表面润湿法合成β沸石体系中晶种作用的研究

系统研究了表面润湿法合成β沸石的体系中,干晶种、润湿态晶种、异晶晶种(Y沸石、ZSM 5沸石)以及碱处理β沸石晶种在此晶化体系中的作用.采用β沸石产品及异晶作晶种时,可使产品的相对结晶度稍有提高,但对沸石微晶核的结构导向作用不明显.经浓碱液处理20min后的β沸石产品(碱处理晶种)作晶种引入晶化体系后,可以显著提高产品的相对结晶度,降低模板剂的用量,缩短晶化诱导期,成为表面润湿法合成β沸石体系的有效晶种形式.     

Electrochemical Characterizations of NaY Zeolite-Entrapped Copper Dicyanoanthraquinone Diimines

Intrazeolite copper dicyanoanthraquinone diimines (NaY/Cu(DCNAQI) were synthesized within NaY zeolite using a “ship-in-a-bottle” technique. These particles were subjected to CV and EIS characterizations based on their associated particulate electrodes. Analysis of the EIS over a wide range of frequency and at potentials around the formal potential of DCNAQI^0/? showed that the charge transfer resistance and the double layer capacitance in the equivalent circuit based on the Fletcher transmission lines were sensitive to the probing potential and the concentration of the free DCNAQI coexisting in the electrolyte solutions. Although CV does not provide much information about the influence of hydrogen on NaY/Cu(DCNAQI), the EIS characterizations suggested hydrogen can significantly accelerate the charge transfer kinetics for most NaY/Cu(DCNAQI) particles.     

Adsorption of Benzene on the Potassium Exchanged Hbeta Zeolites

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Laser oscillation in 5-cm Nd-doped silica fiber fabricated by zeolite method

We have demonstrated a laser oscillation in the highest concentration and the shortest Nd-doped silica fiber, an only 5-cm multimode Nd-doped silica fiber. This fiber-core glass was fabricated by the zeolite method, and the glass contained 1.25 wt.% of Nd₂O₃, which is 10 times higher than previously reported Nd-doped silica fiber. The laser output power was 10 mW at 1062 nm, and the threshold power and slope efficiency of the laser oscillation was 1.39 W and 2.4%, respectively.     

Catalytic Hydration of Aromatic Alkynes to Ketones over H-MFI Zeolites

The hydration of alkyne represents the most straightforward and simplest route toward the synthesis of ketone. Herein, Brønsted acidic zeolites are explored as potential catalysts for the liquid-phase phenylacetylene hydration. The topology structure and Si/Al ratio are disclosed to be key factors controlling the catalytic activity of zeolites. Typically, H-MFI zeolite with a Si/Al molar ratio of 13 exhibits the highest catalytic activity, with turnover frequency of 6.0 h^-1 at 363 K. Besides, H-MFI zeolite shows good catalytic stability and recyclability in the reaction of phenylacetylene hydration, and the substrate scope can be simply extended to other soluble aromatic alkynes. The reaction mechanism of phenylacetylene hydration is investigated by means of kinetic and spectroscopic analyses. The Markovnikov electrophilic addition of phenylacetylene by hydrated protons is established as the rate-determining step, followed by deprotonation and enol isomerization to derive acetophenone product.     

基于科学核心观念建构的高中化学创新实验研究——以“多彩氧化亚铜纳米粒子的制备”为例

介绍了基于科学核心观念建构下制备多彩氧化亚铜纳米粒子的学生实验。利用葡萄糖还原班氏试剂的方法制备了氧化亚铜纳米粒子,并观察和讨论了不同条件下制备的粒子的颜色和粒径。整个实验安全、简单、现象明显、试剂用量少。本研究通过让学生参与科研的全过程,培养了学生的创新能力,促进了科学核心观念的建构。     

Methane activation over Ag-exchanged ZSM-5 zeolites: A theoretical study

Methane activation catalyzed over Ag-exchanged ZSM-5 zeolites was investigated by using the density functional theory (DFT) with a cluster model. Two different pathways were taken into account in this work: the “alkyl” and the “carbenium” pathways. The activation barriers obtained are 34.09 and 66.63 kcal/mol for the “alkyl” and the “carbenium” pathway, respectively. The calculated results show that the activation barrier of the “alkyl” pathway is smaller than that of “carbenium” pathway. Consequently, the “alkyl” pathway is the preferential reaction pathway. A new mechanism of methane conversion in the presence of ethene was proposed. In the catalytic cycle, the initial step of methane activation proceeds with the “alkyl” pathway and the Ag⁺ cation acts as an acceptor of the methyl group, then ethene reacts with the Ag⁺CH₃⁻ group to form propene. In addition, it is found that the Ag⁺ cations play an important role in the methane activation, compared with the reaction of methane activation over H-ZSM-5.     

