A green protocol for the synthesis of quinoxalines has been developed from catalytic oxidative cyclization of deoxybenzoins with 1,2-phenylenediamines in water.The optimal conditions are involved in the use of a water...A green protocol for the synthesis of quinoxalines has been developed from catalytic oxidative cyclization of deoxybenzoins with 1,2-phenylenediamines in water.The optimal conditions are involved in the use of a water-soluble mononuclear copper(Ⅱ) complex of a zwitterionic calix[4]arene[Cu(Ⅱ)LCH2O)]I2(1,H4L=[5,ll,17,23-tetrakis(trimethylammonium)-25,26,27,28-tetrahydroxycalix[4]arene]) as a catalyst in alkali solution after refluxing for 15 h in O2.The target quinoxaline and its derivatives were obtained in good yields(up to 88%).The procedure described in this paper is simple,practical and environmentally benign.展开更多
Small-crystal TS-1 was synthesized via a seed-induced approach using ammonia as the alkali source and tetrapropylammonium bromide as an auxiliary structure-directing agent. The TS-1 samples were characterized using X-...Small-crystal TS-1 was synthesized via a seed-induced approach using ammonia as the alkali source and tetrapropylammonium bromide as an auxiliary structure-directing agent. The TS-1 samples were characterized using X-ray diffraction, N2 adsorption-desorption, Fourier-transform infrared spectroscopy, inductively coupled plasma atomic emission spectroscopy, scanning electron microscopy, and ultraviolet-visible spectroscopy. The use of the colloidal seed reduced the crystal size, and an appropriate amount of silicalite-1 seed assisted Ti incorporation into the TS-1 framework. This method reduces the cost of TS- 1 synthesis because a significantly smaller amount of tetrapropylammonium hydroxide is used. The catalytic performance of the synthesized small-crystal TS-1 samples in cyclohexanone ammoximation was better than that of bulk TS-1 as a result of improved diffusion and a larger number of active tetrahedral Ti centers.展开更多
Birnessite-type MnO2 (δ-MnO2) nano-sheets were successfully synthesized by an interracial synthesis method in this work. The properties and electrochemical performance of the as-prepared δ-MnO2 were analyzed and e...Birnessite-type MnO2 (δ-MnO2) nano-sheets were successfully synthesized by an interracial synthesis method in this work. The properties and electrochemical performance of the as-prepared δ-MnO2 were analyzed and evaluated by scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption measurement and electrochemical tests. This facile synthesis method enables δ-MnO2 nanosheets to show a large specific surface area (257.5 m^2 g^-1). The electrochemical test results show that the specific capacitance is 272 F g^-1 and the specific capacitance retention is over 96.7% after 1000 cycles at a scan rate of 10 mV s^-1. All results demonstrate that δ-MnO2 has a great potential application in high- performance electrochemical capacitors, and this interracial synthesis method will be a very promising method to synthesize highly active MnO2 materials in a large scale.展开更多
A series of MgAl-layered double oxides(LDO) doped with different rare-earth elements(Y, La, and Ce)were synthesized by the calcination of Mg-Al layered double hydroxides, and Ru, which were used to prepare ammonia...A series of MgAl-layered double oxides(LDO) doped with different rare-earth elements(Y, La, and Ce)were synthesized by the calcination of Mg-Al layered double hydroxides, and Ru, which were used to prepare ammonia synthesis catalysts. The as-obtained oxides and catalysts were characterized by XRD,TEM, TPD, TPR and XPS to understand their catalytic performances in ammonia synthesis. The H_2-TPR and HRTEM studies reveal that Ru/Y-LDO catalyst possesses more active Ru metal and small particle size.The XPS demonstrates that the electronic interaction between Y and Ru metals is stronger, which can be tentatively explained by most of Y inserted into the hydrotalcites structure. CO_2-TPD demonstrates that Ru/Y-LDO catalyst shows stronger basic site densities than catalysts doped with Ce and La. Higher activity of the Ru/Y-LDO catalyst can be attributed to smaller particle size, more active metal(Ru) and strong Ru-support interaction.展开更多
A nitrogen-doped titanium dioxide composite photocatalyst(N–TiO2) with heterojunction structures is synthesized by three different approaches: a novel UV-assisted thermal synthesis, annealing, and microwave techni...A nitrogen-doped titanium dioxide composite photocatalyst(N–TiO2) with heterojunction structures is synthesized by three different approaches: a novel UV-assisted thermal synthesis, annealing, and microwave technique. Photocatalytic activities of synthesized photocatalysts are evaluated by the degradation of Methyl Orange under ultraviolet light types A(UV-A), B(UV-B), and C(UV-C), visible light, and direct sunlight irradiation. Results show that by using N–TiO_2 photocatalyst prepared by the UV-assisted thermal synthesis and annealing, the degradation increases by 16.5% and 20.4%, respectively, compared to that by bare TiO2. The best results are obtained at a nitrogen to TiO2 mass ratio of 0.15(N:TiO2). The enhancement of the photocatalytic activity observed in the visible range is mainly attributed to the increasing separation rate of photogenerated charge carriers. The novel UV-assisted thermal synthesis has produced encouraging results as a preparation method for the nitrogen-doped TiO2 photocatalyst; thus, further studies are recommended for process optimization, immobilization, and scale-up to evaluate its applicability in wastewater treatment.展开更多
