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1.
采用阳极氧化技术在不锈钢丝网上成功地自生长了结构致密的氧化物膜,并以此为载体,通过电化学沉积工艺制备了Cu/不锈钢丝网催化剂。以甲苯、丙酮、乙酸乙酯及二氯甲烷为模型反应,考察了4种不同种类挥发性有机化合物(VOCs)在该催化剂上的完全氧化活性。结果表明电化学沉积时间为15 min制备得到的催化剂上完全氧化丙酮、甲苯、乙酸乙酯及二氯甲烷的温度分别为240、220、260和440℃。在220℃反应条件下进行60 h的甲苯氧化稳定性试验结果显示该催化剂催化氧化甲苯的转化率一直保持98%以上,表现出较好的稳定性。扫描电镜,X射线衍射及X射线光电子能谱等表征结果表明,不锈钢丝网载体表面的阳极氧化物膜有利于提高活性组分的分散度。设计采用电沉积工艺大大提高了催化剂表面活性物种与载体的结合牢固度。  相似文献   

2.
多孔氧化铝有序膜的制备研究   总被引:20,自引:0,他引:20  
本文用阳极氧化法分别在硫酸和草酸电解液中成功制备出高度有序、具有纳米级孔洞的氧化铝有序阵列模板。采用饱和HgCl2去除Al基体后,得到典型六方形结构的多孔Al2O3有序膜。通过改变氧化电压、氧化时间等条件使模板的孔径、孔深可调、膜厚度可控,并系统研究了对模板有序性、孔径、膜厚度等的影响因素,总结出制备Al2O3有序膜的最佳工艺。  相似文献   

3.
甲烷直接氧化制甲醇:Ⅱ.催化膜反应器(CMR)   总被引:2,自引:2,他引:0  
采用溶胶-凝胶(Sol-Gel)法制备了微孔结构均匀的“SiO2/陶瓷”膜和“Mo-Co-O/SiO2/陶瓷”催化功能膜,并用XRD、SEM和孔径测定等技术进行了表征。在常压,500~700℃的条件下,在催化膜反应器(CMR)中考察了甲烷氧化制甲醇的反应。在相似的反应条件下(转化率为1.0%),用CMR(甲醇选择性1?.2%)可获得较固定床反应器(甲醇选择性4.5%)高得多的甲醇选择性。  相似文献   

4.
马莹  陈敏  宋萃  郑小明 《物理化学学报》2008,24(7):1132-1136
采用阳极氧化法制备了一种用于催化氧化处理挥发性有机化合物(VOCs)的0.1%Pt-0.5%Pd/不锈钢丝网(SSWM)催化剂. 活性测试结果表明, 0.1%Pt-0.5%Pd/不锈钢丝网催化剂具有较高的催化活性和热稳定性. 该催化剂上甲苯、丙酮和乙酸乙酯的完全氧化温度分别为220、260和280 ℃. 通过扫描电镜(SEM)、X射线光电子能谱(XPS)和超声波等手段对催化剂和不锈钢丝网进行了表征. SEM结果表明, 经阳极氧化工艺处理过的不锈钢金属丝网载体表面形成了一层沟壑形态的复合氧化膜. 该阳极氧化膜有利于活性组分Pd、Pt的分散.  相似文献   

5.
VOCs催化燃烧Pd-Y/不锈钢丝网催化剂的性能   总被引:2,自引:0,他引:2  
采用经阳极氧化工艺处理后的不锈钢丝网作为催化剂载体,制备了Pd-Y/不锈钢丝网催化剂。考察了该催化剂对典型的挥发性有机物(VOCs)(甲苯、丙酮和乙酸乙酯)的催化燃烧性能,并用SEM、TPR技术对催化剂的形貌和氧化膜的结构组成进行了表征。结果表明:采用阳极氧化技术在不锈钢表面形成致密的多孔氧化膜,有利于活性组分的负载及均匀分散,明显提高了催化剂的燃烧活性和稳定性,延长了催化剂的使用寿命。Pd-Y/不锈钢丝网催化剂上3种VOCs的完全氧化温度分别为220、280和320 ℃。控制甲苯进料浓度为4~6 g·m  相似文献   

6.
采用铝阳极氧化法制备了Al2O3-Al-体型多孔氧化铝载体,再采用电沉积技术将TiO2沉积到氧化铝多孔的纳米孔道内,制备了催化精馏专用SO42-/TiO2-Al2O3-Al型固体酸催化剂,并以乙酸乙酯合成为模型反应,考察了水封条件,电沉积电压、电沉积时间等制备工艺条件对催化剂活性的影响.实验结果表明,适宜的制备条件为水封温度为50℃,水封时间为1 h,电沉积电压为6V,电沉积时间为30 min,在此制备条件下,醋酸转化率为31.34%.采用扫描电镜(SEM),X射线衍射分析(XRD)手段对所制备催化剂进行了表征.结果表明:阳极氧化铝膜的结构为无定型结构,TiO2在载体上呈高度分散状态.  相似文献   

