高铁高砂煤矸石合成4A沸石分子筛

以六盘水矿区的高铁高砂煤矸石为原料合成4A沸石分子筛,将煤矸石低温焙烧、盐酸酸浸除铁、高温焙烧后再碱融活化获得了活性原料,最后采用水热晶化的方法,合成了4A沸石分子筛产品.本研究采用单因素实验的方法,考察了合成条件对4A沸石分子筛性能的影响,并运用XRD和SEM对产品进行了表征,结果表明所得产品为4A沸石分子筛,粒度分...     

新型膜状金纳米活性基底的制备及拉曼光谱增强研究

贵金属纳米粒子作为增强基底已经广泛应用于表面增强拉曼光谱(SERS)研究,传统的贵金属纳米基底在制备方法、增强能力、准确性等方面仍有待改进和提高。采用一种简易、高效的方法制备出了一种具有膜状结构的新型金纳米增强基底：以聚乙烯吡咯烷酮(PVP)作保护剂和粘结剂,通过化学还原法制备金纳米基底。实验考察了还原剂种类、反应温度、体系pH和柠檬酸钠浓度对反应的影响,制备出增强效果最佳的新型膜状金纳米基底。利用罗丹明B作为探针分子,考察基底的SERS特征,其增强因子可达6.5×105。利用扫描电镜(SEM)对纳米粒子的结构进行了表征,结果表明其具有膜状结构,且比表面积大,利于分子的吸附。相比于传统的贵金属纳米基底,该实验所制备的新型膜状金纳米基底增强效果更佳、灵敏度和准确度更高,具有很大的应用前景。     

生物质催化转化制取芳香化合物

利用分子筛催化剂(NaZSM-5、HZSM-5、ReY和HY)研究了木屑上催化裂解制取芳香物(苯、甲苯、二甲苯)的反应过程,发现HZSM-5催化剂具有最高的生物质裂解制备芳香化合物的活性. 在450 oC、 载气流速为300 mL/min和催化剂/木屑比为2的优化反应条件下,芳香化合物的产率和选择性分别达到26.5%和62.5C-mol%.     

A variable temperature infrared spectroscopy study of NaA zeolite dehydration

Variable temperature diffuse reflectance infrared spectroscopy is used to monitor the dehydration of sodium Linde type A zeolite (NaA). Between ambient temperature and 423 K, water desorbs from NaA α-cages. At 423 K, remaining NaA water molecules are primarily confined to β-cages. Variable temperature infrared difference spectra band shape and intensity trends reflect the influence of water-Na⁺ interactions and hydrogen bonding on α-cage water desorption mechanisms. Difference spectrum variations suggest that water loss is accompanied by rearrangement of the remaining NaA water molecules to establish new interactions and minimize potential energies. Water molecules that do not interact with Na⁺ form multiple water-water hydrogen bonds and attain near bulk water configurations. These waters desorb at the lowest temperatures. Most α-cage waters are involved in Na⁺ interactions. These water molecules participate in hydrogen bonding with neighboring water molecules, but opportunities diminish with increased dehydration, resulting in systematic temperature-dependent vibrational spectrum changes.     

Synthesis,characterization and CO2 adsorption of NaA,NaX and NaZSM-5 from rice husk ash

NaA, NaX and NaZSM-5 zeolites were prepared by using silica extracted from rice hull ash as a raw material, and they were investigated for CO₂ adsorption performance as an adsorbent in order to solve the problem of suppressing the global warming. Three zeolites were synthesized by hydrothermal methods with seed technology, and a series of characterization methods, including XRD, FTIR, nitrogen adsorption-desorption and SEM, were used to demonstrate their advantages compared to traditional hydrothermal methods. The maximum equilibrium adsorption capacity of NaA-RS, NaX-RS and NaZSM-5-RS was 1.46, 3.12 and 2.20 mmol/g at 0 °C and 101.3 kPa, respectively. The CO₂ and N₂ adsorption isotherms recorded at different temperatures were perfectly fitted by the Dual-site Langmuir model. The CO₂/N₂ selectivity and Henry's law constants were calculated to demonstrate that the samples have a stronger affinity for CO₂, especially at low pressures. The isosteric heat of CO₂ and N₂ adsorption of the three zeolites was calculated, which was indicated that they were in an excellent potential for adsorption and separation of CO₂ in industrial flue gas.     

