We present a microwave-assisted one-pot polymerization with three-components of alkynes, aldehydes and amines for the synthesis of new amino-functionalized optoelectronic polymers. The polymerization of diynes （la-lc...We present a microwave-assisted one-pot polymerization with three-components of alkynes, aldehydes and amines for the synthesis of new amino-functionalized optoelectronic polymers. The polymerization of diynes （la-lc）, dialdehydes （2a and 2b） and dibenzylamine catalyzed by InC13 was carried out smoothly within 1 h under microwave radiation, yielding four soluble polymers with high molecular weights. The resulting polymers P1 and P2 could be easily dissolved in alcohol and thus utilized as the cathode interlayer for polymer solar cells （PSCs）. Compared with the control device, the PSCs with P1 and P2 as the cathode interlayer and PTB7-Th：PC71BM as the photoactive layer exhibited significantly higher power conversion efficiencies （PCEs） of 9.49% and 9.16%, respectively. These results suggest that this polycoupling reaction is an efficient approach to construct three-component polymers for the practical applications.展开更多
L-glutamic acid(LA)is a bio-based,non-toxic,environmentally friendly material derived from biomass.The present study reports the application of Passerini three-component polymerization(P-3CP)for the straightforward pr...L-glutamic acid(LA)is a bio-based,non-toxic,environmentally friendly material derived from biomass.The present study reports the application of Passerini three-component polymerization(P-3CP)for the straightforward preparation of LA-based light-responsive polyesters(PLTDs)under mild conditions.PLTDs with molar masses up to 8500 g/mol and high yields exceeding 90%are obtained.The chemical structures and light-responsive self-immolative behavior of PLTDs are comprehensively characterized by employing ultraviolet-visible(UV-Vis)spectroscopy,size exclusion chromatography(SEC),nuclear magnetic resonance(NMR)spectroscopy,and liquid chromatography mass spectrometry(LC-MS).Meanwhile,monodisperse PLTD-based doxorubicin-loaded nanoparticles(PLTD-DOX-NP)(size=193 nm,PDI=0.018)are formulated by nanoprecipitation method.Upon light-induced depolymerization,the PLTD-DOX-NP undergoes rapid decomposition,resulting in a burst release of 80%cargo within 13 s.Furthermore,according to biological toxicity tests,the PLTD-NP possesses adequate biosafety,both before and after irradiation.Overall,the incorporation of P-3CP with biorenewable LA-based monomer adheres to the principles of green chemistry,significantly simplifying the synthetic pathway of light-responsive polymers.展开更多
A simple and efficient method has been developed for the synthesis ofα-amino nitriles from aldehydes,amines and trimethylsilyl cyanide（Me_3SiCN） in the presence of a catalytic amount of cyanuric acid at room temper...A simple and efficient method has been developed for the synthesis ofα-amino nitriles from aldehydes,amines and trimethylsilyl cyanide（Me_3SiCN） in the presence of a catalytic amount of cyanuric acid at room temperature.展开更多
A simple and general strategy is described for preparing network supported catalyst through a one-pot synthetic procedure using supramolecular gel as template.This procedure directly attaches ligand to support during ...A simple and general strategy is described for preparing network supported catalyst through a one-pot synthetic procedure using supramolecular gel as template.This procedure directly attaches ligand to support during fabricating the support.Using this strategy,supported CuBr/di-（2-picolyl） amine catalyst with U-shaped fibrillar network was prepared and used in atom transfer radical polymerization of methyl methacrylate.XPS and SEM characterization of the catalyst revealed homogeneous distribution of ligand,sufficient reactive sites,adequate mechanical strength and macroporosity.The polymerization results demonstrated high activity and reusability of such catalyst.This strategy might be extended to other supported catalysts used in column reactors.展开更多
