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

Pavel A. Kots, Tianjun Xie, Brandon C. Vance, Caitlin M. Quinn, Matheus Dorneles Mello, J. Anibal Boscoboinik, Cong Wang, Pawan Kumar, Eric A. Stach, Nebojsa S. Marinkovic, Lu Ma, Steven N. Ehrlich and Dionisios G. Vlachos ()
Additional contact information
Pavel A. Kots: University of Delaware
Tianjun Xie: University of Delaware
Brandon C. Vance: University of Delaware
Caitlin M. Quinn: University of Delaware
Matheus Dorneles Mello: Brookhaven National Laboratory
J. Anibal Boscoboinik: Brookhaven National Laboratory
Cong Wang: University of Delaware
Pawan Kumar: University of Pennsylvania
Eric A. Stach: University of Pennsylvania
Nebojsa S. Marinkovic: Columbia University
Lu Ma: Brookhaven National Laboratory
Steven N. Ehrlich: Brookhaven National Laboratory
Dionisios G. Vlachos: University of Delaware

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-32934-5

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