焙烧对HZSM－5分子筛结构的影响

运用魔角自转固态核磁共振谱（ＭＡＳ－ＮＭＲ），研究了焙烧对ＨＺＳＭ－５分子筛结构的影响．结果表明，高温焙烧将引起ＨＺＳＭ－５分子筛骨架的脱铝，当焙烧温度从５００℃增加到７００℃时，ＨＺＳＭ－５的骨架Ｓｉ／Ａｌ比由１６．７增加至２２．７；而当焙烧温度由７００℃到８００℃时，骨架Ｓｉ／Ａｌ比则由２２．７增加到了４８．５．２７Ａｌ－ＭＡＳＮＭＲ结果表明，从骨架上脱下来的铝，部分地形成了ＮＭＲ不可见的无定形态．随着焙烧温度的升高，ＮＭＲ不可见铝增多     

Rational Positioning of Metal Ions to Stabilize Open Tin Sites in Beta Zeolite for Catalytic Conversion of Sugars

Via hydrothermal synthesis of Sn-Al gels, mild dealumination and ion exchange, a bimetallic Sn-Ni-Beta catalyst was prepared which can convert glucose to methyl lactate (MLA) and methyl vinyl glycolate (MVG) in methanol at yields of 71.2 % and 10.2 %, respectively. Results from solid-state magic-angle spinning nuclear magnetic resonance, X-ray photoelectron spectroscopy, transmission electron microscopy, spectroscopic analysis, probe-temperature-programmed desorption, and density functional theory calculations conclusively reveal that the openness of the Sn sites, such as by the formation of [(SiO)₃−Sn−OH] entities, is governed by an adjacent metal cation such as Ni²⁺, Co²⁺, and Mn²⁺. This relies on the low structure-defective pore channel, provided by the current synthesis scheme, and the specific silica hydroxyl anchor point is associated with the incorporation of Sn for additional and precise metal ion localization. The presence of metal cations significantly improved the catalytic performance of Sn-Ni-Beta for glucose isomerization and conversion to MLA of sugar compared with Sn-Beta.     

NaY zeolite functionalized by sulfamic acid/Cu(OAc)2 as a new and reusable heterogeneous hybrid catalyst for efficient solvent-free formylation of amines

NaY zeolite functionalized by sulfamic acid/Cu(OAc)_2[NaY/SA/Cu(Ⅱ)] was synthesized and used as a new,efficient and recyclable catalyst for preparation of formamides. This novel organic-inorganic hybrid catalyst was characterized by several techniques such as FT-IR, XRD, SEM, EDX and TG analysis.Chemoselectivity, easy procedure, excellent yields, very short reaction times, solvent-free and mild reaction conditions are some benefits of this new protocol.     

Y型沸石脱铝机制和铝状态的NMR研究

对Y型沸石原粉及几种不同脱铝样品进行了几种不同NMR方法的测量,确定了不同处理过程的脱铝机制和骨架内外铝状态的变化,²⁹Si MAS NMR谱给出了骨架Si、Al分布的信息,反映了不同方法处理样品其脱铝机制的差异,据此可以控制Y沸石脱铝过程获得更高的硅铝比,²⁷Al MAS NMR谱、二维章动NMR及¹H-²⁷Al CP/MAS NMR测量表明:水热处理的Y沸石中存在4种不同的铝状态。综合²⁹Si和²⁷Al MAS NMR观测,可相当程度地推断Y型沸石分子筛脱铝改性所发生的内部过程。     

分子筛和担体中主含量元素和杂质元素的同时测定

本文研究了用微波消化试样，ICP－AES法同时测定分子筛及担体中的主含量元素Si、Al和杂质元素Fe、Na、Ca、Mg的方法。相对标准偏差：Si、Al＜2％，Fe、Na、Ca、Mg≤4％，杂质元素回收率为97％－107％。方法快速，简便、准确，可靠。