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
Synthesizing nitrogen(N)-containing molecules from biomass derivatives is a new strategy for production of this kind of chemicals.Herein,for the first time we present the synthesis of N-substituted aryl pyrroles via r...Synthesizing nitrogen(N)-containing molecules from biomass derivatives is a new strategy for production of this kind of chemicals.Herein,for the first time we present the synthesis of N-substituted aryl pyrroles via reductive amination/cyclization of levulinic acid(LA)with primary aromatic amines and hydrosilanes(e.g.,PMHS)over Cs F,and a series of N-substituted aryl pyrroles could be obtained in good to excellent yields at 120○C.The mechanism investigation indicates that the reaction proceeds in two steps:the cyclization between amine and LA occurs first to form intermediate 5-methyl-N-alkyl-1,3-dihydro-2H-pyrrolones and their isomeride(B),and then the chemo-and region-selective reduction of intermediates take place to produce the final products.This approach for synthesis of N-substituted aryl pyrroles can be performed under mild and green conditions,which may have promising applications.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
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
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
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.
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
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
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.
We herein disclose a series of novel pyrrole derivatives as well as fused pyrrolopyridines 6a,b and 7a,b, pyrrolopyrazoles 8a, b, pyrrolo[2,3-d]pyrimidine derivatives 10a-d, 12a,b, 14a,b, 18a,b, 20a,b, 21a,b, 22a,b, 2...We herein disclose a series of novel pyrrole derivatives as well as fused pyrrolopyridines 6a,b and 7a,b, pyrrolopyrazoles 8a, b, pyrrolo[2,3-d]pyrimidine derivatives 10a-d, 12a,b, 14a,b, 18a,b, 20a,b, 21a,b, 22a,b, 23a,b, 24a,b, 31a,b, 36a,b, 40a,b, pyrrolo[1,2,6]thiadiazine derivatives 19a,b, pyrrolotriazolopyrimidines 25a,b, 26a,b, 27a,b and 28a,b, pyrrolo[2,3-d][1,2,3]triazine derivatives 32a,b and pyrrolo[2,3-d][1,3]oxazine derivatives 39a,b as novel compounds. All compounds were evaluated for their anti-inflammatory, analgesic (compared to the reference drug Indomethacin) and antimicrobial activities (compared to the reference drug Ampicillin and Fluconazole). Compounds 4d, 5b-d, 6a,b, 9c,d, 10d, 12ab, 13b, 19a,b, 21b, 23b, 31a,b, 38b and 40a were found to be the most active anti-inflammatory drugs exhibiting potency ranging from 1 - 1.01 compared to the reference drug indomethacin. In addition to docking study of these highly active twenty compounds against the active site of cyclooxygenase-2 enzyme (COX-2), among the tested compounds, compounds 5d, 9d, 11b, 12a, 13b and 32a showed multiple activities;anti-inflammatory, analgesic and anti-bacterial activities.展开更多
The synthesis of C-substituted and N-substituted pyrrole is described by the reaction of phenacyl bromides, pentane-2, 4-dione and amine in aqueous medium using DABCO as a catalyst. The method is very convenient and a...The synthesis of C-substituted and N-substituted pyrrole is described by the reaction of phenacyl bromides, pentane-2, 4-dione and amine in aqueous medium using DABCO as a catalyst. The method is very convenient and applicable for alkyl as well as aryl amines and phenacyl bromides. The procedure is amenable for the synthesis of new substituted pyrroles. Moreover, aqueous medium makes the method more eco-friendly.展开更多
Four organic smallmolecule hole transport materials(D41, D42,D43 and D44) of tetraarylpyrrolo[3,2-b]pyrroles were prepared. They can be used without doping in the manufacture of the inverted planar perovskite solar ce...Four organic smallmolecule hole transport materials(D41, D42,D43 and D44) of tetraarylpyrrolo[3,2-b]pyrroles were prepared. They can be used without doping in the manufacture of the inverted planar perovskite solar cells. Tetraarylpyrrolo[3,2-b]pyrroles are accessible for one-pot synthesis.D42, D43 and D44 possess acceptor-π-donor-π-acceptor structure, on which the aryl bearing substitutes of cyan, fluorine and trifluoromethyl, respectively. Instead, the aryl moiety of D41 is in presence of methyl with a donor-π-donor-π-donor structure. The different substitutes significantly affected their molecular surface charge distribution and thin-film morphology, attributing to the electron-rich properties of fused pyrrole ring. The size of perovskite crystalline growth particles is affected by different molecular structures,and the electron-withdrawing cyan group of D42 is most conducive to the formation of large perovskite grains. The D42 fabricated devices with power conversion efficiency of17.3% and retained 55% of the initial photoelectric conversion efficiency after 22 days in dark condition. The pyrrolo[3,2-b]pyrrole is efficient electron-donating moiety for hole transporting materials to form good substrate in producing perovskite thin film.展开更多