Transition metal cation ordering is essential for controlling the electrochemical performance of cubic spinel LiNi_(0.5)Mn_(1.5)O_(4)(LNMO),which is conventionally adjusted by optimizing the high temperature sintering...Transition metal cation ordering is essential for controlling the electrochemical performance of cubic spinel LiNi_(0.5)Mn_(1.5)O_(4)(LNMO),which is conventionally adjusted by optimizing the high temperature sintering and annealing procedures.In this present work,multiple characterization techniques,including 6,7Li NMR,XRD and HRTEM,have been combined to trace the phase transformation and morphology evolution during synthesis.It has been illustrated that simultaneous formation of LiMn_(2)O_(4)(LMO)and LiNiO_(2)(LNO)binary oxides and their conversion into highly reactive LixNi^(3+)_(y)Mn_(3.5+)_(z)O ternary intermediate is a thermal dynamically difficult but crucial step in the synthesis of LNMO ternary oxide.A new strategy of modifying the intermediates formation pathway from binary mode to ternary mode using thermal regulating agent has been adopted.LNMO synthesized with thermal regulating agent exhibits supreme rate capability,long-cycling performance(even at elevated temperature)and excellent capacity efficiency.At a high rate of 100 C,the assembled battery delivers a discharge capacity of 99 mAh g^(-1).This study provides a way to control the formation pathway of complex oxides using thermal regulating agent.展开更多
The use of nanostructured composites as catalyst supports is a promising route to prepare catalysts with high selectivity and productivity. In this work, reduced graphene oxide-TiO_2(rGP-x) composites with a variation...The use of nanostructured composites as catalyst supports is a promising route to prepare catalysts with high selectivity and productivity. In this work, reduced graphene oxide-TiO_2(rGP-x) composites with a variation of reduced graphene oxide(rGO) content were synthesized by hydrothermal method. Pd/rGP-x catalysts were prepared in incipient-wetness impregnation method for the direct synthesis of H_2O_2 from H2 and O_2. The morphology and electronic properties of catalysts were investigated by XPS, TEM, and Raman spectroscopy.The ratio of Pd^(2+)/Pd^0 and the hydrophobicity of the catalysts were increased with the rising content of rGO. As the amount of rGO in the catalysts varied in the range of 0.025 wt%–2 wt%, the selectivity of H_2O_2 exhibited a tendency of increasing firstly and then decreasing from 0.1 wt% to 2 wt%. It indicates that good catalytic performance for H_2O_2 synthesis can be achieved only when appropriate amount of rGO is introduced. The H_2O_2 selectivity and productivity of Pd/r GP-0.025 both improved remarkably compared with Pd/P25. This enhancement originated from the combined effects of the proper ratio of Pd^(2+)/Pd^0 and hydrophobicity of the catalyst.展开更多
A simple ultrasound-assisted co-precipitation method was developed to prepare ferroferric oxide/graphene oxide magnetic nanoparticles(Fe_3O_4/CO MNPs).The hysteresis loop of Fe_3O_4/GO MNPs demonstrated that the sampl...A simple ultrasound-assisted co-precipitation method was developed to prepare ferroferric oxide/graphene oxide magnetic nanoparticles(Fe_3O_4/CO MNPs).The hysteresis loop of Fe_3O_4/GO MNPs demonstrated that the sample was typical of superparamagnetic material.The samples were characterized by transmission electron microscope,and it is found that the particles are of small size.The Fe_3O_4/GO MNPs were further used as an adsorbent to remove Rhodamine B.The effects of initial pH of the solution,the dosage of adsorbent,temperature,contact time and the presence of interfering dyes on adsorption performance were investigated as well.The adsorption equilibrium and kinetics data were fitted well with the Freundlich isotherm and the pseudosecond-order kinetic model respectively.The adsorption process followed intra-particle diffusion model with more than one process affecting the adsorption of Rhodamine B.And the adsorption process was endothermic in nature.Furthermore,the magnetic composite with a high adsorption capacity of Rhodamine B could be effectively and simply separated using an external magnetic field.And the used particles could be regenerated and recycled easily.The magnetic composite could find potential applications for the removal of dye pollutants.展开更多
Two types of alumina dispersion-strengthened copper(ADSC) alloys were fabricated by a novel in-situ reactive synthesis(IRS) and a traditional internal oxidation(IO) process. The features of alumina dispersoids i...Two types of alumina dispersion-strengthened copper(ADSC) alloys were fabricated by a novel in-situ reactive synthesis(IRS) and a traditional internal oxidation(IO) process. The features of alumina dispersoids in these ADSC alloys were investigated by X-ray diffraction, scanning electron microscopy, and high-resolution transmission electron microscopy. It is found that nano-sized γ-Al2O3 particles of approximately 10 nm in diameter are homogeneously distributed in the IRS-ADSC composites. Meanwhile, larger-sized, mixed crystal structure alumina with rod-shaped morphology is embedded in the IO-ADSC alloy. The IRS-ADSC composites can obtain better mechanical and physical properties than the IO-ADSC composites; the tensile strength of the IRS-ADSC alloy can reach 570 MPa at room temperature, its electrical conductivity is 85% IACS, and the Rockwell hardness can reach 86 HRB.展开更多
Microflowers made of interconnected MnO2 nanosheets have been successfully synthesized in a microwave reactor through a hydrothermal reduction of KMnO4 with aqueous HCI at elevated temperatures in the presence of supe...Microflowers made of interconnected MnO2 nanosheets have been successfully synthesized in a microwave reactor through a hydrothermal reduction of KMnO4 with aqueous HCI at elevated temperatures in the presence of superparamagnetic Fe3O4SiO2 core-shell nanoparticles.Due to the chemical compatibility between SiO2 and MnO2,the heterogeneous reaction leads to the spontaneous encapsulation of the Fe3O4@SiO2 core-shell nanoparticles in the MnO2 microflowers.The resulting hybrid particles exhibit multiple properties including high surface area associated with the MnO2nanosheets and superparamagnetism originated from the Fe3O4@SiO2 core-shell nanoparticles.which are beneficial for applications requiring both high surface area and magnetic separation.展开更多
