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In Situ Generation of Brønsted Acidity in the Pd-I Bifunctional Catalysts for Selective Reductive Etherification of Carbonyl Compounds under Mild Conditions
ACS Catalysis ( IF 11.3 ) Pub Date : 2019-02-21 00:00:00 , DOI: 10.1021/acscatal.8b04925
Dan Wu 1, 2 , Willinton Y. Hernández 1 , Songwei Zhang 3 , Evgeny I. Vovk 3 , Xiaohong Zhou 3 , Yong Yang 3 , Andrei Y. Khodakov 2 , Vitaly V. Ordomsky 1, 2
Affiliation  

Selective synthesis of ethers from biomass-derived carbonyl compounds is an important academic and industrial challenge. The existing processes based on strong acid or metallic catalysts cannot provide high selectivity to ethers due to the occurrence of side reactions. Hereby we propose a Pd-I bifunctional heterogeneous catalyst for the selective reductive etherification of aldehydes with alcohols. Extensive catalyst characterizations uncovered the presence of iodine species on the surface of Pd nanoparticles. Heterolytic dissociation of hydrogen on the I-Pd surface sites leads to the “in situ” generation of a Brønsted acid, which promotes the reaction toward the corresponding ethers with extremely high selectivity under very mild reaction conditions.

中文翻译:

在温和条件下用于羰基化合物选择性还原醚化的Pd-I双功能催化剂中原位生成Brønsted酸

从生物质衍生的羰基化合物选择性合成醚是一项重要的学术和工业挑战。由于发生副反应,基于强酸或金属催化剂的现有方法不能提供对醚的高选择性。因此,我们提出了一种Pd-1双功能多相催化剂,用于醛与醇的选择性还原醚化。广泛的催化剂表征揭示了Pd纳米颗粒表面上碘的存在。氢在I-Pd表面位点的异质解离导致布朗斯台德酸的“原位”生成,这在非常温和的反应条件下以极高的选择性促进了向相应醚的反应。
更新日期:2019-02-21
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