Pyrrole is a heterocycle with four carbon atoms and a nitrogen atom,which is extensively used in the pesticide and pharmaceutical industries.In addition,it has a series of analogs such as pyrrolidine,pyrroline,and pyr...Pyrrole is a heterocycle with four carbon atoms and a nitrogen atom,which is extensively used in the pesticide and pharmaceutical industries.In addition,it has a series of analogs such as pyrrolidine,pyrroline,and pyrrolidone.Pesticides containing pyrrole and its analogs have been formally marketed as fungicides,including fenpiclonil,fludioxonil,the insecticide chlorfenapyr,and the herbicide fluorochloridone.In this paper,we analyze the structure-activity relationships(SARs)of pesticides containing these structures.We summarize the characteristics possessed by the most highly active pyrrole and its analogs and provide an overview of research on pyrrole compounds with insecticidal,antimicrobial,herbicidal,and antiviral properties in the past 20 years.It is hoped to provide ideas for the development and design of this type compounds in pesticides and to assist researchers in this area.展开更多
Pyrrolo[3,2-b]pyrrole is a good building block for radical photoini-tiators.In this study,free-radical photoinitiator 1,4-bis(4-bro-mophenyl)-2,5-bis(4-(trifluo-romethyl)phenyl)-1,4-dihydropy-rrolo[3,2-b]pyrrole(PyBF)...Pyrrolo[3,2-b]pyrrole is a good building block for radical photoini-tiators.In this study,free-radical photoinitiator 1,4-bis(4-bro-mophenyl)-2,5-bis(4-(trifluo-romethyl)phenyl)-1,4-dihydropy-rrolo[3,2-b]pyrrole(PyBF),con-taining a symmetric trifluo-romethyl(-CF3)end group,is syn-thesized via a one-step aldehyde-ketone condensation re-action for light-emitting diode(LED)photopolymerization.The-CF3 groups are incorporated into the 2,5-phenyl on the pyrrolo[3,2-b]pyrrole core.PyBF rapidly initiates the photopolymerization of acrylate pre-polymers and monomers under LED illumination at 365 and 405 nm.A possible photolysis mechanism is provided.In the presence of amines,PyBF increases the gel fraction rate of polyethylene glycol diacrylate(PEGDA)from 63.4%to 80.0%,indicating good potential as a two-component photoinitiator.PyBF exhibits a thermal decomposition temperature in an ex-cess of 300℃,comparable to that of a commercial photoinitiator(diphenyl(2,4,6-trimethyl-benzoyl)phosphine oxide,TPO),indicating its thermal stability.PyBF shows low migration in light-curing materials.Scanning electron microscopy images indicate that the materials of the PyBF/TPO/PEGDA mixture cured using the PyBF/TPO two-component photoinitia-tor system exhibit a smooth surface,in contrast to those cured with PyBF/PEGDA and TPO/PEGDA systems.The cured materials also display low curing shrinkage.Therefore,the pyrrolo[3,2-b]pyrrole radical photoinitiator exhibits high photoactivity in visible-light pho-topolymerization reactions.展开更多
Pyrroles are important structural units of natural products,drug molecules,biomolecules and functional material molecules.Efficient synthesis ofα-functionalized pyrroles with different substituents from easily access...Pyrroles are important structural units of natural products,drug molecules,biomolecules and functional material molecules.Efficient synthesis ofα-functionalized pyrroles with different substituents from easily accessible starting materials is still challenging.Herein,a facile and regioselective coarctate reaction of enynals involving a free carbene intermediate has been developed,which allows the divergent and practical de novo synthesis of variousα-furanyl pyrroles andα-cyclopropenyl pyrroles derivatives with good to excellent yields and high efficiency under mild conditions.This approach features readily accessible starting materials,high functional group compatibility,step economy and scalability,which would complement previous methods and support expansion of the toolbox for the synthesis of valuable,but previously inaccessible,highly substituted and electron-richα-functionalized pyrroles.展开更多