Novel pyrido[2,3-d]pyrimidine derivatives were synthesized through a one-pot three-component approach using HAp-encapsulated-γ-Fe2O3[γ-Fe2O3@HAp-SO3H]catalyzed condensation of 6-arnino-2-（methylthio or ethylthio）p...Novel pyrido[2,3-d]pyrimidine derivatives were synthesized through a one-pot three-component approach using HAp-encapsulated-γ-Fe2O3[γ-Fe2O3@HAp-SO3H]catalyzed condensation of 6-arnino-2-（methylthio or ethylthio）pyrimidin-4（3H）-one,Meldrum＇s acid and aryl aldehydes at 60 ℃ and under solvent-free conditions.In this protocol the use of nanocatalyst provided a green,useful and rapid method to generate the products in short reaction times and excellent yields（88%-94%）.展开更多
Polyimides are well-known for their high chemical inertness and thermal stability. However, it is usually challenging to synthesize UV-curable polyimides since the imidization reaction requires such harsh conditions t...Polyimides are well-known for their high chemical inertness and thermal stability. However, it is usually challenging to synthesize UV-curable polyimides since the imidization reaction requires such harsh conditions that acrylate type double bonds cannot withstand. In this work, synthetic methods are developed to obtain polyester-imide type binder polymers with high thermal stability, high compatibility with the other components of the black photoresist, and fine photolithographic patterning property for the negative-tone black photoresist. The syntheses of diimide-diacid or diimide-diol intermediates for the polyesterification with dianhydride gave polyester imides which meets this requirement. The photolithographic tests have shown that the patterning of the micron-sized PDL of the organic light emitting diode (OLED) panel could be obtained. This work will interest the researchers working on the design and optimization of thermally stable binder polymers.展开更多
Poly(ester amide)s(PEAs)attract much attention as a new kind of biodegradable polymers.However,the synthesis of PEAs with sequence-regulated chain structures is still complicated due to the multistep polymerization,hi...Poly(ester amide)s(PEAs)attract much attention as a new kind of biodegradable polymers.However,the synthesis of PEAs with sequence-regulated chain structures is still complicated due to the multistep polymerization,high monomer purity,as well as the usage of organic solvents,which greatly inhibits its development and applications.Herein,a one-pot strategy without solvent was developed to synthesize the alternating PEA fromα,ω-amino alcohol and dicarboxylic acid by sequential polycondensation,where water was used as the controlling agent for amidation and esterification.Specifically,the amidation and esterification were controlled to proceed in turn by adding or removing water,realizing the one-pot preparation of alternating PEAs.The resultant PEA is characterized by^1H-and^(13)C-NMR,and its chain structure is confirmed to be highly quasi-alternating similar to alternating PEAs prepared by classical methods The evaluations from DSC and DMA demonstrate that the properties of quasi-alternating PEA(T_(m)=102℃,ΔH_(m)=30J·g^(-1))are far superior to those of random PEA(T_(m)=72℃,ΔH_(m)<1 J·g^(-1)).展开更多
A one-pot sequential reaction for efficient synthesis of pyrrolo[2,1-a]isoquinoline and pyrrolo[1,2-a]quinoline derivatives has been developed.The reaction included firstly the Cu-catalyzed three-component reaction of...A one-pot sequential reaction for efficient synthesis of pyrrolo[2,1-a]isoquinoline and pyrrolo[1,2-a]quinoline derivatives has been developed.The reaction included firstly the Cu-catalyzed three-component reaction of isoquinoline（quinoline）,acetylenedicarboxylate and alkynylbenzene and then Cs 2 CO 3-promoted intramolecular cyclization reaction of initially formed 1-alkenyl-2-alkynyl-1,2-dihydroisoquinoline（1,2-dihydroquinoline）.展开更多
A simple and fastthree-component synthesis of new and biologically active hexahydro-2-quinolinecarboxylic acid scaf-fold 4 was carried out using cyclocondensation reaction of arylmethylidenepyruvic acids 1, 1,3-cycloh...A simple and fastthree-component synthesis of new and biologically active hexahydro-2-quinolinecarboxylic acid scaf-fold 4 was carried out using cyclocondensation reaction of arylmethylidenepyruvic acids 1, 1,3-cyclohexandiones 2 and ammonium acetate 3 under solvent-free conditions and at room temperature. This protocol has the advantages of facility, easy work-up, high yields, short reaction time and environmentally friendly character.展开更多
