A series of novel 1,5-benzothiazepine derivatives containing COOC2H5/COONa groups at the C(2)-position were synthesized and evaluated for their antifungal and antibacterial activities by both disc diffusion and mini...A series of novel 1,5-benzothiazepine derivatives containing COOC2H5/COONa groups at the C(2)-position were synthesized and evaluated for their antifungal and antibacterial activities by both disc diffusion and minimal inhibition concentration (MIC) methods. Most of the compounds have been shown to have moderate to good antibacterial activity against S. aureus, S. epidermidis and excellent antifungal activity against C. albicans.展开更多
Facile production of high quality activated carbons from biomass materials has greatly triggered much attention presently. In this paper, a series of interconnected porous carbon materials from lotus root shells bioma...Facile production of high quality activated carbons from biomass materials has greatly triggered much attention presently. In this paper, a series of interconnected porous carbon materials from lotus root shells biomass are prepared via simple pyrolysis and followed by a KOH activation process. The prepared carbons exhibit high specific surface areas of up to 2961 m^2/g and large pore volume~1.47 cm3/g. In addition, the resultant porous carbons served as electrode materials in supercapacitor exhibit high specific capacitance and outstanding recycling stability and high energy density. In particular, their specific capacitance retention was almost 100% after 10500 cycles at a current density of 2 A/g. Remarkabely, the impact of the tailored specific surface areas of various carbon samples on their capacitive performances is systematically investigated.Generally, it was believed that the highly-developed porosity features(including surface areas and pore volume and pore size-distributions), together with the good conductivity of activated carbon species, play a key role in effectively improving the storage energy performances of the porous carbon electrode materials in supercapacitor.展开更多
Two new a-aminophosphonate derivatives containing thieno[2,3-d]pyrimidine, diethyl(((6-ethyl-2-methyl-4-oxothieno[2,3-d]pyrimidin-3 (4H)-yl)amino)(4-methoxyphenyl)methyl) phosphonate (1) and diethyl((4-b...Two new a-aminophosphonate derivatives containing thieno[2,3-d]pyrimidine, diethyl(((6-ethyl-2-methyl-4-oxothieno[2,3-d]pyrimidin-3 (4H)-yl)amino)(4-methoxyphenyl)methyl) phosphonate (1) and diethyl((4-bromophenyl)((6-ethyl-2-methyl-4-oxothieno[2,3-d]pyrimidin-3 (4//)-yl)amino)methyl)phosphonate (2), have been synthesized by a facial phosphorylated reaction, and their structures were characterized by NMR, IR, HRMS and X-ray single-crystal diffraction. Compound 1 (C21H28N3O5PS, Mr = 465.49) belongs to the orthorhombic system, space group P212121, with a = 10.83653(16), b = 12.04906(19), c = 18.0061(3) A, V= 2351.06(6) A3, Z= 4, Dc= 1.315 g/cm3, p = 2.177 mm-1, F(000) = 984.0, the final R = 0.0389 and wR = 0.0985 for all data. Compound 2 (C20H25BrN304PS, Mr = 514.37) belongs to the orthorhombic system, space group P212121, with a = 10.9187(5), b = 11.9522(4), c = 17.7667(7) A, V= 2318.60(16) A3, Z = 4, Dc= 1.474 g/cm3,μ = 4.175 mm^-1, F(000) = 1056.0, the final R = 0.0367 and wR = 0.0946 for all data.展开更多
ZnO is a semiconductor photocatalyst widely applied in photodegradation of organic pollutants and in photoelectric conversion. ZnO exhibits low photocatalytic activity due to poor absorption in the visible region. In ...ZnO is a semiconductor photocatalyst widely applied in photodegradation of organic pollutants and in photoelectric conversion. ZnO exhibits low photocatalytic activity due to poor absorption in the visible region. In this work, a novel cobalt-induced electrochemical growth method was developed to synthesize cobalt-doped ZnO/rGO nanoparticles in an aqueous solution at room temperature. Cobalt-doped ZnO/rGO nanoparticles exhibited wider visible-light absorption band ranging from 400 nm to 700 nm due to cobalt doping. The surface structure of ZnO formed by the cobalt-induced electrochemical method without other ions is suitable for photocatalytic reactions. The cobalt-doped ZnO/rGO nanoparticles were found to exhibit in photodegradation and photo-electrochemical measurements and exhibited enhanced photocatalytic activity under visible-light irradiation.展开更多
