降解CTMABr组装介-微孔分子筛的实验研究

通过考察实验影响因素以在最佳条件合成一种具有潜在应用价值的高水热稳定性材料。通过降解NaY分子筛形成其前驱体,以CTMABr(十六烷基三甲基溴化铵)为模板剂合成介-微孔分子筛。XRD和FT IR表征结果表明材料的孔壁含有沸石结构单元,在750?℃,100%水蒸汽中处理2?h后介孔结构依然存在。研究认为在最佳条件下合成的材料是一种高水热稳定性的孔壁含有沸石结构单元的介孔材料,且与直接制备分子筛前驱体的过程相比,降解微孔分子筛制备前驱体有沸石回收和成本低廉两方面的优点。     

强酸性和水热稳定的MCM-41分子筛的合成

以ZSM 5沸石分子筛为原始硅铝源,在碱性条件下,通过水热法合成出了孔壁含有ZSM 5预结构单元的MCM 41介孔分子筛。采用XRD、N2 吸附脱附、FT IR和NH3 TPD等表征手段对样品进行分析,结果表明该分子筛是含有ZSM 5 沸石预结构单元的六方晶相结构,该介孔分子筛的孔壁明显厚于常规方法合成的MCM 41,具有较高的水热稳定性和较强的酸性。     

在低表面活性剂浓度下合成含Y沸石次级结构单元的介孔分子筛

以表面Mol比很低(xsurf／xSiO2=0．07)的阳离子表面活性剂十六烷基三甲基溴化铵(CTAB)和阴离子表面活性剂(SL)的混合水溶液为模板，以具有Y沸石次级结构单元的溶胶为前驱体，在碱性条件下合成了孔道结构类似于MCM-41的介孔分子筛，样品的XRD、FT—IR、N2吸附-脱附、SEM等表征表明合成的介孔分子筛是孔壁含Y沸石次级结构单元的六角相结构，该介孔分子筛的孔壁厚于常规水热方法得到的MCM-41材料的孔壁，它的形貌有别于常规水热方法得到的MCM—41的疏松形貌，为网状交叉结构。对样品水热稳定性的考察显示，在600℃ 100％水蒸气下处理10h，仍然可以保持其中孔结构。     

用ZSM-5降解液进行SBA-15分子筛合成的研究

以商用ZSM-5沸石为原料,采用降解法合成了孔壁含有沸石结构单元的Z-SBA-15介孔分子筛。利用XRD、TEM技术,考察了温度、时间、ZSM-5的硅铝比、降解液用量和初始凝胶pH值对合成产物的影响。结果表明:在晶化温度100～110℃,晶化时间36～48h,硅铝比为25～36,ZSM-5沸石降解液量15～30mL,初始凝胶pH值0.5～1.0时为合成适宜条件。此外,经Z-SBA-15样品结构分析,Z-SBA-15为具有Al—Si—O单元结构成分的SBA-15介孔材料。     

MCM-41/HY介-微孔复合分子筛的合成与表征

以介孔MCM-41凝胶为母液,通过滴加HY浆液,应用水热反应釜合成了一种介-微孔复合分子筛MCM-41/HY.通过XRD、BET、NH3-TPD等手段对复合材料进行了表征,并对复合分子筛的水热稳定性进行了考察.结果表明,复合材料同时具有介孔分子筛MCM-41和微孔HY型沸石的特征,并且和纯MCM-41分子筛相比,复合分子筛的酸性明显增强,水热稳定性显著提高.     