Polyimides are well known for their high chemical and thermal stability. However, a few polyimide samples have been reported which are completely soluble in such environmentally friendly and common organic solvent as ...Polyimides are well known for their high chemical and thermal stability. However, a few polyimide samples have been reported which are completely soluble in such environmentally friendly and common organic solvent as propyleneglycol monomethyl ether acetate (PGMEA). In this work thermally stable, organosoluble and photocurable acidic polyimides were synthesized by simple and cost effective one-pot solution method. They polyimides obtained by this method showed much higher thermal stability (1 wt% loss temperature 345°C) than melt polymerized polyimides owing to the photocrosslinking reactions by the terminal double bonds.展开更多
The development of degradable polymers represents an appealing strategy to address ever-growing concerns for treating waste plastics.Olefin metathesis polymerization has been extensively explored for the synthesis of ...The development of degradable polymers represents an appealing strategy to address ever-growing concerns for treating waste plastics.Olefin metathesis polymerization has been extensively explored for the synthesis of various degradable polymers.Cyclic–acyclic monomers metathesis polymerization(CAMMP)has recently been reported to produce degradable polymers via copolymerization of cyclic monomers with acyclic diene comonomers.Unfortunately,this strategy suffers from poor product material properties,especially at high contents of diene comonomers.To address this issue,we have designed a tandem olefin metathesis polymerization(TOMP)system that combines olefin ringclosing metathesis(RCM)of diene comonomers,followed by ring-opening metathesis copolymerization(ROMCP)with cyclic olefin monomers(dicyclopentadiene,cyclooctene,or alkyl-substituted cyclooctene).This strategy overcame the intrinsic limitations of diene-induced chain-transfer reactions during olefin metathesis,leading to degradable polymers with high molecular weights and excellent material properties.The selection of different cyclic olefin monomers provided access to degradable and recyclable cross-linked thermosets,linear thermoplastics,and elastomers.Notably,this one-pot,two-step process was highly efficient and required the addition of only one metathesis catalyst.展开更多
Multicomponent metal sulfides have been recognized as promising anode materials for lithium/sodiumion storage given their enticing theoretical capacities. However, the simplification of synthetic processes and the con...Multicomponent metal sulfides have been recognized as promising anode materials for lithium/sodiumion storage given their enticing theoretical capacities. However, the simplification of synthetic processes and the construction of heterogeneous interfaces of multimetal sulfides remain great challenges. Herein,a hierarchical 1T-MoS2/carbon nanosheet decorated Co1–xS/N-doped carbon(Co1–xS/NC@MoS2/C) hollow nanofiber was designed and constructed via a one-pot hydrothermal method using a cobalt-based coordination polymer nanofiber. This nanofiber can transform in-situ into conductive N-doped carbon hollow fibers embedded with active Co1–xS nanoparticles, enabling the epitaxial growth of MoS2 nanosheets.Consequently, the Co1–xS/NC@MoS2/C composites achieve exceptional lithium/sodium-ion storage performance. Compared to MoS2/C microspheres and Co1–xS/NC hollow nanofibers alone, the Co1–xS/NC@MoS2/C hollow nanofibers deliver higher discharge capacities(1085.9 mAh g^-1 for lithium-ion batteries(LIBs) and 748.5 mAh g^-1 for sodium-ion batteries(SIBs) at 100 mA g^-1), better capacity retention(910 mAh g^-1 for LIBs and 636.5 mAh g^-1 for SIBs after 150 cycles at 100 mA g^-1), and increased cycling stability(407.2 mAh g^-1 after 1000 cycles for SIBs at 1000 m A g^-1). Furthermore, the kinetic analysis shows that the lithium/sodium-ion storage processes of the Co1–xS/NC@MoS2/C electrode are mainly controlled by pseudocapacitance behavior. The excellent electrochemical properties can thus be ascribed to the synergy of the MoS2/C nanosheets with the enlarged interlayer spacing, good conductivity of the carbon layers, and the Co1–xS nanoparticles embedded in the hollow nanofibers with extensive reaction sites.展开更多
