The aging process of pure copper precursors and copper-zinc binary precursorswere studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnOwere tested using fixed-bed flow reactor, and...The aging process of pure copper precursors and copper-zinc binary precursorswere studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnOwere tested using fixed-bed flow reactor, and the physical properties of the catalysts and Cuspecies were characterized with N_2 adsorption and N_2O passivation method, respectively. For theCu-Zn binary system prepared at the precipitating condition of pH=8.0 and temperature=80℃, theinitial phase was a mixture of copper nitrate hydroxide Cu_2(NO_3)(OH)_3, georgeite and hydrozinciteZn_5(CO_3)_2(OH)_6. By increasing the duration of its aging time, the phase of Cu_2(NO_3)(OH)_2first transited to georgeite, and then interdiffused into Zn_5(CO_3)_2(OH)_6 and resulted in two newphases: rosasite (Cu,Zn)_2CO_3(OH)_2 and au-richalcite (Zn,Cu)_5(CO_3)_2(OH)_6. The former phasewas much easier to be formed than the latter one, while the latter phase was more responsible forthe activity of methanol synthesis than the former one. It is found that the composition andstructure of the precursors altered obviously after the colour transition point. The experimentalresults showed that methanol synthesis is a structure-sensitive catalytic reaction.展开更多
Ensuring a sufficient energy supply is essential to a country. Natural gas constitutes a vital part in energy supply and therefore forecasting natural gas consumption reliably and accurately is an essential part of a ...Ensuring a sufficient energy supply is essential to a country. Natural gas constitutes a vital part in energy supply and therefore forecasting natural gas consumption reliably and accurately is an essential part of a country's energy policy. Over the years, studies have shown that a combinative model gives better projected results compared to a single model. In this study, we used Polynomial Curve and Moving Average Combination Projection (PCMACP) model to estimate the future natural gas consumption in China from 2009 to 2015. The new proposed PCMACP model shows more reliable and accurate results: its Mean Absolute Percentage Error (MAPE) is less than those of any previous models within the investigated range. According to the PCMACP model, the average annual growth rate will increase for the next 7 years and the amount of natural gas consumption will reach 171600 million cubic meters in 2015 in China.展开更多
La(0.6)Sr(0.4)Co(0.2)Fe(0.8)O(3-δ)(LSCF) anodes were infiltrated by Gd(0.2)Ce(0.8)O(1.9)GDC) nanoparticles to improve the oxygen evolution reaction(OER) performance of solid oxide electrolysis ce...La(0.6)Sr(0.4)Co(0.2)Fe(0.8)O(3-δ)(LSCF) anodes were infiltrated by Gd(0.2)Ce(0.8)O(1.9)GDC) nanoparticles to improve the oxygen evolution reaction(OER) performance of solid oxide electrolysis cells(SOECs) in CO2 electroreduction. The effect of GDC loading was investigated, and 10 wt% GDC nanoparticle infiltration of the LSCF(10 GDC/LSCF) anode results in the highest OER performance. Electrochemical impedance spectra measurements indicate that the infiltration by GDC nanoparticles greatly decreases the polarization resistance of the SOECs with the 10 GDC/LSCF anodes. The following distribution of relaxation time analysis suggests that four individual electrode processes are involved in the OER and that all of them are accelerated on the 10 GDC/LSCF anode. Three phase boundaries, surface oxygen vacancies, and bulk oxygen mobility increased, based on scanning electron microscopy and temperature-programmed desorption of O2 characterizations, and contributed to the enhancement of the four electrode processes of the OER and electrochemical performance of SOECs.展开更多
