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A general strategy and a consolidated mechanism for low-methane hydrogenolysis of polyethylene over ruthenium

https://doi.org/10.1016/j.apcatb.2022.121899

Wang, Cong ; Yu, Kewei ; Sheludko, Boris ; Xie, Tianjun ; Kots, Pavel A. ; Vance, Brandon C. ; Kumar, Pawan ; Stach, Eric A. ; Zheng, Weiqing ; Vlachos, Dionisios G. ( December 2022 , Applied Catalysis B: Environmental)

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

https://doi.org/10.1038/s41467-022-32934-5

Kots, Pavel A. ; Xie, Tianjun ; Vance, Brandon C. ; Quinn, Caitlin M. ; de Mello, Matheus Dorneles ; Boscoboinik, J. Anibal ; Wang, Cong ; Kumar, Pawan ; Stach, Eric A. ; Marinkovic, Nebojsa S. ; et al ( September 2022 , Nature Communications)

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. H₂activation 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 TiO₂and 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.

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Structure–Property Relationships for Nickel Aluminate Catalysts in Polyethylene Hydrogenolysis with Low Methane Selectivity

https://doi.org/10.1021/jacsau.3c00232

Vance, Brandon C. ; Najmi, Sean ; Kots, Pavel A. ; Wang, Cong ; Jeon, Sungho ; Stach, Eric A. ; Zakharov, Dmitri N. ; Marinkovic, Nebojsa ; Ehrlich, Steven N. ; Ma, Lu ; et al ( July 2023 , JACS Au)