4-Arylmethylidene-4,5-dihydro-3-phenylisoxazol-5-ones were synthesized by the convenient three-component reaction of ethyl benzoylacetate,hydroxylamine and aromatic aldehydes in the presence of pyridine.The target com...4-Arylmethylidene-4,5-dihydro-3-phenylisoxazol-5-ones were synthesized by the convenient three-component reaction of ethyl benzoylacetate,hydroxylamine and aromatic aldehydes in the presence of pyridine.The target compounds were also obtained by the reaction between 3-phenylisoxazol-5-one and aromatic aldehydes at 105℃under solvent free condition.Yields of products depended considerably on the aldehyde used.展开更多
The one-pot three-component reaction of arylmethylidenepyruvic acids, 1,3-cyclohexandiones and ammonium acetate provides an economical and efficient synthetic route to 5-oxo-4-aryl-1,4,5,6,7,8-hexahydro-2-quinolinecar...The one-pot three-component reaction of arylmethylidenepyruvic acids, 1,3-cyclohexandiones and ammonium acetate provides an economical and efficient synthetic route to 5-oxo-4-aryl-1,4,5,6,7,8-hexahydro-2-quinolinecarboxylic acid 4 under solvent-free conditions using a catalytic amount of TiO2 nanoparticles （TiO2 NPs） as an effective heterogeneous catalyst.展开更多
An efficient ultrasound-assisted preparation of a series of novel 4-aryl-3-methyl-4,5-dihydro-l//-pyrazolo[34-b]pyridin-6（7H）ones via the reaction of 5-amino-3-methyl-1H-pyrazole,Meldrum＇s acid and various arylalde...An efficient ultrasound-assisted preparation of a series of novel 4-aryl-3-methyl-4,5-dihydro-l//-pyrazolo[34-b]pyridin-6（7H）ones via the reaction of 5-amino-3-methyl-1H-pyrazole,Meldrum＇s acid and various arylaldehydes using one-pot three-component approach is described.This rapid method produced the products in short reaction times（3-4 min） and excellent yields（87-95%）.展开更多
In this study,a method was developed to form C(sp^(3))-C(sp^(2))bonds via copper catalyst-promoted cross coupling of 2-methylquinoline and in-situ-activated 3-haloisoquinoline under mild conditions.The multi-component...In this study,a method was developed to form C(sp^(3))-C(sp^(2))bonds via copper catalyst-promoted cross coupling of 2-methylquinoline and in-situ-activated 3-haloisoquinoline under mild conditions.The multi-component tandem reaction was used to construct new C-N,C=O and C-C bonds in one pot via sequential functionalization of the N1,C3 and C1 positions of 3-haloisoquinoline.This method can be used to efficiently access 1,2-disubstituted isoquinolinones by the three-component reaction of 3-halogen isoquinoline,alkyl halide,and 2-methylquinoline.展开更多
A new cerium polyoxomolybdate { [Ce （ H2 O） 7 Al （ OH ） 6 Mo6 O18 ] · 4H20 } （ compound 1 ） was synthesized and characterized by X-ray diffraction analysis, elemental analysis, TG analysis and IR spectromet...A new cerium polyoxomolybdate { [Ce （ H2 O） 7 Al （ OH ） 6 Mo6 O18 ] · 4H20 } （ compound 1 ） was synthesized and characterized by X-ray diffraction analysis, elemental analysis, TG analysis and IR spectrometry. Compound 1 exhibits a zigzag chain-like structure, which is constructed from an Anderson type anion and rare earth metal, Ce（ Ⅲ ）. These 1-D chains are further extended into a 3-D network by the aid of muhipoint hydrogen-bonding interactions.展开更多
4-（Succinimido）-1-butane sulfonic acid as an efficient and reusable Bronsted acid catalyzed the synthesis of pyrano[4,3-b]pyran derivatives under solvent-free conditions.The catalyst can be prepared by mixing succin...4-（Succinimido）-1-butane sulfonic acid as an efficient and reusable Bronsted acid catalyzed the synthesis of pyrano[4,3-b]pyran derivatives under solvent-free conditions.The catalyst can be prepared by mixing succinimide and 1,4-butanesultone that is more simple and safer than the preparation of succinimide sulfonic acid.This method has the advantages of high yield,clean reaction,simple methodology and short reaction time.The catalyst could be recycled without significant loss of activity.展开更多
A one-pot three-component reaction of aldehydes, nitroalkanes and NaN3 for the synthesis ofNH-1,2,3-triazoles has been developed. The reaction provides a safe, efficient and step-economic approach for the synthesis of...A one-pot three-component reaction of aldehydes, nitroalkanes and NaN3 for the synthesis ofNH-1,2,3-triazoles has been developed. The reaction provides a safe, efficient and step-economic approach for the synthesis of various NH-1,2,3-triazoles in good to excellent yields.展开更多