The possible configurations of pyrrole absorbed on a Si(100)surface have been investigated by x-ray photoelectron spectroscopy(XPS)and near-edge x-ray absorption fine structure(NEXAFS)spectra.The C-1s XPS and NEXAFS s...The possible configurations of pyrrole absorbed on a Si(100)surface have been investigated by x-ray photoelectron spectroscopy(XPS)and near-edge x-ray absorption fine structure(NEXAFS)spectra.The C-1s XPS and NEXAFS spectra of these adsorption configurations have been calculated by using the density functional theory(DFT)method and fullcore hole(FCH)approximation to investigate the relationship between the adsorption configurations and the spectra.The result shows that the XPS and NEXAFS spectra are structurally dependent on the configurations of pyrrole absorbed on the Si(100)surface.Compared with the XPS,the NEXAFS spectra are relatively sensitive to the adsorption configurations and can accurately identify them.The NEXAFS decomposition spectra produced by non-equivalent carbon atoms have also been calculated and show that the spectral features vary with the diverse types of carbon atoms and their structural environments.展开更多
Calix[4]pyrroles, as a class of new molecular receptor in the area of supramolecular chemistry, have displayed interesting anion and neutral substrate binding properties. In this paper, several new calix[4]pyrrole mac...Calix[4]pyrroles, as a class of new molecular receptor in the area of supramolecular chemistry, have displayed interesting anion and neutral substrate binding properties. In this paper, several new calix[4]pyrrole macrocycles were synthesised and characterized.展开更多
The polymerization thermokinetics of pyrrole in the presence of iron trichloride art studied by using a Calvet microcalorimoter. The apparent activation energy, the pre-exponential constant and reaction order of this ...The polymerization thermokinetics of pyrrole in the presence of iron trichloride art studied by using a Calvet microcalorimoter. The apparent activation energy, the pre-exponential constant and reaction order of this reaction in the temperature range of 25.2—37℃ are 34.5 KJ·mol^(-1), 10^(2.74)S^(-1) and 1 respectively. The activation free-energies of this reaction at 25.2°, 30°and 37℃ are 91.8, 92.9 and 94.2 KJ·mol^(-1) respectively.展开更多
Michael addition of indole and pyrrole to a variety of α, β-unsaturated ketones was efficiently promoted by a catalytic amount of GaCl3 in aqueous media to afford the corresponding products in good to excellent yields.
With home-made multi-walled carbon nanotubes （MWCNTs, simplified as CNTs in later text） as support, CNT-supported Co-Mo-S catalysts, denoted as x%（mass percentage）MoiCoj/CNTs, were prepared. Their catalytic perfor...With home-made multi-walled carbon nanotubes （MWCNTs, simplified as CNTs in later text） as support, CNT-supported Co-Mo-S catalysts, denoted as x%（mass percentage）MoiCoj/CNTs, were prepared. Their catalytic performance for thiophene hydrodesulfurization （HDS） and pyrrole hydrodenitrification （HDN） reactions was studied, and compared with the reference system sup- ported by AC. Over the 7.24%Mo3Co1/CNTs catalyst at reaction condition of 1.5 MPa, 613 K, C4H4S/H2=3.7/96.3（molar ratio） and GHSV≈8000 mlswP/（g-cat.h）, the specific HDS activity of thiophene reached 3.29 mmolc4H4S/（s.molMo）, which was 1.32 times as high as that （2.49 mmolc4H4S/（s.molMo）） of the AC-based counterpart, and was 2.47 times as high as that （1.33 mmolc4H4S/（s-molMo）） of the catalysts supported by AC with the respective optimal MoaCol-loading amount, 16.90%Mo3Co1/AC. Analogous reaction-chemical behaviours were also observed in the case of pyrrole HDN. It was experimentally found that using the CNTs in place of AC as support of the catalyst caused little change in the apparent activation energy for the thiophene HDS or pyrrole HDN reaction, but led to a significant increase in the concentration of catalytically active Mo-species （Mo^4＋） at the surface of the functioning catalyst. On the other hand, H2-TPD measurements revealed that the CNT-supported catalyst could reversibly adsorb a greater amount of hydrogen under atmospheric pressure at temperatures ranging from room temperature to about 673 K. This unique feature would help to generate microenvironments with higher stationarystate concentration of active hydrogen-adspecies at the surface of the functioning catalyst. Both factors mentioned above were favorable to increasing the rate of thiophene HDS and pyrrole HDN reactions.展开更多