Octadecylsilanized silica (ODS) was coated with meso-octamethylcalix[4]pyrrole to obtain a novel calix[4]pyrrole containing stationary phase for HPLC. Compared to ODS, the new stationary phase showed a relatively larg...Octadecylsilanized silica (ODS) was coated with meso-octamethylcalix[4]pyrrole to obtain a novel calix[4]pyrrole containing stationary phase for HPLC. Compared to ODS, the new stationary phase showed a relatively large retention and an improved separation for phenolic compounds and organic anions, using pure water as mobile phase. The results can be ascribed to the interaction between analytes and calix[4]pyrrole.展开更多
Resorcarens 1a-b (R'=Ph, p-MeOC6H4) were fully alkylated with alkyl iodides or bromides in TEBA/KOH/DMF solid-liquid PTC process with 63-82% yields, whereas the three calix[4]pyrroles 3a-b (2R= 2Me, (CH2)(4), (CH2...Resorcarens 1a-b (R'=Ph, p-MeOC6H4) were fully alkylated with alkyl iodides or bromides in TEBA/KOH/DMF solid-liquid PTC process with 63-82% yields, whereas the three calix[4]pyrroles 3a-b (2R= 2Me, (CH2)(4), (CH2)(5)) were alkylated with alkyl iodides in TBAB/ 50%NaOH/ CH2Cl2 liquid-liquid PTC system with lower yields (10-38%).展开更多
Chikungunya fever(CHIKF)is an arboviral disease that typically consists of an acute illness with fever,skin rash,and incapacitating arthralgia.The causative agent of CHIKF is Chikungunya virus(CHIKV),an alphavirus tha...Chikungunya fever(CHIKF)is an arboviral disease that typically consists of an acute illness with fever,skin rash,and incapacitating arthralgia.The causative agent of CHIKF is Chikungunya virus(CHIKV),an alphavirus that is transmitted by the Aedes mosquitoes.Despite the re-emergence of CHIKV as an epidemic threat,there is no approved effective anti-viral treatment currently available for CHIKV.In our preliminary studies,selected small molecule inhibitors of arboviruses related to CHIKV were investigated and this led us to identify compounds with thieno[3,2-b]pyrrole scaffold as hits.Building on the discovery of our best hit compounds,5-carboxylic acid thieno[3,2-b]pyrrole 1 and 5-carboxamide thieno[3,2-b]pyrrole 2,the main aim of this study is to optimize their anti-viral activities by synthesizing analogs of thieno[3,2-b]pyrroles 1 and 2 and examine their activities against CHIKV.In these two parallel optimization studies,we synthesized two series of thieno[3,2-b]pyrroles,namely the 5-carboxylic acids and 5-carboxamides that possessed a variety of substituents at N4,C2,C6 or C5positions of the thieno[3,2-b]pyrrole scaffold.These compounds were then examined for their cytotoxicity effects and anti-viral activities using a luminescence-labelled CHIKV infectious clone.The most potent compound in our studies was found in the 5-carboxamide series.The synthesis,biological activity and structure-activity relationship(SAR)will be presented and discussed in detail.展开更多
Under the catalysis of Yb(OTf)3, nucleophilic conjugate addition of pyrrole to electron deficient olefins in CH2Cl2 at ambient temperature gives corresponding 2-alkylated pyrrole derivatives in good yields with high s...Under the catalysis of Yb(OTf)3, nucleophilic conjugate addition of pyrrole to electron deficient olefins in CH2Cl2 at ambient temperature gives corresponding 2-alkylated pyrrole derivatives in good yields with high selectivity.展开更多
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.
基金supported by Chinese Academy of Sciences,China(Grant No.QYZDY-SSW-SLH013-2)Henan Normal University,China。
文摘Synthesizing nitrogen(N)-containing molecules from biomass derivatives is a new strategy for production of this kind of chemicals.Herein,for the first time we present the synthesis of N-substituted aryl pyrroles via reductive amination/cyclization of levulinic acid(LA)with primary aromatic amines and hydrosilanes(e.g.,PMHS)over Cs F,and a series of N-substituted aryl pyrroles could be obtained in good to excellent yields at 120○C.The mechanism investigation indicates that the reaction proceeds in two steps:the cyclization between amine and LA occurs first to form intermediate 5-methyl-N-alkyl-1,3-dihydro-2H-pyrrolones and their isomeride(B),and then the chemo-and region-selective reduction of intermediates take place to produce the final products.This approach for synthesis of N-substituted aryl pyrroles can be performed under mild and green conditions,which may have promising applications.
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.
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.
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.
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.
