Snapshots of Cooperative Trimetallic Alkene Hydrogenation
Bimetallic cooperativity and synergistic effects have emerged as powerful tools that can enhance the reactivity and selectivity of catalytic systems, offering a pathway toward the development of catalysts based on Earth-abundant elements. Although not uncommon in nature, discrete molecular systems f...
| Autores: | , , |
|---|---|
| Tipo de recurso: | artículo |
| Fecha de publicación: | 2025 |
| País: | España |
| Institución: | Universidad Complutense de Madrid (UCM) |
| Repositorio: | Docta Complutense |
| Idioma: | inglés |
| OAI Identifier: | oai:docta.ucm.es:20.500.14352/131544 |
| Acceso en línea: | https://hdl.handle.net/20.500.14352/131544 |
| Access Level: | acceso abierto |
| Palabra clave: | 54 Catalytic reactions Hydrocarbons Hydrogenation Ligands Metals Química 23 Química |
| Sumario: | Bimetallic cooperativity and synergistic effects have emerged as powerful tools that can enhance the reactivity and selectivity of catalytic systems, offering a pathway toward the development of catalysts based on Earth-abundant elements. Although not uncommon in nature, discrete molecular systems featuring more than two cooperative metal sites are virtually unknown. Herein we report the design of a well-defined molecular heterotrimetallic [Ga2Ni] system, which is effective in alkene hydrogenation catalysis. Species representing ‘snapshots’ of the catalytic cycle are isolated through consecutive addition of ethylene and dihydrogen, allowing for in-depth experimental mechanistic elucidation of two sequential 2-electron oxidative processes. Alongside combined computational, kinetic, and isotopic labeling studies, these findings reveal a fully mapped hydrogenation mechanism in which all three metal sites partake in the alkene hydrogenation process. This system thus provides unique insights into cooperative molecular multimetallic catalysis and establishes a blueprint for rationally designed multicentered cooperativity beyond established diatomic concepts. |
|---|