Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 56, Issue 35, Pages 10367-10372Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201703808
Keywords
heterogeneous catalysis; structure-activity relationships; X-ray absorption spectroscopy; X-ray diffraction; zeolites
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Funding
- Danish National Research Foundation [DNRF93]
- Center for Materials Crystallography (CMC)
- Danish Agency for Science, Technology and Innovation (DANSCATT)
- Ministry of Education and Science of the Russian Federation [14.Y26.31.0001]
- Innovation Fund Denmark [5190-00018B]
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Using quasi-simultaneous in situ PXRD and XANES, the direct correlation between the oxidation state of Cu ions in the commercially relevant deNO(X)NH(3)-SCR zeolite catalyst Cu-CHA and the Cu ion migration in the zeolitic pores was revealed during catalytic activation experiments. A comparison with recent reports further reveals the high sensitivity of the redox-active centers concerning heating rates, temperature, and gas environment during catalytic activation. Previously, Cu+ was confirmed present only in the 6R. Results verify a novel 8R monovalent Cu site, an eventually large Cu+ presence upon healing to high temperatures in oxidative conditions, and demonstrate the unique potential in combining in situ PXRD and XANES techniques, with which both oxidation state and structural location of the redox-active centers in the zeolite framework could be tracked.
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