首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 78 毫秒
1.
羟基铝柱撑二硫化钼的制备及其催化加氢性能   总被引:6,自引:0,他引:6  
 采用单分子层技术将羟基铝聚合物Al7+13阳离子嵌入到二硫化钼板层间,得到层间距为1.488~1.599 nm的柱撑复合材料. X射线粉末衍射等研究表明,羟基铝聚合物Al7+13经60 ℃恒温陈化2 d即可作为稳定的柱撑液使用; 在柱撑反应体系中,较小的Al/Mo摩尔比有利于获得客体物种较均一和结晶度较好的柱撑复合材料. 与原料 2H-MoS2 相比,柱撑二硫化钼的层间距增大,晶粒变小,比表面积增加. 差示扫描量热分析结果表明,柱撑材料具有较好的热稳定性. 选择苯饱和加氢反应为探针,测定了柱撑材料的催化活性. 气相色谱测定结果表明,柱撑二硫化钼的催化性能显著优于未柱撑的 2H-MoS2 和Raney Ni催化剂. 这与柱撑材料比表面积的增大、可能存在的缺陷增多而导致活性位增多以及对氢气的有效吸附增加有关.  相似文献   

2.
张进飞  林碧洲  孙东亚  许百环  丁聪 《催化学报》2006,27(12):1133-1138
 采用单分子层技术将羟基铬聚合离子[Cr4(OH)6(H2O)10]6+嵌入到二硫化钼板层间,得到层间距为1.319~1.341 nm的柱撑复合材料. X射线粉末衍射表明,羟基铬聚合物溶液经70 ℃恒温下陈化4 d即可作为稳定的柱撑液使用; 在柱撑反应体系中,较小的n(Cr)/n(Mo)比和较低的Cr3+浓度有利于获得结晶度较好的柱撑材料. 与原料2H-MoS2相比,柱撑材料的层间距增大,晶粒变小,比表面积增加并且热稳定性提高. 对催化苯饱和加氢反应表明,柱撑材料Cr-MoS2的催化活性明显优于未柱撑的2H-MoS2和Raney Ni催化剂,且结晶度较好的柱撑材料更具有较高的催化活性和较好的可重复性.  相似文献   

3.
锆钇柱撑蒙脱土负载Pd催化剂的催化性能研究   总被引:1,自引:0,他引:1  
合成了锆钇柱撑蒙脱土(Zr-Y-MMT)载体,并用于丙酮、甲苯和乙酸乙酯的催化氧化。通过XRD、TEM及N2吸附-脱附技术对Zr-Y-MMT载体和负载Pd催化剂(Pd/Zr-Y-MMT)进行了表征。XRD结果显示,经锆钇柱撑后蒙脱土的层间距由1.27 nm增大至1.78 nm;N2吸脱附结果表明,经锆钇柱撑后,其比表面积有了很大的增加,由62 m2·g-1增大至395 m2·g-1。活性评价结果发现,Zr-Y-MMT载体比Na-MMT有更好的催化活性,其完全氧化丙酮、甲苯和乙酸乙酯的温度分别为320 ℃、350 ℃和290 ℃。此外,当此载体上负载0.1wt%Pd时,其用于完全氧化甲苯的活性有了明显的改进。  相似文献   

4.
制备了一系列羟基铁柱撑蒙脱土-δ-MnO2复合材料,采用X射线粉末衍射(XRD)、比表面积(SBET)及扫描电子显微镜(SEM)研究其结构特征。结果显示:钙基蒙脱土的层间距为1.47nm,经过柱撑之后,羟基铁撑蒙脱土的层间距增大到1.51nm,羟基铁柱撑蒙脱土-δ-MnO2复合体为1.55nm左右,并且比表面积较原土也有明显的增大。以亚甲基蓝为目标污染物,研究了其作为异相催化剂的催化性能,考察了溶液H2O2加入量、δ-MnO2含量及pH值等对亚甲基蓝降解性能的影响。结果表明,在实验条件下,催化剂的催化活性随H2O2浓度的增加而升高,当nFe/nMn=0.241时,催化活性最好,且有较大的pH适用范围。亚甲基蓝的异相催化降解过程符合准一级动力学方程。催化剂循环使用3次,仍然具有良好的活性。  相似文献   