Surface self-magnetization of siderite is achieved by generating ferromagnetic substance on the surface of siderite by adjusting slurry temperature,pH value,stirring rate and reaction time.No addition of any iron-cont...Surface self-magnetization of siderite is achieved by generating ferromagnetic substance on the surface of siderite by adjusting slurry temperature,pH value,stirring rate and reaction time.No addition of any iron-containing reagent is required.The temperature of 60 ℃,NaOH concentration of 0.10 mol/L;stirring rate of 900 r/min and the reaction time of 10 min are the optimal conditions.The results show that the siderite recovery in magnetic separation increased from 26.9% to 88.8% after surface magnetization.Magnetization kinetic equation is expressed as 1 [1(e0.269)]1/3 = Kt.Activation energy for the magnetization reaction is 4.30 kJ/mol.VSM,SEM and XPS were used to characterize the siderite,and results show that the saturated magnetization(rs) of siderite increased from 0.652 to 2.569Am2 /kg,the magnetic hysteresis was detected with a coercive force of 0.976 A/m after magnetization;Fe2P3/2 electron binding energy changed which reflects the valence alteration in iron on the surface and the formation of ferromagnetic Fe3O4.展开更多
An efficient method was developed for chlorination of aromatic compounds with electron-donating groups using iodobenzene as the catalyst and m-chloroperbenzoic acid as the terminal oxidant in the presence of 4-methylb...An efficient method was developed for chlorination of aromatic compounds with electron-donating groups using iodobenzene as the catalyst and m-chloroperbenzoic acid as the terminal oxidant in the presence of 4-methylbenzenesulfonic acid in THF at room temperature for 24 h,and a series of the monochlorinated compounds was obtained in good yields.In this protocol,the catalyst iodobenzene was first oxidized into the hypervalent iodine intermediate,which then treated with lithium chloride and finally reacted with aromatic compounds to form the chlorinated compounds.展开更多
Rational designing and controlling of nanostructures is a key factor in realizing appropriate properties required for the high-performance energy fields. In the present study, hollow Sn O2@C nanoparticles(NPs) with ...Rational designing and controlling of nanostructures is a key factor in realizing appropriate properties required for the high-performance energy fields. In the present study, hollow Sn O2@C nanoparticles(NPs) with a mean size of 50 nm have been synthesized in large-scale via a facile hydrothermal approach.The morphology and composition of as-obtained products were studied by various characterized techniques. As an anode material for lithium ion batteries(LIBs), the as-prepared hollow Sn O2@C NPs exhibit significant improvement in cycle performances. The discharge capacity of lithium battery is as high as 370 m Ah g 1, and the current density is 3910 m A g 1(5 C) after 573 cycles. Furthermore, the capacity recovers up to 1100 m Ah g 1at the rate performances in which the current density is recovered to 156.4 m A g 1(0.2 C). Undoubtedly, sub-100 nm Sn O2@C NPs provide significant improvement to the electrochemical performance of LIBs as superior-anode nanomaterials, and this carbon coating strategy can pave the way for developing high-performance LIBs.展开更多
ZnO nanoparticles(ZnO NPs) were synthesized by chemical method(coprecipitation) and biological method using aqueous extracts of garlic(Allium sativum),rosemary(Rosmarinus officinalis) and basil(Ocimum basili...ZnO nanoparticles(ZnO NPs) were synthesized by chemical method(coprecipitation) and biological method using aqueous extracts of garlic(Allium sativum),rosemary(Rosmarinus officinalis) and basil(Ocimum basilicum).The influence of plant extract on the antibacterial and antioxidant activities of green synthesized nanoparticles was investigated.The X-ray diffraction studies reveal that all ZnO samples have hexagonal wurtzite structure.The particle size of ZnO NPs estimated by transmission electron microscopy analysis(between 14 and 27 nm) varies depending on the synthesis method of nanoparticles and the type of extracts from the plants used.The functional groups involved in the biosynthetic procedure were evidenced by Fourier transform infrared spectroscopy.The presence of Mn^(2+)ions,Zn vacancy complexes and oxygen vacancies in ZnO samples was highlighted by electron paramagnetic resonance spectroscopy.The green synthesized ZnO NPs have shown a good bactericidal activity against Staphylococcus aureus,Bacillus subtilis,Listeria monocytogenes,Escherichia coli,Salmonella typhimurium and Pseudomonas aeruginosa bacterial strains.ZnO NPs synthesized using extracts of the selected plant species have been found to exhibit more enhanced antibacterial and antioxidant activities as compared to chemical ZnO NPs.展开更多
The effect of cerous nitrate on activity of NOS and expression of iNOS in rat hepatocyte was studied by means of reverse transcription - polymerase chain reaction ( RT-PCR). The result shows that neither high ( 50 mg....The effect of cerous nitrate on activity of NOS and expression of iNOS in rat hepatocyte was studied by means of reverse transcription - polymerase chain reaction ( RT-PCR). The result shows that neither high ( 50 mg.kg(-1)) nor low( 1 mg.kg(-1)) dose of cerous nitrate can induce the increase of expression of iNOS mRNA, but an increase of activity was observed after administration of cerous nitrate. Possible mechanism for these phenomena was discussed.展开更多
