Formation, Operation and Deactivation of Cr Catalysts in Ethylene Tetramerization Directly Assessed by Operando EPR and XAS

被引:70
作者
Rabeah, Jabor [1 ]
Bauer, Matthias [1 ]
Baumann, Wolfgang [1 ]
McConnell, Ann E. C. [1 ]
Gabrielli, William F. [1 ]
Webb, Paul B. [1 ]
Selent, Detlef [1 ]
Brueckner, Angelika [1 ]
机构
[1] Univ Rostock, Leibniz Inst Katalyse, D-18059 Rostock, Germany
来源
ACS CATALYSIS | 2013年 / 3卷 / 01期
关键词
chromium complexes; ethylene tetramerization; homogeneous catalysis; operando EPR; reaction mechanisms; IN-SITU; LIGAND STRUCTURE; OXIDATION-STATE; CHROMIUM; TRIMERIZATION; COMPLEXES; XANES; OLIGOMERIZATION; MECHANISM;
D O I
10.1021/cs300686m
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Operando EPR under elevated ethylene pressure supported by in situ XAS was for the first time applied to discriminate between active and deactivating Cr species in ethylene tetramerization. Starting from Cr(III) in the Cr(acac)(3) precursor, a (PNP)Cr(II)-(CH3)(2) complex is most likely formed upon adding PNP and MMAO, which is regarded as the active species that converts ethylene to 1-octene by passing a reversible redox cycle, while reduction to Cr(I) leads to deactivation.
引用
收藏
页码:95 / 102
页数:8
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