Kopacka, Gabriela; Wasiluk, Kinga; Majewski, Pawel W.; Kopyt, Michal; Kwiatkowski, Piotr; Megiel, Elzbieta

DOI: PMID:

Abstract

The fixation of carbon dioxide with is one of the most attractive methods for the green utilization of this greenhouse gas and leads to many valuable chems. This process is characterised by 100% atom efficiency; however, an efficient catalyst is required to achieve satisfactory yields. are recognized as being extremely promising for this purpose. Nevertheless, many of the proposed catalysts are based on ions of rare elements or elements not entirely safe for the environment; this is notable with com. unavailable ligands. In an effort to develop novel catalysts for CO2 fixation on an industrial scale, we propose novel , which consist of aluminum ions coordinated with commercially available (Al@NDC) and their nanocomposites with gold nanoparticles entrapped inside their structure (AlAu@NDC). Due to the application of and 5-amino tetrazole as crystallization mediators, the morphol. of the synthesized materials can be modified. The introduction of gold nanoparticles (AuNPs) into the structure of the synthesized Al-based causes the change in morphol. from nano cuboids to nanoflakes, simultaneously decreasing their porosity. However, the homogeneity of the nanostructures in the system is preserved. All synthesized MOF materials are highly crystalline, and the simulation of PXRD patterns suggests the same tetragonal crystallog. system for all fabricated . The fabricated materials are proven to be highly efficient catalysts for carbon dioxide oxide; and propylene oxide. Applying the synthesized catalysts enables the reactions to be performed under mild conditions (90℃; 1 MPa CO2) within a short time and with high conversion and yield (90% conversion of towards with 89% product yield within 2 h). The developed nanocatalysts can be easily separated from the reaction mixture and reused several times (both conversion and yield do not change after five cycles). The excellent performance of the fabricated catalytic materials might be explained by their high microporosity (from 421 m2 g-1 to 735 m2 g-1); many catalytic centers in the structure exhibit Lewis acids' behavior, increased capacity for CO2 adsorption, and high stability. The presence of AuNPs in the synthesized nanocatalysts (0.8% weight/weight) enables the reaction to be performed with a higher yield within a shorter time; this is especially important for less-active such as propylene oxide (two times higher yield was obtained using a nanocomposite, in comparison with Al- without nanoparticles).

Keywords

metal-organic frameworks ; cyclic carbonates ; heterogeneous catalysts ; nanoparticles ; CO2 fixation ; epoxides

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