Acicular goethite(a-Fe OOH) and worm-like maghamite(γ-Fe2O3) nanostructures have been prepared adopting a novel route, using Na2[Fe(HL)2(H2O)2] chelate complex in alkaline medium. It is found that concentrati...Acicular goethite(a-Fe OOH) and worm-like maghamite(γ-Fe2O3) nanostructures have been prepared adopting a novel route, using Na2[Fe(HL)2(H2O)2] chelate complex in alkaline medium. It is found that concentration of hydrated Fe(III) ions increased with increasing temperature, which later play a key role in generation of different phases of iron oxide. Phase and morphology of the products are investigated using XRD, FTIR, SEM, and TEM analysis. Using UV–Vis spectra, various electronic transitions of goethite and maghamite particles are examined. Maghamite nanostructures exhibit superparamagnetic property at room temperature. On the basis of experimental observations and analytical data, growth mechanism of the nanostructures is discussed.展开更多
Two europium oxide/sulfide silicates, Eu2O(SiO4) (1) and Eu5S(SiO4)3 (2), have been synthesized using high-temperature solid-state reactions. 1 crystallizes in the monoclinic space group P21/c with a = 9.1459...Two europium oxide/sulfide silicates, Eu2O(SiO4) (1) and Eu5S(SiO4)3 (2), have been synthesized using high-temperature solid-state reactions. 1 crystallizes in the monoclinic space group P21/c with a = 9.1459(7), b = 7.1280(5), c = 6.7655(5) ? and ? = 107.611(2), belonging to the Gd2O(SiO4) structure type; 2 crystallizes in space group P63/m of the hexagonal system with a = 9.786(4) and c = 6.789(3) , belonging to the apatite Ca5Cl(PO4)3 structure type. The structure chemistry of related RE2O(SiO4) and RE5S(SiO4)3 compounds is also discussed. The optical energy gap of 2 is determined to be 2.05 eV.展开更多
To assess the role of oxidative metabolism and nitric oxide synthesis for elucid a ting their pathophysiological mechanisms in a Tibetan patient with essential hyp ertension Methods The serum levels of total supero...To assess the role of oxidative metabolism and nitric oxide synthesis for elucid a ting their pathophysiological mechanisms in a Tibetan patient with essential hyp ertension Methods The serum levels of total superoxide dismutase (T SOD), malondialdehyde (MDA), total antioxidant capacity (T AOC), nitric oxide (NO) and nitric oxide synthase (NOS) were assayed in sixty native Tibetans (thirty hypertensive patients and t hirty healthy volunteers as control) Results The levels of T SOD, T AOC, NO and NOS were significantly lower in the patien t group than in the control group ( P <0 01); MDA was significantly higher in the patient group than in the control group ( P <0 01) The level of MDA ha d a strong negative correlation with T SOD, T AOC, NO and NOS ( r =-0 82, -0 76, -0 79, -0 73, respectively, P <0 001 for all) Conclusion Tibetan patients with essential hypertension (EH) may have underlying oxidative metabolism dysfunction and depressed NO synthesis, both responsible for the hype rtensive process展开更多
The aim of this study is to investigate the effects of nitric oxide, formed from L-arginine, on the production of endothelin?1 in vivo and in cultured endothelial cells. In mechanically ventilated anesthetized dogs (n...The aim of this study is to investigate the effects of nitric oxide, formed from L-arginine, on the production of endothelin?1 in vivo and in cultured endothelial cells. In mechanically ventilated anesthetized dogs (n = 5), mean pulmonary arterial pressure (PAPm) and pulmonary vascular resistance (PVR) during hypoxic ventilation (FIO2 = 0.10) was 25 ?3.1 kPa and 68.7 ?10.2 kPa.s / L respectively. IG-nitro-L-arginine methylester (L-NAME), an inhibitor of nitric oxide synthase, increased the peak value of PAPm and PVR during hypoxic ventilation to 36.6 ?4.7 kPa and 158.4 ?25 kPa.s / L and its effect lasted for 2-3 hours. Meanwhile, plasma endothelin? level in the femoral artery increased by 20.9+ 7.1, 25.6?7.7, 28.6?7.9 pg / ml at the 60 th, 120th, 180th minute after the injection of L-NAME respectively (P<0.05 vs hypoxic control before the injection). In cultured endothelial cells from umbilical veins, endothelin-1 level of culture medium in control group was 35.1 ?.9 pg / 105 cells /ml (n=9). L-NAME increased endothelin-1 level to 42.8 ?4.9pg / 105 cells / ml (n = 9, P < 0.05) in case of 10-11 mol / L and to 43.0+ 4.7 pg / 105 cells / ml in case of 10 -7 mol/L (n=9, F<0.05). These findings indicate that endogenous nitric oxide is an inhibitory modulator of hypoxic pulmonary vasoconstriction and that nitric oxide inhibits the production of endothelin? in vivo and in cultured vascular endothelial cells.展开更多
基金the financial supports from the National Natural Science Foundation of China(Nos.21271134, 21373142,21531006 and 21671144)the State Key Laboratory of Organometallic Chemistry,Shanghai Institute of Organic Chemistry(No.2015kf-07)+2 种基金supports from the "333" Project of Jiangsu Provincethe Priority Academic Program Development of Jiangsu Higher Education Institutionsthe "SooChow Scholar" Program of Soochow University
文摘A green protocol for the synthesis of quinoxalines has been developed from catalytic oxidative cyclization of deoxybenzoins with 1,2-phenylenediamines in water.The optimal conditions are involved in the use of a water-soluble mononuclear copper(Ⅱ) complex of a zwitterionic calix[4]arene[Cu(Ⅱ)LCH2O)]I2(1,H4L=[5,ll,17,23-tetrakis(trimethylammonium)-25,26,27,28-tetrahydroxycalix[4]arene]) as a catalyst in alkali solution after refluxing for 15 h in O2.The target quinoxaline and its derivatives were obtained in good yields(up to 88%).The procedure described in this paper is simple,practical and environmentally benign.