A series of main chain liquid crystal aromatic copolyesters with X-shaped and rod-shaped mesogenic units were synthesized via solution condensation polymerizations of 4,4'-(alpha,omega-octanedioyloxy)-dibenzoyl di...A series of main chain liquid crystal aromatic copolyesters with X-shaped and rod-shaped mesogenic units were synthesized via solution condensation polymerizations of 4,4'-(alpha,omega-octanedioyloxy)-dibenzoyl dichlorides with 2,5-bis(p-octanoxy benzoyloxy)-hydroquinone and diphenol. All of the copolyesters showed thermotropic liquid crystalline behaviors through observations using DSC, polarized microscopy and X-ray diffraction. The melting point (T-m) and the isotropization temperature (T-i) change regularly with varying the content of diphenol unit in the copolymers.展开更多
A new series of liquid crystal polyesters with T-shaped two-dimensional mesogenic units weresynthesized by melt polycondensation of the diacetates of 2-(4'-alkoxy -phenyl)-hydroquinones with 4,4'-alkylenedioxy...A new series of liquid crystal polyesters with T-shaped two-dimensional mesogenic units weresynthesized by melt polycondensation of the diacetates of 2-(4'-alkoxy -phenyl)-hydroquinones with 4,4'-alkylenedioxydibenzoic acid. The polymers were characterized by using polarized microscopy, DSC and X-ray diffraction. It was realized that all the polymers have nematic thermotropic liquid crystallinecharacteristics. The melting temperature (T_m) and isotropization temperature (T_i) of the polymers changeregularly with varying lengths of the alkoxy side group and the length of the alkylene group in the main chainin company with an even-odd effect. The mesophase temperature range also varies regularly with the polymerstructure. It is shown that the mesophase range has been widened.展开更多
Thermal treatment of the pyridyl side chain functionalized tetramethyl cyclopen- tadiene C5Me4CH2(C5H4N) with Fe(CO)5, Ru3(CO)12 and Mo(CO)6 in refluxing xylene respectively gave the corresponding dinuclear me...Thermal treatment of the pyridyl side chain functionalized tetramethyl cyclopen- tadiene C5Me4CH2(C5H4N) with Fe(CO)5, Ru3(CO)12 and Mo(CO)6 in refluxing xylene respectively gave the corresponding dinuclear metal carbonyl complexes 1~3. These complexes have been characterized by elemental analysis, IR and IH NMR spectra. The molecular structures of 1~3 were determined by X-ray diffraction analysis.展开更多
Ce/BiVO4 nanocomposites photocatalyst was synthesized by direct feeding microwave synthesis method, using bismuth nitrate (Bi (NO3)3·5H2O), cerium?nitrate hexahydrate (Ce (NO3)3·6H2O) and ammonium metavanada...Ce/BiVO4 nanocomposites photocatalyst was synthesized by direct feeding microwave synthesis method, using bismuth nitrate (Bi (NO3)3·5H2O), cerium?nitrate hexahydrate (Ce (NO3)3·6H2O) and ammonium metavanadate (NH4VO3) as raw material and sodium dodecyl sulfate (SDS) as surfactant. The X-ray diffractometer (XRD) and the scanning electron microscopy (SEM) technology were used to characterize the Ce/BiVO4 nanocomposites. We investigated the photocatalytic activity of the as-prepared photocatalyst, and methyl orange was used as organic pollutant. The results show that the Ce/BiVO4 nanocomposite was a good photocatalyst under visible light. In 100 ml of 5 mg/L methylene orange solution, when the catalyst calcined at 673 K was 0.1 g, hydrogen peroxide was 0.5 ml, pH was 2.0, and the degradation ratio of catalyst for methylene orange reached 90.26% within 70 min.展开更多
Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of nove...Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and Au.The electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and HER.Impressively,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 V.Moreover,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was assembled.Accordingly,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS equipment.The interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.展开更多
A new thermomorphic catalytic system for the Baylis-Hillman coupling of aromatic aldehydes with a, β-unsaturated ketone has been described, in which the alkyl-functionalized dendritic catalyst preferred to dissolve i...A new thermomorphic catalytic system for the Baylis-Hillman coupling of aromatic aldehydes with a, β-unsaturated ketone has been described, in which the alkyl-functionalized dendritic catalyst preferred to dissolve in non-polar organic layer in the thermomorphic biphasic system, leading to easy separation of the catalyst from the polar products by changing the temperature of the system at end of the reaction.展开更多
Excited state structures and spectroscopic properties of mercury( 11 ) complexes, Hg-TFT(1) and its electronwithdrawing substituents Hg-TFOT ( 2 ), Hg-TFCNT ( 3 ), where TFT = dietbynylfluorenyl, TFOT = diethy...Excited state structures and spectroscopic properties of mercury( 11 ) complexes, Hg-TFT(1) and its electronwithdrawing substituents Hg-TFOT ( 2 ), Hg-TFCNT ( 3 ), where TFT = dietbynylfluorenyl, TFOT = diethynylfluorenone, and TFCNT = diethynyl-[9-(dicyanomethylene) fluorene], were studied using singlet excitation configuration interaction(CIS) and time-dependent density functional theory(TDDFT) methods. The results of the theoretical calculations indicate that the electron-withdrawing substitutions lead to a significant decrease in the energy gap between the ground state and the first excited states. In the case of Hg-TFCNT, the second singlet excited state (S2 ) may contribute to the luminescence because of its large S1-S2 separation.展开更多
Building well-developed ion-conductive highways is highly desirable for anion exchange membranes(AEMs).Grafting side chain is a highly effective approach for constructing a well-defined phaseseparated morphological st...Building well-developed ion-conductive highways is highly desirable for anion exchange membranes(AEMs).Grafting side chain is a highly effective approach for constructing a well-defined phaseseparated morphological structure and forming unblocked ion pathways in AEMs for fast ion transport.Fluorination of side chains can further enhance phase separation due to the superhydrophobic nature of fluorine groups.However,their electronic effect on the alkaline stability of side chains and membranes is rarely reported.Here,fluorine-containing and fluorine-free side chains are introduced into the polyaromatic backbone in proper configuration to investigate the impact of the fluorine terminal group on the stability of the side chains and membrane properties.The poly(binaphthyl-co-p-terphenyl piperidinium)AEM(QBNp TP)has the highest molecular weight and most dimensional stability due to its favorable backbone arrangement among ortho-and meta-terphenyl based AEMs.Importantly,by introducing both a fluorinated piperidinium side chain and a hexane chain into the p-terphenyl-based backbone,the prepared AEM(QBNp TP-QFC)presents an enhanced conductivity(150.6 m S cm^(-1))and a constrained swelling at 80℃.The electronic effect of fluorinated side chains is contemplated by experiments and simulations.The results demonstrate that the presence of strong electro-withdrawing fluorine groups weakens the electronic cloud of adjacent C atoms,increasing OH^(-)attack on the C atom and improving the stability of piperidinium cations.Hence QBNp TP-QFC possesses a robust alkaline stability at 80℃(95.3%conductivity retention after testing in 2 M Na OH for 2160 h).An excellent peak power density of 1.44 W cm^(-2)and a remarkable durability at 80℃(4.5%voltage loss after 100 h)can be observed.展开更多
Metal-free g-C_3N_4 is widely used in photocatalytic reactions owing to its suitable band structure.However, it has low specific surface area and insufficient absorbance for visible light, and its photoexcited carrier...Metal-free g-C_3N_4 is widely used in photocatalytic reactions owing to its suitable band structure.However, it has low specific surface area and insufficient absorbance for visible light, and its photoexcited carriers have high recombination rates. In this study, the 3 D macropore C-vacancy g-C_3N_4 was prepared through a facile one-step route. Polymethylmethacrylate is used as a template to increase the surface reaction sites of g-C_3N_4 and extend its visible-light range. Compared to unmodified g-C_3N_4, the H2 production and CO_2 reduction rates of the fabricated g-C_3N_4 significantly improved. The special pore structure significantly improved the light utilization efficiency of g-C_3N_4 and increased the number of surface-active sites. The introduction of C-vacancy extended the absorption band of visible-light and suppressed the carrier recombination. The newly developed synthesis strategy can improve solar energy conversion efficiency and potentially modifies g-C_3N_4.展开更多
It is still challenging for conductive polymer composite-based electromagnetic interference(EMI)shielding materials to achieve long-term stability while maintaining high EMI shielding effectiveness(EMI SE),especially ...It is still challenging for conductive polymer composite-based electromagnetic interference(EMI)shielding materials to achieve long-term stability while maintaining high EMI shielding effectiveness(EMI SE),especially undergoing external mechanical stimuli,such as scratches or large deformations.Herein,an electrostatic assembly strategy is adopted to design a healable and segregated carbon nanotube(CNT)/graphene oxide(GO)/polyurethane(PU)composite with excellent and reliable EMI SE,even bearing complex mechanical condition.The negatively charged CNT/GO hybrid is facilely adsorbed on the surface of positively charged PU microsphere to motivate formation of segregated conductive networks in CNT/GO/PU composite,establishing