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Published in: Topics in Catalysis 8-9/2016

21-03-2016 | Original Paper

Operando Molecular Spectroscopy During Ethylene Polymerization by Supported CrO x /SiO2 Catalysts: Active Sites, Reaction Intermediates, and Structure-Activity Relationship

Authors: Anisha Chakrabarti, Maciej Gierada, Jaroslaw Handzlik, Israel E. Wachs

Published in: Topics in Catalysis | Issue 8-9/2016

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Abstract

Time-resolved operando molecular spectroscopy was applied during ethylene polymerization by supported CrO x /SiO2 catalysts to investigate the structure-activity relationships for this important industrial catalytic reaction. A combination of spectroscopic techniques (Raman, UV–Vis, XAS, DRIFTS and TPSR) during ethylene polymerization allows for the first time to monitor the molecular events taking place during activation of supported CrO x /SiO2 catalysts by ethylene and establishment of the structure-activity relationships for this reaction. Based on complementary DFT computational studies, a new initiation mechanism for ethylene polymerization is proposed. During reaction, the initial surface Cr+6O x sites reduce to Cr+3 sites to form Cr–(CH2)2CH=CH2 and Cr–CH=CH2 reaction intermediates with the latter representing the catalytic active site.

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Appendix
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Metadata
Title
Operando Molecular Spectroscopy During Ethylene Polymerization by Supported CrO x /SiO2 Catalysts: Active Sites, Reaction Intermediates, and Structure-Activity Relationship
Authors
Anisha Chakrabarti
Maciej Gierada
Jaroslaw Handzlik
Israel E. Wachs
Publication date
21-03-2016
Publisher
Springer US
Published in
Topics in Catalysis / Issue 8-9/2016
Print ISSN: 1022-5528
Electronic ISSN: 1572-9028
DOI
https://doi.org/10.1007/s11244-016-0546-6

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