含铝富锗 IWV:通过沸石间转化快速合成并应用于 Baeyer-Villiger 氧化反应

IF 10.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Meichen Jiao, Chunmin Jia, Hao Xu, Peng Wu, Xian-Ming Zhang
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引用次数: 0

摘要

含 Ge 的路易斯酸性沸石通常采用传统的水热法从无定形二氧化硅中合成,这种耗时耗能的方法限制了沸石的广泛应用。本研究报告了一种通过脱铝 FAU(DA-FAU)的沸石间转化,快速合成一系列具有宽范围 Si/Ge 摩尔比(5-15)的 IWV 铝锗硅酸盐沸石(T-x-Al)的策略。值得注意的是,通过等分子硅/锗比凝胶可在短至一天的结晶时间内获得富含锗的 IWV。研究了合成参数的影响,并通过 XRD、SEM、EDS、ICP、29Si 和 27Al MAS NMR、FTIR 和 N2 物理吸附分析对获得的 T-x-Al 样品进行了表征。与之前报道的一种 IWV 锗硅酸盐(H-3)相比,T-x-Al 在拜尔-维利格(BV)氧化反应中显示出更好的催化活性,这归因于活性框架 Ge 位点的存在以及框架外 Al 物种的辅助。循环催化测试表明,框架 Al 物种的存在提高了 T-x-Al 的稳定性。具体来说,在大酮类 2-admantanone 的 BV 氧化过程中,具有 14 元环(MR)超笼的 T-x-Al 的性能优于典型的 12-MR Sn-beta 催化剂,这表明其在大分子催化过程中具有广阔的应用前景。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Al-containing Ge-rich IWV: rapid synthesis via interzeolite transformation and application in Baeyer-Villiger oxidation

Ge-containing Lewis acidic zeolites are typically synthesized using a conventional hydrothermal strategy from amorphous silica sources, through a long time- and energy-consuming approach limiting their wide applications. This study reports a rapid synthesis strategy for a series of IWV aluminogermanosilicate zeolites (T-x-Al) with a wide range of Si/Ge molar ratios (5–15) by interzeolite transformation of dealuminated FAU (DA-FAU). Notably, Ge-rich IWV could be obtained with crystallization time as short as one day by the equimolecular Si/Ge ratio gel. The effect of synthetic parameters was investigated and the obtained T-x-Al samples were characterized by XRD, SEM, EDS, ICP, 29Si and 27Al MAS NMR, FTIR, and N2 physisorption analyses. Compared with a previously reported IWV germanosilicate (H-3), T-x-Al displayed a better catalytic activity in Baeyer-Villiger (BV) oxidation, attributed to the presence of the active framework Ge sites with the assistance of the extra-framework Al species. The cyclic catalysis tests revealed that the presence of framework Al species contributed to the stability of the T-x-Al. Specifically, T-x-Al, with 14-membered ring (MR) supercages, outperformed the typical 12-MR Sn-beta catalyst in the BV oxidation of large ketone-like 2-admantanone, indicating a promising potential application in the macromolecular catalytic process.

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来源期刊
Science China Chemistry
Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
7.30%
发文量
3787
审稿时长
2.2 months
期刊介绍: Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.
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