a high EMI SE of 52.7 dB at only 10 wt%CNT/GO loading.The Diels–Alder bonds in PU microsphere endow the CNT/GO/PU composite suffering three cutting/healing cycles with EMI SE retention up to 90%.Additionally,the electrostatic attraction between CNT/GO hybrid and PU microsphere helps to strong interfacial bonding in the composite,resulting in high tensile strength of 43.1 MPa and elongation at break of 626%.The healing efficiency of elongation at break achieves 95%when the composite endured three cutting/healing cycles.This work demonstrates a novel strategy for developing segregated EMI shielding composite with healable features and excellent mechanical performance and shows great potential in the durable and high precision electrical instruments.展开更多
A facile and efficient method for the synthesis of tetrasubstituted olefins in supercritical carbon dioxide was developed by using carbon nanotubes-supported palladium nanoparticles (Pd/CNTs) as the catalyst. Compared...A facile and efficient method for the synthesis of tetrasubstituted olefins in supercritical carbon dioxide was developed by using carbon nanotubes-supported palladium nanoparticles (Pd/CNTs) as the catalyst. Compared with common Pd/C, Pd/CNTs could more effectively catalyze the reaction of dibromo-substituted olefins with boronic acids, affording the corresponding tetrasubstituted olefins with moderate to good yields. This environmentally benign route with an easy-to-handle catalyst provides an appealing alternative to the currently available methods.展开更多
Two series of thieno[2,3-d]pyrimidine derivatives were designed and synthesized, in which bioactive α-aminophosphonate subunits were introduced at the N3 position through an N-N bond connection. The in vitro cytotoxi...Two series of thieno[2,3-d]pyrimidine derivatives were designed and synthesized, in which bioactive α-aminophosphonate subunits were introduced at the N3 position through an N-N bond connection. The in vitro cytotoxic activity of the novel compounds was tested against human esophageal carcinoma cells (EC109), human hepatocarcinoma cells (HepG2), human gastric carcinoma cells (MGC-803), respectively, by the MTT method. The evaluation results revealed that compounds fimb, 6mf, 6mg, 6rid and 6nh exerted the most potent inhibition against HepG2, MGC-803 and EC109 cells, respectively. In particular, compound 6rag presented excellent inhibitory effect against HepG2 (91.2%) and MGC-803 (94.4%) cells.展开更多
A general, mild and efficient protocol for the synthesis of ethyl 4-methyl-2-(thiophen)-2,5-dihydro-1,5- benzodiazepine-3-carboxylate is achieved for first time using H3PMo12O40 in ethanol at 0 ℃ by a one- pot, th...A general, mild and efficient protocol for the synthesis of ethyl 4-methyl-2-(thiophen)-2,5-dihydro-1,5- benzodiazepine-3-carboxylate is achieved for first time using H3PMo12O40 in ethanol at 0 ℃ by a one- pot, three-component condensation of various thiophene aldehydes, substituted o-phenylenediamines and ethyl acetoacetate. Compared with the conventional synthesis method, this procedure has the advantages of convenient operation, excellent yields, and environmentally benign. A plausible formation mechanism has been proposed. The structure of the products is characterized by1H NMR, IR, MS and elemental analysis.展开更多
We report a 2-iodoxybenzoic acid(IBX)-mediated intarmolecular oxidative spiro-fused tandem cyclization reaction of tryptophan analogs bearing an N-arylamides side-chain to rapidly afford polycyclic spiroindolines feat...We report a 2-iodoxybenzoic acid(IBX)-mediated intarmolecular oxidative spiro-fused tandem cyclization reaction of tryptophan analogs bearing an N-arylamides side-chain to rapidly afford polycyclic spiroindolines featuring multiple stereocenters including a quaternary stereocenters under mild reaction conditions.Among them,a novelty azaphosphol idine-containing spiroindoline compound is synthesized for the first time.It may open the door to azaphos pholidine-containing spiroindoline compound of potential interest in synthetic and medicinal chemistry.A plausible mechanism is proposed.展开更多
基金support from National Natural Science Foundation of China(No.20772021)the Natural Science Foundation of Hebei Province,China(No.2007000239)
文摘A series of novel 1,5-benzothiazepine derivatives containing COOC2H5/COONa groups at the C(2)-position were synthesized and evaluated for their antifungal and antibacterial activities by both disc diffusion and minimal inhibition concentration (MIC) methods. Most of the compounds have been shown to have moderate to good antibacterial activity against S. aureus, S. epidermidis and excellent antifungal activity against C. albicans.
