Aim To synthesize trans and cis-3, 4′, 5-trihydroxystilbene by a new convenient route. Methods The reaction of 3, 5-dimethoxybenzaldehyde (3) and 4-methoxy phenylacetonitrile (4) formed the stilbene skeleton. Aft...Aim To synthesize trans and cis-3, 4′, 5-trihydroxystilbene by a new convenient route. Methods The reaction of 3, 5-dimethoxybenzaldehyde (3) and 4-methoxy phenylacetonitrile (4) formed the stilbene skeleton. After hydrolyzation, decarboxylation, and demethylation, we obtained trans-3, 4′, 5-trihydroxystilbene (resveratrol), which can be converted to its cis-isomer by photochemical isomerization. Results Starting from 3 and 4, trans and cis-3, 4′, 5-trihydroxystilbene were synthesized, respectively. Conclusion A facile method for the synthesis of trans and cis-hydroxystilbenes from readily available materials was established.展开更多
The phase equilibria and compositions in Mg-rich side at 300 ℃ were investigated in Mg-Zn-Ca ternary system through the equilibrated alloy method by using scanning electron microscopy,electron probe microanalysis,X-r...The phase equilibria and compositions in Mg-rich side at 300 ℃ were investigated in Mg-Zn-Ca ternary system through the equilibrated alloy method by using scanning electron microscopy,electron probe microanalysis,X-ray diffraction and transmission electron microscopy.The results show that two ternary compounds T1 and T2 can be in equilibrium with the Mg-based solid solution in Mg-Zn-Ca system.T1 phase is a linear compound with the composition region(molar fraction) of 15% Ca,20.5%-48.9% Zn and balanced Mg at 300 ℃.Its hexagonal structure parameters decrease with increasing Zn content,i.e.a=0.992-0.945 nm,c=1.034-1.003 nm.T2 phase has hexagonal structure with the composition region of 26.4%-28.4% Mg,63.2%-65.5% Zn and 7.1%-8.4% Ca.At 300 ℃,the solubility of Zn in the Mg-based solid solution increases for the addition of Ca,the maximum solubility of Zn is 3.7%.Three-phase fields consisting of--Mg+Mg2Ca+T1,--Mg+T1+T2,--Mg+T2+MgZn and MgZn+T2+Mg2Zn3 exist in the Mg-Zn-Ca system at 300 ℃.展开更多
Mesh-like Bi2MoO6 product was successfully synthesized by a hydrothermal method without using any surfactant or template. The pH value played an important role in the formation of this morphology. The as-prepared mesh...Mesh-like Bi2MoO6 product was successfully synthesized by a hydrothermal method without using any surfactant or template. The pH value played an important role in the formation of this morphology. The as-prepared mesh-like Bi2MoO6 sample exhibited excellent visible-light-driven photocatalytic e ciency. The photocatalytic activity of the mesh-like Bi2MoO6 sample was much higher than that of bulk Bi2MoO6 sample prepared by solid-state reac-tion. Di erence in the photocatalytic activities of the mesh-like Bi2MoO6 sample and bulk Bi2MoO6 sample was further investigated.展开更多
To study the antifungal effect of chalcone derivatives. Methods Sixteenchalcone derivatives were synthesized and confirmed by ~1H NMR and IR spectra, and tested forantifungal activity against four common pathogenic fu...To study the antifungal effect of chalcone derivatives. Methods Sixteenchalcone derivatives were synthesized and confirmed by ~1H NMR and IR spectra, and tested forantifungal activity against four common pathogenic fungi. Their structure-activity relationship isdiscussed. Results Among 16 title compounds, there were 5 new compounds, which have not beenreported before. The preliminary antifungal test showed that all title compounds exhibitedantifungal activities to a certain extent. The activity of compound 8 against Trichophyton rubrumhad a potency equal to that of fluconazole, with a MIC of 4 μg·mL^(-1) . Conclusion Sixteenchalcones were prepared and their antifungal activities against four common pathogenic fungi invitro were examined. Some of them exhibited antifungal activities to a certain extent.展开更多
The textural features and acidic properties of sulfated mesoporous lanthana‐zirconia solid acids (SO42?/meso‐La0.1Zr0.9Oδ) were efficiently tuned by modifying the conditions used to prepare the meso‐La0.1Zr0.9O...The textural features and acidic properties of sulfated mesoporous lanthana‐zirconia solid acids (SO42?