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通过钴和磷酸根有效调控原子分散铑的微环境以提高烯烃氢甲酰化反应的选择性

Effectively Regulating the Microenvironment of Atomically Dispersed Rh through Co and Pi to Promote the Selectivity in Olefin Hydroformylation.

作者信息

Wei Baiyin, Liu Xiaofang, Hua Kaimin, Deng Yuchao, Wang Hui, Sun Yuhan

机构信息

School of Physical Science and Technology, ShanghaiTech University, Shanghai 201203, People's Republic of China.

CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, People's Republic of China.

出版信息

ACS Appl Mater Interfaces. 2021 Apr 7;13(13):15113-15121. doi: 10.1021/acsami.0c21749. Epub 2021 Mar 23.

Abstract

In the study of heterogeneity of homogeneous processes, effective control of the microenvironment of active sites is a reliable means to improve the selectivity of products. Here, we develop a high-performance Rh-based atomically dispersed catalyst for olefin hydroformylation by controlling the electronic environment and spatial distribution of active metals on the supports, which is achieved through wet impregnation of Rh on ZnO modified with Pi and Co. Various characterizations demonstrate that Co weakens Rh-CO interactions and Pi promotes the formation of atomically dispersed Rh, which thereby improves the selectivity of linear aldehydes in hydroformylation. This strategy of rationally designing the local microenvironment of active metals is important to optimize the catalytic performance.

摘要

在均相过程的非均相性研究中,有效控制活性位点的微环境是提高产物选择性的可靠手段。在此,我们通过控制活性金属在载体上的电子环境和空间分布,开发了一种用于烯烃氢甲酰化的高性能铑基原子分散催化剂,这是通过将铑湿浸渍在经Pi和Co改性的ZnO上实现的。各种表征表明,Co减弱了Rh-CO相互作用,Pi促进了原子分散Rh的形成,从而提高了氢甲酰化反应中线性醛的选择性。这种合理设计活性金属局部微环境的策略对于优化催化性能至关重要。

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