5.
采用单分子层剥离-重堆积技术将聚合羟基锆离子嵌入到钛酸盐板层间,制得层间距为1.92~2.01nm的介孔钛酸盐柱撑复合材料。X-射线衍射(XRD)、热重-示差扫描热分析(TG-DSC)、扫描/透射电镜(SEM/HR-TEM)和N2吸附等手段对材料物化性质进行了分析。结果表明,客体锆离子主要以[Zr4(OH)16-n(H2O)8+n]n+(记为Zr4)的形式存在于主体层间域中,且柱撑体系中nZr/nTi比越小,越有利于获得层间距和比表面积较大的柱撑材料。紫外光降解亚甲基蓝实验表明,柱撑材料对亚甲基蓝降解率为钛酸盐主体的3.5倍,这与柱撑形成的介孔结构以及主客体间的电子耦合有关;350℃热处理后材料对亚甲基蓝的降解率进一步提高,说明主客体间形成了更有效的欧姆接触。  相似文献   

6.
以Al2O3为催化剂催化臭氧化处理邻苯二甲酸二甲酯. 通过XRD、比表面积、孔结构、FTIR和活性评价等方法对催化剂的物化性质及催化活性进行了研究, 考察了焙烧温度、成型粒径对催化剂活性的影响. 结果表明, Al2O3催化剂对臭氧化降解邻苯二甲酸二甲酯具有很高的催化活性, 反应120 min后, 总有机碳(TOC)的去除率从单独臭氧氧化的23.9%提高到55.1%; 焙烧温度对催化剂的活性具有很大的影响, 600 ℃催化剂催化活性最高; 随着焙烧温度的升高, Al2O3晶型经历了从γ-Al2O3到θ-Al2O3到α-Al2O3的转变, 催化剂的比表面积、焙烧得到的孔容逐渐变小, 晶体粒径变大, 表面•OH数量减少, 催化活性下降. Al2O3成型粒径的减小, 提高了催化剂的外比表面积, 减小了内部传质扩散的影响, 从而提高了催化活性.  相似文献   

7.
含铁的柱撑膨润土光催化降解甲基橙   总被引:11,自引:0,他引:11  
将两种含铁柱撑膨润土(Fe-Al-Bent和Fe-Bent)用作复相光催化剂, 表征结果证实它们具有很高的比表面积, 铁以高催化活性的α-Fe2O3存在于复相催化剂中. 以甲基橙为目标降解物, 考察了不同类型的催化剂、催化剂用量以及H2O2浓度对其降解的影响, 并与相应的均相Fenton反应进行了比较. 结果表明: 两种复相光催化剂的催化脱色性能和CODCr去除率都很高, 明显优于相应的均相Fenton反应, 且复合铁铝柱撑膨润土(Fe-Al-Bent)比单一的铁柱撑膨润土(Fe-Bent)催化性能更好, 此外它们还具有分离简单、重复使用性好等特点.  相似文献   

8.
Al2O3催化剂结构对催化臭氧化活性的影响   总被引:6,自引:0,他引:6  
以Al2O3为催化剂催化臭氧化处理邻苯二甲酸二甲酯. 通过XRD、比表面积、孔结构、FTIR和活性评价等方法对催化剂的物化性质及催化活性进行了研究, 考察了焙烧温度、成型粒径对催化剂活性的影响. 结果表明, Al2O3催化剂对臭氧化降解邻苯二甲酸二甲酯具有很高的催化活性, 反应120 min后, 总有机碳(TOC)的去除率从单独臭氧氧化的23.9%提高到55.1%; 焙烧温度对催化剂的活性具有很大的影响, 600 ℃催化剂催化活性最高; 随着焙烧温度的升高, Al2O3晶型经历了从γ-Al2O3θ-Al2O3α-Al2O3的转变, 催化剂的比表面积、焙烧得到的孔容逐渐变小, 晶体粒径变大, 表面•OH数量减少, 催化活性下降. Al2O3成型粒径的减小, 提高了催化剂的外比表面积, 减小了内部传质扩散的影响, 从而提高了催化活性.  相似文献   

