the DOX-loaded MSN@PBLGF nanohybrid shows outstanding cellular uptake and cell-growth inhibition effects on human lung cancer cell line A549 in comparison with healthy human cells such as hepatocyte cells LO2.展开更多
Aggregation-induced emission(AIE),as an exciting photophysical phenomenon,has been regarded as one frontier research topic within both ranges of molecular luminescence and materials science over the last two decades.S...Aggregation-induced emission(AIE),as an exciting photophysical phenomenon,has been regarded as one frontier research topic within both ranges of molecular luminescence and materials science over the last two decades.Since controllable molecular ensembles with particular morphologies and tunable functions can be elegantly constructed in the realm of supramolecular chemistry,the integration of supramolecular assembly and AIE systems can expectedly bring about luminescent materials with tunable emission and tailorable well-ordered architectures.In this review,we will provide a summary of the creation and working mechanisms of AIE systems involving supramolecular systems that are driven by different supramolecular driving forces including hydrogen bonding,host−guest interactions,metal coordination,and π-π interactions.The morphological and photoluminescent features of these AIE-active supramolecular assemblies will be elucidated,and the regulated fluorescence properties of the AIEgens induced by the assembling-disassembling processes will be discussed in detail.展开更多
The production of high-purity n-hexane under mild conditions is of great significance in both the petrochemical industry and synthetic chemistry.Here,we report an easy-to-operate and energy-efficient n-hexane purifica...The production of high-purity n-hexane under mild conditions is of great significance in both the petrochemical industry and synthetic chemistry.Here,we report an easy-to-operate and energy-efficient n-hexane purification strategy using nonporous adaptive crystals of perethylated leaning pillar[6]arene(EtLP6).Adaptive EtLP6 crystals preferentially absorb n-hexane over other branched or cyclic C6 alkanes with similar boiling points.This selectivity arises from the different thermodynamic stabilities and variabilities of EtLP6 crystalloids loaded with n-hexane and other C6 alkanes.Moreover,the reversible transformations between the nonporous guest-free and n-hexane-containing structures make the EtLP6 crystals highly recyclable.展开更多
With the highly interdisciplinary of research and great development of microfabrication techniques,patterned surfaces have attracted great attention of researchers since they possess specific regularity and orderness ...With the highly interdisciplinary of research and great development of microfabrication techniques,patterned surfaces have attracted great attention of researchers since they possess specific regularity and orderness of structures.In recent years,series of two dimensional patterned structures have been successfully fabricated,and widely used in anti-reflection,anti-fogging,self-cleaning,and sensing,etc.In the meantime,patterned structures have been gradually used in biologically relative fields such as biomaterials,aiming to deepen the perception of organism and understand the vital movements of human body.In this review,we provide a brief introduction on current status of techniques for two dimensional patterns fabrication,the applications of patterned surfaces in biologically related fields,and give out a prospective on the development of these patterned surfaces in the future.展开更多
We report here a one-pot synthetic method for the synthesis of a bisester-functionalized copillar[5]arene(BECP5A) with yield up to 20%. The properties of BECP5A in solution and in solid state were deeply investigated ...We report here a one-pot synthetic method for the synthesis of a bisester-functionalized copillar[5]arene(BECP5A) with yield up to 20%. The properties of BECP5A in solution and in solid state were deeply investigated with the aid of 1D and 2D NMR spectra and X-ray diffraction, showing that this molecule has a fully self-included conformation in chloroform and partial self-inclusion in DMSO, and the compound has an asymmetrical structure with only one self-included side in the cavity of pillar[5]arene in the solid state. This compound will be used as the precursor of complex systems such as polymers and mechanically interlocked molecules.展开更多
Two strategies for the design of new pillar[5]arene-based mechanically self-interlocked molecules (MSMs) are reported here. The first strategy is based on the construction of an intermediate pseudo[1]rotaxane followed...Two strategies for the design of new pillar[5]arene-based mechanically self-interlocked molecules (MSMs) are reported here. The first strategy is based on the construction of an intermediate pseudo[1]rotaxane followed by the desired bis-[l]rotaxane. The other one is based on the construction of the desired bis-[1]rotaxane directly via a condensation reaction through host-guest interactions between a mono-functionalized pillar[5]arene and the axle. The newly synthesized bis-[1]rotaxane BR was characterized by ~1H NMR, ^(13)C NMR, 2D NMRs (~1H-^(13)C HSQC,~1H-~1H COSY and NOESY) and LC-ESI-MS,which indicated compound BR displayed an self-interlocked structure in CDCl_3. Surprisingly, the results of SEM, TEM and DLS showed that the compound BR could assemble into spherical nanoparticles in MeOH.展开更多
A well-known deep-blue emitting iridium(III) complex was selected for deuterium isotope effect evalua- tion, both on deuterated locations and numbers, through theoretical investigation. It was revealed that the cont...A well-known deep-blue emitting iridium(III) complex was selected for deuterium isotope effect evalua- tion, both on deuterated locations and numbers, through theoretical investigation. It was revealed that the containment of the d site deuteriation of ancillary ligand picolinate enabled the non-radiative deactivation process to be repessed, and thereby improving the quantum efficiency through such a simple and controllable approach.展开更多
Transformation of DNA into microbial cells via heat-shock approach has been well established in the fieldof molecular biology for decades. Herein we described an unexpected finding that heat-shock may not play an esse...Transformation of DNA into microbial cells via heat-shock approach has been well established in the fieldof molecular biology for decades. Herein we described an unexpected finding that heat-shock may not play an essen-tial role in the transformation process. This observation was verified via UV-Vis and fluorescence spectroscopies, andconfocal microscopy images for various DNAs and bacterial cells. The non-heat-shock approach proposed in thisstudy can be a convenient and beneficial modification for DNA transformation, especially for those laboratorieslacking ice machine and heat-shock equipment.展开更多
We made an extended study on the structure and properties of the low-lying electronic states of ethynyl substituted aniline and their cations. We performed these calculations using density functional theory method(B3...We made an extended study on the structure and properties of the low-lying electronic states of ethynyl substituted aniline and their cations. We performed these calculations using density functional theory method(B3LYP and CAM-B3LYP DFT) and the complete active space self-consistent field(CASSCF) approach in connection with the aug-cc-pVZ Dunning's basis sets and concerted ANO-L-VDZP basis sets. Our results included their equilibrium geometries, the vertical excitation spectra and the vertical and adiabatic ionization energies. The effect of ethynyl substitution on the electronic structure and the spectroscopy of aniline was probed.展开更多
Pillar[n]arenes(pillarenes for short)are a relatively new generation of macrocyclic host compounds with rigid cylinder architectures containing several hydroquinone units that are bridged by methylene(−CH2−)at their p...Pillar[n]arenes(pillarenes for short)are a relatively new generation of macrocyclic host compounds with rigid cylinder architectures containing several hydroquinone units that are bridged by methylene(−CH2−)at their para positions.The investigation of pillarenes has expanded from the sole domain of supramolecular chemistry to invoke immense interest among scientists striving to exploit intelligent materials or functional systems,with regard to their fascinating attributes such as symmetric structures,tailorable functionalization,and unique host−guest properties.Over the past few years,researchers have focused on the construction of prominent supramolecular architectures such as supramolecular switches,supramolecular polymers,and self-assembled amphiphilic systems on the basis of host−guest chemistry in collaboration with other noncovalent interactions.One of the most attractive characteristics of these supramolecular assemblies relies on the tunable mechanical motions via switching of the most conformationally and thermally stable structures in a dynamic and reversible manner,which could be affected by the external conditions and enable the reciprocal effect with surrounding environments.Consequently,macrocyclic arenes are the key components of stimuli-responsive supramolecular assemblies,serving as important candidates in the construction of advanced supramolecular materials,including organic functional systems and organic−inorganic hybrid systems.In this Account,we present a relatively elaborate summary of the significant and typical intelligent systems containing pillarenes and their extended versions with a focus on our own contributions to this field during the past decade.Finally,in the last section of the review,challenges and perspectives are given.展开更多
基金the Jilin Province University Cooperative Construction Project-Special Funds for New Materials(No.SXGJSF2017-3)for financial support。
文摘A stimuli-responsive supramolecular polymer network(G-(CN)_(2)⊂BXDSP5)with aggregation-induced emission(AIE)properties has been efficiently constructed by host-guest interactions between pillar[5]arene derivative BXDSP5 and a homoditopic guest G-(CN)_(2),which shows not only excellent fluorescence properties due to the AIE effect but also desirable ion-sensing abilities in both solution and solid states,holding great potential in the applicable fluorescence detection for Fe^(3+).The resultant G-(CN)_(2)⊂BXDSP5 can be transformed into supramolecular polymer gel at high concentration via multiple noncovalent interactions,showing multi-stimuli-responsiveness in response to temperature change,mechanical force,and competitive agent.Meanwhile,the xerogel of supramolecular polymer material has been successfully used to remove Fe^(3+)from water with high adsorption efficiency.In addition,an ionresponsive film based on supramolecular polymer has also been developed,which can serve as a practical and convenient fluorescence test kit for detecting Fe^(3+).
基金‘14th Five-Year’Science and Technology Project of the Education Department of Jilin Province,China(No.JJKH20220966KJ)Open Fund of the State Key Laboratory of Luminescent Materials and Devices of South China University of Technology,China(No.2022-skllmd-09)LIXIN Outstanding Young Scholar Training Program of Jilin University,China.
文摘The geometries and electronic structures of a series of electron donor-acceptor radical molecules have been studied theoretically.The computational results show that the introduction of substituents with strong electron donating ability into tri-(2,4,6-trichlorophenyl)methyl(TTM)radicals enables the radical molecules to form the non-Aufbau electronic structure.The difficulty of forming the non-Aufbau electronic structure decreases with the enhancement of the electron donating ability of the substituent,but the expansion of the molecular conjugated system is not conducive to the formation.The hybridization of different fragments in molecular orbitals results in the disproportionation of orbital energy level and forms a staggered energy level structure.The electronic structure of radical molecules can be adjusted by substituents and molecular skeleton profoundly,which is a very effective means for molecular design.
基金Acknowledgements This work received financial support from the National Natural Science Foundation of China (No, 51472226) and Dean Fund of Chinese Academy of Inspection and Quarantine (Nos. 2014JK005 and 2014JK006).
文摘Cubic-perovskite (SrTiO3) has a great potential to be utilized in a wide range of applications. However, currently very little is known about the shape and facet effects of SrTiO3 on their physicochemical properties. This is largely owing to the difficulties in controlling the morphology of facets during synthesis. Herein, we describe a facile route for the facet- and size-controlled fabrication of single- crystalline SrTiO3 triangular prisms with highly exposed {101} side faces and {111} end faces. Theoretical and experimental studies of their photocatalytic performance have shown that triangular prisms exhibit superior photocatalytic activities than nanocubes with exposed (001) faces for the degradation of organic contaminants, which may be primarily attributed to the much higher surface energy of {101} facets (2.97 J/m^2) and {111} facets (2.80 J/m^2) than of that of {001} facets (0.98 J/m^2).
基金financially supported by the National Natural Science Foundation of China (21835001, 51773080, 21674041, 51573068, 21221063, and 81870117)the Program for Changbaishan Scholars of Jilin Province, Jilin Province project (20160101305JC)+1 种基金Jilin Province Science and Technology Development Plan (20190201252JC)“Talents Cultivation Program” of Jilin University
基金the National Natural Science Foundation of China(Nos.51673084,51473061)the JLU Cultivation Fund for the National Science Fund for Distinguished Young Scholars,for financial support
文摘Covalent organic frameworks(COFs) are an emerging class of porous covalent organic structures whose backbones were composed of light elements(B,C,N,O,Si) and linked by robust covalent bonds to endow such material with desirable properties,i.e.,inherent porosity,well-defined pore aperture,ordered channel structure,large surface area,high stability,and multi-dimension.As expected,the abovementioned properties of COFs broaden the applications of this class of materials in various fields such as gas storage and separation,catalysis,optoelectronics,sensing,small molecules adsorption,and drug delivery.In this review,we outlined the synthesis of COFs and highlighted their applications ranging from the initial gas storage and separation to drug delivery.
基金the National Natural Science Foundation of China (No. 21871108) for financial support
文摘A fluorescent supramolecular polymer network with an excellent triple-stimuli responsive property based on metal-ligand coordination and host-guest interactions has been constructed from a terpyridine-monofunctionalized leaning tower[6]arene,a tetraphenylethylene AIEgen,and a bridging coordination ion(Zn^2+).Addition of competitive binding agents,trifluoroacetic acid,and/or pillar[5]arene can break the metal coordination and/or host-guest inclusion complexation,and thermal heating can weaken the non-covalent interactions in the supramolecular polymer gel,all leading to the gel-to-sol transition.
基金the Nationla Key R&D Program of China(No.2016YFA0203203)the National Natural Science Foundation of China(Nos.22074137 and 21721003).