The one-pot hydrothermal reaction of CuCl2 with H2CPOA and 4,4＇-bpy results in two new coordination polymers, [Cu（CPOA）（4,4＇-bpy）（H2O）2]·1.5H2O （1） and [Cu2（HCPOA）4（4,4＇-bpy）4] （2） （H2CPOA=4-car...The one-pot hydrothermal reaction of CuCl2 with H2CPOA and 4,4＇-bpy results in two new coordination polymers, [Cu（CPOA）（4,4＇-bpy）（H2O）2]·1.5H2O （1） and [Cu2（HCPOA）4（4,4＇-bpy）4] （2） （H2CPOA=4-carboxyphenoxy acetic acid, 4,4＇-bpy=4,4＇-bipyridine） since CPOA^2- anions reach equilibrium with HCPOA^- anions in the reaction system. The crystal structure of 1 shows a triple interpenetration CdSO4-like net with 1D channel, in which lattice water molecules are located. Complex 2 is a ladder-like 1D double chain structure assembled through coordination bonds and O—H…N hydrogen bonds.展开更多
基金financially supported by the National Natural Science Foundation of China(No.21490573)
文摘We present a microwave-assisted one-pot polymerization with three-components of alkynes, aldehydes and amines for the synthesis of new amino-functionalized optoelectronic polymers. The polymerization of diynes （la-lc）, dialdehydes （2a and 2b） and dibenzylamine catalyzed by InC13 was carried out smoothly within 1 h under microwave radiation, yielding four soluble polymers with high molecular weights. The resulting polymers P1 and P2 could be easily dissolved in alcohol and thus utilized as the cathode interlayer for polymer solar cells （PSCs）. Compared with the control device, the PSCs with P1 and P2 as the cathode interlayer and PTB7-Th：PC71BM as the photoactive layer exhibited significantly higher power conversion efficiencies （PCEs） of 9.49% and 9.16%, respectively. These results suggest that this polycoupling reaction is an efficient approach to construct three-component polymers for the practical applications.
基金This work was financially supported by the International Science and Technology Assistance Program of the Ministry of Science and Technology(No.KY202001016)Shandong Provincial Natural Science Foundation Magnitude Fundamental Research,China(No.ZR2022ZD11)Qingdao New Energy Shandong Laboratory Open Project(No.QNESL OP202312).
文摘L-glutamic acid(LA)is a bio-based,non-toxic,environmentally friendly material derived from biomass.The present study reports the application of Passerini three-component polymerization(P-3CP)for the straightforward preparation of LA-based light-responsive polyesters(PLTDs)under mild conditions.PLTDs with molar masses up to 8500 g/mol and high yields exceeding 90%are obtained.The chemical structures and light-responsive self-immolative behavior of PLTDs are comprehensively characterized by employing ultraviolet-visible(UV-Vis)spectroscopy,size exclusion chromatography(SEC),nuclear magnetic resonance(NMR)spectroscopy,and liquid chromatography mass spectrometry(LC-MS).Meanwhile,monodisperse PLTD-based doxorubicin-loaded nanoparticles(PLTD-DOX-NP)(size=193 nm,PDI=0.018)are formulated by nanoprecipitation method.Upon light-induced depolymerization,the PLTD-DOX-NP undergoes rapid decomposition,resulting in a burst release of 80%cargo within 13 s.Furthermore,according to biological toxicity tests,the PLTD-NP possesses adequate biosafety,both before and after irradiation.Overall,the incorporation of P-3CP with biorenewable LA-based monomer adheres to the principles of green chemistry,significantly simplifying the synthetic pathway of light-responsive polymers.
文摘A simple and efficient method has been developed for the synthesis ofα-amino nitriles from aldehydes,amines and trimethylsilyl cyanide（Me_3SiCN） in the presence of a catalytic amount of cyanuric acid at room temperature.
基金support from the National Natural Science Foundation of China(Nos.20574041 and 20874055)Hi-tech Research and Development Program(863 plan) of China(No.2009AA062903)
文摘A simple and general strategy is described for preparing network supported catalyst through a one-pot synthetic procedure using supramolecular gel as template.This procedure directly attaches ligand to support during fabricating the support.Using this strategy,supported CuBr/di-（2-picolyl） amine catalyst with U-shaped fibrillar network was prepared and used in atom transfer radical polymerization of methyl methacrylate.XPS and SEM characterization of the catalyst revealed homogeneous distribution of ligand,sufficient reactive sites,adequate mechanical strength and macroporosity.The polymerization results demonstrated high activity and reusability of such catalyst.This strategy might be extended to other supported catalysts used in column reactors.