气相水解法介孔分子筛MCM-41组装纳米TiO2研究

以水玻璃为硅源,表面活性剂十六烷基三甲基溴化铵为结构模板剂,合成出MCM-41介孔分子筛,并以钛酸丁酯为前驱体,在高温气相炉中进行水解,羟基缩合对介孔分子筛MCM-41进行了纳米TiO2的修饰。XRD、FTIR、N2吸附脱附、SEM表征手段对其结构特征的测试结果表明:纳米TiO2不仅进入介孔分子筛MCM-41介孔孔道,较均匀地修饰了介孔分子筛MCM-41的孔壁,而且使介孔分子筛MCM-41能够保持有序的孔道结构。     

碱处理法制备微孔 介孔ZSM-5分子筛及其在苯酚叔丁醇烷基化反应中的应用#br#

首先, 以微孔结构的ZSM-5沸石为前驱物, 经碱液处理不同时间后与介孔模板剂十六烷基三甲基溴化铵（CTAB）混合, 水热处理后制备微孔-介孔ZSM-5分子筛, 并用X射线衍射（XRD）、 Fourier变换红外光谱（FT-IR）、 N₂吸附 脱附和透射电镜（TEM）等方法表征微孔-介孔ZSM-5分子筛的理化性质. 其次, 将微孔 介孔ZSM-5分子筛作为苯酚叔丁醇烷基化反应的催化剂, 利用苯酚转化率与2,4-二叔丁基苯酚的选择性测试所得材料的催化性能. 结果表明: [JP2]碱处理1 h可获得微孔和介孔复合较好的ZSM-5, 且该催化剂具有较好的苯酚叔丁基化催化性能, 苯酚的转化率最高为86.2%, 大分子2,4 二叔丁基苯酚的选择性可达57.9%.     

碱处理法制备微孔-介孔ZSM-5分子筛及其在苯酚叔丁醇烷基化反应中的应用

首先,以微孔结构的ZSM-5沸石为前驱物,经碱液处理不同时间后与介孔模板剂十六烷基三甲基溴化铵(CTAB)混合,水热处理后制备微孔-介孔ZSM-5分子筛,并用X射线衍射(XRD)、Fourier变换红外光谱(FT-IR)、N2吸附-脱附和透射电镜(TEM)等方法表征微孔-介孔ZSM-5分子筛的理化性质.其次,将微孔-介孔ZSM-5分子筛作为苯酚叔丁醇烷基化反应的催化剂,利用苯酚转化率与2,4-二叔丁基苯酚的选择性测试所得材料的催化性能.结果表明:碱处理1h可获得微孔和介孔复合较好的ZSM-5,且该催化剂具有较好的苯酚叔丁基化催化性能,苯酚的转化率最高为86.2%,大分子2,4-二叔丁基苯酚的选择性可达57.9%.     

Y/SBA-15的微波水热法合成及其表征分析

研究了微波水热法合成微孔-介孔复合分子筛Y/SBA-15,以XRD为表征手段,考察了pH、二氧化硅与P123物质的量比、微波功率、搅拌速度和晶化温度等因素对复合分子筛结构的影响.经过研究确定了复合分子筛的合成条件:pH值为2.5,SiO2和P123物质的量比为58,微波功率为200W,搅拌速度为250r/min,晶化温度为120℃.采用氮气吸附脱附、透射电镜等分析方法对复合分子筛进行了表征分析,结果表明:合成产物同时具有微孔介孔结构特征,结晶度良好、短棒状大小均匀,微孔、介孔2种孔径分布均匀,平均孔径为4.050 13nm,孔壁厚度为2.2nm,BET孔容为0.350 525cm3/g.     

微孔——介孔复合分子筛的合成近况

微孔－介孔复合分子筛是近年来沸石研究人员颇感兴趣的一类新催化材料。概述了该类催化剂合成方法的进展情况，主要介绍了原位合成法和后合成法。     

Supramolecular self-assembled molecules as organic directing agent for synthesis of zeolites

