In order to achieve effective, economic, and easily achievable photocatalyst for the degradation of dye methyl orange（MeO）, ZnO, ZnO/ZnS and ZnO/ZnS/α-Fe2O3 nanocomposites were prepared by simple chemical synthetic...In order to achieve effective, economic, and easily achievable photocatalyst for the degradation of dye methyl orange（MeO）, ZnO, ZnO/ZnS and ZnO/ZnS/α-Fe2O3 nanocomposites were prepared by simple chemical synthetic route in the aqueous medium. Phase, crystallinity, surface structure and surface behavior of the synthesized materials were determined by X-ray diffraction（XRD） and Brunauer-Emmett-Teller analysis（BET） techniques. XRD study established formation of good crystalline ZnO, ZnO/ZnS and ZnO/ZnS/α-Fe2O3 nanomaterials. By using intensity of constituent peaks in the XRD pattern, the compositions of nanocomposites were determined. From the BET analysis, the prepared materials show mesoporous behavior, type Ⅳ curves along with H4 hysteresis. The ZnO/ZnS/α-Fe2O3 composite shows the largest surface area among three materials. From the UV-visible spectra, the band gap energy of the materials was determined. Photoluminescence spectra（PL） were used to determine the emission behavior and surface defects in the materials. In PL spectra, the intensity of UV peak of ZnO/ZnS is lowered than that of ZnO while in case of ZnO/ZnS/α-Fe2O3, the intensity further decreased. The visible emission spectra of ZnO/ZnS increased compared with ZnO while in ZnO/ZnS/α-Fe2O3 it is further increased compared with ZnO/ZnS. The as-synthesized materials were used as photocatalysts for the degradation of dye MeO. The photo-degradation data revealed that the ZnO/ZnS/α-Fe2O3 is the best photocatalyst among three specimens for the degradation of dye MeO. The decrease of intensity of UV emission peak and the increase of intensity of visible emission cause the decrease of recombination of electrons and holes which are ultimately responsible for the highest photocatalytic activity of ZnO/ZnS/α-Fe2O3.展开更多
采用柠檬酸为络合剂,溶胶-凝胶法制备系列CeO_2-CuO/ZnO/Al_2O_3,在3.0 MPa压力和220~230℃反应条件下,甲苯二胺(TDA)和乙烯催化合成二乙基甲苯二胺(DETDA)为探针反应,考察其催化性能,其中CeO_2掺杂量为3%,催化活性最高。通过X射线衍射(...采用柠檬酸为络合剂,溶胶-凝胶法制备系列CeO_2-CuO/ZnO/Al_2O_3,在3.0 MPa压力和220~230℃反应条件下,甲苯二胺(TDA)和乙烯催化合成二乙基甲苯二胺(DETDA)为探针反应,考察其催化性能,其中CeO_2掺杂量为3%,催化活性最高。通过X射线衍射(XRD)、傅里叶红外光谱(FT-IR)、差热重量分析法(DTG-DTA)、核磁氢谱1 H NMR对CeO_2-CuO/ZnO/Al_2O_3、DETDA、TDA进行检测和表征,揭示了它们的微观结构和内在规律性。XRD检测发现CeO_2掺杂量增多,CeO_2-CuO/ZnO/Al_2O_3衍射峰强度增强,提高了晶化程度,金属原子存在协同效应,增多了活性中心。FT-IR揭示了DETDA内部化学键键型,拥有甲基、亚甲基的多取代芳胺。DTG-DTA检测出的质量变化与热效应两种信息,DETDA的DTG-DTA曲线在66.0、271.0℃存在二个吸热峰,分别为氨基脱离苯环、DETDA的分解产生。通过1 H NMR对DETDA、TDA检测,得到DETDA、TDA的氢原子的数目分别为18和10,分子中各个氢核对应所归属的吸收峰,分别和它们分子式中的氢原子数目吻合。CeO_2-CuO/ZnO/Al_2O_3催化合成DETDA,反应条件温和,工艺流程简单,容易实现高效率和连续化工业生产,因此具有广阔的发展前景。展开更多
A novel coprecipitation-reduction process has been proposed for preparing highly selective Cu/ZnO/Al 2O 3 catalysts for methanol synthesis from CO 2 hydrogenation. Compared to the catalysts prepared by the conventiona...A novel coprecipitation-reduction process has been proposed for preparing highly selective Cu/ZnO/Al 2O 3 catalysts for methanol synthesis from CO 2 hydrogenation. Compared to the catalysts prepared by the conventional method, the new catalysts prepared via the new method exhibit much higher BET surface area and pore size, much smaller crystallite size and higher catalytic activity and selectivity in CO 2 hydrogenation to methanol. It is also found that the molar ratio of Cu + to Cu 0 on the surface of the catalyst obtained by coprecipitation-reduction is much higher than that on the reduced catalyst obtained by the conventional method, which could be crucial for its high activity and selectivity for catalytic hydrogenation of CO 2 to methanol.展开更多
