Direct aerobic oxidation of monoalcohol and diols to acetals using tandem Ru@MOF catalysts  

作　　者：Songwei Zhang Jerry Pui Ho Li Jingpeng Zhao Dan Wu Biao Yuan Willinton Yesid Hernandez Wen-Juan Zhou Tao He Yi Yu Yong Yang Vitaly Ordomsky Tao Li 

机构地区：[1]School of Physical Science and Technology,ShartghaiTech University,Shanghai 201210,China [2]Eco-Efficient Products and Processes Laboratory(E2P2L),UM I3464 CNRS-Solvay,Shanghai 201108,China [3]University of Chinese Academy of Sciences,Beijing 100049,China [4]Laboratory for Membrane Materials and Separation Technologies,Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai 201210,China [5]School of Chemistry and Chemical Engineering,Queens University Belfast,Belfast,BT95AG,UK

出　　处：《Nano Research》2021年第2期479-485,共7页纳米研究（英文版）

基　　金：the National Natural Science Foundation of China(No.21701110,T.L.);Solvay China(T.L.,V.O.,Y.Y.);and the start-up funding from ShanghaiTech University(T.L.).This work made use of the resources of the Instrum ental Analysis Center of SPST at ShanghaiTech University.This work is partially supported by CfiEM of SPST at ShanghaiTech(No.EM02161943).

摘　　要：The aerobic oxidation of monoalcohols and diols to acetals is an important academic and industrial challenge for the production of fine chemicals and intermediates.The existing methods usually rely on a two-step process in which alcohols are first oxidized to aldehydes over metal catalysts(Ru,Pt,Pd)and then acetalized using acids.Due to the instability of aldehydes,how to avoid over-oxidation to their respective carboxylic acids and esters is a long-standing challenge.For this reason,certain non-conjugated dialdehydes have never been successfully produced from diol oxidation.Hereby we report a Ru@metal-organic framework(MOF)tandem catalyst containing ultra-fine Ru nanoparticles(<2 nm)for direct alcohol to acetal conversion of monoalcohol and diols with noformation of carboxylic acids.Mechanistic study reveals that the presence of Lewis acid sites in the MOF work in concert with Ru active sites to promptly convert aldehydes to acetals thereby effectively suppressing the formation of over-oxidation byproducts.

关 键 词：metal-organic framework Ru nanoparticles aerobic oxidation ALCOHOLS ACETALIZATION 

分 类 号：O643.36[理学—物理化学]