A convenient and effective Paal-Knorr condensations of 2,5-hexanedione with most amines have been carried out at room temperature under solvent-free condition.Macroporous strongly acidic styrol resin(D001) as a novel,...A convenient and effective Paal-Knorr condensations of 2,5-hexanedione with most amines have been carried out at room temperature under solvent-free condition.Macroporous strongly acidic styrol resin(D001) as a novel,efficient,cost-effective,and reusable solid acid catalyst for the synthesis of pyrroles under the same conditions.The pyrroles were obtained in high yields in short reaction times.展开更多
The electrochemical performance of lithium-sulfur(Li-S)batteries is strongly hampered by the shuttle effect and slow redox kinetics of lithium polysulfides(Li PSs).Surface modified interlayer of a separator of Li-S ba...The electrochemical performance of lithium-sulfur(Li-S)batteries is strongly hampered by the shuttle effect and slow redox kinetics of lithium polysulfides(Li PSs).Surface modified interlayer of a separator of Li-S batteries is demonstrated to be an effective strategy to overcome this problem.Herein,cobalt nanoparticles confined in nitrogen co-doped porous carbon framework(Co-CN)were developed from pyrolysis of ZIF-67 and used as interlayer of PP separator for Li-S batteries,and were functionalized by four pyrrole derivatives,1-phenylpyrrole,1-methyl pyrrole,1-(p-toluenesulfonyl)pyrrole,and 1-pyrrole,respectively,which were screened in terms of the electron-withdrawing/donating ability of the substituent groups on the pyrrolic nitrogen.The impact of the molecular structure of pyrrole derivatives on the interaction with Li PSs and the electrochemical performance of Li-S batteries were explored by nuclear magnetic resonance and theoretical calculation.It is uncovered that 1-phenylpyrrole shows the highest enhancement of redox kinetics of Li PSs,attributing to the optimal interaction with Co nanoparticles and Li PSs.Therefore,1-phenylpyrrole modified Co-CN interlayer enables the best electrochemical performance for the Li-S batteries,delivering a specific capacity of 562 m Ah g^(-1)at 5 C and a capacity of 538,526,and 449 m Ah g^(-1)after 500 cycles at 1,2,and 3 C,respectively.At a high sulfur loading of 5.5 mg cm^(-2),it achieves a capacity of 440 m Ah g^(-1)after 500 cycles at 1 C.This work reveals the interaction mechanism among Li PSs,Co nanoparticles and the molecular modifiers in improving the electrochemical performance of Li-S batteries.展开更多
A phytochemical investigation of the EtOH extract of the flowers of Lagerstroemia indica L.led to the isolation and char-acterization of a new pyrrole alkaloid,named lagerindicine(1),along with four known compounds(2-...A phytochemical investigation of the EtOH extract of the flowers of Lagerstroemia indica L.led to the isolation and char-acterization of a new pyrrole alkaloid,named lagerindicine(1),along with four known compounds(2-5).Their structures were elucidated by the detailed spectroscopic analysis and comparison with literature data,whereas the structure,in par-ticularly,the absolute configuration(AC)of 1,was firmly determined by total synthesis.All the isolates were evaluated for their cytotoxic effects against human colon cancer cell(HCT-116),and compound 3 exhibited weak cytotoxicity with IC50 value of 28.4μM.展开更多
Polysubstituted pyrroles are very important scaffolds in many bioactive natural products and synthetic pharmaceuticals.Here,a new gold-catalyzed cycloaddition of alkynes with azadienes to access tetrasubstituted pyrro...Polysubstituted pyrroles are very important scaffolds in many bioactive natural products and synthetic pharmaceuticals.Here,a new gold-catalyzed cycloaddition of alkynes with azadienes to access tetrasubstituted pyrroles is demonstrated.The neighboring hydroxylmethyl group serves a very important directing group through an addition/cycloaddition/elimination cascade.Diverse polysubstituted pyrroles were synthesized in good yields under mild conditions in one step,and tricyclic pyrrole containing heterocycles were easily obtained through derivatization.展开更多
A palladium-catalyzed formal[2+2+1]cyclization of 1-alkynyl-8-iodonaphthalene with double isocyanides is developed herein.The transformation worked well to produce a series of 7 H-acenaphtho[1,2-b]pyrrole with a broad...A palladium-catalyzed formal[2+2+1]cyclization of 1-alkynyl-8-iodonaphthalene with double isocyanides is developed herein.The transformation worked well to produce a series of 7 H-acenaphtho[1,2-b]pyrrole with a broad reaction scope.Isocyanides play a dual role in the reaction.One is a C1 building block,and another is used as C1 N1 component.In the process,the[2+2+1]cyclization involves imidoylation,regioselective addition of imidoylpalladium species into alkyne,double imidoylation,and another addition of the resulting imidoylpalladium species into imine bonds.展开更多
