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铁硅酸盐分子筛乙苯氧化脱氢催化性能研究—平衡阳离子性… 总被引:1,自引:0,他引:1
在823K和乙苯/O2=1.0的条件下考察了乙苯在FeZSM-5上的催化活性,比较了平衡阳离子性质,水热处理及Fe2O3的分散程度对乙苯氧化脱氢性能的影响,结合XPS、ESR及TPR测试结果讨论了FeZSM-5中铁的存在状态与乙苯氧化脱氢的关系,结果表明,FeZSM-5催化剂上作为L酸中心的骨架Fe(Ⅲ),水热处理产生的高分散非骨架Fe(Ⅲ)和适当强度的碱中心共同构成了乙七氧化脱氢活性中心。 相似文献
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用XPS、DRS及Mossbauer谱对水热处理改性的FeZSM-5中Fe(Ⅲ)的化学状态进行了研究,并定量地考察了水热处理时间对骨架铁含量的影响,比较了不同水热处理时间及不同平衡阳离子交换的FeZSM-5上乙苯的吸附及扩散性质。水热处理将使骨架铁从骨架析出,但析出的骨架铁并不阻塞孔道,而是高分散在分子筛的表面上,乙苯的吸附量随水热处理时间增加而增大。阳离子交换的FeZSM-5上乙苯的扩散系数及吸附量均按H、Li、Na、K离子半径增大的顺序递减。乙苯的氧化脱氢活性主要取决于Fe(Ⅲ)活性中心的性质,也与乙苯的吸附量及扩散系数有关。 相似文献
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本文应用碱性气体吸附的红外光谱和TPD技术研究了FeZSM-5(F_4)的酸性,酸性顺序为:H-F_4>Fe_2O_3/F_4>F_4原粉>水热处理的K-F_4>Li-F_4>NaF_4>K-F_4>NaOH/F_4,比较了酸强度和积炭对乙苯氧化脱氢性能的影响,以及催化剂酸碱性质与积炭的关系.结果表明,乙苯氧化脱氢反应是在酸碱协同作用下进行的,积炭也参与了氧化脱氢反应,催化剂表面上L酸中心产生的具有一定C、H、O比的积炭具有高的氧化脱氢活性.碱金属阳离子改性的具有L酸中心的FeZSM-5是乙苯氧化脱氢的高活性催化剂。 相似文献
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Fe—ZSM—5分子筛中Fe的化学环境研究 总被引:4,自引:1,他引:4
本文应用ESR、XPS、DRS、Mossbauer谱和首次运用TPR技术结合XPS、XRD对Fe-ZSM-5中Fe的化学环境进行了研究。结果表明,碱性介质条件下合成的Fe-ZSM-5分子筛中,铁仅有一种价态Fe(Ⅲ),但却有多种存在形式。非骨架Fe(Ⅲ)包括分子筛孔道内及外表面上沉积的氧化铁;骨架Fe至少有两种状态,即骨架不饱和配位Fe(Ⅲ)和骨架畸变四配位的Fe(Ⅲ).各种测试方法的结果表明Fe主要位于分子筛的骨架上,非骨架Fe(Ⅲ)很少. 相似文献
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用XDPS、DRS及Mossbauer谱对水热处理改性的FeZSM-5中F(Ⅱ)的化学状态进行了研究,并定量地考察了水热处理时间对骨架铁含量的影响,比较了不同水热处理时间及不同平衡阳离子交换的FeZSM-5上乙苯的吸附及扩散性质。水热处理将骨架析出,但析出的骨架铁并不阻塞孔道,而高分散在分子筛的表面上,乙苯的吸附量随水热处理时间增加而增大。 相似文献
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本文应用碱性气体吸附的红外光谱和TPD技术研究了FeZSM-5(F4)的酸性,酸性为:H-F4〉Fe2O3/F4〉F4原粉〉水热处理的K-F4〉Li-F4〉Na-F4〉K-F4〉NaOH/F4。比较了酸强度和积炭对乙苯氧化脱氢性能的影响,以及催化剂酸碱性质与积炭的关系。结果表明,乙苯氧化脱氢反应是在酸碱协同作用下进行的,积炭也参与了氧化脱氢反应,催化剂表面上L酸中心产生的具有一定C、H、O比的积炭 相似文献
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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
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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
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Toward new camptothecins. Part 6: Synthesis of crucial ketones and their use in Friedländer reaction
Laurent Gavara Thomas Boisse Jean-Pierre Hénichart Adam Daïch Philippe Gautret 《Tetrahedron》2010,66(38):7544-5571
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
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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
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Rebecca J. Burton Mandy L. CrowtherNeal J. Fazakerley Shaun M. FilleryBarry M. Hayter Jason G. KettleCaroline A. McMillan Paula PerkinsPeter Robins Peter M. SmithEmma J. Williams Gail L. Wrigley 《Tetrahedron letters》2013
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
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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
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N. A. Nedolya 《Chemistry of Heterocyclic Compounds》2008,44(10):1165-1219
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
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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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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
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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