/meso‐La0.1Zr0.9Oδ) were efficiently tuned by modifying the conditions used to prepare the meso‐La0.1Zr0.9Oδcomposites, such as the molar ratio of the template to La and Zr metal ions (Nt/m), molar ratio of ammonia to La and Zr metal ions (Na/m), hydrothermal temperature (Thydro), and hy‐drothermal time (thydro). The effect of the textural features and acidic properties on the catalytic performance of solid acid catalysts for alkenylation of p‐xylene with phenylacetylene was investi‐gated. Various characterization techniques such as N2 physisorption, X‐ray diffraction, NH3 temper‐ature‐programmed desorption, and thermogravimetric analysis were employed to reveal the rela‐tionship between the nature of catalyst and its catalytic performance. It was found that the catalytic performance significantly depended on the textural features and acidic properties, which were strongly affected by preparation conditions of the meso‐La0.1Zr0.9Oδcomposite. Appropriate acidic sites and high accessibility were required to obtain satisfactory catalytic reactions for this reaction. It was also found that the average crystallite size of t‐ZrO2 affected by the preparation conditions had significant influence on the ultrastrong acidic sites of the catalysts. The optimized SO42?/meso‐La0.1Zr0.9Oδcatalyst exhibited much superior catalytic activity and coke‐resistant stabil‐ity. Moreover, the developed SO42?/meso‐La0.1Zr0.9Oδcatalyst demonstrated excellent catalytic per‐formance for alkenylation of diverse aromatics with phenylacetylene to their correspondingα‐arylstyrenes. Combining the previously established complete regeneration of used catalysts by a facile calcination process with the improved catalytic properties, the developed SO42?/meso‐La0.1Zr0.9Oδ solid acid could be a potential catalyst for industrial production ofα‐arylstyrenes through clean and atom efficient solid‐acid‐mediated Friedel‐Crafts alkenylation of diverse aromatics with phenylacetylene.展开更多
The two major challenges in industrial enzymatic catalysis are the limited number of chemical reaction types that are catalyzed by enzymes and the instability of enzymes under harsh conditions in industrial catalysis....The two major challenges in industrial enzymatic catalysis are the limited number of chemical reaction types that are catalyzed by enzymes and the instability of enzymes under harsh conditions in industrial catalysis.Expanding enzyme catalysis to a larger substrate scope and greater variety of chemical reactions and tuning the microenvironment surrounding enzyme molecules to achieve high enzyme performance are urgently needed.In this account,we focus on our efforts using the de novo approach to synthesis hybrid enzyme catalysts that can address these two challenges and the structure-function relationship is discussed to reveal the principles of designing hybrid enzyme catalysts.We hope that this account will promote further efforts toward fundamental research and wide applications of designed enzyme hybrid catalysts for expanding biocatalysis.展开更多
Tricalcium silicate cement(TSC)has been widely used in dental materials because of its self-setting behavior,good bioactivity,biocompatibility,osteoinductivity,and antibacterial effect.Tricalcium silicate(C3S)powder w...Tricalcium silicate cement(TSC)has been widely used in dental materials because of its self-setting behavior,good bioactivity,biocompatibility,osteoinductivity,and antibacterial effect.Tricalcium silicate(C3S)powder was prepared by Pechini technique with a calcining temperature of 1300℃ for 3 h.The influence of liquid/powder(L/P)rate on the setting time and the mechanical property of TSC was studied.Characterization methods including XRD,FTIR,SEM-EDS,TEM,and ICP-AES were utilized to study the properties of C3S powder and its hydrated cement.The bioactivity and biocompatibility of the cement were investigated by soaking test and cell culture,respectively.The results show that the L/P rate plays an important role in the setting time and the compressive strength of TSC.The surface of TSC was covered by hydroxyapatite deposition during the immersion experiment and the cells attachment on the surface of TSC was well,which indicated that TSC has good bioactivity and biocompatibility.In addition,TSC has excellent antibacterial properties against Staphylococcus aureus.In conclusion,TSC is a promising candidate for root canal filling materials.展开更多
In order to broaden the application of wrought Mg alloy sheets in the automotive industry,the influence of Ca and Sm alloying on the texture evolution,mechanical properties,and formability of a hot-rolled Mg-2Zn-0.2Mn...In order to broaden the application of wrought Mg alloy sheets in the automotive industry,the influence of Ca and Sm alloying on the texture evolution,mechanical properties,and formability of a hot-rolled Mg-2Zn-0.2Mn alloy was investigated by OM,XRD,SEM,EBSD,tensile tests,and Erichsen test.The results showed that the average grain size and basal texture intensity of Mg-2Zn-0.2Mn alloys were remarkably decreased after Ca and Sm additions.0.64 wt.%Ca or 0.48 wt.%Sm addition significantly increased the tensile strength,ductility and formability.Moreover,the synergetic addition of Sm and Ca improved the ductility and formability of Mg-2Zn-0.2Mn alloy,which was due to the change of Ca distribution and further reduction of the size of Ca-containing particles by Sm addition.The results provided a possibility of replacing RE elements with Ca and Sm in Mg alloys which bring about outstanding mechanical properties and formability.展开更多