Hydrogen production by catalytic steam reforming of methanol over a series of coprecipitated Cu/ZnO/Al2O3 catalysts under atmospheric pressure in a microreactor has been studied Effects of catalyst composition...Hydrogen production by catalytic steam reforming of methanol over a series of coprecipitated Cu/ZnO/Al2O3 catalysts under atmospheric pressure in a microreactor has been studied Effects of catalyst composition, reaction temperature and activation conditions on the catalytic activity have been investigated Crystal phases of catalysts were analyzed by XRD The results showed that Cu/ZnO/Al2O3 catalysts displayed high activity and selectivity for hydrogen and stability The optimized molar ratio is Cu/Zn=10, a maximum methanol conversion of 994?mol%, hydrogen selectivity of 999?mol% and CO molar fraction of 0007% were obtained in the steam reforming reaction with the catalyst containing 45?mol% copper XRD results showed that the diffraction peaks of CuO in the catalyst were clearly lower and broaden It indicated that high dispersion of small copper crystallites on the catalyst surface was formed under the calcination conditions It is suggested that the good performance of Cu/ZnO/Al2O3 catalysts partly resulted from well dispersed展开更多
We demonstrate for the first time that a short time of microwave irradiation on the oxide precursor of a Cu/ZnO/Al2O3 catalyst can provide unique opportunity for tailoring the microstructure and activity of the cataly...We demonstrate for the first time that a short time of microwave irradiation on the oxide precursor of a Cu/ZnO/Al2O3 catalyst can provide unique opportunity for tailoring the microstructure and activity of the catalyst for methanol steam reforming. It is shown by in situ XRD that a considerable increase in the microstrain of Cu nanocrystals could be achieved in the catalysts processed by microwave irradiation for 310 min, which correlates well with the enhanced CH3OH conversion as observed on the corresponding samples. The present work also confirms that although the high specific surface area of Cu is a prerequisite for catalytic activity, it does not account for the observed changes in activity and selectivity alone without taking bulk microstructural changes into account.展开更多
文摘In order to achieve effective, economic, and easily achievable photocatalyst for the degradation of dye methyl orange（MeO）, ZnO, ZnO/ZnS and ZnO/ZnS/α-Fe2O3 nanocomposites were prepared by simple chemical synthetic route in the aqueous medium. Phase, crystallinity, surface structure and surface behavior of the synthesized materials were determined by X-ray diffraction（XRD） and Brunauer-Emmett-Teller analysis（BET） techniques. XRD study established formation of good crystalline ZnO, ZnO/ZnS and ZnO/ZnS/α-Fe2O3 nanomaterials. By using intensity of constituent peaks in the XRD pattern, the compositions of nanocomposites were determined. From the BET analysis, the prepared materials show mesoporous behavior, type Ⅳ curves along with H4 hysteresis. The ZnO/ZnS/α-Fe2O3 composite shows the largest surface area among three materials. From the UV-visible spectra, the band gap energy of the materials was determined. Photoluminescence spectra（PL） were used to determine the emission behavior and surface defects in the materials. In PL spectra, the intensity of UV peak of ZnO/ZnS is lowered than that of ZnO while in case of ZnO/ZnS/α-Fe2O3, the intensity further decreased. The visible emission spectra of ZnO/ZnS increased compared with ZnO while in ZnO/ZnS/α-Fe2O3 it is further increased compared with ZnO/ZnS. The as-synthesized materials were used as photocatalysts for the degradation of dye MeO. The photo-degradation data revealed that the ZnO/ZnS/α-Fe2O3 is the best photocatalyst among three specimens for the degradation of dye MeO. The decrease of intensity of UV emission peak and the increase of intensity of visible emission cause the decrease of recombination of electrons and holes which are ultimately responsible for the highest photocatalytic activity of ZnO/ZnS/α-Fe2O3.
