丙烷脱氢反应中焙烧温度和反应气氛对 Pt-Sn/SAPO-34 催化性能的影响

 在不同的焙烧温度下制备了 Pt-Sn/SAPO-34 催化剂, 并使用 X 射线衍射、N2 吸附、X 射线荧光光谱、O2 脉冲烧炭、H2 程序升温还原和透射电镜等手段对催化剂进行了表征. 在微型反应器中评价了 Pt-Sn/SAPO-34 催化剂对丙烷脱氢制丙烯反应的催化性能, 考察了焙烧温度和反应气氛对催化剂性能的影响. 结果表明, 焙烧温度为 500 oC 时, 催化剂具有最佳的反应活性. 当焙烧温度高于 500 oC 时, 催化剂出现不希望的表面变化, 例如活性 Pt 位点的聚集、Pt 的团聚、Sn 的流失等. 当反应温度为 595 oC 时, Pt-Sn/SAPO-34 催化性能稳定, 且能够保持表面金属状态.     

煅烧温度对Cu掺杂ZnO纳米粉体的制备及发光性能的影响

在PVA溶液中制备ZnO∶Cu纳米粉体的前驱体,经过煅烧获得ZnO∶Cu纳米粉体,考察煅烧温度对制备过程及发光性能的影响。利用XRD、TEM分析了产物的结构和形貌,XRD分析结果表明,当煅烧温度高于500℃时,可以使PVA完全分解,制备出具有六角纤锌矿结构的ZnO∶Cu粉体。TEM结果表明,粉体呈球形,大小均匀,分散性好,平均粒径为20～25 nm。在342 nm波长光的激发下,在ZnO∶Cu的室温PL光谱中可以观察到两个中心波长位于458 nm和486 nm的较强的蓝光发射峰,经400℃煅烧处理的ZnO∶Cu纳米粉体的蓝光发射最强。煅烧后的ZnO∶Cu只有微弱的绿光发射(510～530 nm),Cu的掺杂使ZnO的绿光发射变为蓝光发射。蓝紫光的发射波长随煅烧温度的升高产生明显的红移,由300℃时的404 nm红移至600℃时的422nm,发射强度随温度升高先增大后减小。     

Electrospinning preparation of NiO/ZnO composite nanofibers for photodegradation of binary mixture of rhodamine B and methylene blue in aqueous solution: Central composite optimization

One‐dimensional nanofiber of p‐type NiO/n‐type ZnO heterojunctions with various molar ratios of Ni to Zn at different calcination temperatures were successfully synthesized using the electrospinning method, and they were fully characterized. The photocatalysts thus obtained were applied in aqueous solutions for rhodamine B (RDB) and methylene blue (MB) degradation. The p–n heterojunctions built among the cubic structure NiO and hexagonal structure ZnO in the composite nanofiber are responsible for generation of electrons and holes and subsequently superoxide and hydroxyl radical production by carriers which lead to degradation of the dyes in solution. The composite nanofibers (ZnNi1) calcined at 550 °C for 3 h showed the highest photocatalytic activity for degradation of the dyes in aqueous solution. The optimum values were found to be 180 min, 7.0, 1 g l^?1 and 3.0 and 3.0 mg l^?1 for irradiation time, pH, photocatalyst dosage and initial concentration of RDB and MB, respectively. For these optimum conditions, the photocatalytic degradation of RDB and MB was found to be 99.37 and 98.44%, respectively. The maximum photodegradation of RDB and MB using ZnNi1 was 59.41 and 65.43%, respectively. First‐order kinetics based on the Langmuir–Hinshelwood model successfully fitted the experimental data.     

Influence of the Template Removal Method on the Mechanical Stability of SBA-15

Removing the template from the pores after the polycondensation of the silica precursor is a necessary step in the synthesis of mesoporous silica materials. In our previous work, we developed a method for the efficient and spatially controlled functionalization of SBA-15. First, the silanol groups on the particle surface and in the pore entrances were passivated. After extraction of the template, a pretreatment step in N₂ converted the silanol groups to the single and geminal state. Afterwards, an azide functionality was introduced exclusively into the mesopores. This ensured that the catalyst could afterwards be immobilized unambiguously in the mesopores. The mechanical stability of a material functionalized in such a spatially controlled manner is studied and compared to other template removal methods. Even though several studies investigated the influence of the calcination temperature, the presence or the absence of oxygen during the template removal, the specific conditions used during the herein reported selective functionalization procedure have not been covered yet.     

Influence of Drying and Calcination on Remaining Amount and Immobile Character of Titanium on Titanium‐pillared Montmorillonite