Nanosize cerium-zirconium solid solution(CZO)with a special fluorite structure has received an increasing research interest due to their remarkable advantages such as excellent oxygen storage capacity and great flexib...Nanosize cerium-zirconium solid solution(CZO)with a special fluorite structure has received an increasing research interest due to their remarkable advantages such as excellent oxygen storage capacity and great flexibility in their composition and structure.By partial metal(including rare earth,transition,alkaline earth or other metal)doping into CZO,the physicochemical properties of these catalytic materials can be controllable adjusted for the study of specific reactions.To date,nanosize CZO has been prepared by co-precipitation,sol-gel,surfactant-assisted approach,solution combustion,micro-emulsion,high energy mechanical milling,etc.The advent of these methodologies has prompted researchers to construct well-defined networks with customized micromorphology and functionalities.In this review,we describe not only the basic structure and synthetic strategies of CZO,but also their relevant applications in environmental catalysis,such as the purification for CO,nitrogen oxides(NOx),volatile organic compounds(VOC),soot,hydrocarbon(HC),CO2 and solid particulate matters(PM),and some reaction mechanisms are also summarized.展开更多
At room temperature, the reaction of dibenzoyl peroxide with metallic copper powder in the presence of pyridine affords the copper(Ⅱ) complex [Cu(C 5H 5N) 2(H 2O)\|(C 6H 5COO) 2]. Crystal is monoclinic, M r =483.002,...At room temperature, the reaction of dibenzoyl peroxide with metallic copper powder in the presence of pyridine affords the copper(Ⅱ) complex [Cu(C 5H 5N) 2(H 2O)\|(C 6H 5COO) 2]. Crystal is monoclinic, M r =483.002, space group Cc with parameters: a=6\^078(4), b=15.879(4), c=23.091(3), β=97.61(2)°, V=2209.1(2) 3, Z=4, D c =1\^464g/cm 3, μ =10.279 cm -1 , F(000)=996, R=0\^031, R w =0.036, 1595 reflections with I≥3σ(I ) were considered to be observed. Each copper(Ⅱ) ion is coordinated by two monodentate benzoate ligands, two pyridines and one water molecule. The complex is also characterized by its IR, XPS and thermal properties.展开更多
Converting sunlight directly to fuels and chemicals is a great latent capacity for storing renewable energy.Due to the advantages of large surface area,short diffusion paths for electrons,and more exposed active sites...Converting sunlight directly to fuels and chemicals is a great latent capacity for storing renewable energy.Due to the advantages of large surface area,short diffusion paths for electrons,and more exposed active sites,few‐layer carbon nitride(FLCN)materials present great potential for production of solar fuels and chemicals and set off a new wave of research in the last few years.Herein,the recent progress in synthesis and regulation of FLCN‐based photocatalysts,and their applications in the conversion of sunlight into fuels and chemicals,is summarized.More importantly,the regulation strategies from chemical modification to microstructure control toward the production of solar fuels and chemicals has been deeply analyzed,aiming to inspire critical thinking about the effective approaches for photocatalyst modification rather than developing new materials.At the end,the key scientific challenges and some future trend of FLCN‐based materials as advanced photocatalysts are also discussed.展开更多
Calcium lignosulphonate was used to synthesize a spherical lignosulphonate resin in a cheap and non-toxic disperse medium by reversed phase suspension polymerization. The process conditions were optimized by orthog...Calcium lignosulphonate was used to synthesize a spherical lignosulphonate resin in a cheap and non-toxic disperse medium by reversed phase suspension polymerization. The process conditions were optimized by orthogonal experiments. Under .the optxmal conditxons (T=95 ℃, CHCl= 3 mol·L^-1, mHCHO: mCLS=7%, WCLS=50%), globulation took about 20 min and the product was featured with excellent spherical shape, narrow particle size range, 61.20% of water retention capacity, 0.83 mmol·ml^- 1 of total volume exchange capacity and 3.46 mmol·g^- 1 of total exchange capacity. The results of Scanning Electron Micrograph and Scanning Probe Micrograph indicate that spherical lignosulphonate resin has a rugged surface with porous microstructure in the gel skeleton. The average pore size of dry samples was determined to be 10.46 nm. by the BET method.展开更多