9.
对不同硅铝比的MCM-22分子筛进行气相硅烷化处理,并采用X射线衍射、固体核磁、N2吸附-脱附和甲苯吸附等技术对样品进行了表征. 结果显示,原料硅铝比为50~100的MCM-22分子筛均可以利用气相硅烷化,在不脱除骨架铝的基础上,将Si(OH)2柱撑结构引入其层间超笼系统,从而使层间距增大,孔体积增加; 将密度泛函理论用于计算硅烷化前后的MCM-22分子筛的N2吸附等温线,成功得到十元环孔道和超笼体系的比表面积和孔体积,发现气相硅烷化使MCM-22分子筛超笼体系的比表面积和孔体积增大,而十元环孔道减小.另外,气相硅烷化可有效提高不同硅铝比MCM-22分子筛的甲苯平衡吸附量.  相似文献   

10.
膨润土纳米复合材料的制备、表征及吸附性能研究   总被引:7,自引:0,他引:7  
用有机螯合剂(CA)和十六烷基三甲基溴化铵(HDTMAB)共同改性膨润土(IMB),制得一系列膨润土纳米复合材料IMB-HDTMA-CA。X射线衍射(XRD)、热分析(TG-DTA)、红外光谱(FTIR)以及N2-吸附脱附技术等研究发现,HDTMA+和CA已稳定柱撑在膨润土的片层结构中,其层间距增大、比表面积减小而疏水性增强。吸附实验表明,IMB-HDTMA-CA能协同吸附水中有机物对硝基苯酚(PNP)和重金属镉(Cd2+)。对水中对硝基苯酚的吸附源于PNP在膨润土层间有机相中分配作用的增加,其吸附容量和膨润土内有机碳含量和层间距大小一致,而与比表面积无关,依次为IMB-HDTMA-TEPA>IMB-HDTMA-TETA>IMB-HDTMA-En>IMB-HDTMA 》IMB;FTIR图谱显示,IMB-HDTMA-CA吸附Cd2+后的N-H吸收峰向低频方向移动,其吸附能力和所形成配合物的稳定性一致。  相似文献   

11.
用溶胶-凝胶法以磷钼酸(MPA)的镍盐溶液水解钛酸四丁酯制备了NiPMo/TiO2催化剂.使用ICP、 XRD、 TG-DTA、 IR、 TPD-MS和微反应技术研究了催化剂的化学组成、热稳定性、化学吸附性质和催化反应性能.杂多钼酸盐与TiO2通过O2-在TiO2表面发生了键合.在623 K下,杂多阴离子仍保持原有的Keggin结构.CO2在Lewis酸位Ni(Ⅱ)和Lewis碱位Ni-O-Mo的桥氧协同作用下生成CO2卧式吸附态Ni(Ⅱ)←O-(CO)←(O--Ni).丙烯有多种吸附态在催化剂上吸附.在563 K、 1 MPa和空速1500 h-1的反应条件下,丙烯的摩尔转化率为3.2%,产物MAA选择性为95%.  相似文献   

12.
Different approaches for the synthesis of 1-benzyloxypyrazin-2(1H)-one derivatives from simple amino acids have been investigated. A library of 33 precursors for the preparation of N-hydroxy pyrazinones was obtained in moderate to good yields.  相似文献   

13.
In the context of the preparation of camptothecin and luotonin A analogs, the synthesis of some key keto-precursors and their use in Friedländer condensation are described. This paper also focuses on the stability of these keto intermediates and emphasizes the major differences between indolizinones and pyrroloquinazolinones series. Noteworthy is also the report of some original structures isolated as by-products of some experiments.  相似文献   