An efficient 1-methylimidazole-catalyzed synthesis of dialkyl 2-[（4-methylphenyl）sulfonyl]-1H-pyrrole-3,4-dicarboxylates is described.The reactive 1：1 zwitterionic intermediate formed by the addition of 1-methylimi...An efficient 1-methylimidazole-catalyzed synthesis of dialkyl 2-[（4-methylphenyl）sulfonyl]-1H-pyrrole-3,4-dicarboxylates is described.The reactive 1：1 zwitterionic intermediate formed by the addition of 1-methylimidazole to dialkyl acetylenedicarboxylates is trapped by tosylmethyl isocyanide（TOSMIC） to afford the title compounds in excellent yields.展开更多
An undescribed pyrrole acid,1-(4′-methoxy-4′-oxobutyl)-1 H-pyrrole-2,5-dicarboxylic acid(1)and one known pyr-role acid(2)were isolated from the fruits of Phyllanthus emblica.The structures of these compounds were el...An undescribed pyrrole acid,1-(4′-methoxy-4′-oxobutyl)-1 H-pyrrole-2,5-dicarboxylic acid(1)and one known pyr-role acid(2)were isolated from the fruits of Phyllanthus emblica.The structures of these compounds were elucidated via the comprehensive analyses of IR,HRESIMS,1D and 2D spectroscopic data.A series of biological assays revealed that compounds 1 and 2 could inhibit LPS-induced over-production of nitric oxide(NO),interleukin-6(IL-6),monocyte chemotactic protein 1(MCP-1)and tumor necrosis factor-α(TNF-α)by reducing the phosphorylation of extracellular regulated protein kinases(ERK)and c-Jun N-terminal kinases(JNK)in RAW 264.7 cells.Additionally,compounds 1 and 2 were found to reduce lipid deposition and increase the mRNA expression of ATP-binding cassette transporter A1 in oxidized low-density lipoprotein-treated RAW264.7 macrophages.展开更多
Three new pyrrole alkaloids albifipyrrols A-C(1-3),were isolated from the endophytic fungus Albifimbria viridis col-lected from the Chinese medicinal plant.Their structures were elucidated by extensive NMR and HRESIMS...Three new pyrrole alkaloids albifipyrrols A-C(1-3),were isolated from the endophytic fungus Albifimbria viridis col-lected from the Chinese medicinal plant.Their structures were elucidated by extensive NMR and HRESIMS spectro-metric analyses.All compounds were evaluated for immunosuppressive activity.Fortunately,compound 2 exhibits certain inhibition specifically against the LPS-induced proliferation of B lymphocyte cells with IC50 value 16.16μM.展开更多
Supramolecular interaction of calix[4]pyrroles with several inorganic anions is reported by addition of calix[4]pyrroles to background electrolyte (BGE) in CZE. The retention time (t(R)) of all anions increased with i...Supramolecular interaction of calix[4]pyrroles with several inorganic anions is reported by addition of calix[4]pyrroles to background electrolyte (BGE) in CZE. The retention time (t(R)) of all anions increased with increasing concentration of calix[4]pyrroles. The effect on F- is most evident.展开更多
A simple and quick method for the synthesis of water dispersible stable silver nanoparticles has been developed. Calix[4]pyrrole octahydrazide （CPOH）, has been successfully used as a reducing as well as stabilizing ...A simple and quick method for the synthesis of water dispersible stable silver nanoparticles has been developed. Calix[4]pyrrole octahydrazide （CPOH）, has been successfully used as a reducing as well as stabilizing agent for the synthesis of silver nanoparticles. CPOH-AgNps have been duly characterized by SPR, PSA, TEM and EDX-ray. The ability of CPOH-AgNps as selective and sensitive sensor for various ions （Pb（Ⅱ）, Cd（II）, Mn（Ⅱ）, Fe（Ⅲ）, Ni（Ⅱ）, Zn（Ⅱ）, Hg（Ⅱ）, Co（Ⅱ）, Cu（Ⅱ）） by colorimetry and spectrofluorimetry has been explored. CPOH-AgNps were found to be selective only for Hg（Ⅱ） ions. Nanomolar concentration of Hg（Ⅱ） ions can also be determined by spectrofluorimetry by increase in fluorescence intensity. Linear range of detection of Hg（Ⅱ） ions in water was found to be from 1nmol/L to mol/L. The method has been successfully applied for determination of Hg（Ⅱ） ions in ground water and industrial effluent waste water samples.展开更多
One simple and versatile method is established far the synthesis of DNA recognition molecules-polyamides containing alternating N-methylpyrrole and N-methylimidazole without necessitating NH2- group protection.