Remove of titanium (Ti) from titanium‐pillared montmorillont (TIPM) is not expected during its application as adsorbent and photocatalyst, etc. But studies on immobilization of Ti on TIPM are seldom reported. In this work, TIPM was synthesized from TiCl₄ and Na⁺‐montmorillont (Na⁺‐MMT). Then the prepared TIPM was heated at different temperatures (100, 240 and 450°C) to yield three TIPM samples (TIPM1, TIPM2, and TIPM3). Inductively coupled plasma optical emission spectrometer (ICP‐OES) was used to determine the effect of heating temperature on the remaining amount of Ti on TIPMs. A two‐step treatment method which is often used in the pretreatment and application of TIPM was developed to investigate the immobile character of Ti on TIPMs. X‐ray diffraction (XRD), Fourier transform infrared spectroscopy (FT‐IR), N₂ adsorption/desorption isotherm, thermogravimetric analysis and differential scanning calorimetry (TG‐DSC) were also used to characterize TIPMs before and after the treatment. The results show that with an increase in heating temperature, the amount of Ti species remained on TIPM decreases gradually and Ti immobilization is strengthened on TIPM. For TIPM3, less than 2% Ti is removed from TIPM3 after the treatment required to simulate the practical conditions of TIPM in its application, while those of TIPM1 and TIPM2 are 6.6% and 8.4%, respectively. The reason may be that when TIPM is heated, Ti species intercalated into MMT become chemically bonded with the framework of MMT and partially migrate into the layer structure, which make Ti immobile on TIPM firmly during the treatment process.     

Efficient conversion of fructose to 5‐hydroxymethylfurfural by functionalized γ‐Al2O3 beads

Millimeter size γ‐Al₂O₃ beads were prepared by alginate assisted sol–gel method and grafting organic groups with propyl sulfonic acid and alkyl groups as functionalized γ‐Al₂O₃ bead catalysts for fructose dehydration to 5‐hydroxymethylfurfural (5‐HMF). Experiment results showed that the porous structure of γ‐Al₂O₃ beads was favorable to the loading and dispersion of active components, and had an obvious effect on the properties of the catalyst. The lower calcination temperature of γ‐Al₂O₃ beads increased the specific surface area, the hydrophobicity and the activity of catalysts. Competition between the reaction of alkyl groups and ‐SH groups with surface hydroxyl during the preparation process of the catalyst influenced greatly the acid site densities, hydrophobic properties and activity of the catalyst. With an increase in the alkyl group chain, the hydrophobicity of catalysts increased obviously and the activity of the catalyst was enhanced. The most hydrophobic catalyst C₁₆‐SO₃H‐γ‐Al₂O₃–650°C exhibited the highest yield of 5‐HMF (84%) under the following reaction conditions: reaction medium of dimethylsulfoxide/H₂O (V/V, 4:1), catalyst amount of 30 mg, temperature of 110°C and reaction time of 4 hr.     

Pt2+/Pt0掺杂g-C3N4光催化降解环丙沙星和偶氮染料

以三聚氰胺和氯铂酸(H2PtCl6·6H2O)为原材料,采用简单一步煅烧法制备了不同含量的Pt^2+/Pt^0掺杂石墨相氮化碳(Pt^2+/Pt^0-CN)。运用扫描电镜、透射电子显微镜、X射线光电子能谱、X射线粉末衍射、N2物理吸附-脱附、紫外-可见漫反射光谱和光电流测试等技术对制备的样品的形貌、化学组成、晶体结构、比表面积和光电性能等物理化学性质进行了表征。由XPS可知Pt粒子以二价Pt和零价Pt掺杂在催化剂的表面和内部,其中Pt^0与Pt^2+的比约为1∶7.26。与g-C3N4相比,Pt^2+/Pt^0-CN表现出高效的光催化降解活性。当Pt^2+/Pt^0理论负载质量分数为0.02%时,对环丙沙星、罗丹明B、酸性橙Ⅱ、甲基橙和亚甲基蓝的降解效率分别提升了43%、64%、39%、42%和52%。Pt^2+/Pt0掺杂使催化剂的比表面积大幅度增加,同时增强光催化剂对光的吸收能力,并抑制光生电子(e^-)和空穴(h^+)的复合。     

焙烧温度对费托合成铁基催化剂还原动力学的影响

采用沉淀法和喷雾干燥技术制备了一个典型的费托合成铁基催化剂(100Fe/3K/6SiO_2,质量比)所得样品在不同温度下焙烧5 h.分别利用N_2吸附和穆斯保尔谱表征了催化剂的织构和物相性质,同时利用热重分析仪记录了催化剂在H2气氛中的还原过程,并利用气固反应模型对还原曲线进行了动力学模拟.结果表明,300~600℃焙烧后催化剂的还原过程可用相同的模型拟合,其中由α-Fe_2O_3还原为Fe_3O_4的过程可用一维晶相形成与生长模型或三维相界面反应模型描述,Fe_3O_4还原为α-Fe的过程受二维晶相形成与生长模型控制.而对于700℃焙烧后的催化剂,其还原过程可能受晶相形成与生长模型和收缩核模型共同影响.随着焙烧温度的提高,催化剂的还原能力减弱,还原过程活化能升高.这可能是由于焙烧温度的提高导致晶粒尺寸增大和晶格缺陷减少所致.     

预处理条件对一步法合成吲哚用Ag/SiO2催化剂活性的影响

 以简单浸渍法制备的Ag/SiO2催化剂对苯胺和乙二醇一步法合成吲哚具有很高的催化活性. 研究了预处理条件对催化剂活性的影响. 结果表明,采用程序升温法将催化剂前体在500 ℃焙烧4 h,并在低于150 ℃时用H2-N2混合气(H2含量低于50%)原位还原得到的Ag/SiO2催化剂活性较高; TEM和XRD结果表明,预处理后催化剂表面银晶粒较小,结晶度较低.