Solid materials with uniform micropores, such as zeolites, can act as selective catalysts and adsorbents for molecular mixtures by separating those molecules small enough to enter their pores while leaving the larger molecules behind. Zeolite A is a microporous material with a high void volume. Despite its widespread industrial use in, for example, molecular separations and in detergency, its capability as a petroleum-refining material is limited owing to its poor acid-catalytic activity and hydrothermal stability, and its low hydrophobicity. These characteristics are ultimately a consequence of the low framework Si/Al ratio (normally around one) and the resulting high cationic fraction within the pores and cavities. Researchers have modified the properties of type-A zeolites by increasing the Si/Al compositions up to a ratio of three. Here we describe the synthesis of zeolite A structures exhibiting high Si/Al ratios up to infinity (pure silica). We synthesize these materials, named ITQ-29, using a supramolecular organic structure-directing agent obtained by the self-assembly, through pi-pi type interactions, of two identical organic cationic moieties. The highly hydrophobic pure-silica zeolite A can be used for hydrocarbon separations that avoid oligomerization reactions, whereas materials with high Si/Al ratios give excellent shape-selective cracking additives for increasing propylene yield in fluid catalytic cracking operations. We have also extended the use of our supramolecular structure-directing agents to the synthesis of a range of other zeolites.     

High-throughput synthesis and catalytic properties of a molecular sieve with 18- and 10-member rings

Crystalline molecular sieves with large pores and high adsorption capacities have many potential applications. Of these materials, zeolites are of particular interest owing to their stability in a wide range of experimental conditions. An aluminophosphate with very large circular channels(5) containing 18 oxygen atoms (18-ring channels) has been synthesized, but in the search for large-pore zeolites, most of the materials which have been synthesized up to now contain only 14-ring channels; the synthesis of zeolites with larger ring structures has been believed to be hindered by the low Si-O-Si bond angles available. A silicogaloaluminate (ECR-34) with unidirectional 18-ring channels was recently reported, but exhibited low micropore volume, thus rendering the material less attractive for catalytic applications. Here we report the structure and catalytic activity of the silicogermanate zeolite ITQ-33; this material exhibits straight large pore channels with circular openings of 18-rings along the c axis interconnected by a bidirectional system of 10-ring channels, yielding a structure with very large micropore volume. The conditions for synthesis are easily accessible, but are not typical, and were identified using high-throughput techniques.     

排水性聚氨酯稳定再生集料最佳胶石比与组份比

为了解决废旧路面材料再生利用问题,满足排水路面结构需要,制备了一种新型的排水性聚氨酯稳定再生碎石材料(简称PPSRA)。通过肯塔堡飞散试验、析漏试验、马歇尔试验与透水性试验,对PPSRA的胶石比范围,PPSRA的稳定度随胶石比、胶水组份比和孔隙率的变化规律以及透水性随孔隙率的变化规律进行研究。试验结果表明：PPSRA的胶石比范围为3%-5%,最佳胶石比为4%,最佳组份比为1:2.5,PPSRA的稳定度随着混合料孔隙率的增加而降低,渗透系数与孔隙率成线性正相关。     

表面修饰多孔微晶玻璃的制备及其对废水中钯(II)的吸附分离

以废玻璃为原材料, 制备表面修饰多孔微晶玻璃(Thio-aminopropyltriethoxysilane-modified porous glassceramics, TAMPG), 实现对水溶液中钯(II)的高效吸附分离。通过在废玻璃制成的多孔微晶玻璃上负载有机配体2-噻吩甲醛、2-巯基苯并咪唑和2-巯基苯并噻唑, 得到新型吸附剂TAMPG-1, TAMPG-2和TAMPG-3, 同时对钯(II)吸附过程的pH 值、温度、初始浓度和吸附时间等条件进行优化。由于原材料廉价易得, 吸附性能良好, 可循环使用, 同时具备优良的选择性和稳定性, 所以表面修饰多孔微晶玻璃既可以高效地分离钯(II), 也能产生良好的经济效益。     

Colossal cages in zeolitic imidazolate frameworks as selective carbon dioxide reservoirs