文摘High-entropy-oxides(HEOs),a new class of solids that contain five or more elemental species,have attracted increasing interests owing to their unique structures and fascinating physicochemical properties.However,it is a huge challenge to construct various nanostructured,especially low-dimensional nanostructured HEOs under the high temperature synthetic conditions.Herein,a facile strategy using glucose-urea deep eutectic solvent(DES)as both a solvent and the carbon source of structure-directed template is proposed for the synthesis of various HEOs with two-dimentional(2D)nanonets and one-dimentional(1D)nanowires,including rock-salt(Co,Cu,Mg,Ni,Zn)O,spinel(Co,Cr,Fe,Mn,Ni)_(3)O_(4),and perovskite La(Co,Cr,Fe,Mn,Ni)O_(3).The as-prepared HEOs possessed five or more uniformly dispersed metal elements,large specific surface areas(more than 25 m^(2)·g^(−1)),and a pure single-phase structure.In addition,high cooling rate(cooling in air or liq-N_(2)-quenching)was indispensable to obtain a single-phase rock-salt(Co,Cu,Mg,Ni,Zn)O because of phase separation caused by copper.By taking advantage of unique features of HEOs,rock-salt(Co,Cu,Mg,Ni,Zn)O can function as a promising candidate for lithium-ion batteries(LIBs)anode material,which achieved excellent cycling stability.This work provides a feasible synthetic strategy for low-dimensional hierarchical HEOs,which creates new opportunities for the stable HEOs being highly active functional materials.
基金the National Natural Science Foundation of China (Nos. 21272093 and 51473061)the Fundamental Research Funds for the Central Universities (No. JCKY-QKJC05) for financial support
文摘In recent years, cancer has become the number two cause of death around the world, and scientists have exploited various treatment maps. Calixarenes, with diversified features, have been widely applied into drug delivery systems, which can respond to multi-stimuli and exhibit excellent performance. In this mini-review, we summarize the recent advances on controlled drug delivery systems based on calixarenes, in the form of inclusion complexes, amphiphilic self-assembly nanocarriers including micelles, hydrogels, vesicles and liposomes, and supramolecular nanovalves on mesoporous silica nanomaterials.
基金This work was supported by the National Natural Science Foundation of China(51673084 and 21871108)the Jilin Province-University Cooperative Construction Project-Special Funds for New Materials(SXGJSF2017-3)the Jilin University Talents Cultivation Program for fnancial support.
文摘We construct a fuorescent supramolecular system(TPE-Q_(4)⊂DSP5)of excellent tolerance to a wide range of pH by the facile selfassembly of a new pillar[5]arene bearing disulfonated arms(DSP5)with an AIE-active tetraphenylethene-based tetratopic guest bearing four quaternary ammonium binding sites(TPE-Q_(4)),which exhibits strong blue emission even in dilute aqueous solutions along with much higher quantum yield and longer fuorescence lifetime than TPE-Q_(4) itself.Tis appreciable property can be attributed to the supramolecular assembly-induced emission(SAIE)mechanism endowed by the host-guest inclusion complexation based on synthetic macrocycles.Remarkably,the enhanced fuorescence of the supramolecular assembly is quenched efciently and exclusively by ferric ions in water with a high Stern–Volmer formula constant of 1.3×10^(5) mol^(−1),demonstrating the excellent cation selectivity and visualized responsiveness in ion sensing and detection.
基金financially supported by the National Natural Science Foundation of China(No.21871108)Wuhan University of Science and Technologythe Jilin Province-University Cooperative Construction Project–Special Funds for New Materials(No.SXGJSF2017-3)。
文摘An electrochemical sensor(carboxylatopillar[5]arene-coated nitrogen-doped carbon dots,namely CCDs)based on carboxylatopillar[5]arene(CP[5])functionalized nitrogen-doped carbon dots(N-CDs)has been developed in a facile and economic manner.To improve the performance of this electrochemical sensor in pesticide detection,the optimal solution pH(pH 7)and loading amount of CCDs on the electrode(0.50 mg/mL)have been determined.By virtue of the good conductivity of N-CDs and the molecular recognition property of CP[5],CCDs modified glassy carbon electrode,namely CCDs/GCE,shows excellent anti-interference capability,selectivity,stability,and reproducibility in the sensitive detection of paraquat.The peak currents are proportional to the paraquat concentration(from 0.1μmol/L to 10μmol/L)with a detection limit of 6.4 nmol/L(S/N=3),indicating a great potential in pesticide detection.In comparison with the electrochemical sensors that require expensive metal nanoparticles and complex preparation processes,CCDs/GCE exhibits excellent detection capability of paraquat with lower cost and simpler preparation processes.
