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甲醇气相氧化羰基化合成碳酸二甲酯的研究Ⅲ. 催化剂的失活再生 总被引:1,自引:0,他引:1
碳酸二甲酯 (DMC)是一种对环境友好的绿色化学品 ,其洁净合成工艺的开发 ,已引起国内外研究者的广泛重视。真田等人[1 ] 对PdCl2 存在下CO和亚硝酸甲酯反应合成DMC过程所用催化剂的失活原因和再生方法进行了研究 ,认为PdCl2 中的Cl被还原消除生成氯甲酸甲酯导致催化剂失活 ,并发现氯甲酸甲酯在DMC合成中可使Pd催化剂再生和提高寿命。DOW公司[2 ] 开发的气相氧化羰基化法催化剂CuCl2-KCl AC易失活 ,该催化剂运行 50~ 1 0 0h后需进行再生。再生时 ,于 1 2 0℃条件下通入 1 0 %HCl N2 混合物 ,再生后… 相似文献
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合成低碳醇超细Mo-Co-K催化剂的TPD研究 总被引:1,自引:3,他引:1
近年来 ,Mo基催化剂由于其独特的耐硫性而在各种合成低碳醇催化剂体系中倍受青睐。许多研究表明 ,以Co作为Mo基催化剂的第二组分可明显改善其催化合成低碳醇的反应性能[1~ 4] 。一般认为 ,K是这类催化剂通用的促进剂[1,3 ,5,6] 。我们曾经报道[7] ,还原态超细Mo Co K催化剂具有优良的合成低碳醇性能。同时 ,催化剂的Co Mo比对其合成低碳醇性能具有显著的影响。为了解这种影响的原因 ,本文运用TPD技术对此类催化剂进行了研究。催化剂经还原后 ,在催化剂表面即形成了不同的吸附中心[8] 。了解这些不同的吸附中心 ,对于研… 相似文献
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MCM—48介孔分子筛的合成研究 总被引:14,自引:3,他引:11
利用水热法合成了MCM-48介孔分子筛,通过IR,TG-DTA,XRD,XRD,TEM,N2吸附等方法对产物进行了表征,并系统地研究了晶化温度、晶化时间、凝胶组成等对合成MCM-48介孔分子筛的影响。 相似文献
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复合催化剂中H-ZSM-5酸性对合成气制二甲醚的影响 总被引:23,自引:0,他引:23
对合成气制二甲醚( D M E)复合催化剂中脱水组分 H Z S M 5 分子筛进行水热处理及 N H3 T P D、 C O2 T P D 表征. 研究结果表明, 在 H Z S M 5 分子筛脱水组分上具有两种酸性中心,高温 N H3 的脱附峰代表强酸中心, 低温 N H3 的脱附峰代表弱酸中心. 同时, 亦有两种不同强度的碱中心. 随 H Z S M 5 水热处理温度的提高, 总酸量及强酸中心数量逐渐降低, 碱性中心数目随 H Z S M 5 水热处理温度的提高略有增加, D M E的选择性随之提高. D M E 主要是在 H Z S M5 分子筛的弱酸中心上生成. 对 H Z S M5 于 600 ℃处理后与铜基催化剂混合制得的复合催化剂, 对其反应性能考察后发现, 当 H2/ C O≈2 时, 4~6 M Pa、2 000~3 000 h- 1、260 ℃为最适宜反应条件. 此时, C O 的转化率≥ 90% , 对 D M E 和甲醇的选择性为96% , D M E 在所有有机产物中的选择性≥ 80% , D M E的含量≥ 20% . 提高反应压力, C O 的转化率及 D M E 在产物中的含量有较大提高, 但对 D M E的选择性影响不大. 相似文献
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铜基甲醇合成催化剂的失活研究 总被引:5,自引:0,他引:5
选用了两个化肥厂的失活甲醇合成催化剂,采用XRD、SEM、SEM-EDS、TEM、XPS、TRP、CO-TPD和化学吸附等方法对催化剂进行比较测试。结果表明,硫中毒、积炭、铜粒长大和杂质金属沉积等是造成甲醇合成催化剂失活的因素。由于某一种或几种因素都导致催化剂活性表面积的降低,对反应物CO吸附量减少,或造成催化剂对CO吸附能力的降低,从而降低合成甲醇反应的活性。硫中毒和铜粒长大是普遍存在的最主要因 相似文献
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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
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An efficient tandem approach for the selective synthesis of 4,5-dihydroimidazo[1,5-a]quinoxalines 6a–g and imidazo[1,5-a]quinoxalines 7a–h by the reaction of 2-imidazolyl anilines 4a–c with aryl aldehydes 5a–k under mild reaction conditions is described. Introduction of electron releasing alkyl groups in substrates 4a–b was found to be instrumental for the success of the reaction. 相似文献
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The Diels-Alder reactivity of 1,2-heteroborines (H4C4B(H)X, X?=?NH, PH, AsH; O, S, Se) has been computationally explored by means of Density Functional Theory (DFT) calculations. The influence of the HB?=?X fragment on the reactivity of the system has been quantitatively analyzed in detail by means of the so-called Activation Strain Model (ASM) of reactivity. It is found that the interaction between these species and the dienophile is significantly stronger than that computed for their all-carbon isoelectronic counterpart, benzene. In addition, the strain energy plays a key role in the observed reactivity trends. The role of the aromaticity strength of these heteroarenes on the reactivity is also assessed. 相似文献
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Xi-Liu YunWen-Ying Bi Jian-Hui HuangYu Liu Daisy Zhang-NegrerieYun-Fei Du Kang Zhao 《Tetrahedron letters》2012,53(38):5076-5080
A variety of N-aryl and N-alkyl carbazolones were conveniently achieved in good to high yields via Pd2(dba)3-mediated intramolecular coupling of N-substituted α-iodo enaminones under microwave irradiation. The Pd(0)-catalyzed cyclization was found to proceed favorably with the more electron-deficient phenyl ring during the reactions involving unsymmetrical N,N-diaryl α-iodo enaminones. This unique property enables the construction of carbazolone skeleton containing nitro substituted benzenoid ring. 相似文献