Dimethyl carbonate is an environmentally benign and biodegradable chemical.Based on integration of reactive distillation and pressure-swing distillation technologies,a novel process for synthesis of dimethyl carbonate...Dimethyl carbonate is an environmentally benign and biodegradable chemical.Based on integration of reactive distillation and pressure-swing distillation technologies,a novel process for synthesis of dimethyl carbonate through transesterification with propylene carbonate and methanol has been developed by Huang et al.In this work,the optimization of this process was performed by minimizing the total TAC.The results show that the optimal design flowsheet can save energy consumption by 18.6% with the propylene carbonate conversion of 99.9%.Then,an effective plant-wide control structure for the process was developed.Dynamic simulation results demonstrate that the temperature/flow rate cascade control plus with simple temperature control can keep not only product purity but also the conversion of the reactant at their desired values in the face of the disturbance in reactant feed flow rate and feed composition.展开更多
A series of Co-imbedded zeolite-based catalysts were synthesized following a facile solvent-free grinding route.The catalytic performance for direct syngas conversion to gasoline range hydrocarbons was compared with t...A series of Co-imbedded zeolite-based catalysts were synthesized following a facile solvent-free grinding route.The catalytic performance for direct syngas conversion to gasoline range hydrocarbons was compared with their counterpart Co-impregnated zeolite-based catalysts.Successful transformation of solid raw materials to targeted zeolite was confirmed by XRD,SEM,STEM,and N2 physisorption analysis.An in-depth study of acidic strength and acidic site distribution was conducted by NH3-TPD and Py-IR spectroscopy.Acidic strength showed a pivotal role in defining product range.Co@S1,with the weakest acidic strength of silicalite-1 among three types of zeolites,evaded over-cracking of product and exhibited the highest gasoline and isoparaffin selectivity(≈70%and 30.7%,respectively).Moreover,the solvent-free raw material grinding route for zeolite synthesis accompanies several advantages like the elimination of production of wastewater,high product yield within confined crystallization space,and elimination of safety concerns regarding high pressure due to the absence of the solvent.Facileness and easiness of the solvent-free synthesis route together with promising catalytic performance strongly support its application on the industrial scale.展开更多
The title compound methyl (7,7-dimemyl-2-amino-4-(4-chlorophenyl)-5-oxo-5,6,7,8-tetrahydro-4H-benzo-[b]-pyran-3-yl) carboxylate (C19H20ClNO4, Mr = 361.81) was synthesized and crystallized. The crystal belongs to tricl...The title compound methyl (7,7-dimemyl-2-amino-4-(4-chlorophenyl)-5-oxo-5,6,7,8-tetrahydro-4H-benzo-[b]-pyran-3-yl) carboxylate (C19H20ClNO4, Mr = 361.81) was synthesized and crystallized. The crystal belongs to triclinic, space group P 1 with a = 8.519(2), b = 10.346(2), c = 11.481(3) A, α = 108.16(1), β = 107.78(2), γ= 91.83(2)°, Z = 2, V = 906.5(3) A3, Dc = 1.326 g/cm3, μ(MoKα) = 0.234 mm-1, F(000) = 380, R = 0.0467 and wR = 0.1270 for 3142 observed reflections (I > 2σ(I)). X-ray analysis reveals that the C(7), C(8), C(9), O(1), C(10) and C(11) atoms form a six-membered ring which adopts a boat conformation. In the ring, the distances of C(8)-C(9) and C(10)-C(11) are 1.332(3) and 1.357(3) A, respectively, which indicates that they are C=C double bonds. Another six-membered ring (C(8)-C(9)-C(15)-C(14)-C(13)-C(12)) adopts the half-chair confonnation. In addition, there are intermolecular hydrogen bonds in the crystal structure.展开更多
Anhydrous SmCl 3 reacts with two equal of Li(1,3 tBu 2C 5H 3) to give a complex (1,3 tBu 2C 5H 3) 2Sm( μ Cl) 2Li(THF) 2(C 34 H 58 Cl 2LiO 2Sm, M r =726.99), monoclinic, space group P2 1/n, a=10.615(2), b=21.037(4), c...Anhydrous SmCl 3 reacts with two equal of Li(1,3 tBu 2C 5H 3) to give a complex (1,3 tBu 2C 5H 3) 2Sm( μ Cl) 2Li(THF) 2(C 34 H 58 Cl 2LiO 2Sm, M r =726.99), monoclinic, space group P2 1/n, a=10.615(2), b=21.037(4), c=17.166(3), β=93.60(3)°, V=3825\^7(13) 3, Z=4, D c =1.262Mg/m 3, μ =1.699mm -1 and F (000)=1508, final R= 0.0387 and wR =0.0741 for 5320 observed[ I2σ(I)] reflections. The average Sm-C distance is 2\^73. Sm-Cl1 and Sm-Cl2 distances are 2\^719(2) and 2.697(2), respectively. Two 1,3 tBu 2C 5H 3 ring centroids and two μ 2 bridging chloride atoms around Sm atom form a distorted tetrahedron.展开更多