基金supported by the National Natural Science Foundation of China(21403070 and 21373088)Innovation Program of Shanghai Municipal Education Commission(13zz038)+2 种基金Key Project of the Shanghai Committee of Science and Technology(12JC1403600)National Key Technology R&D Program(2012BAE05B02)Shanghai Leading Academic Discipline Project(B409)~~
文摘Small-crystal TS-1 was synthesized via a seed-induced approach using ammonia as the alkali source and tetrapropylammonium bromide as an auxiliary structure-directing agent. The TS-1 samples were characterized using X-ray diffraction, N2 adsorption-desorption, Fourier-transform infrared spectroscopy, inductively coupled plasma atomic emission spectroscopy, scanning electron microscopy, and ultraviolet-visible spectroscopy. The use of the colloidal seed reduced the crystal size, and an appropriate amount of silicalite-1 seed assisted Ti incorporation into the TS-1 framework. This method reduces the cost of TS- 1 synthesis because a significantly smaller amount of tetrapropylammonium hydroxide is used. The catalytic performance of the synthesized small-crystal TS-1 samples in cyclohexanone ammoximation was better than that of bulk TS-1 as a result of improved diffusion and a larger number of active tetrahedral Ti centers.
基金financial support by the One Hundred Talent Program of the Chinese Academy of Sciences and the National Natural Science Foundation of China(No.51302264)
文摘Birnessite-type MnO2 (δ-MnO2) nano-sheets were successfully synthesized by an interracial synthesis method in this work. The properties and electrochemical performance of the as-prepared δ-MnO2 were analyzed and evaluated by scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption measurement and electrochemical tests. This facile synthesis method enables δ-MnO2 nanosheets to show a large specific surface area (257.5 m^2 g^-1). The electrochemical test results show that the specific capacitance is 272 F g^-1 and the specific capacitance retention is over 96.7% after 1000 cycles at a scan rate of 10 mV s^-1. All results demonstrate that δ-MnO2 has a great potential application in high- performance electrochemical capacitors, and this interracial synthesis method will be a very promising method to synthesize highly active MnO2 materials in a large scale.
基金Project supported by the Natural Science Foundation of Fujian Province(2014J01043)the National Natural Science Foundation of China(21203028)PetroChina Innovation Foundation(2016D-5007-0504)
文摘A series of MgAl-layered double oxides(LDO) doped with different rare-earth elements(Y, La, and Ce)were synthesized by the calcination of Mg-Al layered double hydroxides, and Ru, which were used to prepare ammonia synthesis catalysts. The as-obtained oxides and catalysts were characterized by XRD,TEM, TPD, TPR and XPS to understand their catalytic performances in ammonia synthesis. The H_2-TPR and HRTEM studies reveal that Ru/Y-LDO catalyst possesses more active Ru metal and small particle size.The XPS demonstrates that the electronic interaction between Y and Ru metals is stronger, which can be tentatively explained by most of Y inserted into the hydrotalcites structure. CO_2-TPD demonstrates that Ru/Y-LDO catalyst shows stronger basic site densities than catalysts doped with Ce and La. Higher activity of the Ru/Y-LDO catalyst can be attributed to smaller particle size, more active metal(Ru) and strong Ru-support interaction.
