Highly Selective and Efficient Perdeuteration of n-Pentane via H/D Exchange Catalyzed by a Silica-Supported Hafnium-Iridium Bimetallic Complex.

Autor: Pichugov AV; Laboratory of Catalysis, Polymerization, Processes and Materials, CP2 M UMR 5128, Université de Lyon, Institut de Chimie de Lyon, CNRS, Université Lyon 1, CPE Lyon, 43 Bd du 11 Novembre 1918, F-69616, Villeurbanne, France., Escomel L; Laboratory of Catalysis, Polymerization, Processes and Materials, CP2 M UMR 5128, Université de Lyon, Institut de Chimie de Lyon, CNRS, Université Lyon 1, CPE Lyon, 43 Bd du 11 Novembre 1918, F-69616, Villeurbanne, France., Lassalle S; Laboratory of Catalysis, Polymerization, Processes and Materials, CP2 M UMR 5128, Université de Lyon, Institut de Chimie de Lyon, CNRS, Université Lyon 1, CPE Lyon, 43 Bd du 11 Novembre 1918, F-69616, Villeurbanne, France., Petit J; Laboratory of Catalysis, Polymerization, Processes and Materials, CP2 M UMR 5128, Université de Lyon, Institut de Chimie de Lyon, CNRS, Université Lyon 1, CPE Lyon, 43 Bd du 11 Novembre 1918, F-69616, Villeurbanne, France., Jabbour R; Centre de RMN à Hauts Champs de Lyon CRMN, UMR5082, Université de Lyon, CNRS, ENS Lyon, Université Claude Bernard Lyon 1, 69100, Villeurbanne, France., Gajan D; Centre de RMN à Hauts Champs de Lyon CRMN, UMR5082, Université de Lyon, CNRS, ENS Lyon, Université Claude Bernard Lyon 1, 69100, Villeurbanne, France., Veyre L; Laboratory of Catalysis, Polymerization, Processes and Materials, CP2 M UMR 5128, Université de Lyon, Institut de Chimie de Lyon, CNRS, Université Lyon 1, CPE Lyon, 43 Bd du 11 Novembre 1918, F-69616, Villeurbanne, France., Fonda E; Synchrotron SOLEIL L'Orme des Merisiers, Saint Aubin BP-48, 91192, Gif sur Yvette, France., Lesage A; Centre de RMN à Hauts Champs de Lyon CRMN, UMR5082, Université de Lyon, CNRS, ENS Lyon, Université Claude Bernard Lyon 1, 69100, Villeurbanne, France., Thieuleux C; Laboratory of Catalysis, Polymerization, Processes and Materials, CP2 M UMR 5128, Université de Lyon, Institut de Chimie de Lyon, CNRS, Université Lyon 1, CPE Lyon, 43 Bd du 11 Novembre 1918, F-69616, Villeurbanne, France., Camp C; Laboratory of Catalysis, Polymerization, Processes and Materials, CP2 M UMR 5128, Université de Lyon, Institut de Chimie de Lyon, CNRS, Université Lyon 1, CPE Lyon, 43 Bd du 11 Novembre 1918, F-69616, Villeurbanne, France.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Apr 15; Vol. 63 (16), pp. e202400992. Date of Electronic Publication: 2024 Mar 07.
DOI: 10.1002/anie.202400992
Abstrakt: A Surface OrganoMetallic Chemistry (SOMC) approach is used to prepare a novel hafnium-iridium catalyst immobilized on silica, HfIr/SiO 2 , featuring well-defined [≡SiOHf(CH 2 t Bu) 2 (μ-H) 3 IrCp*] surface sites. Unlike the monometallic analogous materials Hf/SiO 2 and Ir/SiO 2 , which promote n-pentane deuterogenolysis through C-C bond scission, we demonstrate that under the same experimental conditions (1 bar D 2 , 250 °C, 3 h, 0.5 mol %), the heterobimetallic catalyst HfIr/SiO 2 is highly efficient and selective for the perdeuteration of alkanes with D 2 , exemplified on n-pentane, without substantial deuterogenolysis (<2 % at 95 % conversion). Furthermore this HfIr/SiO 2 catalyst is robust and can be re-used several times without evidence of decomposition. This represents substantial advance in catalytic H/D isotope exchange (HIE) reactions of C(sp 3 )-H bonds.
(© 2024 Wiley‐VCH GmbH.)
Databáze: MEDLINE
Externí odkaz: