Vacancy-cluster-mediated Surface Activation for Boosting CO Chemical Fixation

Overview

Journal Chem Sci

Publisher Royal Society of Chemistry

Specialty Chemistry

Date 2023 Feb 16

PMID 36794176

Authors

Wenxiu Liu

Lei Li

Wei Shao

Hui Wang

Yun Dong

Ming Zuo

Jiandang Liu

Hongjun Zhang

Bangjiao Ye

Xiaodong Zhang

Yi Xie

Affiliations

Soon will be listed here.

Abstract

The cycloaddition of CO with epoxides towards cyclic carbonates provides a promising pathway for CO utilization. Given the crucial role of epoxide ring opening in determining the reaction rate, designing catalysts with rich active sites for boosting epoxide adsorption and C-O bond cleavage is necessary for gaining efficient cyclic carbonate generation. Herein, by taking two-dimensional FeOCl as a model, we propose the construction of electron-donor and -acceptor units within a confined region vacancy-cluster engineering to boost epoxide ring opening. By combing theoretical simulations and diffuse reflectance infrared Fourier-transform spectroscopy, we show that the introduction of Fe-Cl vacancy clusters can activate the inert halogen-terminated surface and provide reactive sites containing electron-donor and -acceptor units, leading to strengthened epoxide adsorption and promoted C-O bond cleavage. Benefiting from these, FeOCl nanosheets with Fe-Cl vacancy clusters exhibit enhanced cyclic carbonate generation from CO cycloaddition with epoxides.

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