7.
庄林 《物理化学学报》2018,34(2):115-116
正直接甲醇燃料电池(DMFC)是将甲醇氧化反应的化学能直接转化为电能的一种发电装置,其工作原理非常简单,主要由阴极、阳极、质子交换膜及双极板等组成。工作时,甲醇在阳极上被催化氧化为CO_2和H_2O,同时产生6个电子和6个质子,其中质子经质子交换膜由阳极到达阴极,在催化剂作  相似文献   

8.
铂微粒修饰的氧化钛电极对甲醇的电催化氧化性能   总被引:8,自引:2,他引:6  
直接甲醇质子交换膜燃料电池(DMPEMFC)可用作未来电动车辆的动力电源[1],但要达到实际应用还有大量问题有待进一步解决.目前限制DMPEMFC实际应用的主要问题是甲醇阳极氧化催化剂低的活性、高的价格及催化剂的毒化.就目前对于甲醇氧化电催化剂研究的...  相似文献   

9.
催化剂的宏观反应速率受颗粒内扩散过程的影响,而内扩散过程又取决于催化剂颗粒的孔结构。以铜基甲醇合成催化剂为研究本系,通过改变压片压强和共沉淀条件,制备具有不同孔结构参数(比表面、孔隙率、孔径分布、孔容、颗粒密度、曲折因子)的颗粒催化剂,由反应工程中的扩散-反应方程,按照平行交联孔模型计算有效扩散系数,模拟计算单颗粒催化剂在工业生产条件下的宏观反应速率,从而研究孔结构对未中毒铜基甲醇合成催化剂宏观反  相似文献   

10.
陈敏  宋萃  汪丽娜  张婷  郑小明 《化学学报》2009,67(16):1839-1842
通过阳极氧化技术制备了一种新型的0.75%Ce-0.5%Pd/不锈钢丝网催化剂. 采用扫描电镜(SEM)和程序升温还原技术(TPR)对催化剂进行了表征. 考察了稀土铈的引入对催化剂上甲苯、丙酮和乙酸乙酯氧化活性的影响, 结果显示, 在不锈钢丝网载体表面处理过程中引入阳极氧化技术, 使之自组织生长了一层多孔氧化膜, 提供了活性组分CeO2和Pd相互作用的平台. 氧化铈的引入, 使不锈钢丝网载体表面的多孔氧化膜形成了独特的海绵状蜂窝结构, 有利于活性组分Pd的分散锚定. 0.75%Ce-0.5%Pd/不锈钢丝网催化剂对甲苯、丙酮和乙酸乙酯的完全转化温度分别为200, 240和260 ℃, 具有良好的催化消除活性. 催化剂的反应活性与稀土CeO2的引入及其在阳极氧化膜上形成独特的形貌有关.  相似文献   

11.
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   

12.
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   

13.
A new and simple synthesis of novel N-protected methyl 5-substituted-4-hydroxypyrrole-3-carboxylates, which exist in equilibrium with their 4-oxo tautomers, has been developed in two steps starting from N-protected α-amino acids. The key intermediates are enaminones, which can also be isolated, characterized, and used for the construction of other functionalized heterocycles, before they spontaneously decompose to pyrrole products. 4-Hydroxypyrroles are prone to partial aerial oxidation but can be efficiently alkylated or reduced to stable polysubstituted pyrrolidine derivatives.  相似文献   

14.
The chemoselectivity in the intramolecular CH insertion of various diazosulfonamides has been experimentally studied. The results reveal that the aliphatic 1,4-, 1,5-, or 1,6-C(sp3)?H insertions of diazosulfonamides are not accessible, while the aromatic 1,5-C(sp2)?H insertion can be realized specifically by adjusting the diazo-adjacent group. In addition, the general chemoselectivities in the intramolecular CH insertions of diazosulfonyl compounds are summarized. Generally, diazosulfones undergo both aromatic 1,5-C(sp2)?H and aliphatic 1,5- and 1,6-C(sp3)?H insertions, while diazosulfonates undergo aliphatic 1,5- and 1,6-C(sp3)?H insertions. However, diazosulfonamides only undergo aromatic 1,5-C(sp2)?H insertion.  相似文献   

15.
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   

16.
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   

17.
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   

18.
N-Heterocyclic carbene-palladacyclic complexes 3 were successfully achieved in a one-pot procedure under mild conditions. The structure of 3a was unambiguously confirmed by X-ray single crystal diffraction and it was an active catalyst in the Buchwald-Hartwig amination and α-arylation of ketones even at very low catalyst loadings (0.01?mol%).  相似文献   

19.
An efficient approach to the synthesis of highly congested di, penta and hexacyclic pyrazoles as well as imidazole fragment containing novel heterocyclic molecule has been developed through a carbanion induced transformation of suitably functionalized 2H-pyran-2-ones, benzo[h]chromene and thiochromeno[4,3-b]pyrans. Due to the presence of fluorescence, we report their prime application metal sensor as off/on switching in ferric ions.  相似文献   

20.
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   

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