Zeolitic imidazolate frameworks (ZIFs) are porous crystalline materials with tetrahedral networks that resemble those of zeolites: transition metals (Zn, Co) replace tetrahedrally coordinated atoms (for example, Si), and imidazolate links replace oxygen bridges. A striking feature of these materials is that the structure adopted by a given ZIF is determined by link-link interactions, rather than by the structure directing agents used in zeolite synthesis. As a result, systematic variations of linker substituents have yielded many different ZIFs that exhibit known or predicted zeolite topologies. The materials are chemically and thermally stable, yet have the long-sought-after design flexibility offered by functionalized organic links and a high density of transition metal ions. Here we report the synthesis and characterization of two porous ZIFs-ZIF-95 and ZIF-100-with structures of a scale and complexity previously unknown in zeolites. The materials have complex cages that contain up to 264 vertices, and are constructed from as many as 7,524 atoms. As expected from the adsorption selectivity recently documented for other members of this materials family, both ZIFs selectively capture carbon dioxide from several different gas mixtures at room temperature, with ZIF-100 capable of storing 28 litres per litre of material at standard temperature and pressure. These characteristics, combined with their high thermal and chemical stability and ease of fabrication, make ZIFs promising candidate materials for strategies aimed at ameliorating increasing atmospheric carbon dioxide levels.     

Utilization of waste polyethylene terephthalate as a reducing agent in the reduction of iron ore composite pellets

The increasing consumption of plastics inevitably results in increasing amounts of waste plastics. Because of their long degradation periods, these wastes negatively affect the natural environment. Numerous studies have been conducted to recycle and eliminate waste plastics. The potential for recycling waste plastics in the iron and steel industry has been underestimated; the high C and H contents of plastics may make them suitable as alternative reductants in the reduction process of iron ore. This study aims to substitute plastic wastes for coal in reduction melting process and to investigate their performance during reduction at high temperature. We used a common type of waste plastic, polyethylene terephthalate (PET), because of its high carbon and hydrogen contents. Composite pellets containing PET wastes, coke, and magnetite iron ore were reduced at selected temperatures of 1400 and 1450°C for reduction time from 2 to 10 min to investigate the reduction melting behavior of these pellets. The results showed that an increased temperature and reduction time increased the reduction ratio of the pellets. The optimum experimental conditions for obtaining metallic iron (iron nuggets) were reduction at 1450°C for 10 min using composite pellets containing 60% PET and 40% coke.     

调吡脲生产废液中甲苯和2-氯-4-氨基吡啶的回收利用研究

对调吡脲(氯吡脲/CPPU)生产过程中产生的废液中的甲苯和2-氯-4-氨基吡啶进行了回收利用研究,考察和优化了处理条件,得到甲苯的最佳回收工艺路线:用0.1 mol/L硫酸处理液与废液按1∶30的质量比加热回流2 h,经分液、干燥、过滤、蒸馏后得到回收甲苯,经气相色谱检测,纯度为99.4%.进一步对处理过甲苯的废液进行2-氯-4-氨基吡啶的回收研究,得到2-氯-4-氨基吡啶回收的最佳工艺条件为:废液pH为12～13,萃取时间为6 min,进行萃取剂与废液体积比为2的5级错流萃取,回收率达到94%以上,经液相色谱检测,纯度达到97.5%,实现了废弃物资源化利用的目的.     

垃圾土降解规律及填埋场沉降计算分析

通过垃圾土有机物降解试验,提出垃圾土有机物降解规律的计算公式和参数确定方法,并推导了垃圾土沉降计算模型.以深圳下坪垃圾填埋场为例,根据试验材料中的有机物和降解残余物含量以及特征降解时间,计算得到降解速率和降解量随时间变化规律.实例分析表明:变形计算模型能够反映压缩和降解引起垃圾土的变形特性.     

新型混凝剂聚合氯化铝钙的合成及其初步应用

以Al2O3和CaCO3为原料在高温下进行焙烧后酸溶、聚合、干燥制备了新型的无机高效混凝剂聚合氯化铝钙,并对其合成条件进行了详细的研究,结果表明:最佳的原料配比(Al2O3∶CaCO3)为3∶2,提高焙烧温度利于产品的合成,最佳酸溶时间为3h·对合成的聚合氯化铝钙在废水处理中的应用进行了初步研究,取得了满意的效果·