基金the Research Council of University of Guilan for the financial support of this research work
文摘Novel pyrido[2,3-d]pyrimidine derivatives were synthesized through a one-pot three-component approach using HAp-encapsulated-γ-Fe2O3[γ-Fe2O3@HAp-SO3H]catalyzed condensation of 6-arnino-2-（methylthio or ethylthio）pyrimidin-4（3H）-one,Meldrum＇s acid and aryl aldehydes at 60 ℃ and under solvent-free conditions.In this protocol the use of nanocatalyst provided a green,useful and rapid method to generate the products in short reaction times and excellent yields（88%-94%）.
文摘Polyimides are well-known for their high chemical inertness and thermal stability. However, it is usually challenging to synthesize UV-curable polyimides since the imidization reaction requires such harsh conditions that acrylate type double bonds cannot withstand. In this work, synthetic methods are developed to obtain polyester-imide type binder polymers with high thermal stability, high compatibility with the other components of the black photoresist, and fine photolithographic patterning property for the negative-tone black photoresist. The syntheses of diimide-diacid or diimide-diol intermediates for the polyesterification with dianhydride gave polyester imides which meets this requirement. The photolithographic tests have shown that the patterning of the micron-sized PDL of the organic light emitting diode (OLED) panel could be obtained. This work will interest the researchers working on the design and optimization of thermally stable binder polymers.
基金financially supported by the innovation funding from Wei Qiao Group(Nos.H2872307 and H2872305)Fundamental Research Funds for the Central Universities and Graduate Student Innovation Fund of Donghua University(No.CUSF-DH-D-2024004)。
文摘Poly(ester amide)s(PEAs)attract much attention as a new kind of biodegradable polymers.However,the synthesis of PEAs with sequence-regulated chain structures is still complicated due to the multistep polymerization,high monomer purity,as well as the usage of organic solvents,which greatly inhibits its development and applications.Herein,a one-pot strategy without solvent was developed to synthesize the alternating PEA fromα,ω-amino alcohol and dicarboxylic acid by sequential polycondensation,where water was used as the controlling agent for amidation and esterification.Specifically,the amidation and esterification were controlled to proceed in turn by adding or removing water,realizing the one-pot preparation of alternating PEAs.The resultant PEA is characterized by^1H-and^(13)C-NMR,and its chain structure is confirmed to be highly quasi-alternating similar to alternating PEAs prepared by classical methods The evaluations from DSC and DMA demonstrate that the properties of quasi-alternating PEA(T_(m)=102℃,ΔH_(m)=30J·g^(-1))are far superior to those of random PEA(T_(m)=72℃,ΔH_(m)<1 J·g^(-1)).
基金Supported by the National Natural Science Foundation of China(No.21172189)
文摘A one-pot sequential reaction for efficient synthesis of pyrrolo[2,1-a]isoquinoline and pyrrolo[1,2-a]quinoline derivatives has been developed.The reaction included firstly the Cu-catalyzed three-component reaction of isoquinoline（quinoline）,acetylenedicarboxylate and alkynylbenzene and then Cs 2 CO 3-promoted intramolecular cyclization reaction of initially formed 1-alkenyl-2-alkynyl-1,2-dihydroisoquinoline（1,2-dihydroquinoline）.
文摘A simple and fastthree-component synthesis of new and biologically active hexahydro-2-quinolinecarboxylic acid scaf-fold 4 was carried out using cyclocondensation reaction of arylmethylidenepyruvic acids 1, 1,3-cyclohexandiones 2 and ammonium acetate 3 under solvent-free conditions and at room temperature. This protocol has the advantages of facility, easy work-up, high yields, short reaction time and environmentally friendly character.
文摘Polyimides are well known for their high chemical and thermal stability. However, a few polyimide samples have been reported which are completely soluble in such environmentally friendly and common organic solvent as propyleneglycol monomethyl ether acetate (PGMEA). In this work thermally stable, organosoluble and photocurable acidic polyimides were synthesized by simple and cost effective one-pot solution method. They polyimides obtained by this method showed much higher thermal stability (1 wt% loss temperature 345°C) than melt polymerized polyimides owing to the photocrosslinking reactions by the terminal double bonds.
基金supported by National Key R&D Program of China(grant no.2021YFA1501700)National Natural Science Foundation of China(NSFC+3 种基金grant nos.22301294,52025031,and 22261142664)the Chinese Academy of Sciences(CAS)Project for Young Scientists in Basic Research(grant no.YSBR-094)China Postdoctoral Science Foundation(grant nos.BX20230339 and 2023M743352)the University of Science and Technology of China(USTC)Research Funds of the Double First-Class Initiative(grant no.YD9990002030).