Photocatalysis driven by near-infrared(NIR)light is of scientific and technological interest for ex-ploiting solar energy.In this study,we demonstrate a facile hydrothermal process to synthesize core-shell nanoparti...Photocatalysis driven by near-infrared(NIR)light is of scientific and technological interest for ex-ploiting solar energy.In this study,we demonstrate a facile hydrothermal process to synthesize core-shell nanoparticles combining upconversion nanoparticles(UCNPs)and alloyed ZnxCwhich can be excited using NIR or visible light.Morphologies,phase,and chemical composition have been investigated using field-emission scanning electron microscopy,transmission electron mi-croscopy,X-ray diffraction analysis,and atomic absorption spectroscopy.Moreover,we found that amorphous TiO2 layers existing in the final samples play an important role in formation ofyolk-shell nanoparticles,which bind the as-prepared ZnxCnanoparticlescan be tuna-ble by adjusting the amount of the Cd and Zn source compounds.The photochemical reduction of Cr(Ⅵ)in water has been performed to study the photocatalytic performance under irradiation by NIR light or a simulated solar light,showing efficient photoreduction and Cr(Ⅵ)removal over the/TiO2 yolk-shell nanoparticles.The as-prepared UCNPs@ZnxC/TiO2 nanoparticles show excellent production of hydroxyl radicals,which are responsible for the photochemical reduction of Cr(Ⅵ)to Cr(Ⅲ).This study will provide an alternative strategy for en-vironmental wastewater treatment,making full use of solar energy.展开更多
A series of novel fluorine-containing acrylates 6a-6g were synthesized via the condensation of ethyl cyanoacetate and trifluoroacetic anhydride, followed by chloridization and the coupling reaction with amines. These ...A series of novel fluorine-containing acrylates 6a-6g were synthesized via the condensation of ethyl cyanoacetate and trifluoroacetic anhydride, followed by chloridization and the coupling reaction with amines. These new compounds exhibited some biological activity as preliminary bioassay indicated. A plausible reaction mechanism was outlined and discussed.展开更多
文摘Aim To synthesize trans and cis-3, 4′, 5-trihydroxystilbene by a new convenient route. Methods The reaction of 3, 5-dimethoxybenzaldehyde (3) and 4-methoxy phenylacetonitrile (4) formed the stilbene skeleton. After hydrolyzation, decarboxylation, and demethylation, we obtained trans-3, 4′, 5-trihydroxystilbene (resveratrol), which can be converted to its cis-isomer by photochemical isomerization. Results Starting from 3 and 4, trans and cis-3, 4′, 5-trihydroxystilbene were synthesized, respectively. Conclusion A facile method for the synthesis of trans and cis-hydroxystilbenes from readily available materials was established.
基金Project(50731002) supported by the National Natural Science Foundation of ChinaProject(20082030) supported by the Natural Science Foundation of Liaoning Province,China
文摘The phase equilibria and compositions in Mg-rich side at 300 ℃ were investigated in Mg-Zn-Ca ternary system through the equilibrated alloy method by using scanning electron microscopy,electron probe microanalysis,X-ray diffraction and transmission electron microscopy.The results show that two ternary compounds T1 and T2 can be in equilibrium with the Mg-based solid solution in Mg-Zn-Ca system.T1 phase is a linear compound with the composition region(molar fraction) of 15% Ca,20.5%-48.9% Zn and balanced Mg at 300 ℃.Its hexagonal structure parameters decrease with increasing Zn content,i.e.a=0.992-0.945 nm,c=1.034-1.003 nm.T2 phase has hexagonal structure with the composition region of 26.4%-28.4% Mg,63.2%-65.5% Zn and 7.1%-8.4% Ca.At 300 ℃,the solubility of Zn in the Mg-based solid solution increases for the addition of Ca,the maximum solubility of Zn is 3.7%.Three-phase fields consisting of--Mg+Mg2Ca+T1,--Mg+T1+T2,--Mg+T2+MgZn and MgZn+T2+Mg2Zn3 exist in the Mg-Zn-Ca system at 300 ℃.
文摘Mesh-like Bi2MoO6 product was successfully synthesized by a hydrothermal method without using any surfactant or template. The pH value played an important role in the formation of this morphology. The as-prepared mesh-like Bi2MoO6 sample exhibited excellent visible-light-driven photocatalytic e ciency. The photocatalytic activity of the mesh-like Bi2MoO6 sample was much higher than that of bulk Bi2MoO6 sample prepared by solid-state reac-tion. Di erence in the photocatalytic activities of the mesh-like Bi2MoO6 sample and bulk Bi2MoO6 sample was further investigated.
文摘To study the antifungal effect of chalcone derivatives. Methods Sixteenchalcone derivatives were synthesized and confirmed by ~1H NMR and IR spectra, and tested forantifungal activity against four common pathogenic fungi. Their structure-activity relationship isdiscussed. Results Among 16 title compounds, there were 5 new compounds, which have not beenreported before. The preliminary antifungal test showed that all title compounds exhibitedantifungal activities to a certain extent. The activity of compound 8 against Trichophyton rubrumhad a potency equal to that of fluconazole, with a MIC of 4 μg·mL^(-1) . Conclusion Sixteenchalcones were prepared and their antifungal activities against four common pathogenic fungi invitro were examined. Some of them exhibited antifungal activities to a certain extent.