14.
The Langevin paramagnetic theory can’t describe the relation between magnetization of ferrofluids and applied magnetic field. The structuralization of ferrofluids, which is considered the main influence factor of the magnetization, is regarded. The part of magnetization works is deposited when the structure is forming. This action influences the magnetization of ferrofluids directly or indirectly. On the base of the “compressing” model, the Langevin function that usually describes the magnetization of ferrofluid is modified, and a well-fitted curve is obtained. An equation of the relation between the equivalent volume fraction after being “compressed” and the intensity of magnetic field is discovered, which approximately describes the process of magnetization. The relation between the approximate initial susceptibility and the volume fraction can be obtained from modified formula.  相似文献   

15.
The highly regioselective Buchwald–Hartwig amination at C-2 of the cheap and readily accessible reagent, 2,4-dichloropyridine with a range of anilines and heterocyclic amines is described. This new methodology is robust and provides a facile access to 4-chloro-N-phenylpyridin-2-amines on 0.25 mol scale. These intermediates undergo a further Buchwald–Hartwig amination at higher temperature to enable rapid exploration of the chemical space at C-4 and to provide a library of 2,4-bisaminopyridines.  相似文献   

16.
KMnO4-mediated oxidative CN bond cleavage of tertiary amines producing secondary amine was introduced, which was trapped by electrophiles (acyl chloride and sulfonyl chloride) to form amides and sulfonamides. The reaction could take place at mild condition, tolerating a wide range of function groups and affording products in moderate to excellent yields.  相似文献   

17.
The review contains a concise historical account and information on the most significant researches undertaken by the staff at the A. E. Favorsky Irkutsk Institute of Chemistry, Siberian Branch of the Russian Academy of Sciences on the Chemistry of Heterocyclic Compounds. Dedicated to Academician of the Russian Academy of Sciences B. A. Trofimov on his 70th jubilee. Translated from Khimiya Geterotsiklicheskikh Soedinenii, No. 10, pp. 1443–1502, October, 2008.  相似文献   

18.
A general synthesis of previously unknown semicarbazone-based α-amidoalkylating reagents, 4-(tosylmethyl)semicarbazones, has been developed. The synthesis involved three-component condensation of semicarbazones of aliphatic or aromatic aldehydes with the same or other aldehydes and p-toluenesulfinic acid. The scope and limitations of this reaction were investigated. The compounds obtained were demonstrated to be an efficient α-(4-semicarbazono)alkylating agents. They were reacted with H- (sodium borohydride), O- (sodium methylate), S- (sodium phenylthiolate), N- (pyrrolidine, sodium succinimide), P- (trialkyl phosphites), and C-nucleophiles (sodium diethyl malonate) to give the corresponding products of the tosyl group substitution, 4-substituted semicarbazones, including analogues of nitrofurazone. Among the prepared compounds tested in vitro for antibacterial and antifungal activity, three nitrofuryl-containing semicarbazones exhibited high biological activities with minimum inhibitory concentration (MIC) values of 8–32 μg/mL.  相似文献   

19.
Zhanhui Yang  Shiyi Yang  Jiaxi Xu 《Tetrahedron》2017,73(23):3240-3248
Regiospecific and direct imidation of the methyl C(sp3)–H bond of thioanisoles is realized under mild and metal-free conditions with N-fluorobis(benzenesulfonyl)imide as an oxidant and nitrogen source. Proposed mechanism suggests that thionium ion intermediates and a Pummerer-type reaction are involved. The imidation has advantages such as high step-economy, excellent functionality tolerance, and regiospecificity, giving structurally diverse imidation products.  相似文献   

20.
A small library of new chiral bidentate hydroxyalkyl-imidazolium salts 1 is conveniently synthesized on multi-gram scale from inexpensive and commercially available chiral pool amino acids. The corresponding carbenes, generated by deprotonation of imidazolium salts 1, in combination with palladium(II) chloride were tested in the Mizoroki–Heck coupling reaction. The most significant results in terms of yields and reactivities were achieved with low catalyst loading. The catalytic activities of these imidazolium salts were also investigated in the asymmetric addition of diethylzinc to benzaldehyde. The use of MgO nanoparticles as an additive in conjunction with these ligands played a crucial role in increasing the efficiency of these reactions.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号