Comparing the Nature of Active Sites in Cu-loaded SAPO-34 and SSZ-13 for the Direct Conversion of Methane to Methanol
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 CO<sub>2</sub> emissions in comparison to using petroleum. In this study, we investigate the perfor...
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MDPI AG
2020-02-01
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| Series: | Catalysts |
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| Online Access: | https://www.mdpi.com/2073-4344/10/2/191 |
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doaj-98d738146a5a42e395e929de2db833fa2020-11-25T02:16:09ZengMDPI AGCatalysts2073-43442020-02-0110219110.3390/catal10020191catal10020191Comparing the Nature of Active Sites in Cu-loaded SAPO-34 and SSZ-13 for the Direct Conversion of Methane to MethanolKaroline Kvande0Dimitrios K. Pappas1Michael Dyballa2Carlo Buono3Matteo Signorile4Elisa Borfecchia5Kirill A. Lomachenko6Bjørnar Arstad7Silvia Bordiga8Gloria Berlier9Unni Olsbye10Pablo Beato11Stian Svelle12Center for Materials Science and Nanotechnology (SMN), Department of Chemistry, University of Oslo, 1033 Blindern, 0315 Oslo, NorwayCenter for Materials Science and Nanotechnology (SMN), Department of Chemistry, University of Oslo, 1033 Blindern, 0315 Oslo, NorwayCenter for Materials Science and Nanotechnology (SMN), Department of Chemistry, University of Oslo, 1033 Blindern, 0315 Oslo, NorwayCenter for Materials Science and Nanotechnology (SMN), Department of Chemistry, University of Oslo, 1033 Blindern, 0315 Oslo, NorwayDepartment of Chemistry, NIS Center and INSTM Reference Center, University of Turin, via P. Giuria 7, 10125 Turin, ItalyDepartment of Chemistry, NIS Center and INSTM Reference Center, University of Turin, via P. Giuria 7, 10125 Turin, ItalyEuropean Synchrotron Radiation Facility, 71 avenue des Martyrs, CS 40220, CEDEX 9, 38043 Grenoble, FranceSINTEF Industry, Department of Process Technology, Forskningsveien 1, 0373 Oslo, NorwayDepartment of Chemistry, NIS Center and INSTM Reference Center, University of Turin, via P. Giuria 7, 10125 Turin, ItalyDepartment of Chemistry, NIS Center and INSTM Reference Center, University of Turin, via P. Giuria 7, 10125 Turin, ItalyCenter for Materials Science and Nanotechnology (SMN), Department of Chemistry, University of Oslo, 1033 Blindern, 0315 Oslo, NorwayHaldor Topsøe A/S, Haldor Topsøes Allé 1, DK-2800 Kgs. Lyngby, DenmarkCenter for Materials Science and Nanotechnology (SMN), Department of Chemistry, University of Oslo, 1033 Blindern, 0315 Oslo, NorwayOn 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 CO<sub>2</sub> 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 CH<sub>4</sub>-TPR, it is evident that SAPO-34 requires a higher temperature for CH<sub>4</sub> oxidation, and by changing the CH<sub>4</sub> 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 O<sub>2</sub>-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.https://www.mdpi.com/2073-4344/10/2/191methanemethanolzeolitechabazitespectroscopytpr |
| collection |
DOAJ |
| language |
English |
| format |
Article |
| sources |
DOAJ |
| author |
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 |
| spellingShingle |
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 Comparing the Nature of Active Sites in Cu-loaded SAPO-34 and SSZ-13 for the Direct Conversion of Methane to Methanol Catalysts methane methanol zeolite chabazite spectroscopy tpr |
| author_facet |
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 |
| author_sort |
Karoline Kvande |
| title |
Comparing the Nature of Active Sites in Cu-loaded SAPO-34 and SSZ-13 for the Direct Conversion of Methane to Methanol |
| title_short |
Comparing the Nature of Active Sites in Cu-loaded SAPO-34 and SSZ-13 for the Direct Conversion of Methane to Methanol |
| title_full |
Comparing the Nature of Active Sites in Cu-loaded SAPO-34 and SSZ-13 for the Direct Conversion of Methane to Methanol |
| title_fullStr |
Comparing the Nature of Active Sites in Cu-loaded SAPO-34 and SSZ-13 for the Direct Conversion of Methane to Methanol |
| title_full_unstemmed |
Comparing the Nature of Active Sites in Cu-loaded SAPO-34 and SSZ-13 for the Direct Conversion of Methane to Methanol |
| title_sort |
comparing the nature of active sites in cu-loaded sapo-34 and ssz-13 for the direct conversion of methane to methanol |
| publisher |
MDPI AG |
| series |
Catalysts |
| issn |
2073-4344 |
| publishDate |
2020-02-01 |
| description |
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 CO<sub>2</sub> 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 CH<sub>4</sub>-TPR, it is evident that SAPO-34 requires a higher temperature for CH<sub>4</sub> oxidation, and by changing the CH<sub>4</sub> 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 O<sub>2</sub>-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. |
| topic |
methane methanol zeolite chabazite spectroscopy tpr |
| url |
https://www.mdpi.com/2073-4344/10/2/191 |
| work_keys_str_mv |
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