An efficient and facile method for the synthesis of N-substituted pyrroles in moderate to good yields by the Paal-Knorr reaction of β-diketones with amines in the presence of β-cyclodextrin in aqueous media has been...An efficient and facile method for the synthesis of N-substituted pyrroles in moderate to good yields by the Paal-Knorr reaction of β-diketones with amines in the presence of β-cyclodextrin in aqueous media has been developed. Moreover, this process tolerated diamines （e.g., para-, metaor orthophenylenediamine） to construct bis-pyrrole or mono-pyrrole derivates.β-Cyclodextrin can be recovered easily after the reactions and reused without evident loss in activity.展开更多
基金financial support from the National Natural Science Foundation of China(No.32072445)the Science and Technology Plan Project of Guizhou Province(Qiankehezhicheng[2024]the general 083)+5 种基金the Program of Introducing Talents to Chinese Universities(No.D20023)the Central Government Guides Local Science and Technology Development Fund Projects(Qiankehezhongyindi(2023)001)Key Agricultural Technology R&D Projects of the Xinjiang Production and Construction Corps(NYHXGG,2023AA602)the Frontiers Science Centre for Asymmetric Synthesis and Medicinal Molecules,Department of Education,Guizhou Province[Qianjiaohe KY(2020)004]the specific research fund of The Innovation Platform for Academicians of Hainan Province(No.SQ2020PTZ0009)。
文摘Pyrrole is a heterocycle with four carbon atoms and a nitrogen atom,which is extensively used in the pesticide and pharmaceutical industries.In addition,it has a series of analogs such as pyrrolidine,pyrroline,and pyrrolidone.Pesticides containing pyrrole and its analogs have been formally marketed as fungicides,including fenpiclonil,fludioxonil,the insecticide chlorfenapyr,and the herbicide fluorochloridone.In this paper,we analyze the structure-activity relationships(SARs)of pesticides containing these structures.We summarize the characteristics possessed by the most highly active pyrrole and its analogs and provide an overview of research on pyrrole compounds with insecticidal,antimicrobial,herbicidal,and antiviral properties in the past 20 years.It is hoped to provide ideas for the development and design of this type compounds in pesticides and to assist researchers in this area.
基金the financial support of the Tianjin Technical Expert Project(22YDTPJC00620)。
文摘Pyrrolo[3,2-b]pyrrole is a good building block for radical photoini-tiators.In this study,free-radical photoinitiator 1,4-bis(4-bro-mophenyl)-2,5-bis(4-(trifluo-romethyl)phenyl)-1,4-dihydropy-rrolo[3,2-b]pyrrole(PyBF),con-taining a symmetric trifluo-romethyl(-CF3)end group,is syn-thesized via a one-step aldehyde-ketone condensation re-action for light-emitting diode(LED)photopolymerization.The-CF3 groups are incorporated into the 2,5-phenyl on the pyrrolo[3,2-b]pyrrole core.PyBF rapidly initiates the photopolymerization of acrylate pre-polymers and monomers under LED illumination at 365 and 405 nm.A possible photolysis mechanism is provided.In the presence of amines,PyBF increases the gel fraction rate of polyethylene glycol diacrylate(PEGDA)from 63.4%to 80.0%,indicating good potential as a two-component photoinitiator.PyBF exhibits a thermal decomposition temperature in an ex-cess of 300℃,comparable to that of a commercial photoinitiator(diphenyl(2,4,6-trimethyl-benzoyl)phosphine oxide,TPO),indicating its thermal stability.PyBF shows low migration in light-curing materials.Scanning electron microscopy images indicate that the materials of the PyBF/TPO/PEGDA mixture cured using the PyBF/TPO two-component photoinitia-tor system exhibit a smooth surface,in contrast to those cured with PyBF/PEGDA and TPO/PEGDA systems.The cured materials also display low curing shrinkage.Therefore,the pyrrolo[3,2-b]pyrrole radical photoinitiator exhibits high photoactivity in visible-light pho-topolymerization reactions.
基金the National Natural Science Foundation of China(Nos.22071062 and 22271096)the Fundamental Research Funds for the Central Universities,SCUT(No.2022ZYGXZR107)funded by the National Postdoctoral Research Program(No.GZC20230839)。
文摘Pyrroles are important structural units of natural products,drug molecules,biomolecules and functional material molecules.Efficient synthesis ofα-functionalized pyrroles with different substituents from easily accessible starting materials is still challenging.Herein,a facile and regioselective coarctate reaction of enynals involving a free carbene intermediate has been developed,which allows the divergent and practical de novo synthesis of variousα-furanyl pyrroles andα-cyclopropenyl pyrroles derivatives with good to excellent yields and high efficiency under mild conditions.This approach features readily accessible starting materials,high functional group compatibility,step economy and scalability,which would complement previous methods and support expansion of the toolbox for the synthesis of valuable,but previously inaccessible,highly substituted and electron-richα-functionalized pyrroles.
