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具有铁-儿茶酚位点的微孔纳米管和纳米球:在 CO2 固定反应中高效路易斯酸催化剂和 Ag 纳米颗粒的载体。

Microporous Nanotubes and Nanospheres with Iron-Catechol Sites: Efficient Lewis Acid Catalyst and Support for Ag Nanoparticles in CO Fixation Reaction.

机构信息

Department of Materials Science, Indian Association for the Cultivation of Science, 2A & B, Raja S.C. Mullick Road, Jadavpur, Kolkata-, 700032, India.

S. N. Bose National Centre for Basic Sciences, Block-JD, Sector-III, Salt Lake, Kolkata, 700106, India.

出版信息

Chemistry. 2018 Sep 20;24(53):14189-14197. doi: 10.1002/chem.201802319. Epub 2018 Aug 28.

DOI:10.1002/chem.201802319
PMID:29979469
Abstract

Fe -containing hyper-crosslinked microporous nanotubes (FeNTs) and nanospheres (FeNSs) are synthesized through the reaction of catechol and dimethoxymethane in the presence of FeCl or CF SO H. Both FeNTs and FeNSs demonstrate excellent catalytic activity in Lewis acid catalysis (hydrolysis and regioselective methanolysis of styrene oxide) and tandem catalysis involving a sequential oxidation-cyclization process, which selectively converts benzyl alcohol to 2-phenyl benzimidazole. Apart from Lewis acidity, the FeNTs and FeNSs also showed CO uptake capacities of 2.6 and 2.2 mmol g , respectively, at a pressure of 1 atm and temperature of 273 K. Furthermore, Ag nanoparticles are immobilized successfully on the surfaces of FeNTs and FeNSs by the liquid-phase impregnation method to prepare Ag@FeNT and Ag@FeNS nanocomposites, which show high catalytic activity for the selective fixation of CO to phenylacetylene to yield phenylpropiolic acid at 60 °C and 1 atm CO pressure. Hence, Fe -catechol-containing hyper-crosslinked nanotubes and nanospheres have huge potential not only as Lewis acid catalysts, but also as excellent supports for immobilizing Ag nanoparticles in the design of a robust catalyst for the carboxylation of terminal alkynes, which has wide scope in catalysis and environmental research.

摘要

含 Fe 的超交联微孔纳米管(FeNTs)和纳米球(FeNSs)是通过在 FeCl 或 CF3SO3H 的存在下,儿茶酚和二甲氧基甲烷之间的反应合成的。FeNTs 和 FeNSs 在路易斯酸催化(苯乙烯氧化物的水解和区域选择性甲醇解)和串联催化(涉及顺序氧化-环化过程)中均表现出优异的催化活性,可将苄醇选择性转化为 2-苯基苯并咪唑。除了路易斯酸度外,FeNTs 和 FeNSs 在 1 atm 压力和 273 K 温度下,分别具有 2.6 和 2.2 mmol g 的 CO 吸收能力。此外,通过液相浸渍法成功地将 Ag 纳米颗粒固定在 FeNTs 和 FeNSs 的表面上,制备了 Ag@FeNT 和 Ag@FeNS 纳米复合材料,它们在 60°C 和 1 atm CO 压力下,对 CO 到苯乙炔的选择性固定具有很高的催化活性,生成苯丙炔酸。因此,含 Fe 的儿茶酚超交联纳米管和纳米球不仅具有路易斯酸催化剂的巨大潜力,而且作为在设计用于末端炔烃羧化的坚固催化剂中固定 Ag 纳米颗粒的优异载体也具有很大的潜力,在催化和环境研究中具有广泛的应用前景。

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