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Activation of [CrCl3{R-SN(H)S-R}] Catalysts for Selective Trimerization of Ethene: A Freeze-Quench Cr K-Edge XAFS Study

DOI: 10.1021/cs501017g DOI Help

Authors: Stuart Bartlett (University of Southampton; Research Complex at Harwell) , Jerome Moulin (University of Southampton) , Moniek Tromp (Southampton University) , Gill Reid (University of Southampton) , Andrew Dent (Diamond Light Source Ltd) , Giannantonio Cibin (Diamond Light Source) , David S. Mcguinness (University of Tasmania) , John Evans (University of Southampton; Research Complex at Harwell; Diamond Light Source , Diamond Light Source)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Catalysis , VOL 4 (11) , PAGES 4201-4204

State: Published (Approved)
Published: October 2014
Diamond Proposal Number(s): 8956

Open Access Open Access

Abstract: Homogeneous chromium catalysts for the selective conversion of ethene to hex-1-ene are formed from Cr(III) reagents, aminothioether ligands of the type HN(CH2CH2SR)2, and aluminum reagents. In this study, the early activation steps are investigated by EPR, UV–visible, and Cr K-edge XAFS spectroscopy; rapid stopped-flow mixing and a freeze-quench allows good quality EXAFS analysis of a species formed in ?1 s of reaction. This is shown to involve reduction to Cr(II) and deprotonation of a NH group of the auxiliary ligand. This 4-coordinate metal center may act as precursor for the coordination of ethene and subsequent selective oligomerization.

Journal Keywords: Homogeneous Catalysis; Chromium; Oligomerization; Xafs Spectroscopy; Dft Calculations

Subject Areas: Chemistry

Instruments: B18-Core EXAFS

Other Facilities: ESRF BM26A