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揭示了 Co-Mg-Al 层状双氢氧化物(LTHs)协同作用的独特设计,用于在温和条件下促进吲哚-3-基衍生物的绿色合成的催化活性。

Unveiling the exceptional synergism-induced design of Co-Mg-Al layered triple hydroxides (LTHs) for boosting catalytic activity toward the green synthesis of indol-3-yl derivatives under mild conditions.

机构信息

Fabrication Technology Research Department, Advanced Technology and New Materials Research Institute (ATNMRI), City of Scientific Research and Technological Applications (SRTA-City), New Borg El-Arab City, P.O. Box 21934 Alexandria, Egypt.

Nanotechnology Research Centre (NTRC), The British University in Egypt (BUE), El-Sherouk City, Suez Desert Road, 11837 Cairo, Egypt.

出版信息

J Colloid Interface Sci. 2021 Oct;599:227-244. doi: 10.1016/j.jcis.2021.04.083. Epub 2021 Apr 20.

Abstract

The current study provides a novel insight into the role of synergism of the changes in Mg/ Al in the best catalytic activity of indol-3-yl derivatives. A series of Co-Mg-Al layered triple hydroxides (LTHs) catalysts were produced by altering the Al/Mg ratio with respect to Co. The physicochemical properties of LTHs were well characterized by ICP-AES, XRD, FTIR, FE-SEM, BET, Zeta-sizer, and VSM. The results show that the sample CMA4 (Co:Mg:Al 2:4:4) is an exception to the physicochemical characteristics of the produced Co-Mg-Al LTHs, which is due to the synergism between the changes in Mg and Al. To the best of our knowledge, this is the first study to report the synthesis of indol-3-yl derivatives from indole-3-carbaldehyde using Co-Mg-Al LTHs as highly efficient heterogeneous catalysts, which is an extremely appealing path. The selectivity of the synthesis was studied by condensing various nucleophiles through the one-pot method that established superior reactivity under mild conditions. Notably, the results show that the Co-Mg-Al LTHs system exhibited an extraordinarily catalytic activity, with the highest yield (98%) being obtained under the following optimal conditions: the concentration of Co-Mg-Al LTHs = 5 mol%, 30 min., water/ethanol as solvent. Furthermore, the reusable studies exhibited that the catalysts were found to be stable and reusable for up to six cycles without substantial loss of catalytic activity. Finally, a plausible reaction mechanism of the Co-Mg-Al LTHs system for indol-3-yl derivatives was put forward according to our comprehensive analysis. Our work illuminates a cheap and flexible strategy for the synthesis of indol-3-yl derivatives using Co-Mg-Al LTHs.

摘要

当前的研究为镁/铝变化协同作用在吲哚-3-基衍生物最佳催化活性中的作用提供了新的见解。通过改变相对于 Co 的 Al/Mg 比,制备了一系列 Co-Mg-Al 层状双氢氧化物(LTHs)催化剂。LTHs 的物理化学性质通过 ICP-AES、XRD、FTIR、FE-SEM、BET、Zeta 粒度仪和 VSM 进行了很好的表征。结果表明,样品 CMA4(Co:Mg:Al 2:4:4)是所制备的 Co-Mg-Al LTHs 的物理化学特性的例外,这是由于 Mg 和 Al 的变化之间的协同作用。据我们所知,这是首次报道使用 Co-Mg-Al LTHs 作为高效多相催化剂从吲哚-3-甲醛合成吲哚-3-基衍生物的研究,这是一条极具吸引力的途径。通过一锅法缩合各种亲核试剂研究了合成的选择性,该方法在温和条件下建立了优异的反应性。值得注意的是,结果表明 Co-Mg-Al LTHs 体系表现出异常高的催化活性,在以下最佳条件下获得了最高产率(98%):Co-Mg-Al LTHs 的浓度= 5 mol%,30 分钟,水/乙醇为溶剂。此外,可重复使用研究表明,催化剂在六个循环内稳定且可重复使用,没有明显的催化活性损失。最后,根据我们的综合分析,提出了 Co-Mg-Al LTHs 体系用于吲哚-3-基衍生物的可能反应机制。我们的工作为使用 Co-Mg-Al LTHs 合成吲哚-3-基衍生物提供了一种廉价且灵活的策略。

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