Rapid Polyolefin Hydrogenolysis by a Single-Site Organo-Tantalum Catalyst on a Super-Acidic Support: Structure and Mechanism.
Angew Chem Int Ed Engl
; 62(50): e202312546, 2023 Dec 11.
Article
em En
| MEDLINE
| ID: mdl-37948306
ABSTRACT
The novel electrophilic organo-tantalum catalyst AlS/TaNpx (1) (Np=neopentyl) is prepared by chemisorption of the alkylidene Np3 Ta=CHt Bu onto highly Brønsted acidic sulfated alumina (AlS). The proposed catalyst structure is supported by EXAFS, XANES, ICP, DRIFTS, elemental analysis, and SSNMR measurements and is in good agreement with DFT analysis. Catalyst 1 is highly effective for the hydrogenolysis of diverse linear and branched hydrocarbons, ranging from C2 to polyolefins. To the best of our knowledge, 1 exhibits one of the highest polyolefin hydrogenolysis activities (9,800 (CH2 units) â
mol(Ta)-1 â
h-1 at 200 °C/17â
atm H2 ) reported to date in the peer-reviewed literature. Unlike the AlS/ZrNp2 analog, the Ta catalyst is more thermally stable and offers multiple potential C-C bond activation pathways. For hydrogenolysis, AlS/TaNpx is effective for a wide variety of pre- and post-consumer polyolefin plastics and is not significantly deactivated by standard polyolefin additives at typical industrial concentrations.
Texto completo:
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Base de dados:
MEDLINE
Idioma:
En
Ano de publicação:
2023
Tipo de documento:
Article
País de afiliação:
Estados Unidos