AIM: Fourteen urinary nucleosides, primary degradation products of tRNA, were evaluated to know the potential as biological markers for patients with colorectal cancer. METHODS: The concentrations of 14 kinds of urina...AIM: Fourteen urinary nucleosides, primary degradation products of tRNA, were evaluated to know the potential as biological markers for patients with colorectal cancer. METHODS: The concentrations of 14 kinds of urinary nucleosides from 52 patients with colorectal cancer, 10 patients with intestinal villous adenoma and 60 healthy adults were determined by column switching high performance liquid chromatography method. RESULTS: The mean levels of 12 kinds of urinary nucleosides (except uridine and guanosine) in the patients with colorectal cancer were significantly higher than those in patients with intestinal villous adenoma or the healthy adults. Using the levels of 14 kinds of urinary nucleosides as the data vectors for principal component analysis, 71% (37/52) patients with colorectal cancer were correctly classified from healthy adults, in which the identification rate was much higher than that of CEA method (29%). Only 10% (1/10) of patients with intestinal villous adenoma were indistinguishable from patients with colorectal cancer. The levels of m1G, Pseu and m1A were positively related with tumor size and Duke's stages of colorectal cancer. When monitoring the changes in urinary nucieoside concentrations of patients with colorectal cancer associated with surgery, it was found that the overall correlations with clinical assessment were 84% (27/32) and 91% (10/11) in response group and progressive group, respectively. CONCLUSION: These findings indicate that urinary nucleosides determined by column switching high performance liquid chromatography method may be useful as biological markers for colorectal cancer.展开更多
A novel poly-/-arginine microcapsule was prepared due to its nutritional function and pharmacological efficacy. A high-voltage electrostatic droplet generator was used to make uniform microcapsules. The results show t...A novel poly-/-arginine microcapsule was prepared due to its nutritional function and pharmacological efficacy. A high-voltage electrostatic droplet generator was used to make uniform microcapsules. The results show that the membrane strength and permeating property are both remarkably affected with the changes of sodium alginate concentration. With the sodium alginate concentration increasing, gel beads sizes increase from 233μm to 350μm, release ratio is also higher at the same time, but the membrane strength decreases.展开更多
The simultaneous removal of up to 92% of the surfactant template and chemical implantation of transition metal complexes into mesopores has been successfully achieved by treating as-synthesized pure siliceous MCM-41 w...The simultaneous removal of up to 92% of the surfactant template and chemical implantation of transition metal complexes into mesopores has been successfully achieved by treating as-synthesized pure siliceous MCM-41 with supercritical CO2 modified with CH2Cl2/MeOH mixture, resulting in the formation of functionalized material with uniform pore structure.展开更多
The optimum Mo/[H^+] ratio per unit cell of the active precursors in Mo/HZSM-5 catalysts for methane dehydro-aromatization, measured by1H MAS NMR, was found to be about 1 when adjusting the acid sites by altering eith...The optimum Mo/[H^+] ratio per unit cell of the active precursors in Mo/HZSM-5 catalysts for methane dehydro-aromatization, measured by1H MAS NMR, was found to be about 1 when adjusting the acid sites by altering either the SiO2/Al2O3 ratios or the Mo loading. This implies that a concerted interaction between the Mo species and the Bronsted acid sites probably features the bifunctionality of the Mo/HZSM-5 catalyst. On the other hand, it was found that the driving force for Mo species to move into the HSZM-5 zeolite channels and the interaction between the Mo species and the Bronsted acid sites are closely and proportionably related with the amount of Bronsted acid sites per unit cell.展开更多
The elegant 2D multiquantum (MQ) MAS NMR has been applied to investigate the coordination of Al atoms in SAPO-34. The results show that the effects of the template and/or water on the coordination of Al atoms are sig...The elegant 2D multiquantum (MQ) MAS NMR has been applied to investigate the coordination of Al atoms in SAPO-34. The results show that the effects of the template and/or water on the coordination of Al atoms are significant, which lead to the formation of various Al species. Up to four kinds of Al species are distinctly resolved.展开更多