基金National Science Foundation of China(No.21173167)the Science and Technology Committee of Shaanxi Province(Grant No.2014KW09-03)+1 种基金Program for New Century Excellent Talents in University(NCET-13-0953)the Research Fund of the State Key Lab of Solidification Processing(NWPU),China(Grant No.15-BZ-2015)
文摘Facile production of high quality activated carbons from biomass materials has greatly triggered much attention presently. In this paper, a series of interconnected porous carbon materials from lotus root shells biomass are prepared via simple pyrolysis and followed by a KOH activation process. The prepared carbons exhibit high specific surface areas of up to 2961 m^2/g and large pore volume~1.47 cm3/g. In addition, the resultant porous carbons served as electrode materials in supercapacitor exhibit high specific capacitance and outstanding recycling stability and high energy density. In particular, their specific capacitance retention was almost 100% after 10500 cycles at a current density of 2 A/g. Remarkabely, the impact of the tailored specific surface areas of various carbon samples on their capacitive performances is systematically investigated.Generally, it was believed that the highly-developed porosity features(including surface areas and pore volume and pore size-distributions), together with the good conductivity of activated carbon species, play a key role in effectively improving the storage energy performances of the porous carbon electrode materials in supercapacitor.
基金supported by the National Natural Science Foundation of China(Nos.21105091 and 21171149)
文摘Two new a-aminophosphonate derivatives containing thieno[2,3-d]pyrimidine, diethyl(((6-ethyl-2-methyl-4-oxothieno[2,3-d]pyrimidin-3 (4H)-yl)amino)(4-methoxyphenyl)methyl) phosphonate (1) and diethyl((4-bromophenyl)((6-ethyl-2-methyl-4-oxothieno[2,3-d]pyrimidin-3 (4//)-yl)amino)methyl)phosphonate (2), have been synthesized by a facial phosphorylated reaction, and their structures were characterized by NMR, IR, HRMS and X-ray single-crystal diffraction. Compound 1 (C21H28N3O5PS, Mr = 465.49) belongs to the orthorhombic system, space group P212121, with a = 10.83653(16), b = 12.04906(19), c = 18.0061(3) A, V= 2351.06(6) A3, Z= 4, Dc= 1.315 g/cm3, p = 2.177 mm-1, F(000) = 984.0, the final R = 0.0389 and wR = 0.0985 for all data. Compound 2 (C20H25BrN304PS, Mr = 514.37) belongs to the orthorhombic system, space group P212121, with a = 10.9187(5), b = 11.9522(4), c = 17.7667(7) A, V= 2318.60(16) A3, Z = 4, Dc= 1.474 g/cm3,μ = 4.175 mm^-1, F(000) = 1056.0, the final R = 0.0367 and wR = 0.0946 for all data.
基金supported by the National Science Fund of China(51662030,21366020)the Natural Science Foundation of Jiangxi Province(20151BAB216006,20122BAB203009)the Science and Technology Project of Education Department of Jiangxi Province(GJJ14109)
文摘ZnO is a semiconductor photocatalyst widely applied in photodegradation of organic pollutants and in photoelectric conversion. ZnO exhibits low photocatalytic activity due to poor absorption in the visible region. In this work, a novel cobalt-induced electrochemical growth method was developed to synthesize cobalt-doped ZnO/rGO nanoparticles in an aqueous solution at room temperature. Cobalt-doped ZnO/rGO nanoparticles exhibited wider visible-light absorption band ranging from 400 nm to 700 nm due to cobalt doping. The surface structure of ZnO formed by the cobalt-induced electrochemical method without other ions is suitable for photocatalytic reactions. The cobalt-doped ZnO/rGO nanoparticles were found to exhibit in photodegradation and photo-electrochemical measurements and exhibited enhanced photocatalytic activity under visible-light irradiation.
基金The work was supported by the National Natural Science Foundation of China.
文摘A series of main chain liquid crystal aromatic copolyesters with X-shaped and rod-shaped mesogenic units were synthesized via solution condensation polymerizations of 4,4'-(alpha,omega-octanedioyloxy)-dibenzoyl dichlorides with 2,5-bis(p-octanoxy benzoyloxy)-hydroquinone and diphenol. All of the copolyesters showed thermotropic liquid crystalline behaviors through observations using DSC, polarized microscopy and X-ray diffraction. The melting point (T-m) and the isotropization temperature (T-i) change regularly with varying the content of diphenol unit in the copolymers.
基金This work was supported by the National Natural Science Foundation of China.
文摘A new series of liquid crystal polyesters with T-shaped two-dimensional mesogenic units weresynthesized by melt polycondensation of the diacetates of 2-(4'-alkoxy -phenyl)-hydroquinones with 4,4'-alkylenedioxydibenzoic acid. The polymers were characterized by using polarized microscopy, DSC and X-ray diffraction. It was realized that all the polymers have nematic thermotropic liquid crystallinecharacteristics. The melting temperature (T_m) and isotropization temperature (T_i) of the polymers changeregularly with varying lengths of the alkoxy side group and the length of the alkylene group in the main chainin company with an even-odd effect. The mesophase temperature range also varies regularly with the polymerstructure. It is shown that the mesophase range has been widened.
基金financially supported by the National Natural Science Foundation of China(No.21372061)Natural Science Foundation of Hebei Province(Nos.B2013205025 and B2014205018)the Key Research Fund of Hebei Normal University(No.L2012Z02)
文摘Thermal treatment of the pyridyl side chain functionalized tetramethyl cyclopen- tadiene C5Me4CH2(C5H4N) with Fe(CO)5, Ru3(CO)12 and Mo(CO)6 in refluxing xylene respectively gave the corresponding dinuclear metal carbonyl complexes 1~3. These complexes have been characterized by elemental analysis, IR and IH NMR spectra. The molecular structures of 1~3 were determined by X-ray diffraction analysis.
文摘Ce/BiVO4 nanocomposites photocatalyst was synthesized by direct feeding microwave synthesis method, using bismuth nitrate (Bi (NO3)3·5H2O), cerium?nitrate hexahydrate (Ce (NO3)3·6H2O) and ammonium metavanadate (NH4VO3) as raw material and sodium dodecyl sulfate (SDS) as surfactant. The X-ray diffractometer (XRD) and the scanning electron microscopy (SEM) technology were used to characterize the Ce/BiVO4 nanocomposites. We investigated the photocatalytic activity of the as-prepared photocatalyst, and methyl orange was used as organic pollutant. The results show that the Ce/BiVO4 nanocomposite was a good photocatalyst under visible light. In 100 ml of 5 mg/L methylene orange solution, when the catalyst calcined at 673 K was 0.1 g, hydrogen peroxide was 0.5 ml, pH was 2.0, and the degradation ratio of catalyst for methylene orange reached 90.26% within 70 min.
基金supported by the Key projects of intergovernmental international cooperation in the Key R&D programs of the Ministry of Science and Technology of China(No.2021YFE0115800)the National Science Funding Committee of China(No.U20A20250)。
文摘Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and Au.The electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and HER.Impressively,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 V.Moreover,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was assembled.Accordingly,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS equipment.The interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.
文摘A new thermomorphic catalytic system for the Baylis-Hillman coupling of aromatic aldehydes with a, β-unsaturated ketone has been described, in which the alkyl-functionalized dendritic catalyst preferred to dissolve in non-polar organic layer in the thermomorphic biphasic system, leading to easy separation of the catalyst from the polar products by changing the temperature of the system at end of the reaction.