基金Project supported by the Shandong Provincial Natural Science Foundation,China(Grant Nos.ZR2022MA025 and ZR2020MA077).
文摘The possible configurations of pyrrole absorbed on a Si(100)surface have been investigated by x-ray photoelectron spectroscopy(XPS)and near-edge x-ray absorption fine structure(NEXAFS)spectra.The C-1s XPS and NEXAFS spectra of these adsorption configurations have been calculated by using the density functional theory(DFT)method and fullcore hole(FCH)approximation to investigate the relationship between the adsorption configurations and the spectra.The result shows that the XPS and NEXAFS spectra are structurally dependent on the configurations of pyrrole absorbed on the Si(100)surface.Compared with the XPS,the NEXAFS spectra are relatively sensitive to the adsorption configurations and can accurately identify them.The NEXAFS decomposition spectra produced by non-equivalent carbon atoms have also been calculated and show that the spectral features vary with the diverse types of carbon atoms and their structural environments.
文摘Calix[4]pyrroles, as a class of new molecular receptor in the area of supramolecular chemistry, have displayed interesting anion and neutral substrate binding properties. In this paper, several new calix[4]pyrrole macrocycles were synthesised and characterized.
文摘The polymerization thermokinetics of pyrrole in the presence of iron trichloride art studied by using a Calvet microcalorimoter. The apparent activation energy, the pre-exponential constant and reaction order of this reaction in the temperature range of 25.2—37℃ are 34.5 KJ·mol^(-1), 10^(2.74)S^(-1) and 1 respectively. The activation free-energies of this reaction at 25.2°, 30°and 37℃ are 91.8, 92.9 and 94.2 KJ·mol^(-1) respectively.
基金support by the Natural Science Foundation of Zhejiang Province(No.Y4051137,Y405015 and Y4080177)
文摘Michael addition of indole and pyrrole to a variety of α, β-unsaturated ketones was efficiently promoted by a catalytic amount of GaCl3 in aqueous media to afford the corresponding products in good to excellent yields.
基金Supported by National Natural Science Foundation of China (No. 20473063 and No. 20590364).
文摘With home-made multi-walled carbon nanotubes （MWCNTs, simplified as CNTs in later text） as support, CNT-supported Co-Mo-S catalysts, denoted as x%（mass percentage）MoiCoj/CNTs, were prepared. Their catalytic performance for thiophene hydrodesulfurization （HDS） and pyrrole hydrodenitrification （HDN） reactions was studied, and compared with the reference system sup- ported by AC. Over the 7.24%Mo3Co1/CNTs catalyst at reaction condition of 1.5 MPa, 613 K, C4H4S/H2=3.7/96.3（molar ratio） and GHSV≈8000 mlswP/（g-cat.h）, the specific HDS activity of thiophene reached 3.29 mmolc4H4S/（s.molMo）, which was 1.32 times as high as that （2.49 mmolc4H4S/（s.molMo）） of the AC-based counterpart, and was 2.47 times as high as that （1.33 mmolc4H4S/（s-molMo）） of the catalysts supported by AC with the respective optimal MoaCol-loading amount, 16.90%Mo3Co1/AC. Analogous reaction-chemical behaviours were also observed in the case of pyrrole HDN. It was experimentally found that using the CNTs in place of AC as support of the catalyst caused little change in the apparent activation energy for the thiophene HDS or pyrrole HDN reaction, but led to a significant increase in the concentration of catalytically active Mo-species （Mo^4＋） at the surface of the functioning catalyst. On the other hand, H2-TPD measurements revealed that the CNT-supported catalyst could reversibly adsorb a greater amount of hydrogen under atmospheric pressure at temperatures ranging from room temperature to about 673 K. This unique feature would help to generate microenvironments with higher stationarystate concentration of active hydrogen-adspecies at the surface of the functioning catalyst. Both factors mentioned above were favorable to increasing the rate of thiophene HDS and pyrrole HDN reactions.
文摘A convenient and effective Paal-Knorr condensations of 2,5-hexanedione with most amines have been carried out at room temperature under solvent-free condition.Macroporous strongly acidic styrol resin(D001) as a novel,efficient,cost-effective,and reusable solid acid catalyst for the synthesis of pyrroles under the same conditions.The pyrroles were obtained in high yields in short reaction times.