基金financially supported by the National Natural Science Foundation of China (21276041)the Program for New Century Excellent Talents in University of Ministry of Education (NCET-12-0079)+1 种基金the Natural Science Foundation of Liaoning Province (2015020200)the Fundamental Research Funds for the Central Universities (DUT15LK41)~~
文摘The textural features and acidic properties of sulfated mesoporous lanthana‐zirconia solid acids (SO42?/meso‐La0.1Zr0.9Oδ) were efficiently tuned by modifying the conditions used to prepare the meso‐La0.1Zr0.9Oδcomposites, such as the molar ratio of the template to La and Zr metal ions (Nt/m), molar ratio of ammonia to La and Zr metal ions (Na/m), hydrothermal temperature (Thydro), and hy‐drothermal time (thydro). The effect of the textural features and acidic properties on the catalytic performance of solid acid catalysts for alkenylation of p‐xylene with phenylacetylene was investi‐gated. Various characterization techniques such as N2 physisorption, X‐ray diffraction, NH3 temper‐ature‐programmed desorption, and thermogravimetric analysis were employed to reveal the rela‐tionship between the nature of catalyst and its catalytic performance. It was found that the catalytic performance significantly depended on the textural features and acidic properties, which were strongly affected by preparation conditions of the meso‐La0.1Zr0.9Oδcomposite. Appropriate acidic sites and high accessibility were required to obtain satisfactory catalytic reactions for this reaction. It was also found that the average crystallite size of t‐ZrO2 affected by the preparation conditions had significant influence on the ultrastrong acidic sites of the catalysts. The optimized SO42?/meso‐La0.1Zr0.9Oδcatalyst exhibited much superior catalytic activity and coke‐resistant stabil‐ity. Moreover, the developed SO42?/meso‐La0.1Zr0.9Oδcatalyst demonstrated excellent catalytic per‐formance for alkenylation of diverse aromatics with phenylacetylene to their correspondingα‐arylstyrenes. Combining the previously established complete regeneration of used catalysts by a facile calcination process with the improved catalytic properties, the developed SO42?/meso‐La0.1Zr0.9Oδ solid acid could be a potential catalyst for industrial production ofα‐arylstyrenes through clean and atom efficient solid‐acid‐mediated Friedel‐Crafts alkenylation of diverse aromatics with phenylacetylene.
文摘The two major challenges in industrial enzymatic catalysis are the limited number of chemical reaction types that are catalyzed by enzymes and the instability of enzymes under harsh conditions in industrial catalysis.Expanding enzyme catalysis to a larger substrate scope and greater variety of chemical reactions and tuning the microenvironment surrounding enzyme molecules to achieve high enzyme performance are urgently needed.In this account,we focus on our efforts using the de novo approach to synthesis hybrid enzyme catalysts that can address these two challenges and the structure-function relationship is discussed to reveal the principles of designing hybrid enzyme catalysts.We hope that this account will promote further efforts toward fundamental research and wide applications of designed enzyme hybrid catalysts for expanding biocatalysis.
基金Project(2019JJ50797)supported by Hunan Provincial Natural Science Foundation of China。
文摘Tricalcium silicate cement(TSC)has been widely used in dental materials because of its self-setting behavior,good bioactivity,biocompatibility,osteoinductivity,and antibacterial effect.Tricalcium silicate(C3S)powder was prepared by Pechini technique with a calcining temperature of 1300℃ for 3 h.The influence of liquid/powder(L/P)rate on the setting time and the mechanical property of TSC was studied.Characterization methods including XRD,FTIR,SEM-EDS,TEM,and ICP-AES were utilized to study the properties of C3S powder and its hydrated cement.The bioactivity and biocompatibility of the cement were investigated by soaking test and cell culture,respectively.The results show that the L/P rate plays an important role in the setting time and the compressive strength of TSC.The surface of TSC was covered by hydroxyapatite deposition during the immersion experiment and the cells attachment on the surface of TSC was well,which indicated that TSC has good bioactivity and biocompatibility.In addition,TSC has excellent antibacterial properties against Staphylococcus aureus.In conclusion,TSC is a promising candidate for root canal filling materials.
基金financially supported by the National Key Research and Development Program of China(Nos.2018YFA0702903,2016YFB0701204)the Fundamental Research Funds for the Central Universities,China(No.DUT20GF102)。
文摘In order to broaden the application of wrought Mg alloy sheets in the automotive industry,the influence of Ca and Sm alloying on the texture evolution,mechanical properties,and formability of a hot-rolled Mg-2Zn-0.2Mn alloy was investigated by OM,XRD,SEM,EBSD,tensile tests,and Erichsen test.The results showed that the average grain size and basal texture intensity of Mg-2Zn-0.2Mn alloys were remarkably decreased after Ca and Sm additions.0.64 wt.%Ca or 0.48 wt.%Sm addition significantly increased the tensile strength,ductility and formability.Moreover,the synergetic addition of Sm and Ca improved the ductility and formability of Mg-2Zn-0.2Mn alloy,which was due to the change of Ca distribution and further reduction of the size of Ca-containing particles by Sm addition.The results provided a possibility of replacing RE elements with Ca and Sm in Mg alloys which bring about outstanding mechanical properties and formability.