基金The financial support of Natural Sciences and Engineering Research Council of Canada (NSERC)Ontario Graduate Scholarship (OGS) programRyerson University is greatly appreciated
文摘A nitrogen-doped titanium dioxide composite photocatalyst(N–TiO2) with heterojunction structures is synthesized by three different approaches: a novel UV-assisted thermal synthesis, annealing, and microwave technique. Photocatalytic activities of synthesized photocatalysts are evaluated by the degradation of Methyl Orange under ultraviolet light types A(UV-A), B(UV-B), and C(UV-C), visible light, and direct sunlight irradiation. Results show that by using N–TiO_2 photocatalyst prepared by the UV-assisted thermal synthesis and annealing, the degradation increases by 16.5% and 20.4%, respectively, compared to that by bare TiO2. The best results are obtained at a nitrogen to TiO2 mass ratio of 0.15(N:TiO2). The enhancement of the photocatalytic activity observed in the visible range is mainly attributed to the increasing separation rate of photogenerated charge carriers. The novel UV-assisted thermal synthesis has produced encouraging results as a preparation method for the nitrogen-doped TiO2 photocatalyst; thus, further studies are recommended for process optimization, immobilization, and scale-up to evaluate its applicability in wastewater treatment.
基金financially supported by the National Natural Science Foundation of China(Grant No.21673065 and 21875057)the Key-Area Research and Development Program of Guangdong Province(No.1934212200002)the Innovation and Entrepreneurship Team Project of Zhuhai(No.ZH01110405170016PWC)。
文摘Transition metal cation ordering is essential for controlling the electrochemical performance of cubic spinel LiNi_(0.5)Mn_(1.5)O_(4)(LNMO),which is conventionally adjusted by optimizing the high temperature sintering and annealing procedures.In this present work,multiple characterization techniques,including 6,7Li NMR,XRD and HRTEM,have been combined to trace the phase transformation and morphology evolution during synthesis.It has been illustrated that simultaneous formation of LiMn_(2)O_(4)(LMO)and LiNiO_(2)(LNO)binary oxides and their conversion into highly reactive LixNi^(3+)_(y)Mn_(3.5+)_(z)O ternary intermediate is a thermal dynamically difficult but crucial step in the synthesis of LNMO ternary oxide.A new strategy of modifying the intermediates formation pathway from binary mode to ternary mode using thermal regulating agent has been adopted.LNMO synthesized with thermal regulating agent exhibits supreme rate capability,long-cycling performance(even at elevated temperature)and excellent capacity efficiency.At a high rate of 100 C,the assembled battery delivers a discharge capacity of 99 mAh g^(-1).This study provides a way to control the formation pathway of complex oxides using thermal regulating agent.
基金Supported by the National Key Basic Research Program of China(2013CB733505,2013CB733501)the National Natural Science Foundation of China(91334202)+2 种基金the Natural Science Foundation of Jiangsu Province of China(BK2012421,BK20130062)the Research Fund for the Doctoral Program of Higher Education of China(20123221120015)the Project for Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘The use of nanostructured composites as catalyst supports is a promising route to prepare catalysts with high selectivity and productivity. In this work, reduced graphene oxide-TiO_2(rGP-x) composites with a variation of reduced graphene oxide(rGO) content were synthesized by hydrothermal method. Pd/rGP-x catalysts were prepared in incipient-wetness impregnation method for the direct synthesis of H_2O_2 from H2 and O_2. The morphology and electronic properties of catalysts were investigated by XPS, TEM, and Raman spectroscopy.The ratio of Pd^(2+)/Pd^0 and the hydrophobicity of the catalysts were increased with the rising content of rGO. As the amount of rGO in the catalysts varied in the range of 0.025 wt%–2 wt%, the selectivity of H_2O_2 exhibited a tendency of increasing firstly and then decreasing from 0.1 wt% to 2 wt%. It indicates that good catalytic performance for H_2O_2 synthesis can be achieved only when appropriate amount of rGO is introduced. The H_2O_2 selectivity and productivity of Pd/r GP-0.025 both improved remarkably compared with Pd/P25. This enhancement originated from the combined effects of the proper ratio of Pd^(2+)/Pd^0 and hydrophobicity of the catalyst.
基金Supported by the National Natural Science Foundation of China(21107143,21207033)the Fundamental Research Funds for the Central Universities,South-Central University for Nationalities(CZY15003)
文摘A simple ultrasound-assisted co-precipitation method was developed to prepare ferroferric oxide/graphene oxide magnetic nanoparticles(Fe_3O_4/CO MNPs).The hysteresis loop of Fe_3O_4/GO MNPs demonstrated that the sample was typical of superparamagnetic material.The samples were characterized by transmission electron microscope,and it is found that the particles are of small size.The Fe_3O_4/GO MNPs were further used as an adsorbent to remove Rhodamine B.The effects of initial pH of the solution,the dosage of adsorbent,temperature,contact time and the presence of interfering dyes on adsorption performance were investigated as well.The adsorption equilibrium and kinetics data were fitted well with the Freundlich isotherm and the pseudosecond-order kinetic model respectively.The adsorption process followed intra-particle diffusion model with more than one process affecting the adsorption of Rhodamine B.And the adsorption process was endothermic in nature.Furthermore,the magnetic composite with a high adsorption capacity of Rhodamine B could be effectively and simply separated using an external magnetic field.And the used particles could be regenerated and recycled easily.The magnetic composite could find potential applications for the removal of dye pollutants.
