Electronic modulation of metal-support interactions improves polypropylene hydrogenolysis over ruthenium catalysts.

ABSTRACT: Ruthenium (Ru) is the one of the most promising catalysts for polyolefin hydrogenolysis. Its performance varies widely with the support, but the reasons remain unknown. Here, we introduce a simple synthetic strategy (using ammonia as a modulator) to tune metal-support interactions and apply it to Ru deposited on titania (TiO₂). We demonstrate that combining deuterium nuclear magnetic resonance spectroscopy with temperature variation and density functional theory can reveal the complex nature, binding strength, and H amount. H₂ activation occurs heterolytically, leading to a hydride on Ru, an H⁺ on the nearest oxygen, and a partially positively charged Ru. This leads to partial reduction of TiO₂ and high coverages of H for spillover, showcasing a threefold increase in hydrogenolysis rates. This result points to the key role of the surface hydrogen coverage in improving hydrogenolysis catalyst performance.

SUBMITTER: Kots PA 

PROVIDER: S-EPMC9440920 | biostudies-literature | 2022 Sep

REPOSITORIES: biostudies-literature