基金financially supported by the National Natural Science Foundation of China (21673290, U1662103)~~
文摘Nanosize cerium-zirconium solid solution(CZO)with a special fluorite structure has received an increasing research interest due to their remarkable advantages such as excellent oxygen storage capacity and great flexibility in their composition and structure.By partial metal(including rare earth,transition,alkaline earth or other metal)doping into CZO,the physicochemical properties of these catalytic materials can be controllable adjusted for the study of specific reactions.To date,nanosize CZO has been prepared by co-precipitation,sol-gel,surfactant-assisted approach,solution combustion,micro-emulsion,high energy mechanical milling,etc.The advent of these methodologies has prompted researchers to construct well-defined networks with customized micromorphology and functionalities.In this review,we describe not only the basic structure and synthetic strategies of CZO,but also their relevant applications in environmental catalysis,such as the purification for CO,nitrogen oxides(NOx),volatile organic compounds(VOC),soot,hydrocarbon(HC),CO2 and solid particulate matters(PM),and some reaction mechanisms are also summarized.
文摘At room temperature, the reaction of dibenzoyl peroxide with metallic copper powder in the presence of pyridine affords the copper(Ⅱ) complex [Cu(C 5H 5N) 2(H 2O)\|(C 6H 5COO) 2]. Crystal is monoclinic, M r =483.002, space group Cc with parameters: a=6\^078(4), b=15.879(4), c=23.091(3), β=97.61(2)°, V=2209.1(2) 3, Z=4, D c =1\^464g/cm 3, μ =10.279 cm -1 , F(000)=996, R=0\^031, R w =0.036, 1595 reflections with I≥3σ(I ) were considered to be observed. Each copper(Ⅱ) ion is coordinated by two monodentate benzoate ligands, two pyridines and one water molecule. The complex is also characterized by its IR, XPS and thermal properties.
文摘Converting sunlight directly to fuels and chemicals is a great latent capacity for storing renewable energy.Due to the advantages of large surface area,short diffusion paths for electrons,and more exposed active sites,few‐layer carbon nitride(FLCN)materials present great potential for production of solar fuels and chemicals and set off a new wave of research in the last few years.Herein,the recent progress in synthesis and regulation of FLCN‐based photocatalysts,and their applications in the conversion of sunlight into fuels and chemicals,is summarized.More importantly,the regulation strategies from chemical modification to microstructure control toward the production of solar fuels and chemicals has been deeply analyzed,aiming to inspire critical thinking about the effective approaches for photocatalyst modification rather than developing new materials.At the end,the key scientific challenges and some future trend of FLCN‐based materials as advanced photocatalysts are also discussed.
基金the Ph.D. Programs Foundation of Ministry of Education of China (20020561001)
文摘Calcium lignosulphonate was used to synthesize a spherical lignosulphonate resin in a cheap and non-toxic disperse medium by reversed phase suspension polymerization. The process conditions were optimized by orthogonal experiments. Under .the optxmal conditxons (T=95 ℃, CHCl= 3 mol·L^-1, mHCHO: mCLS=7%, WCLS=50%), globulation took about 20 min and the product was featured with excellent spherical shape, narrow particle size range, 61.20% of water retention capacity, 0.83 mmol·ml^- 1 of total volume exchange capacity and 3.46 mmol·g^- 1 of total exchange capacity. The results of Scanning Electron Micrograph and Scanning Probe Micrograph indicate that spherical lignosulphonate resin has a rugged surface with porous microstructure in the gel skeleton. The average pore size of dry samples was determined to be 10.46 nm. by the BET method.
基金Supported by the National Natural Science Foundation of China(21306025,21576053)the International Science&Technology Cooperation Program of China(2013DFR90540)
文摘Dimethyl carbonate is an environmentally benign and biodegradable chemical.Based on integration of reactive distillation and pressure-swing distillation technologies,a novel process for synthesis of dimethyl carbonate through transesterification with propylene carbonate and methanol has been developed by Huang et al.In this work,the optimization of this process was performed by minimizing the total TAC.The results show that the optimal design flowsheet can save energy consumption by 18.6% with the propylene carbonate conversion of 99.9%.Then,an effective plant-wide control structure for the process was developed.Dynamic simulation results demonstrate that the temperature/flow rate cascade control plus with simple temperature control can keep not only product purity but also the conversion of the reactant at their desired values in the face of the disturbance in reactant feed flow rate and feed composition.