The electrocatalysts of Pt/C, PtRu/C and Ru/C were prepared by the impregnation method. The facet characterization, the dispersion and the particle size for the catalysts were determined by means of X ray diffractio...The electrocatalysts of Pt/C, PtRu/C and Ru/C were prepared by the impregnation method. The facet characterization, the dispersion and the particle size for the catalysts were determined by means of X ray diffraction and transmission electron microscopy. X ray photoelectron spectroscopy was also used to analyze the state and the valency of the noble metals. The results show that the particle size was in nanometer range and the binary metals have come into being an alloy. The platinum in the catalysts existed in zero valency. The valency of the ruthenium on the surface is different from that in the body, while the ruthenium on the surface existed in oxide form. PtRu/C and Pt/C are of good activity to the electrooxidation of hydrogen except Ru/C. PtRu/C is more tolerant of CO than Pt/C, and CO is only adsorbed on Pt.展开更多
DNL-6, a silicoaluminophosphate(SAPO) molecular sieve with RHO topology, was hydrothermally synthesized using a new structure-directing agent(SDA), N,N'-dimethylethylenediamine. The obtained samples were characte...DNL-6, a silicoaluminophosphate(SAPO) molecular sieve with RHO topology, was hydrothermally synthesized using a new structure-directing agent(SDA), N,N'-dimethylethylenediamine. The obtained samples were characterized by X-ray diffraction, X-ray fluorescence, X-ray photoelectron spectroscopy, scanning electron microscopy, and N2 adsorption, which indicated that the synthesized DNL-6 s have high crystallinity and relatively high Si content ranging from 20% to 35%. Solid-state magic-angle-spinning(MAS) nuclear magnetic resonance(13 C, 29 Si, 27 Al, 31 P, and 27 Al multiple-quantum(MQ)) was conducted to investigate the status of the SDA and local atomic environment in the as-synthesized DNL-6. Thermal analysis revealed the presence of a large amount of amines in the DNL-6 crystals(about 4.4 SDAs per α-cage), which was the reason for the formation of DNL-6 with an ultrahigh Si content(36.4% Si per mole). Interestingly, DNL-6 exhibited excellent catalytic performance for methanol amination. More than 88% methanol conversion and 85% methylamine plus dimethylamine selectivity could be achieved due to the combined contribution of strong acid sites, suitable acid distribution, and narrow pore dimensions of DNL-6.展开更多
trans-PtH(PCy3)2[S2CN(CH2C6H5)2] crystallizes in triclinic space group P1 with a=10. 961 (9),b= 13. 247 (6), c= 18. 331(4) A ,α=82. 97(2) ,β= 103. 89(5),γ=103. 79(7)°,Mr=1029. 39,V = 2503(4)A3,Z = 2,Dc = 1. 36...trans-PtH(PCy3)2[S2CN(CH2C6H5)2] crystallizes in triclinic space group P1 with a=10. 961 (9),b= 13. 247 (6), c= 18. 331(4) A ,α=82. 97(2) ,β= 103. 89(5),γ=103. 79(7)°,Mr=1029. 39,V = 2503(4)A3,Z = 2,Dc = 1. 366g/cm3, μ= 30. 06cm-1,F(000) = 1068,R=0. 033 and Rw = 0. 039 for 6940 unique observed reflections. The platinum atom is coordinated by one hydrogen,one sulfur and two phosphorus atoms to form a distorted square plane.展开更多
文摘The aging process of pure copper precursors and copper-zinc binary precursorswere studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnOwere tested using fixed-bed flow reactor, and the physical properties of the catalysts and Cuspecies were characterized with N_2 adsorption and N_2O passivation method, respectively. For theCu-Zn binary system prepared at the precipitating condition of pH=8.0 and temperature=80℃, theinitial phase was a mixture of copper nitrate hydroxide Cu_2(NO_3)(OH)_3, georgeite and hydrozinciteZn_5(CO_3)_2(OH)_6. By increasing the duration of its aging time, the phase of Cu_2(NO_3)(OH)_2first transited to georgeite, and then interdiffused into Zn_5(CO_3)_2(OH)_6 and resulted in two newphases: rosasite (Cu,Zn)_2CO_3(OH)_2 and au-richalcite (Zn,Cu)_5(CO_3)_2(OH)_6. The former phasewas much easier to be formed than the latter one, while the latter phase was more responsible forthe activity of methanol synthesis than the former one. It is found that the composition andstructure of the precursors altered obviously after the colour transition point. The experimentalresults showed that methanol synthesis is a structure-sensitive catalytic reaction.