文摘采用柠檬酸为络合剂,溶胶-凝胶法制备系列CeO_2-CuO/ZnO/Al_2O_3,在3.0 MPa压力和220~230℃反应条件下,甲苯二胺(TDA)和乙烯催化合成二乙基甲苯二胺(DETDA)为探针反应,考察其催化性能,其中CeO_2掺杂量为3%,催化活性最高。通过X射线衍射(XRD)、傅里叶红外光谱(FT-IR)、差热重量分析法(DTG-DTA)、核磁氢谱1 H NMR对CeO_2-CuO/ZnO/Al_2O_3、DETDA、TDA进行检测和表征,揭示了它们的微观结构和内在规律性。XRD检测发现CeO_2掺杂量增多,CeO_2-CuO/ZnO/Al_2O_3衍射峰强度增强,提高了晶化程度,金属原子存在协同效应,增多了活性中心。FT-IR揭示了DETDA内部化学键键型,拥有甲基、亚甲基的多取代芳胺。DTG-DTA检测出的质量变化与热效应两种信息,DETDA的DTG-DTA曲线在66.0、271.0℃存在二个吸热峰,分别为氨基脱离苯环、DETDA的分解产生。通过1 H NMR对DETDA、TDA检测,得到DETDA、TDA的氢原子的数目分别为18和10,分子中各个氢核对应所归属的吸收峰,分别和它们分子式中的氢原子数目吻合。CeO_2-CuO/ZnO/Al_2O_3催化合成DETDA,反应条件温和,工艺流程简单,容易实现高效率和连续化工业生产,因此具有广阔的发展前景。
文摘A novel coprecipitation-reduction process has been proposed for preparing highly selective Cu/ZnO/Al 2O 3 catalysts for methanol synthesis from CO 2 hydrogenation. Compared to the catalysts prepared by the conventional method, the new catalysts prepared via the new method exhibit much higher BET surface area and pore size, much smaller crystallite size and higher catalytic activity and selectivity in CO 2 hydrogenation to methanol. It is also found that the molar ratio of Cu + to Cu 0 on the surface of the catalyst obtained by coprecipitation-reduction is much higher than that on the reduced catalyst obtained by the conventional method, which could be crucial for its high activity and selectivity for catalytic hydrogenation of CO 2 to methanol.
文摘Hydrogen production by catalytic steam reforming of methanol over a series of coprecipitated Cu/ZnO/Al2O3 catalysts under atmospheric pressure in a microreactor has been studied Effects of catalyst composition, reaction temperature and activation conditions on the catalytic activity have been investigated Crystal phases of catalysts were analyzed by XRD The results showed that Cu/ZnO/Al2O3 catalysts displayed high activity and selectivity for hydrogen and stability The optimized molar ratio is Cu/Zn=10, a maximum methanol conversion of 994?mol%, hydrogen selectivity of 999?mol% and CO molar fraction of 0007% were obtained in the steam reforming reaction with the catalyst containing 45?mol% copper XRD results showed that the diffraction peaks of CuO in the catalyst were clearly lower and broaden It indicated that high dispersion of small copper crystallites on the catalyst surface was formed under the calcination conditions It is suggested that the good performance of Cu/ZnO/Al2O3 catalysts partly resulted from well dispersed
文摘We demonstrate for the first time that a short time of microwave irradiation on the oxide precursor of a Cu/ZnO/Al2O3 catalyst can provide unique opportunity for tailoring the microstructure and activity of the catalyst for methanol steam reforming. It is shown by in situ XRD that a considerable increase in the microstrain of Cu nanocrystals could be achieved in the catalysts processed by microwave irradiation for 310 min, which correlates well with the enhanced CH3OH conversion as observed on the corresponding samples. The present work also confirms that although the high specific surface area of Cu is a prerequisite for catalytic activity, it does not account for the observed changes in activity and selectivity alone without taking bulk microstructural changes into account.