基金the financial support from the Zhejiang Province Natural Science Foundation(LY19B060001)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(2018-K25)the Foundation of Zhejiang University of Science and Technology(2019QN18,2019QN23)~~
文摘A series of Co-imbedded zeolite-based catalysts were synthesized following a facile solvent-free grinding route.The catalytic performance for direct syngas conversion to gasoline range hydrocarbons was compared with their counterpart Co-impregnated zeolite-based catalysts.Successful transformation of solid raw materials to targeted zeolite was confirmed by XRD,SEM,STEM,and N2 physisorption analysis.An in-depth study of acidic strength and acidic site distribution was conducted by NH3-TPD and Py-IR spectroscopy.Acidic strength showed a pivotal role in defining product range.Co@S1,with the weakest acidic strength of silicalite-1 among three types of zeolites,evaded over-cracking of product and exhibited the highest gasoline and isoparaffin selectivity(≈70%and 30.7%,respectively).Moreover,the solvent-free raw material grinding route for zeolite synthesis accompanies several advantages like the elimination of production of wastewater,high product yield within confined crystallization space,and elimination of safety concerns regarding high pressure due to the absence of the solvent.Facileness and easiness of the solvent-free synthesis route together with promising catalytic performance strongly support its application on the industrial scale.
基金This work was supported by the foundation of the "Surpassing Project" of Jiangsu province
文摘The title compound methyl (7,7-dimemyl-2-amino-4-(4-chlorophenyl)-5-oxo-5,6,7,8-tetrahydro-4H-benzo-[b]-pyran-3-yl) carboxylate (C19H20ClNO4, Mr = 361.81) was synthesized and crystallized. The crystal belongs to triclinic, space group P 1 with a = 8.519(2), b = 10.346(2), c = 11.481(3) A, α = 108.16(1), β = 107.78(2), γ= 91.83(2)°, Z = 2, V = 906.5(3) A3, Dc = 1.326 g/cm3, μ(MoKα) = 0.234 mm-1, F(000) = 380, R = 0.0467 and wR = 0.1270 for 3142 observed reflections (I > 2σ(I)). X-ray analysis reveals that the C(7), C(8), C(9), O(1), C(10) and C(11) atoms form a six-membered ring which adopts a boat conformation. In the ring, the distances of C(8)-C(9) and C(10)-C(11) are 1.332(3) and 1.357(3) A, respectively, which indicates that they are C=C double bonds. Another six-membered ring (C(8)-C(9)-C(15)-C(14)-C(13)-C(12)) adopts the half-chair confonnation. In addition, there are intermolecular hydrogen bonds in the crystal structure.
文摘Anhydrous SmCl 3 reacts with two equal of Li(1,3 tBu 2C 5H 3) to give a complex (1,3 tBu 2C 5H 3) 2Sm( μ Cl) 2Li(THF) 2(C 34 H 58 Cl 2LiO 2Sm, M r =726.99), monoclinic, space group P2 1/n, a=10.615(2), b=21.037(4), c=17.166(3), β=93.60(3)°, V=3825\^7(13) 3, Z=4, D c =1.262Mg/m 3, μ =1.699mm -1 and F (000)=1508, final R= 0.0387 and wR =0.0741 for 5320 observed[ I2σ(I)] reflections. The average Sm-C distance is 2\^73. Sm-Cl1 and Sm-Cl2 distances are 2\^719(2) and 2.697(2), respectively. Two 1,3 tBu 2C 5H 3 ring centroids and two μ 2 bridging chloride atoms around Sm atom form a distorted tetrahedron.
基金supported by the National Natural Science Foundation of China (21471043, 51603059, 31501576)~~
文摘Photocatalysis driven by near-infrared(NIR)light is of scientific and technological interest for ex-ploiting solar energy.In this study,we demonstrate a facile hydrothermal process to synthesize core-shell nanoparticles combining upconversion nanoparticles(UCNPs)and alloyed ZnxCwhich can be excited using NIR or visible light.Morphologies,phase,and chemical composition have been investigated using field-emission scanning electron microscopy,transmission electron mi-croscopy,X-ray diffraction analysis,and atomic absorption spectroscopy.Moreover,we found that amorphous TiO2 layers existing in the final samples play an important role in formation ofyolk-shell nanoparticles,which bind the as-prepared ZnxCnanoparticlescan be tuna-ble by adjusting the amount of the Cd and Zn source compounds.The photochemical reduction of Cr(Ⅵ)in water has been performed to study the photocatalytic performance under irradiation by NIR light or a simulated solar light,showing efficient photoreduction and Cr(Ⅵ)removal over the/TiO2 yolk-shell nanoparticles.The as-prepared UCNPs@ZnxC/TiO2 nanoparticles show excellent production of hydroxyl radicals,which are responsible for the photochemical reduction of Cr(Ⅵ)to Cr(Ⅲ).This study will provide an alternative strategy for en-vironmental wastewater treatment,making full use of solar energy.
基金The project supported by the National Natural Science Foundation of China(No.2017203 1)the Chinese Research Fund for the Doctoral Pr ogram of High Education.
文摘A series of novel fluorine-containing acrylates 6a-6g were synthesized via the condensation of ethyl cyanoacetate and trifluoroacetic anhydride, followed by chloridization and the coupling reaction with amines. These new compounds exhibited some biological activity as preliminary bioassay indicated. A plausible reaction mechanism was outlined and discussed.