基金Supported by the"973"Program of China(No 2002CB613406) and Youth Science Foundation of Northeast Normal University(No 111494018)
文摘Excited state structures and spectroscopic properties of mercury( 11 ) complexes, Hg-TFT(1) and its electronwithdrawing substituents Hg-TFOT ( 2 ), Hg-TFCNT ( 3 ), where TFT = dietbynylfluorenyl, TFOT = diethynylfluorenone, and TFCNT = diethynyl-[9-(dicyanomethylene) fluorene], were studied using singlet excitation configuration interaction(CIS) and time-dependent density functional theory(TDDFT) methods. The results of the theoretical calculations indicate that the electron-withdrawing substitutions lead to a significant decrease in the energy gap between the ground state and the first excited states. In the case of Hg-TFCNT, the second singlet excited state (S2 ) may contribute to the luminescence because of its large S1-S2 separation.
基金the financial support from the National Natural Science Foundation of China(22078272&22278340)。
文摘Building well-developed ion-conductive highways is highly desirable for anion exchange membranes(AEMs).Grafting side chain is a highly effective approach for constructing a well-defined phaseseparated morphological structure and forming unblocked ion pathways in AEMs for fast ion transport.Fluorination of side chains can further enhance phase separation due to the superhydrophobic nature of fluorine groups.However,their electronic effect on the alkaline stability of side chains and membranes is rarely reported.Here,fluorine-containing and fluorine-free side chains are introduced into the polyaromatic backbone in proper configuration to investigate the impact of the fluorine terminal group on the stability of the side chains and membrane properties.The poly(binaphthyl-co-p-terphenyl piperidinium)AEM(QBNp TP)has the highest molecular weight and most dimensional stability due to its favorable backbone arrangement among ortho-and meta-terphenyl based AEMs.Importantly,by introducing both a fluorinated piperidinium side chain and a hexane chain into the p-terphenyl-based backbone,the prepared AEM(QBNp TP-QFC)presents an enhanced conductivity(150.6 m S cm^(-1))and a constrained swelling at 80℃.The electronic effect of fluorinated side chains is contemplated by experiments and simulations.The results demonstrate that the presence of strong electro-withdrawing fluorine groups weakens the electronic cloud of adjacent C atoms,increasing OH^(-)attack on the C atom and improving the stability of piperidinium cations.Hence QBNp TP-QFC possesses a robust alkaline stability at 80℃(95.3%conductivity retention after testing in 2 M Na OH for 2160 h).An excellent peak power density of 1.44 W cm^(-2)and a remarkable durability at 80℃(4.5%voltage loss after 100 h)can be observed.
基金financial support from the National Natural Science Foundation of China (51862023, 51662030, 21868016)the Natural Science Foundation of Jiangxi Province (20171BAB206014, 2018BCD40004)。
文摘Metal-free g-C_3N_4 is widely used in photocatalytic reactions owing to its suitable band structure.However, it has low specific surface area and insufficient absorbance for visible light, and its photoexcited carriers have high recombination rates. In this study, the 3 D macropore C-vacancy g-C_3N_4 was prepared through a facile one-step route. Polymethylmethacrylate is used as a template to increase the surface reaction sites of g-C_3N_4 and extend its visible-light range. Compared to unmodified g-C_3N_4, the H2 production and CO_2 reduction rates of the fabricated g-C_3N_4 significantly improved. The special pore structure significantly improved the light utilization efficiency of g-C_3N_4 and increased the number of surface-active sites. The introduction of C-vacancy extended the absorption band of visible-light and suppressed the carrier recombination. The newly developed synthesis strategy can improve solar energy conversion efficiency and potentially modifies g-C_3N_4.
基金The authors gratefully acknowledge the financial support from the National Natural Science Foundation of China(Grant Nos.51973142,51721091,21878194)the National Key Research and Development Program of China(2018YFB0704200)the funds of the State Key Laboratory of Solidification Processing(Northwestern Polytechnical University)(SKLSP201918).
