期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 27, 期 50, 页码 12890-12899出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202102089
关键词
CO2 conversion; CO2 fixation; Cyclic carbonates; MOP; Zr-based metal-organic polyhedron
资金
- China Postdoctoral Science Foundation [2019M663663]
- Basic and Applied Basic Research Foundation of Guangdong Province [2019A1515110551]
- Science Foundation for Distinguished Scholars of Dongguan University of Technology [196100041051]
- National Natural Science Foundation of China [51773165, 51973171]
- Young Talent Support Plan of Xi'an Jiaotong University
A novel catalyst Zr-AZDA was prepared and exhibited efficient performance in CO2 fixation with epoxides, providing an effective multi-functional cooperative method for improvement of CO2 cycloaddition.
Chemical fixation of CO2 as C1 source at ambient temperature and low pressure is an energy-saving way to make use of the green-house gas, but it still remains a challenge since efficient catalyst with high catalytic active sites is required. Here, a novel monoclinic azo-functionalized Zr-based metal-organic polyhedron (Zr-AZDA) has been prepared and applied in CO2 fixation with epoxides. The inherent azo groups not only endow Zr-AZDA with good solubilization, but also act as basic sites to enrich CO2 showing efficient synergistic catalysis as confirmed by TPD-CO2 analysis. XPS results demonstrate that the Zr active sites in Zr-AZDA possess suitable Lewis acidity, which satisfies both substrates activation and products desorption. DFT calculation indicates the energy barrier of the rate-determining step in CO2 cycloaddition could be reduced remarkably (by ca. 60.9 %) in the presence of Zr-AZDA, which may rationalize the mild and efficient reaction condition employed (80 degrees C and 1 atm of CO2). The work provides an effective multi-functional cooperative method for improvement of CO2 cycloaddition.
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