Spectral Studies of a Cr(PNP)–MAO System for Selective Ethylene Trimerization Catalysis: Searching for the Active Species
作者： Loi H. Do , Jay A. Labinger , John E. Bercaw
DOI: 10.1021/CS400778A
关键词:
摘要: Variable temperature spectroscopic, kinetic, and chemical studies were performed on a soluble Cr^(III)Cl_3(PNP) (PNP = bis(diarylphosphino)alkylamine) ethylene trimerization precatalyst to map out its methylaluminoxane (MAO) activation sequence. These indicate that treatment of with MAO leads first replacement chlorides alkyl groups, followed by abstraction, then reduction lower–valent species. Reactivity demonstrate the majority chromium species detected are not catalytically active.
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Lucia McDyre, James A. Platts, David M. Smith, Damien M. Murphy, Emma Carter, Kingsley J. Cavell, William F. Gabrielli, Martin J. Hanton, Andrew J. Hallett, Formation of [Cr(CO)x(Ph2PN(iPr)PPh2)]+ Structural Isomers by Reaction of Triethylaluminum with a Chromium N,N-Bis(diarylphosphino)amine Complex [Cr(CO)4(Ph2PN(iPr)PPh2)]+: An EPR and DFT Investigation Organometallics. ,vol. 32, pp. 1924- 1931 ,(2013) , 10.1021/OM400029Y
Lucia McDyre, Emma Carter, Kingsley J. Cavell, Damien M. Murphy, James A. Platts, Katharine Sampford, Benjamin D. Ward, William F. Gabrielli, Martin J. Hanton, David M. Smith, Intramolecular Formation of a CrI(bis-arene) Species via TEA Activation of [Cr(CO)4(Ph2P(C3H6)PPh2)]+: An EPR and DFT Investigation Organometallics. ,vol. 30, pp. 4505- 4508 ,(2011) , 10.1021/OM2006062
Randolf D Köhn, David Smith, Mary F Mahon, Martina Prinz, Shahram Mihan, Gabriele Kociok-Köhn, Coordination chemistry of the activation of [(triazacyclohexane)CrCl3] with [PhNMe2H][B(C6F5)(4)] and AlR3 Journal of Organometallic Chemistry. ,vol. 683, pp. 200- 208 ,(2003) , 10.1016/S0022-328X(03)00634-X
Theodor Agapie, Susan J. Schofer, Jay A. Labinger, John E. Bercaw, Mechanistic Studies of the Ethylene Trimerization Reaction with Chromium−Diphosphine Catalysts: Experimental Evidence for a Mechanism Involving Metallacyclic Intermediates Journal of the American Chemical Society. ,vol. 126, pp. 1304- 1305 ,(2004) , 10.1021/JA038968T
Angelika Brückner, Jabor K. Jabor, Ann E. C. McConnell, Paul B. Webb, Monitoring Structure and Valence State of Chromium Sites during Catalyst Formation and Ethylene Oligomerization by in Situ EPR Spectroscopy Organometallics. ,vol. 27, pp. 3849- 3856 ,(2008) , 10.1021/OM800316M
David S. McGuinness, Olefin oligomerization via metallacycles: dimerization, trimerization, tetramerization, and beyond. Chemical Reviews. ,vol. 111, pp. 2321- 2341 ,(2011) , 10.1021/CR100217Q
Alceo Macchioni, Ion pairing in transition-metal organometallic chemistry. Chemical Reviews. ,vol. 105, pp. 2039- 2073 ,(2005) , 10.1021/CR0300439
Amir Jabri, Claire Temple, Patrick Crewdson, Sandro Gambarotta, Ilia Korobkov, Robbert Duchateau, Role of the metal oxidation state in the SNS-Cr catalyst for ethylene trimerization: isolation of di- and trivalent cationic intermediates. Journal of the American Chemical Society. ,vol. 128, pp. 9238- 9247 ,(2006) , 10.1021/JA0623717
Dorothée Coevoet, Henri Cramail, Alain Deffieux, Caroline Mladenov, Jean-Noël Pedeutour, Frédéric Peruch, New catalysts for olefin polymerization : from elementary processes to the synthesis of polyolefins Polymer International. ,vol. 48, pp. 257- 263 ,(1999) , 10.1002/(SICI)1097-0126(199904)48:4<257::AID-PI99>3.0.CO;2-M
Tom E. Stennett, Mairi F. Haddow, Duncan F. Wass, Avoiding MAO: Alternative Activation Methods in Selective Ethylene Oligomerization Organometallics. ,vol. 31, pp. 6960- 6965 ,(2012) , 10.1021/OM300739M