文摘It is still challenging for conductive polymer composite-based electromagnetic interference(EMI)shielding materials to achieve long-term stability while maintaining high EMI shielding effectiveness(EMI SE),especially undergoing external mechanical stimuli,such as scratches or large deformations.Herein,an electrostatic assembly strategy is adopted to design a healable and segregated carbon nanotube(CNT)/graphene oxide(GO)/polyurethane(PU)composite with excellent and reliable EMI SE,even bearing complex mechanical condition.The negatively charged CNT/GO hybrid is facilely adsorbed on the surface of positively charged PU microsphere to motivate formation of segregated conductive networks in CNT/GO/PU composite,establishing a high EMI SE of 52.7 dB at only 10 wt%CNT/GO loading.The Diels–Alder bonds in PU microsphere endow the CNT/GO/PU composite suffering three cutting/healing cycles with EMI SE retention up to 90%.Additionally,the electrostatic attraction between CNT/GO hybrid and PU microsphere helps to strong interfacial bonding in the composite,resulting in high tensile strength of 43.1 MPa and elongation at break of 626%.The healing efficiency of elongation at break achieves 95%when the composite endured three cutting/healing cycles.This work demonstrates a novel strategy for developing segregated EMI shielding composite with healable features and excellent mechanical performance and shows great potential in the durable and high precision electrical instruments.
基金Supported by the National Natural Science Foundation of China (Grant Nos. 20332030, 20572027, 20625205 and 20772034) Guangdong Natural Science Foundation (No. 07118070).
文摘A facile and efficient method for the synthesis of tetrasubstituted olefins in supercritical carbon dioxide was developed by using carbon nanotubes-supported palladium nanoparticles (Pd/CNTs) as the catalyst. Compared with common Pd/C, Pd/CNTs could more effectively catalyze the reaction of dibromo-substituted olefins with boronic acids, affording the corresponding tetrasubstituted olefins with moderate to good yields. This environmentally benign route with an easy-to-handle catalyst provides an appealing alternative to the currently available methods.
基金supported by the National Natural Sciences Foundations of China (Nos.21171149,21105091)
文摘Two series of thieno[2,3-d]pyrimidine derivatives were designed and synthesized, in which bioactive α-aminophosphonate subunits were introduced at the N3 position through an N-N bond connection. The in vitro cytotoxic activity of the novel compounds was tested against human esophageal carcinoma cells (EC109), human hepatocarcinoma cells (HepG2), human gastric carcinoma cells (MGC-803), respectively, by the MTT method. The evaluation results revealed that compounds fimb, 6mf, 6mg, 6rid and 6nh exerted the most potent inhibition against HepG2, MGC-803 and EC109 cells, respectively. In particular, compound 6rag presented excellent inhibitory effect against HepG2 (91.2%) and MGC-803 (94.4%) cells.
基金financial support from the National Natural Science Foundation of China(No.21276064)the Natural Science Foundation of Hebei Education Department(No.2008320)the Science Foundation of Hebei Normal University(No.2011Y04)
文摘A general, mild and efficient protocol for the synthesis of ethyl 4-methyl-2-(thiophen)-2,5-dihydro-1,5- benzodiazepine-3-carboxylate is achieved for first time using H3PMo12O40 in ethanol at 0 ℃ by a one- pot, three-component condensation of various thiophene aldehydes, substituted o-phenylenediamines and ethyl acetoacetate. Compared with the conventional synthesis method, this procedure has the advantages of convenient operation, excellent yields, and environmentally benign. A plausible formation mechanism has been proposed. The structure of the products is characterized by1H NMR, IR, MS and elemental analysis.
基金the National Natural Science Foundation of China(Nos.U1604285,21772032 and 21702051)Program for Changjiang Scholars and Innovative Research Team in University(PCSIRT)of Ministry of Education of China(No.IRT1061)+3 种基金the 111 Project(No.D17007)Henan Provincial Natural Science Foundation(No.162300410180)Key Project of Henan Educational Committee(No.18A150009)Program for Innovative Research Team of Science and Technology in the University of Henan Province(No.18IRTSTHN004)。
文摘We report a 2-iodoxybenzoic acid(IBX)-mediated intarmolecular oxidative spiro-fused tandem cyclization reaction of tryptophan analogs bearing an N-arylamides side-chain to rapidly afford polycyclic spiroindolines featuring multiple stereocenters including a quaternary stereocenters under mild reaction conditions.Among them,a novelty azaphosphol idine-containing spiroindoline compound is synthesized for the first time.It may open the door to azaphos pholidine-containing spiroindoline compound of potential interest in synthetic and medicinal chemistry.A plausible mechanism is proposed.