文摘The development of degradable polymers represents an appealing strategy to address ever-growing concerns for treating waste plastics.Olefin metathesis polymerization has been extensively explored for the synthesis of various degradable polymers.Cyclic–acyclic monomers metathesis polymerization(CAMMP)has recently been reported to produce degradable polymers via copolymerization of cyclic monomers with acyclic diene comonomers.Unfortunately,this strategy suffers from poor product material properties,especially at high contents of diene comonomers.To address this issue,we have designed a tandem olefin metathesis polymerization(TOMP)system that combines olefin ringclosing metathesis(RCM)of diene comonomers,followed by ring-opening metathesis copolymerization(ROMCP)with cyclic olefin monomers(dicyclopentadiene,cyclooctene,or alkyl-substituted cyclooctene).This strategy overcame the intrinsic limitations of diene-induced chain-transfer reactions during olefin metathesis,leading to degradable polymers with high molecular weights and excellent material properties.The selection of different cyclic olefin monomers provided access to degradable and recyclable cross-linked thermosets,linear thermoplastics,and elastomers.Notably,this one-pot,two-step process was highly efficient and required the addition of only one metathesis catalyst.
基金This work was supported by the National Natural Science Foundation of China(51673117,21805193 and 51973118)Postdoctoral Science Foundation of China(2019M650212)+2 种基金Key R&D Program of Guangdong Province(2019B010929002 and 2019B010941001)Science and Technology Innovation Commission of Shenzhen(JCYJ20170817094628397,JCYJ20170818093832350,JCYJ20170818112409808,JCYJ20170818100112531,JCYJ20180507184711069,and JCYJ20180305125319991)The authors also thank the Materials and Devices Testing Center of Tsinghua University Shenzhen Graduate School.
文摘Multicomponent metal sulfides have been recognized as promising anode materials for lithium/sodiumion storage given their enticing theoretical capacities. However, the simplification of synthetic processes and the construction of heterogeneous interfaces of multimetal sulfides remain great challenges. Herein,a hierarchical 1T-MoS2/carbon nanosheet decorated Co1–xS/N-doped carbon(Co1–xS/NC@MoS2/C) hollow nanofiber was designed and constructed via a one-pot hydrothermal method using a cobalt-based coordination polymer nanofiber. This nanofiber can transform in-situ into conductive N-doped carbon hollow fibers embedded with active Co1–xS nanoparticles, enabling the epitaxial growth of MoS2 nanosheets.Consequently, the Co1–xS/NC@MoS2/C composites achieve exceptional lithium/sodium-ion storage performance. Compared to MoS2/C microspheres and Co1–xS/NC hollow nanofibers alone, the Co1–xS/NC@MoS2/C hollow nanofibers deliver higher discharge capacities(1085.9 mAh g^-1 for lithium-ion batteries(LIBs) and 748.5 mAh g^-1 for sodium-ion batteries(SIBs) at 100 mA g^-1), better capacity retention(910 mAh g^-1 for LIBs and 636.5 mAh g^-1 for SIBs after 150 cycles at 100 mA g^-1), and increased cycling stability(407.2 mAh g^-1 after 1000 cycles for SIBs at 1000 m A g^-1). Furthermore, the kinetic analysis shows that the lithium/sodium-ion storage processes of the Co1–xS/NC@MoS2/C electrode are mainly controlled by pseudocapacitance behavior. The excellent electrochemical properties can thus be ascribed to the synergy of the MoS2/C nanosheets with the enlarged interlayer spacing, good conductivity of the carbon layers, and the Co1–xS nanoparticles embedded in the hollow nanofibers with extensive reaction sites.
基金the Natural Science Foundation of Xinjiang Science Technology Agency(No.2009211A02) for the support
文摘4-Arylmethylidene-4,5-dihydro-3-phenylisoxazol-5-ones were synthesized by the convenient three-component reaction of ethyl benzoylacetate,hydroxylamine and aromatic aldehydes in the presence of pyridine.The target compounds were also obtained by the reaction between 3-phenylisoxazol-5-one and aromatic aldehydes at 105℃under solvent free condition.Yields of products depended considerably on the aldehyde used.
