Reaction of Molecular Oxygen with an NHC-Coordinated Pd0 Complex: Computational Insights and Experimental Implications†
Brian V. Popp
Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue, Madison, WI 53706, USA, Fax: (+1) 608-262-6143
Search for more papers by this authorJohanna E. Wendlandt
Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue, Madison, WI 53706, USA, Fax: (+1) 608-262-6143
Search for more papers by this authorClark R. Landis Prof.
Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue, Madison, WI 53706, USA, Fax: (+1) 608-262-6143
Search for more papers by this authorShannon S. Stahl Prof.
Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue, Madison, WI 53706, USA, Fax: (+1) 608-262-6143
Search for more papers by this authorBrian V. Popp
Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue, Madison, WI 53706, USA, Fax: (+1) 608-262-6143
Search for more papers by this authorJohanna E. Wendlandt
Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue, Madison, WI 53706, USA, Fax: (+1) 608-262-6143
Search for more papers by this authorClark R. Landis Prof.
Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue, Madison, WI 53706, USA, Fax: (+1) 608-262-6143
Search for more papers by this authorShannon S. Stahl Prof.
Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue, Madison, WI 53706, USA, Fax: (+1) 608-262-6143
Search for more papers by this authorWe thank M. Konnick for providing (IMes)2Pd0. Financial support and computational resources from the following agencies and the UW Parallel Computing Center are gratefully acknowledged: NSF (CHE-0094344 and CHE-0091916), NCSA (CHE-060010T), and gifts from Intel Corporation. NHC=N-heterocyclic carbene.
Graphical Abstract
O2-Aktivierung: Bei der Umsetzung von molekularem Sauerstoff mit einem [Pd0(NHC)2]-Komplex (NHC=N-heterocyclisches Carben) ist die Triebkraft für die Bildung des PdII(η2-O2)-Produkts Berechnungen zufolge unerwartet gering. Entsprechend konnte experimentell eine reversible Koordination von O2 an die Pd(NHC)2-Einheit nachgewiesen werden. Rechnerisch wurde eine schrittweise Reaktion von O2 mit Pd0 über einen η1-O2-Übergangszustand ermittelt.
Supporting Information
Supporting information for this article is available on the WWW under http://www.wiley-vch.de/contents/jc_2001/2007/z603667_s.pdf or from the author.
Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.
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