Mechanochemical preparation of Cu-CHA zeolites for gas phase methane activation
Principal investigator
Project description:
There is a great economic opportunity in developing methods for direct conversion of methane into liquid fuel and chemicals due to its high availability. Currently, the commercial processes involve indirect conversion which is feasible only at large scales. However, the direct conversion of methane into valuable products concerns the challenge of activating one of the most stable of all hydrocarbons. To address these issues, new catalyst and process design are a necessity. Metal-containing zeolite materials comprising copper and iron species as active sites, inspired by the natural enzyme systems represent the most promising catalysts for the methane activation. In the frame of this project, Cu-containing zeolite materials are going to be prepared applying milling processes, an environment-friendly route. The obtained materials will be tested as catalysts in the direct methane conversion into hydrocarbons. The results are expected to serve as the foundation for development of an industrial process thus providing a cost- and energy-efficient solving of the energy feedstocks issue. The work on the topic of direct methane conversion is going to enable new possibilities in finding the appropriate solution of the aim to increase the independence of the Republic of Croatia from the energetical perspective.
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Results:
During this project a series of CHA-type SSZ-13 zeolite materials has been prepared. Powder X-ray diffraction showed all the samples exhibit high crystallinity and that indeed CHA-type materials were attained. SEM micrographs reveal cubic crystal morphology of the synthesized materials and indicate that the changes in the composition of the initial reaction mixture affect the crystal size distribution of the end products. The prepared materials have been ion-exchanged with copper(II) nitrate and copper(II) acetate. According to the XRD measurements, the CHA crystal structure remained preserved after ion-exchange and calcination post-synthesis treatment. Further characterization of the materials showed that the copper occupies cationic positions within the zeolite voids. In addition, copper oxide has been detected as well.
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