基金the Jilin Province-University Cooperative Construction Project-Special Funds for New Materials (No. SXGJSF2017-3) for financial support
文摘A biopolymer-inorganic hybrid system(MSN@PBLGF) is designed and fabricated from mesoporous silica nanoparticles(MSNs) and folic acid(FA)-terminated temperature-sensitive synthetic polypeptide,i.e.,poly(γ-benzyl-L-glutamate)(PBLG) derivative,through a thiol-disulfide exchange reaction,where MSNs with high drug loading capacity serve as drug nanocarriers and the biocompatible PBLG biopolymer brushes installed on MSN surface through disulfide bonds endow the system with tumor-specific recognition ability and GSH/temperature dual-stimuli responsiveness.Controlled drug release experiments indicate that DOX can be tightly hosted in the system with limited premature release,but efficiently released in response to an increased concentration of GSH and/or an elevated temperature.Intracellular experiments demonstrate that the DOX-loaded MSN@PBLGF nanohybrid shows outstanding cellular uptake and cell-growth inhibition effects on human lung cancer cell line A549 in comparison with healthy human cells such as hepatocyte cells LO2.
基金National Natural Science Foundation of China,Grant/Award Numbers:51673084,21871108Jilin Province-University Cooperative Construction Project--Special Funds for New Materials,Grant/Award Number:SXGJSF2017-3。
文摘Aggregation-induced emission(AIE),as an exciting photophysical phenomenon,has been regarded as one frontier research topic within both ranges of molecular luminescence and materials science over the last two decades.Since controllable molecular ensembles with particular morphologies and tunable functions can be elegantly constructed in the realm of supramolecular chemistry,the integration of supramolecular assembly and AIE systems can expectedly bring about luminescent materials with tunable emission and tailorable well-ordered architectures.In this review,we will provide a summary of the creation and working mechanisms of AIE systems involving supramolecular systems that are driven by different supramolecular driving forces including hydrogen bonding,host−guest interactions,metal coordination,and π-π interactions.The morphological and photoluminescent features of these AIE-active supramolecular assemblies will be elucidated,and the regulated fluorescence properties of the AIEgens induced by the assembling-disassembling processes will be discussed in detail.
基金the National Natural Science Foundation of China(21871108)Jilin Province-University Cooperative Construction Project-Special Funds for New Materials(SXGJSF2017-3)Jilin University Talents Cultivation Program for financial support.
文摘The production of high-purity n-hexane under mild conditions is of great significance in both the petrochemical industry and synthetic chemistry.Here,we report an easy-to-operate and energy-efficient n-hexane purification strategy using nonporous adaptive crystals of perethylated leaning pillar[6]arene(EtLP6).Adaptive EtLP6 crystals preferentially absorb n-hexane over other branched or cyclic C6 alkanes with similar boiling points.This selectivity arises from the different thermodynamic stabilities and variabilities of EtLP6 crystalloids loaded with n-hexane and other C6 alkanes.Moreover,the reversible transformations between the nonporous guest-free and n-hexane-containing structures make the EtLP6 crystals highly recyclable.
基金financially supported by the National Basic Research Program of China(973 program,No.2012CB933800)the National Natural Science Foundation of China(NSFC,No.91123031)
文摘With the highly interdisciplinary of research and great development of microfabrication techniques,patterned surfaces have attracted great attention of researchers since they possess specific regularity and orderness of structures.In recent years,series of two dimensional patterned structures have been successfully fabricated,and widely used in anti-reflection,anti-fogging,self-cleaning,and sensing,etc.In the meantime,patterned structures have been gradually used in biologically relative fields such as biomaterials,aiming to deepen the perception of organism and understand the vital movements of human body.In this review,we provide a brief introduction on current status of techniques for two dimensional patterns fabrication,the applications of patterned surfaces in biologically related fields,and give out a prospective on the development of these patterned surfaces in the future.