文摘The one-pot three-component reaction of arylmethylidenepyruvic acids, 1,3-cyclohexandiones and ammonium acetate provides an economical and efficient synthetic route to 5-oxo-4-aryl-1,4,5,6,7,8-hexahydro-2-quinolinecarboxylic acid 4 under solvent-free conditions using a catalytic amount of TiO2 nanoparticles （TiO2 NPs） as an effective heterogeneous catalyst.
基金Financial support from the Research Council of University of Guilan is sincerely acknowledged
文摘An efficient ultrasound-assisted preparation of a series of novel 4-aryl-3-methyl-4,5-dihydro-l//-pyrazolo[34-b]pyridin-6（7H）ones via the reaction of 5-amino-3-methyl-1H-pyrazole,Meldrum＇s acid and various arylaldehydes using one-pot three-component approach is described.This rapid method produced the products in short reaction times（3-4 min） and excellent yields（87-95%）.
基金Foundation of the National Natural Science Foundation of China(No.22101212)“Climbing Program”(No.pdjh2021a0505)Special Funds+2 种基金Science Foundation for Young Teachers of Wuyi University(No.2019td06)Guangdong Basic and Applied Basic Research Foundation(Nos.2019A1515110866,2019A1515110522)College Students Innovation and Entrepreneurship Training Program of Wuyi University(Nos.202111349020,202111349308S)for financial support。
文摘In this study,a method was developed to form C(sp^(3))-C(sp^(2))bonds via copper catalyst-promoted cross coupling of 2-methylquinoline and in-situ-activated 3-haloisoquinoline under mild conditions.The multi-component tandem reaction was used to construct new C-N,C=O and C-C bonds in one pot via sequential functionalization of the N1,C3 and C1 positions of 3-haloisoquinoline.This method can be used to efficiently access 1,2-disubstituted isoquinolinones by the three-component reaction of 3-halogen isoquinoline,alkyl halide,and 2-methylquinoline.
文摘A new cerium polyoxomolybdate { [Ce （ H2 O） 7 Al （ OH ） 6 Mo6 O18 ] · 4H20 } （ compound 1 ） was synthesized and characterized by X-ray diffraction analysis, elemental analysis, TG analysis and IR spectrometry. Compound 1 exhibits a zigzag chain-like structure, which is constructed from an Anderson type anion and rare earth metal, Ce（ Ⅲ ）. These 1-D chains are further extended into a 3-D network by the aid of muhipoint hydrogen-bonding interactions.
文摘4-（Succinimido）-1-butane sulfonic acid as an efficient and reusable Bronsted acid catalyzed the synthesis of pyrano[4,3-b]pyran derivatives under solvent-free conditions.The catalyst can be prepared by mixing succinimide and 1,4-butanesultone that is more simple and safer than the preparation of succinimide sulfonic acid.This method has the advantages of high yield,clean reaction,simple methodology and short reaction time.The catalyst could be recycled without significant loss of activity.
基金Supporting information for this article is available on the WWW under http：//dx.doi.org/10.1002/cjoc. 201700367 or from the author.Acknowledgement This work was supported by the National Natural Science Foundation of China （Nos. 21622203, 21472147） and the Fund of the Shanxi Province （No. 2016JM2007）.
文摘A one-pot three-component reaction of aldehydes, nitroalkanes and NaN3 for the synthesis ofNH-1,2,3-triazoles has been developed. The reaction provides a safe, efficient and step-economic approach for the synthesis of various NH-1,2,3-triazoles in good to excellent yields.
基金Project supported by National Natural Science Foundation of China （Nos. 20331010, 20501003）.
文摘The one-pot hydrothermal reaction of CuCl2 with H2CPOA and 4,4＇-bpy results in two new coordination polymers, [Cu（CPOA）（4,4＇-bpy）（H2O）2]·1.5H2O （1） and [Cu2（HCPOA）4（4,4＇-bpy）4] （2） （H2CPOA=4-carboxyphenoxy acetic acid, 4,4＇-bpy=4,4＇-bipyridine） since CPOA^2- anions reach equilibrium with HCPOA^- anions in the reaction system. The crystal structure of 1 shows a triple interpenetration CdSO4-like net with 1D channel, in which lattice water molecules are located. Complex 2 is a ladder-like 1D double chain structure assembled through coordination bonds and O—H…N hydrogen bonds.