基金supported by the Youth Fund of Chinese Academy of Sciences Knowledge Innovation Program area frontier projects (No. S200603)the Innovation Team Project of Education Department of Liaoning Province (No. 2007T050)
文摘Ensuring a sufficient energy supply is essential to a country. Natural gas constitutes a vital part in energy supply and therefore forecasting natural gas consumption reliably and accurately is an essential part of a country's energy policy. Over the years, studies have shown that a combinative model gives better projected results compared to a single model. In this study, we used Polynomial Curve and Moving Average Combination Projection (PCMACP) model to estimate the future natural gas consumption in China from 2009 to 2015. The new proposed PCMACP model shows more reliable and accurate results: its Mean Absolute Percentage Error (MAPE) is less than those of any previous models within the investigated range. According to the PCMACP model, the average annual growth rate will increase for the next 7 years and the amount of natural gas consumption will reach 171600 million cubic meters in 2015 in China.
基金This work was supported by the National Key R&D Program of China(2017YFA0700102)the National Natural Science Foundation of China(21703237,21573222,91545202)+1 种基金Dalian Institute of Chemical Physics(DICP DMTO201702)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020200)and CAS Youth Innovation Promotion(2015145)~~
文摘La(0.6)Sr(0.4)Co(0.2)Fe(0.8)O(3-δ)(LSCF) anodes were infiltrated by Gd(0.2)Ce(0.8)O(1.9)GDC) nanoparticles to improve the oxygen evolution reaction(OER) performance of solid oxide electrolysis cells(SOECs) in CO2 electroreduction. The effect of GDC loading was investigated, and 10 wt% GDC nanoparticle infiltration of the LSCF(10 GDC/LSCF) anode results in the highest OER performance. Electrochemical impedance spectra measurements indicate that the infiltration by GDC nanoparticles greatly decreases the polarization resistance of the SOECs with the 10 GDC/LSCF anodes. The following distribution of relaxation time analysis suggests that four individual electrode processes are involved in the OER and that all of them are accelerated on the 10 GDC/LSCF anode. Three phase boundaries, surface oxygen vacancies, and bulk oxygen mobility increased, based on scanning electron microscopy and temperature-programmed desorption of O2 characterizations, and contributed to the enhancement of the four electrode processes of the OER and electrochemical performance of SOECs.
基金Supported by the High-tech R and D Plan, No. 2003AA223061the Sociality Commonweal Project of State Ministry of Science and Technology of Chinathe Knowledge Innovation Program of the Chinese Academy of Sciences, No. K2003A16 and Liaoning Province Foundation of Science and Technology
文摘AIM: Fourteen urinary nucleosides, primary degradation products of tRNA, were evaluated to know the potential as biological markers for patients with colorectal cancer. METHODS: The concentrations of 14 kinds of urinary nucleosides from 52 patients with colorectal cancer, 10 patients with intestinal villous adenoma and 60 healthy adults were determined by column switching high performance liquid chromatography method. RESULTS: The mean levels of 12 kinds of urinary nucleosides (except uridine and guanosine) in the patients with colorectal cancer were significantly higher than those in patients with intestinal villous adenoma or the healthy adults. Using the levels of 14 kinds of urinary nucleosides as the data vectors for principal component analysis, 71% (37/52) patients with colorectal cancer were correctly classified from healthy adults, in which the identification rate was much higher than that of CEA method (29%). Only 10% (1/10) of patients with intestinal villous adenoma were indistinguishable from patients with colorectal cancer. The levels of m1G, Pseu and m1A were positively related with tumor size and Duke's stages of colorectal cancer. When monitoring the changes in urinary nucieoside concentrations of patients with colorectal cancer associated with surgery, it was found that the overall correlations with clinical assessment were 84% (27/32) and 91% (10/11) in response group and progressive group, respectively. CONCLUSION: These findings indicate that urinary nucleosides determined by column switching high performance liquid chromatography method may be useful as biological markers for colorectal cancer.
文摘A novel poly-/-arginine microcapsule was prepared due to its nutritional function and pharmacological efficacy. A high-voltage electrostatic droplet generator was used to make uniform microcapsules. The results show that the membrane strength and permeating property are both remarkably affected with the changes of sodium alginate concentration. With the sodium alginate concentration increasing, gel beads sizes increase from 233μm to 350μm, release ratio is also higher at the same time, but the membrane strength decreases.
文摘The simultaneous removal of up to 92% of the surfactant template and chemical implantation of transition metal complexes into mesopores has been successfully achieved by treating as-synthesized pure siliceous MCM-41 with supercritical CO2 modified with CH2Cl2/MeOH mixture, resulting in the formation of functionalized material with uniform pore structure.
