Comparing the Nature of Active Sites in Cu-loaded SAPO-34 and SSZ-13 for the Direct Conversion of Methane to Methanol

Autor: Karoline Kvande, Dimitrios K. Pappas, Michael Dyballa, Carlo Buono, Matteo Signorile, Elisa Borfecchia, Kirill A. Lomachenko, Bjørnar Arstad, Silvia Bordiga, Gloria Berlier, Unni Olsbye, Pablo Beato, Stian Svelle
Jazyk: angličtina
Rok vydání: 2020
Předmět:
Zdroj: Catalysts, Vol 10, Iss 2, p 191 (2020)
Druh dokumentu: article
ISSN: 2073-4344
DOI: 10.3390/catal10020191
Popis: On our route towards a more sustainable future, the use of stranded and underutilized natural gas to produce chemicals would be a great aid in mitigating climate change, due to the reduced CO2 emissions in comparison to using petroleum. In this study, we investigate the performance of Cu-exchanged SSZ-13 and SAPO-34 microporous materials in the stepwise, direct conversion of methane to methanol. With the use of X-ray absorption spectroscopy, infrared (in combination with CO adsorption) and Raman spectroscopy, we compared the structure−activity relationships for the two materials. We found that SSZ-13 performed significantly better than SAPO-34 at the standard conditions. From CH4-TPR, it is evident that SAPO-34 requires a higher temperature for CH4 oxidation, and by changing the CH4 loading temperature from 200 to 300 °C, the yield (μmol/g) of SAPO-34 was increased tenfold. As observed from spectroscopy, both three- and four-fold coordinated Cu-species were formed after O2-activation; among them, the active species for methane activation. The Cu speciation in SAPO-34 is distinct from that in SSZ-13. These deviations can be attributed to several factors, including the different framework polarities, and the amount and distribution of ion exchange sites.
Databáze: Directory of Open Access Journals
Nepřihlášeným uživatelům se plný text nezobrazuje