基金supported by the National Key Research and Development Program of China(Grant No.2017YFA0206703)the National Natural Science Foundation of China(Grant No.U2032151)。
文摘The electrochemical performance of lithium-sulfur(Li-S)batteries is strongly hampered by the shuttle effect and slow redox kinetics of lithium polysulfides(Li PSs).Surface modified interlayer of a separator of Li-S batteries is demonstrated to be an effective strategy to overcome this problem.Herein,cobalt nanoparticles confined in nitrogen co-doped porous carbon framework(Co-CN)were developed from pyrolysis of ZIF-67 and used as interlayer of PP separator for Li-S batteries,and were functionalized by four pyrrole derivatives,1-phenylpyrrole,1-methyl pyrrole,1-(p-toluenesulfonyl)pyrrole,and 1-pyrrole,respectively,which were screened in terms of the electron-withdrawing/donating ability of the substituent groups on the pyrrolic nitrogen.The impact of the molecular structure of pyrrole derivatives on the interaction with Li PSs and the electrochemical performance of Li-S batteries were explored by nuclear magnetic resonance and theoretical calculation.It is uncovered that 1-phenylpyrrole shows the highest enhancement of redox kinetics of Li PSs,attributing to the optimal interaction with Co nanoparticles and Li PSs.Therefore,1-phenylpyrrole modified Co-CN interlayer enables the best electrochemical performance for the Li-S batteries,delivering a specific capacity of 562 m Ah g^(-1)at 5 C and a capacity of 538,526,and 449 m Ah g^(-1)after 500 cycles at 1,2,and 3 C,respectively.At a high sulfur loading of 5.5 mg cm^(-2),it achieves a capacity of 440 m Ah g^(-1)after 500 cycles at 1 C.This work reveals the interaction mechanism among Li PSs,Co nanoparticles and the molecular modifiers in improving the electrochemical performance of Li-S batteries.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.81991521,41676073)the National Key Research and Development Program of China(No.2018YFC0310903)+2 种基金the Drug Innovation Major Project(No.2018ZX09711-001-001-009)the SKLDR/SIMM Project(No.SIMM1903ZZ-04)Changsha Engineering Technology Research Center of Woody flower(kq1907081).
文摘A phytochemical investigation of the EtOH extract of the flowers of Lagerstroemia indica L.led to the isolation and char-acterization of a new pyrrole alkaloid,named lagerindicine(1),along with four known compounds(2-5).Their structures were elucidated by the detailed spectroscopic analysis and comparison with literature data,whereas the structure,in par-ticularly,the absolute configuration(AC)of 1,was firmly determined by total synthesis.All the isolates were evaluated for their cytotoxic effects against human colon cancer cell(HCT-116),and compound 3 exhibited weak cytotoxicity with IC50 value of 28.4μM.
基金the financial support from the Natural Science Foundation of China and Shandong Province(Nos.21971149,92156007,ZR2019ZD45,ZR2020KB005)the Fundamental Research Funds of Shandong University。
文摘Polysubstituted pyrroles are very important scaffolds in many bioactive natural products and synthetic pharmaceuticals.Here,a new gold-catalyzed cycloaddition of alkynes with azadienes to access tetrasubstituted pyrroles is demonstrated.The neighboring hydroxylmethyl group serves a very important directing group through an addition/cycloaddition/elimination cascade.Diverse polysubstituted pyrroles were synthesized in good yields under mild conditions in one step,and tricyclic pyrrole containing heterocycles were easily obtained through derivatization.
基金Financial supports from the Natural Science Foundation of Zhejiang Province(No.LY22B020010)the National Natural Science Foundation of China(Nos.21772067,21801096 and 22161043)The Youth Jinggang Scholars Program in Jiangxi Province。
文摘A palladium-catalyzed formal[2+2+1]cyclization of 1-alkynyl-8-iodonaphthalene with double isocyanides is developed herein.The transformation worked well to produce a series of 7 H-acenaphtho[1,2-b]pyrrole with a broad reaction scope.Isocyanides play a dual role in the reaction.One is a C1 building block,and another is used as C1 N1 component.In the process,the[2+2+1]cyclization involves imidoylation,regioselective addition of imidoylpalladium species into alkyne,double imidoylation,and another addition of the resulting imidoylpalladium species into imine bonds.
基金supported by the Research Council of the University of Tehran as research project(No6102036/ 1/03)
文摘An efficient 1-methylimidazole-catalyzed synthesis of dialkyl 2-[（4-methylphenyl）sulfonyl]-1H-pyrrole-3,4-dicarboxylates is described.The reactive 1：1 zwitterionic intermediate formed by the addition of 1-methylimidazole to dialkyl acetylenedicarboxylates is trapped by tosylmethyl isocyanide（TOSMIC） to afford the title compounds in excellent yields.