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Both substituted 2,4,5,6-tetrahydrocyclopenta[c]pyrazoles and 2,4,5,6-tetrahydropyrrolo[3,4-c]pyrazoles have been synthesized by the 3+2 intramolecular dipolar cycloaddition of nitrilimines to alkynes. This cyclization has been extended to more versatile 3-bromo derivatives by the use of alkynylbromides as dipolarophiles. 相似文献
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An efficient and benign method for the preparation of aminomethyl-substituted fullerenes has been developed. The process, involving catalyst free, visible-light irradiation of 10% EtOH-toluene solutions containing fullerene C60 and N-trimethylsilylmethyl-substituted amines by using a 20 W compact fluorescent lamp, leads to formation of aminomethyl-substituted fullerene adducts in a highly efficient manner. The photoaddition reaction takes place via a pathway initiated by visible light absorption by C60, followed by SET from the amine to the triplet excited state of C60. Ethanol-promoted desilylation of the resulting a minimum radical then generates the corresponding α-amino radical which couples with the C60 radical anion to form the anion precursor of the fullerene adducts. The new approach using visible-light takes place under mild conditions and it does not require the use of photocatalysts. Thus, the method developed in this effort could broadens the range of functionalized fullerene derivatives that can be readily prepared. 相似文献
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Viktor A. Dmitriev Mariia M. Efremova Alexander S. Novikov Vladimir V. Zarubaev Alexander V. Slita Anastasia V. Galochkina Galina L. Starova Andrey V. Ivanov Alexander P. Molchanov 《Tetrahedron letters》2018,59(24):2327-2331
The reactions of various nitrones with indolyl- and pyrrolylacrylates proceeds regioselectively with high diastereoselectivity in the case of aldonitrones, and represents an effective method for obtaining new indolyl- and pyrrolyl-substituted isoxazolidine carboxylates stabilized by weak (CH?O) and moderate (NH?N) strength intramolecular hydrogen bonding. The resulting cycloadducts exhibit promising in vitro anti-influenza activities. 相似文献
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A transition metal-free method for the direct amination of benzoxazoles using formamides as nitrogen sources is reported, which was mediated by an inexpensive and environmentally friendly tetrabutylammonium iodide/tert-butyl hydroperoxide system and gave the 2-aminobenzoxazole derivatives with moderate to good yields. 相似文献
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Multifunctionalized 1,2,3,4-tetrahydropyridines are concisely synthesized in good yields via l-proline-catalyzed or l-proline/FeCl3-cocatalyzed one-pot multicomponent reactions (MCRs). The MCRs involve a domino hydroamination/prins reaction/Mannich-type reaction/intramolecular dehydration-cyclization process. The molecular structure of 5baa, one of multifunctionalized 1,2,3,4-tetrahydropyridines, was confirmed by single-crystal X-ray diffraction. 相似文献
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M. Saeed Abaee Atefeh Hadizadeh Mohammad M. Mojtahedi Mohammad R. Halvagar 《Tetrahedron letters》2017,58(14):1408-1412
An efficient four-component reaction was developed to take advantage of the reactivity of the 2-aminothiophene-3-carbonitrile functionality, which is obtained during the classical three-component Gewald reaction. Various α-methylene bearing ketones were reacted with malononitrile, elemental sulfur, and aryl/heteroarylnitrile derivatives in t-BuOH/NaOH to afford 2-arylthieno[2,3-d]pyrimidin-4-amines in high yields. Preliminary studies revealed the photophysical properties of the products and their potential for use as metal sensors. 相似文献