Azo-Functionalized Zirconium-Based Metal-Organic Polyhedron as an Efficient Catalyst for CO2 Fixation with Epoxides.
Chemistry
; 27(50): 12890-12899, 2021 Sep 06.
Article
em En
| MEDLINE
| ID: mdl-34288181
ABSTRACT
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 °C and 1â
atm of CO2 ). The work provides an effective multi-functional cooperative method for improvement of CO2 cycloaddition.
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Bases de dados:
MEDLINE
Idioma:
En
Revista:
Chemistry
Assunto da revista:
QUIMICA
Ano de publicação:
2021
Tipo de documento:
Article