Li Jingwen, Hu Riming, Liu Wei, Gao Daowei, Zhao Huaiqing, Li Chunsheng, Jiang Xuchuan, Chen Guozhu
School of Chemistry and Chemical Engineering, University of Jinan, Jinan, Shandong 250022 P. R. China.
Institute for Smart Materials & Engineering, University of Jinan, Jinan, Shandong 250022 P. R. China.
Inorg Chem. 2023 Feb 27;62(8):3692-3702. doi: 10.1021/acs.inorgchem.3c00095. Epub 2023 Feb 10.
Direct oxidative coupling of alcohols with amines over cheap but efficient catalysts is a promising choice for imine formation. In this study, porous CeO-MnO binary oxides were prepared via an interfacial reaction between Ce(SO) and KMnO at room temperature without any additives. The as-prepared porous CeO-MnO catalyst has a higher fraction of Ce, Mn, and Mn and contains larger surface area and more oxygen vacancies. During the oxidative coupling reaction of alcohol with amine to imine, the as-obtained CeO-MnO catalyst is motivated by the above encouraging characteristics and exhibits superior catalytic activity (98% conversion and 97% selectivity) and can also work effectively under a wide scope of temperatures and substrates. The in-depth DRIFTS and density functional theory (DFT) results demonstrate that there is a strong interaction between CeO and MnO in the CeO-MnO catalyst, exhibiting especially a positive synergistic effect in the direct coupling of alcohol and amine reaction.
在廉价而高效的催化剂上，醇与胺直接氧化偶联是形成亚胺的一个有前景的选择。在本研究中，通过Ce(SO)与KMnO在室温下的界面反应，无需任何添加剂，制备了多孔CeO-MnO二元氧化物。所制备的多孔CeO-MnO催化剂具有更高比例的Ce、Mn和Mn，且具有更大的表面积和更多的氧空位。在醇与胺氧化偶联生成亚胺的反应中，所得到的CeO-MnO催化剂受上述令人鼓舞的特性驱动，表现出优异的催化活性（转化率98%，选择性97%），并且在很宽的温度范围和底物条件下都能有效工作。深入的漫反射红外傅里叶变换光谱（DRIFTS）和密度泛函理论（DFT）结果表明，CeO-MnO催化剂中CeO和MnO之间存在强烈的相互作用，在醇与胺的直接偶联反应中尤其表现出正协同效应。