文摘We herein disclose a series of novel pyrrole derivatives as well as fused pyrrolopyridines 6a,b and 7a,b, pyrrolopyrazoles 8a, b, pyrrolo[2,3-d]pyrimidine derivatives 10a-d, 12a,b, 14a,b, 18a,b, 20a,b, 21a,b, 22a,b, 23a,b, 24a,b, 31a,b, 36a,b, 40a,b, pyrrolo[1,2,6]thiadiazine derivatives 19a,b, pyrrolotriazolopyrimidines 25a,b, 26a,b, 27a,b and 28a,b, pyrrolo[2,3-d][1,2,3]triazine derivatives 32a,b and pyrrolo[2,3-d][1,3]oxazine derivatives 39a,b as novel compounds. All compounds were evaluated for their anti-inflammatory, analgesic (compared to the reference drug Indomethacin) and antimicrobial activities (compared to the reference drug Ampicillin and Fluconazole). Compounds 4d, 5b-d, 6a,b, 9c,d, 10d, 12ab, 13b, 19a,b, 21b, 23b, 31a,b, 38b and 40a were found to be the most active anti-inflammatory drugs exhibiting potency ranging from 1 - 1.01 compared to the reference drug indomethacin. In addition to docking study of these highly active twenty compounds against the active site of cyclooxygenase-2 enzyme (COX-2), among the tested compounds, compounds 5d, 9d, 11b, 12a, 13b and 32a showed multiple activities;anti-inflammatory, analgesic and anti-bacterial activities.
文摘The synthesis of C-substituted and N-substituted pyrrole is described by the reaction of phenacyl bromides, pentane-2, 4-dione and amine in aqueous medium using DABCO as a catalyst. The method is very convenient and applicable for alkyl as well as aryl amines and phenacyl bromides. The procedure is amenable for the synthesis of new substituted pyrroles. Moreover, aqueous medium makes the method more eco-friendly.
基金supported by the National Natural Sci-ence Foundation of China(No.21671148)Tianjin Natural Science Foundation(18JCZDJC97000).
文摘Four organic smallmolecule hole transport materials(D41, D42,D43 and D44) of tetraarylpyrrolo[3,2-b]pyrroles were prepared. They can be used without doping in the manufacture of the inverted planar perovskite solar cells. Tetraarylpyrrolo[3,2-b]pyrroles are accessible for one-pot synthesis.D42, D43 and D44 possess acceptor-π-donor-π-acceptor structure, on which the aryl bearing substitutes of cyan, fluorine and trifluoromethyl, respectively. Instead, the aryl moiety of D41 is in presence of methyl with a donor-π-donor-π-donor structure. The different substitutes significantly affected their molecular surface charge distribution and thin-film morphology, attributing to the electron-rich properties of fused pyrrole ring. The size of perovskite crystalline growth particles is affected by different molecular structures,and the electron-withdrawing cyan group of D42 is most conducive to the formation of large perovskite grains. The D42 fabricated devices with power conversion efficiency of17.3% and retained 55% of the initial photoelectric conversion efficiency after 22 days in dark condition. The pyrrolo[3,2-b]pyrrole is efficient electron-donating moiety for hole transporting materials to form good substrate in producing perovskite thin film.
基金supported by the National Natural Science Foundation of China(NO.20275041)
文摘Octadecylsilanized silica (ODS) was coated with meso-octamethylcalix[4]pyrrole to obtain a novel calix[4]pyrrole containing stationary phase for HPLC. Compared to ODS, the new stationary phase showed a relatively large retention and an improved separation for phenolic compounds and organic anions, using pure water as mobile phase. The results can be ascribed to the interaction between analytes and calix[4]pyrrole.
文摘Resorcarens 1a-b (R'=Ph, p-MeOC6H4) were fully alkylated with alkyl iodides or bromides in TEBA/KOH/DMF solid-liquid PTC process with 63-82% yields, whereas the three calix[4]pyrroles 3a-b (2R= 2Me, (CH2)(4), (CH2)(5)) were alkylated with alkyl iodides in TBAB/ 50%NaOH/ CH2Cl2 liquid-liquid PTC system with lower yields (10-38%).
文摘Chikungunya fever(CHIKF)is an arboviral disease that typically consists of an acute illness with fever,skin rash,and incapacitating arthralgia.The causative agent of CHIKF is Chikungunya virus(CHIKV),an alphavirus that is transmitted by the Aedes mosquitoes.Despite the re-emergence of CHIKV as an epidemic threat,there is no approved effective anti-viral treatment currently available for CHIKV.In our preliminary studies,selected small molecule inhibitors of arboviruses related to CHIKV were investigated and this led us to identify compounds with thieno[3,2-b]pyrrole scaffold as hits.Building on the discovery of our best hit compounds,5-carboxylic acid thieno[3,2-b]pyrrole 1 and 5-carboxamide thieno[3,2-b]pyrrole 2,the main aim of this study is to optimize their anti-viral activities by synthesizing analogs of thieno[3,2-b]pyrroles 1 and 2 and examine their activities against CHIKV.In these two parallel optimization studies,we synthesized two series of thieno[3,2-b]pyrroles,namely the 5-carboxylic acids and 5-carboxamides that possessed a variety of substituents at N4,C2,C6 or C5positions of the thieno[3,2-b]pyrrole scaffold.These compounds were then examined for their cytotoxicity effects and anti-viral activities using a luminescence-labelled CHIKV infectious clone.The most potent compound in our studies was found in the 5-carboxamide series.The synthesis,biological activity and structure-activity relationship(SAR)will be presented and discussed in detail.
文摘Under the catalysis of Yb(OTf)3, nucleophilic conjugate addition of pyrrole to electron deficient olefins in CH2Cl2 at ambient temperature gives corresponding 2-alkylated pyrrole derivatives in good yields with high selectivity.