共沉淀法制备纳米多晶La2／3Sr1／3MnO3及其低场磁电阻性质

利用共沉淀法制备了纳米多晶La2/3Sr1/3MnO3粉体,并研究了相应烧结陶瓷的相结构、显微形貌、电性质以及磁电阻效应.样品中存在高密的晶界,对电子的疏运过程产生明显的散射作用,从而使得样品具有较大的电阻值,并且只有当烧结温度大于800℃时才出现金属绝缘体温度相变.样品的磁电阻是低场磁电阻效应,源于晶界处电子的自旋极化隧穿.烧结温度越低的样品,其磁电阻越大.     

The effect of triethyl citrate on the dispersibility and water vapor sorption behavior of polylactic acid/zeolite composites

The aim of this study was to investigate the water vapor adsorption behavior and mechanical properties of poly (lactic acid) (PLA)/zeolite (5, 10, or 15 phr) composites prepared with triethyl citrate (TEC; 20 phr) via a melting process. TEC was used to improve the flexibility of the PLA and the dispersibility of the zeolite in TEC-zeolite suspensions that were ultra-sonicated. It was found that zeolite was uniformly dispersed in the PLA matrix, and the interfacial adhesion between the PLA matrix and zeolite was enhanced by TEC. In addition, the tensile strengths and Young's modulus of the composites improved with increasing zeolite content. The PLA/zeolite composites prepared with TEC had increased water vapor permeability and contact angles compared to neat PLA and standard PLA/zeolite due to the presence of TEC. In particular, TEC accelerated the hydrolysis of the PLA surface in a high humidity environment, resulting in an improvement in water vapor sorption capacity. At the same zeolite content of 15 phr, the equilibrium moisture content (EMC) values of PLA/zeolite films prepared with TEC increased by up to 39.25 mg/g whereas those prepared without TEC only increased by up to 24.33 mg/g. The results suggest the possibility of applying PLA/zeolite films prepared with TEC as a flexible active packaging material.     

Ultrasound-assisted regeneration of zeolite/water adsorption pair

The use of ultrasound to enhance the regeneration of zeolite 13X for efficient utilization of thermal energy was investigated as a substitute to conventional heating methods. The effects of ultrasonic power and frequency on the desorption of water from zeolite 13X were analyzed to optimize the desorption efficiency. To determine and justify the effectiveness of incorporating ultrasound from an energy-savings point of view, an approach of constant overall input power of 20 or 25 W was adopted. To measure the extent of the effectiveness of using ultrasound, the ultrasonic-power-to-total power ratios of 0.2, 0.25, 0.4 and 0.5 were investigated and the results compared with those of no-ultrasound (heat only) at the same total power. To analyze the effect of ultrasonic frequency, identical experiments were performed at three nominal ultrasonic frequencies of ~28, 40 and 80 kHz. The experimental results showed that using ultrasound enhances the regeneration of zeolite 13X at all the aforementioned power ratios and frequencies without increasing the total input power. With regard to energy consumption, the highest energy-savings power ratio (0.25) resulted in a 24% reduction in required input energy and with an increase in ultrasonic power, i.e. an increase in acoustic-to-total power ratio, the effectiveness of applying ultrasound decreased drastically. At a power ratio of 0.2, the time required for regeneration was reduced by 23.8% compared to the heat-only process under the same experimental conditions. In terms of ultrasonic frequency, lower frequencies resulted in higher efficiency and energy savings, and it was concluded that the effect of ultrasonic radiation becomes more significant at lower ultrasonic frequencies. The observed inverse proportionality between the frequency and ultrasound-assisted desorption enhancement suggests that acoustic dissipation is not a significant mechanism to enhance mass transfer, but rather other mechanisms must be considered.