基于层状氢氧化铝构建的用于氢化反应的固体表面受阻路易斯酸碱对。
Solid surface frustrated Lewis pair constructed on layered AlOOH for hydrogenation reaction.
作者信息
Liu Shulin, Dong Minghua, Wu Yuxuan, Luan Sen, Xin Yu, Du Juan, Li Shaopeng, Liu Huizhen, Han Buxing
机构信息
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
出版信息
Nat Commun. 2022 Apr 28;13(1):2320. doi: 10.1038/s41467-022-29970-6.
Designing heterogeneous solid surface frustrated Lewis pair (ssFLP) catalyst for hydrogenation is a new challenge in catalysis and no research has been reported on the construction of ssFLP on boehmite (AlOOH) surfaces up to now as far as we know. Herein, AlOOH with a layer structure is prepared and it is found that the Lewis basic O site (one H removed from OH) and an adjacent Lewis acidic unsaturated Al site (Al.) proximal to a surface OH (OH vacancy) on AlOOH layers could form the ssFLP. The layered structure of AlOOH and its abundant OH defects over the surface result in a high concentration of O/Al. FLPs, which are conducive to highly efficient hydrogen activation for hydrogenation of olefins and alkynes with low H-H bond dissociates activation energy of 0.16 eV under mild conditions (T = 80°C and P(H) = 2.0 MPa). This work develops a new kind of hydrogenation catalyst and provides a new perspective for creating solid surface FLP.
设计用于氢化的非均相固体表面受阻路易斯对（ssFLP）催化剂是催化领域的一项新挑战，据我们所知，迄今为止尚未有关于在勃姆石（AlOOH）表面构建ssFLP的研究报道。在此，制备了具有层状结构的AlOOH，发现AlOOH层上的路易斯碱性O位点（从OH中除去一个H）和与表面OH（OH空位）相邻的路易斯酸性不饱和Al位点（Al.）可以形成ssFLP。AlOOH的层状结构及其表面丰富的OH缺陷导致O/Al FLP的高浓度，这有利于在温和条件下（T = 80°C，P(H) = 2.0 MPa）以低H-H键解离活化能0.16 eV对烯烃和炔烃进行高效氢活化用于氢化反应。这项工作开发了一种新型氢化催化剂，并为创建固体表面FLP提供了新的视角。
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