Lewis Acid Strength of Interfacial Metal Sites Drives CH 3 OH Selectivity and Formation Rates on Cu‐Based CO 2 Hydrogenation Catalysts
| Autor: | David W. Flaherty, Erwin Lam, Christophe Copéret, Daniel T. Bregante, Petr Šot, Gina Noh, Jordan Meyet |
|---|---|
| Rok vydání: | 2021 |
| Předmět: |
010405 organic chemistry
General Chemistry General Medicine 010402 general chemistry Heterogeneous catalysis 01 natural sciences Catalysis 0104 chemical sciences chemistry.chemical_compound Adsorption chemistry Pyridine Polymer chemistry Formate Reactivity (chemistry) Lewis acids and bases Organometallic chemistry |
| Zdroj: | Angewandte Chemie. 133:9736-9745 |
| ISSN: | 1521-3757 0044-8249 |
| DOI: | 10.1002/ange.202100672 |
| Popis: | CH3 OH formation rates in CO2 hydrogenation on Cu-based catalysts sensitively depend on the nature of the support and the presence of promoters. In this context, Cu nanoparticles supported on tailored supports (highly dispersed M on SiO2 ; M=Ti, Zr, Hf, Nb, Ta) were prepared via surface organometallic chemistry, and their catalytic performance was systematically investigated for CO2 hydrogenation to CH3 OH. The presence of Lewis acid sites enhances CH3 OH formation rate, likely originating from stabilization of formate and methoxy surface intermediates at the periphery of Cu nanoparticles, as evidenced by metrics of Lewis acid strength and detection of surface intermediates. The stabilization of surface intermediates depends on the strength of Lewis acid M sites, described by pyridine adsorption enthalpies and 13 C chemical shifts of -OCH3 coordinated to M; these chemical shifts are demonstrated here to be a molecular descriptor for Lewis acid strength and reactivity in CO2 hydrogenation. |
| Databáze: | OpenAIRE |
| Externí odkaz: |
|
| Nepřihlášeným uživatelům se plný text nezobrazuje | K zobrazení výsledku je třeba se přihlásit. |