基金financially supported by the National Natural Science Foundation of China(NO.51464013)the Dr.Initialization Fund of Jiangxi University of Science and Technology(No.jxxjbs14013)
文摘Two types of alumina dispersion-strengthened copper(ADSC) alloys were fabricated by a novel in-situ reactive synthesis(IRS) and a traditional internal oxidation(IO) process. The features of alumina dispersoids in these ADSC alloys were investigated by X-ray diffraction, scanning electron microscopy, and high-resolution transmission electron microscopy. It is found that nano-sized γ-Al2O3 particles of approximately 10 nm in diameter are homogeneously distributed in the IRS-ADSC composites. Meanwhile, larger-sized, mixed crystal structure alumina with rod-shaped morphology is embedded in the IO-ADSC alloy. The IRS-ADSC composites can obtain better mechanical and physical properties than the IO-ADSC composites; the tensile strength of the IRS-ADSC alloy can reach 570 MPa at room temperature, its electrical conductivity is 85% IACS, and the Rockwell hardness can reach 86 HRB.
基金supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,under Contract No.DE-AC02-06CH11357
文摘Microflowers made of interconnected MnO2 nanosheets have been successfully synthesized in a microwave reactor through a hydrothermal reduction of KMnO4 with aqueous HCI at elevated temperatures in the presence of superparamagnetic Fe3O4SiO2 core-shell nanoparticles.Due to the chemical compatibility between SiO2 and MnO2,the heterogeneous reaction leads to the spontaneous encapsulation of the Fe3O4@SiO2 core-shell nanoparticles in the MnO2 microflowers.The resulting hybrid particles exhibit multiple properties including high surface area associated with the MnO2nanosheets and superparamagnetism originated from the Fe3O4@SiO2 core-shell nanoparticles.which are beneficial for applications requiring both high surface area and magnetic separation.
基金the financial support from the National Natural Science Foundation of China(No.51274256)
文摘Surface self-magnetization of siderite is achieved by generating ferromagnetic substance on the surface of siderite by adjusting slurry temperature,pH value,stirring rate and reaction time.No addition of any iron-containing reagent is required.The temperature of 60 ℃,NaOH concentration of 0.10 mol/L;stirring rate of 900 r/min and the reaction time of 10 min are the optimal conditions.The results show that the siderite recovery in magnetic separation increased from 26.9% to 88.8% after surface magnetization.Magnetization kinetic equation is expressed as 1 [1(e0.269)]1/3 = Kt.Activation energy for the magnetization reaction is 4.30 kJ/mol.VSM,SEM and XPS were used to characterize the siderite,and results show that the saturated magnetization(rs) of siderite increased from 0.652 to 2.569Am2 /kg,the magnetic hysteresis was detected with a coercive force of 0.976 A/m after magnetization;Fe2P3/2 electron binding energy changed which reflects the valence alteration in iron on the surface and the formation of ferromagnetic Fe3O4.
基金Financial support from the Natural Science Foundation of China (No.21072176)
文摘An efficient method was developed for chlorination of aromatic compounds with electron-donating groups using iodobenzene as the catalyst and m-chloroperbenzoic acid as the terminal oxidant in the presence of 4-methylbenzenesulfonic acid in THF at room temperature for 24 h,and a series of the monochlorinated compounds was obtained in good yields.In this protocol,the catalyst iodobenzene was first oxidized into the hypervalent iodine intermediate,which then treated with lithium chloride and finally reacted with aromatic compounds to form the chlorinated compounds.
基金the Program for the NSFC (Nos. 51302325, 51201115, 51471121)New Century Excellent Talents in University (No. NCET-12-0553)+4 种基金Program for Shenghua Overseas Talent (No. 1681-7607030005) from Central South UniversityHubei Provincial Natural Science Foundation (No. 2014CFB261)the partial financial support from the Open-End Fund for the Valuable and Precision Instruments of Central South University (No. CSUZC2014032)Fundamental Research Funds for the Central Universities (No. 2042015kf0184)Wuhan University
文摘Rational designing and controlling of nanostructures is a key factor in realizing appropriate properties required for the high-performance energy fields. In the present study, hollow Sn O2@C nanoparticles(NPs) with a mean size of 50 nm have been synthesized in large-scale via a facile hydrothermal approach.The morphology and composition of as-obtained products were studied by various characterized techniques. As an anode material for lithium ion batteries(LIBs), the as-prepared hollow Sn O2@C NPs exhibit significant improvement in cycle performances. The discharge capacity of lithium battery is as high as 370 m Ah g 1, and the current density is 3910 m A g 1(5 C) after 573 cycles. Furthermore, the capacity recovers up to 1100 m Ah g 1at the rate performances in which the current density is recovered to 156.4 m A g 1(0.2 C). Undoubtedly, sub-100 nm Sn O2@C NPs provide significant improvement to the electrochemical performance of LIBs as superior-anode nanomaterials, and this carbon coating strategy can pave the way for developing high-performance LIBs.
基金supported by the Romanian Ministry of Education and Research within the Nucleu Programme(Project PN 09-44)
文摘ZnO nanoparticles(ZnO NPs) were synthesized by chemical method(coprecipitation) and biological method using aqueous extracts of garlic(Allium sativum),rosemary(Rosmarinus officinalis) and basil(Ocimum basilicum).The influence of plant extract on the antibacterial and antioxidant activities of green synthesized nanoparticles was investigated.The X-ray diffraction studies reveal that all ZnO samples have hexagonal wurtzite structure.The particle size of ZnO NPs estimated by transmission electron microscopy analysis(between 14 and 27 nm) varies depending on the synthesis method of nanoparticles and the type of extracts from the plants used.The functional groups involved in the biosynthetic procedure were evidenced by Fourier transform infrared spectroscopy.The presence of Mn^(2+)ions,Zn vacancy complexes and oxygen vacancies in ZnO samples was highlighted by electron paramagnetic resonance spectroscopy.The green synthesized ZnO NPs have shown a good bactericidal activity against Staphylococcus aureus,Bacillus subtilis,Listeria monocytogenes,Escherichia coli,Salmonella typhimurium and Pseudomonas aeruginosa bacterial strains.ZnO NPs synthesized using extracts of the selected plant species have been found to exhibit more enhanced antibacterial and antioxidant activities as compared to chemical ZnO NPs.