基金Scientific and technological innovation project of China Academy of Chinese Medical Sciences(CI2021A04409,CI2021A04404,CI2021A04405)the fundamental research funds for the central public welfare research institutes(No.ZZ13-YQ-061,ZXKT22012,ZXKT22039).
文摘An undescribed pyrrole acid,1-(4′-methoxy-4′-oxobutyl)-1 H-pyrrole-2,5-dicarboxylic acid(1)and one known pyr-role acid(2)were isolated from the fruits of Phyllanthus emblica.The structures of these compounds were elucidated via the comprehensive analyses of IR,HRESIMS,1D and 2D spectroscopic data.A series of biological assays revealed that compounds 1 and 2 could inhibit LPS-induced over-production of nitric oxide(NO),interleukin-6(IL-6),monocyte chemotactic protein 1(MCP-1)and tumor necrosis factor-α(TNF-α)by reducing the phosphorylation of extracellular regulated protein kinases(ERK)and c-Jun N-terminal kinases(JNK)in RAW 264.7 cells.Additionally,compounds 1 and 2 were found to reduce lipid deposition and increase the mRNA expression of ATP-binding cassette transporter A1 in oxidized low-density lipoprotein-treated RAW264.7 macrophages.
基金National Natural Science Foundation of China (31870513)Zheng-Hui Li,National Aerospace Science Foundation of China (32000011),Hong-Lian Ai.
文摘Three new pyrrole alkaloids albifipyrrols A-C(1-3),were isolated from the endophytic fungus Albifimbria viridis col-lected from the Chinese medicinal plant.Their structures were elucidated by extensive NMR and HRESIMS spectro-metric analyses.All compounds were evaluated for immunosuppressive activity.Fortunately,compound 2 exhibits certain inhibition specifically against the LPS-induced proliferation of B lymphocyte cells with IC50 value 16.16μM.
基金the Nature Science Foundation of Gansu Provice (NO. A52).
文摘Supramolecular interaction of calix[4]pyrroles with several inorganic anions is reported by addition of calix[4]pyrroles to background electrolyte (BGE) in CZE. The retention time (t(R)) of all anions increased with increasing concentration of calix[4]pyrroles. The effect on F- is most evident.
基金financial assistance provided by University Grants Commission (New Delhi. India), GUJCOST (Gandhinagar, India)
文摘A simple and quick method for the synthesis of water dispersible stable silver nanoparticles has been developed. Calix[4]pyrrole octahydrazide （CPOH）, has been successfully used as a reducing as well as stabilizing agent for the synthesis of silver nanoparticles. CPOH-AgNps have been duly characterized by SPR, PSA, TEM and EDX-ray. The ability of CPOH-AgNps as selective and sensitive sensor for various ions （Pb（Ⅱ）, Cd（II）, Mn（Ⅱ）, Fe（Ⅲ）, Ni（Ⅱ）, Zn（Ⅱ）, Hg（Ⅱ）, Co（Ⅱ）, Cu（Ⅱ）） by colorimetry and spectrofluorimetry has been explored. CPOH-AgNps were found to be selective only for Hg（Ⅱ） ions. Nanomolar concentration of Hg（Ⅱ） ions can also be determined by spectrofluorimetry by increase in fluorescence intensity. Linear range of detection of Hg（Ⅱ） ions in water was found to be from 1nmol/L to mol/L. The method has been successfully applied for determination of Hg（Ⅱ） ions in ground water and industrial effluent waste water samples.
基金Professor Pang Zhang for his encouragementthe National Natural Science Foundation of China !298
文摘One simple and versatile method is established far the synthesis of DNA recognition molecules-polyamides containing alternating N-methylpyrrole and N-methylimidazole without necessitating NH2- group protection.
基金the National Natural Science Foundation of China(No.21172175)Natural Science Foundation of Zhejiang Province(Nos.LY12B02011 and Y4110491)for financial support
文摘An efficient and facile method for the synthesis of N-substituted pyrroles in moderate to good yields by the Paal-Knorr reaction of β-diketones with amines in the presence of β-cyclodextrin in aqueous media has been developed. Moreover, this process tolerated diamines （e.g., para-, metaor orthophenylenediamine） to construct bis-pyrrole or mono-pyrrole derivates.β-Cyclodextrin can be recovered easily after the reactions and reused without evident loss in activity.