文摘The optimum Mo/[H^+] ratio per unit cell of the active precursors in Mo/HZSM-5 catalysts for methane dehydro-aromatization, measured by1H MAS NMR, was found to be about 1 when adjusting the acid sites by altering either the SiO2/Al2O3 ratios or the Mo loading. This implies that a concerted interaction between the Mo species and the Bronsted acid sites probably features the bifunctionality of the Mo/HZSM-5 catalyst. On the other hand, it was found that the driving force for Mo species to move into the HSZM-5 zeolite channels and the interaction between the Mo species and the Bronsted acid sites are closely and proportionably related with the amount of Bronsted acid sites per unit cell.
基金We are grateful to the support of the National Natural Science Foundation of China and the Ministry of Science and Technology of China. We appreciate Dr. R. Fu (NHMFL Tallahassee) for his kind help regarding the MQ MAS NMR experiments.
文摘The elegant 2D multiquantum (MQ) MAS NMR has been applied to investigate the coordination of Al atoms in SAPO-34. The results show that the effects of the template and/or water on the coordination of Al atoms are significant, which lead to the formation of various Al species. Up to four kinds of Al species are distinctly resolved.
基金Supported by the National 973project(No.G2 0 0 0 0 2 6 4 10 ) and Inovation Funds of Dalian Insitute of Chem icalPhysics
文摘The electrocatalysts of Pt/C, PtRu/C and Ru/C were prepared by the impregnation method. The facet characterization, the dispersion and the particle size for the catalysts were determined by means of X ray diffraction and transmission electron microscopy. X ray photoelectron spectroscopy was also used to analyze the state and the valency of the noble metals. The results show that the particle size was in nanometer range and the binary metals have come into being an alloy. The platinum in the catalysts existed in zero valency. The valency of the ruthenium on the surface is different from that in the body, while the ruthenium on the surface existed in oxide form. PtRu/C and Pt/C are of good activity to the electrooxidation of hydrogen except Ru/C. PtRu/C is more tolerant of CO than Pt/C, and CO is only adsorbed on Pt.
基金supported by the National Natural Science Foundation of China(21476228,21676262)the Key Research Program of Frontier Sciences,CAS(QYZDB-SSW-JSC040)~~
文摘DNL-6, a silicoaluminophosphate(SAPO) molecular sieve with RHO topology, was hydrothermally synthesized using a new structure-directing agent(SDA), N,N'-dimethylethylenediamine. The obtained samples were characterized by X-ray diffraction, X-ray fluorescence, X-ray photoelectron spectroscopy, scanning electron microscopy, and N2 adsorption, which indicated that the synthesized DNL-6 s have high crystallinity and relatively high Si content ranging from 20% to 35%. Solid-state magic-angle-spinning(MAS) nuclear magnetic resonance(13 C, 29 Si, 27 Al, 31 P, and 27 Al multiple-quantum(MQ)) was conducted to investigate the status of the SDA and local atomic environment in the as-synthesized DNL-6. Thermal analysis revealed the presence of a large amount of amines in the DNL-6 crystals(about 4.4 SDAs per α-cage), which was the reason for the formation of DNL-6 with an ultrahigh Si content(36.4% Si per mole). Interestingly, DNL-6 exhibited excellent catalytic performance for methanol amination. More than 88% methanol conversion and 85% methylamine plus dimethylamine selectivity could be achieved due to the combined contribution of strong acid sites, suitable acid distribution, and narrow pore dimensions of DNL-6.
文摘trans-PtH(PCy3)2[S2CN(CH2C6H5)2] crystallizes in triclinic space group P1 with a=10. 961 (9),b= 13. 247 (6), c= 18. 331(4) A ,α=82. 97(2) ,β= 103. 89(5),γ=103. 79(7)°,Mr=1029. 39,V = 2503(4)A3,Z = 2,Dc = 1. 366g/cm3, μ= 30. 06cm-1,F(000) = 1068,R=0. 033 and Rw = 0. 039 for 6940 unique observed reflections. The platinum atom is coordinated by one hydrogen,one sulfur and two phosphorus atoms to form a distorted square plane.