文摘The effect of cerous nitrate on activity of NOS and expression of iNOS in rat hepatocyte was studied by means of reverse transcription - polymerase chain reaction ( RT-PCR). The result shows that neither high ( 50 mg.kg(-1)) nor low( 1 mg.kg(-1)) dose of cerous nitrate can induce the increase of expression of iNOS mRNA, but an increase of activity was observed after administration of cerous nitrate. Possible mechanism for these phenomena was discussed.
文摘Acicular goethite(a-Fe OOH) and worm-like maghamite(γ-Fe2O3) nanostructures have been prepared adopting a novel route, using Na2[Fe(HL)2(H2O)2] chelate complex in alkaline medium. It is found that concentration of hydrated Fe(III) ions increased with increasing temperature, which later play a key role in generation of different phases of iron oxide. Phase and morphology of the products are investigated using XRD, FTIR, SEM, and TEM analysis. Using UV–Vis spectra, various electronic transitions of goethite and maghamite particles are examined. Maghamite nanostructures exhibit superparamagnetic property at room temperature. On the basis of experimental observations and analytical data, growth mechanism of the nanostructures is discussed.
基金supported by Yangzhou Engineering Technology Research Center of Petrochemical New Materials(YZM2015086)Yangzhou Science and Technology Bureau(YZ2016269)
文摘Two europium oxide/sulfide silicates, Eu2O(SiO4) (1) and Eu5S(SiO4)3 (2), have been synthesized using high-temperature solid-state reactions. 1 crystallizes in the monoclinic space group P21/c with a = 9.1459(7), b = 7.1280(5), c = 6.7655(5) ? and ? = 107.611(2), belonging to the Gd2O(SiO4) structure type; 2 crystallizes in space group P63/m of the hexagonal system with a = 9.786(4) and c = 6.789(3) , belonging to the apatite Ca5Cl(PO4)3 structure type. The structure chemistry of related RE2O(SiO4) and RE5S(SiO4)3 compounds is also discussed. The optical energy gap of 2 is determined to be 2.05 eV.
文摘To assess the role of oxidative metabolism and nitric oxide synthesis for elucid a ting their pathophysiological mechanisms in a Tibetan patient with essential hyp ertension Methods The serum levels of total superoxide dismutase (T SOD), malondialdehyde (MDA), total antioxidant capacity (T AOC), nitric oxide (NO) and nitric oxide synthase (NOS) were assayed in sixty native Tibetans (thirty hypertensive patients and t hirty healthy volunteers as control) Results The levels of T SOD, T AOC, NO and NOS were significantly lower in the patien t group than in the control group ( P <0 01); MDA was significantly higher in the patient group than in the control group ( P <0 01) The level of MDA ha d a strong negative correlation with T SOD, T AOC, NO and NOS ( r =-0 82, -0 76, -0 79, -0 73, respectively, P <0 001 for all) Conclusion Tibetan patients with essential hypertension (EH) may have underlying oxidative metabolism dysfunction and depressed NO synthesis, both responsible for the hype rtensive process
文摘The aim of this study is to investigate the effects of nitric oxide, formed from L-arginine, on the production of endothelin?1 in vivo and in cultured endothelial cells. In mechanically ventilated anesthetized dogs (n = 5), mean pulmonary arterial pressure (PAPm) and pulmonary vascular resistance (PVR) during hypoxic ventilation (FIO2 = 0.10) was 25 ?3.1 kPa and 68.7 ?10.2 kPa.s / L respectively. IG-nitro-L-arginine methylester (L-NAME), an inhibitor of nitric oxide synthase, increased the peak value of PAPm and PVR during hypoxic ventilation to 36.6 ?4.7 kPa and 158.4 ?25 kPa.s / L and its effect lasted for 2-3 hours. Meanwhile, plasma endothelin? level in the femoral artery increased by 20.9+ 7.1, 25.6?7.7, 28.6?7.9 pg / ml at the 60 th, 120th, 180th minute after the injection of L-NAME respectively (P<0.05 vs hypoxic control before the injection). In cultured endothelial cells from umbilical veins, endothelin-1 level of culture medium in control group was 35.1 ?.9 pg / 105 cells /ml (n=9). L-NAME increased endothelin-1 level to 42.8 ?4.9pg / 105 cells / ml (n = 9, P < 0.05) in case of 10-11 mol / L and to 43.0+ 4.7 pg / 105 cells / ml in case of 10 -7 mol/L (n=9, F<0.05). These findings indicate that endogenous nitric oxide is an inhibitory modulator of hypoxic pulmonary vasoconstriction and that nitric oxide inhibits the production of endothelin? in vivo and in cultured vascular endothelial cells.