基金the JLU Cultivation Fund for the National Science Fund for Distinguished Young ScholarsNMAC, College of Chemistry at Jilin University for financial support
文摘We report here a one-pot synthetic method for the synthesis of a bisester-functionalized copillar[5]arene(BECP5A) with yield up to 20%. The properties of BECP5A in solution and in solid state were deeply investigated with the aid of 1D and 2D NMR spectra and X-ray diffraction, showing that this molecule has a fully self-included conformation in chloroform and partial self-inclusion in DMSO, and the compound has an asymmetrical structure with only one self-included side in the cavity of pillar[5]arene in the solid state. This compound will be used as the precursor of complex systems such as polymers and mechanically interlocked molecules.
文摘Two strategies for the design of new pillar[5]arene-based mechanically self-interlocked molecules (MSMs) are reported here. The first strategy is based on the construction of an intermediate pseudo[1]rotaxane followed by the desired bis-[l]rotaxane. The other one is based on the construction of the desired bis-[1]rotaxane directly via a condensation reaction through host-guest interactions between a mono-functionalized pillar[5]arene and the axle. The newly synthesized bis-[1]rotaxane BR was characterized by ~1H NMR, ^(13)C NMR, 2D NMRs (~1H-^(13)C HSQC,~1H-~1H COSY and NOESY) and LC-ESI-MS,which indicated compound BR displayed an self-interlocked structure in CDCl_3. Surprisingly, the results of SEM, TEM and DLS showed that the compound BR could assemble into spherical nanoparticles in MeOH.
基金Supported by the National Natural Science Foundation of China(No.21171065) and the Young Scholar Training Program of Jilin University, China.
文摘A well-known deep-blue emitting iridium(III) complex was selected for deuterium isotope effect evalua- tion, both on deuterated locations and numbers, through theoretical investigation. It was revealed that the containment of the d site deuteriation of ancillary ligand picolinate enabled the non-radiative deactivation process to be repessed, and thereby improving the quantum efficiency through such a simple and controllable approach.
文摘Transformation of DNA into microbial cells via heat-shock approach has been well established in the fieldof molecular biology for decades. Herein we described an unexpected finding that heat-shock may not play an essen-tial role in the transformation process. This observation was verified via UV-Vis and fluorescence spectroscopies, andconfocal microscopy images for various DNAs and bacterial cells. The non-heat-shock approach proposed in thisstudy can be a convenient and beneficial modification for DNA transformation, especially for those laboratorieslacking ice machine and heat-shock equipment.
基金Supported by the National Natural Science Foundation of China(No.21173096) and the National Basic Research Program of China(No. 2013CB83480).
文摘We made an extended study on the structure and properties of the low-lying electronic states of ethynyl substituted aniline and their cations. We performed these calculations using density functional theory method(B3LYP and CAM-B3LYP DFT) and the complete active space self-consistent field(CASSCF) approach in connection with the aug-cc-pVZ Dunning's basis sets and concerted ANO-L-VDZP basis sets. Our results included their equilibrium geometries, the vertical excitation spectra and the vertical and adiabatic ionization energies. The effect of ethynyl substitution on the electronic structure and the spectroscopy of aniline was probed.
基金the National Natural Science Foundation of China(21871108)the Jilin Province-University Cooperative Construction Project-Special Funds for New Materials(SXGJSF2017-3)the Jilin University Talents Cultivation Program for financial support.
文摘Pillar[n]arenes(pillarenes for short)are a relatively new generation of macrocyclic host compounds with rigid cylinder architectures containing several hydroquinone units that are bridged by methylene(−CH2−)at their para positions.The investigation of pillarenes has expanded from the sole domain of supramolecular chemistry to invoke immense interest among scientists striving to exploit intelligent materials or functional systems,with regard to their fascinating attributes such as symmetric structures,tailorable functionalization,and unique host−guest properties.Over the past few years,researchers have focused on the construction of prominent supramolecular architectures such as supramolecular switches,supramolecular polymers,and self-assembled amphiphilic systems on the basis of host−guest chemistry in collaboration with other noncovalent interactions.One of the most attractive characteristics of these supramolecular assemblies relies on the tunable mechanical motions via switching of the most conformationally and thermally stable structures in a dynamic and reversible manner,which could be affected by the external conditions and enable the reciprocal effect with surrounding environments.Consequently,macrocyclic arenes are the key components of stimuli-responsive supramolecular assemblies,serving as important candidates in the construction of advanced supramolecular materials,including organic functional systems and organic−inorganic hybrid systems.In this Account,we present a relatively elaborate summary of the significant and typical intelligent systems containing pillarenes and their extended versions with a focus on our own contributions to this field during the past decade.Finally,in the last section of the review,challenges and perspectives are given.