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Lithium Ion Battery Materials as Tunable, Redox Non-Innocent Catalyst Supports
preprintsubmitted on 09.02.2021, 23:18 and posted on 09.02.2021, 23:51 by Alon Chapovetsky, Ryan J. Witzke, Robert Kennedy, Evan Wegener, Fulya Dogan, Prajay Patel, Magali Ferrandon, Jens Niklas, Oleg Poluektov, Ning Rui, Sanjaya D. Senanayake, José A. Rodriguez, Christopher Johnson, Cynthia Jenks, A. Jeremy Kropf, Cong Liu, Massimiliano Delferro, David Kaphan
The development of general strategies for the electronic tuning of a catalyst’s active site is an ongoing challenge in heterogeneous catalysis. To this end we report the application of cathode and anode materials as redox non-innocent catalyst supports that can be continuously modulated as a function of lithium intercalation. A zero valent nickel complex was oxidatively grafted onto the surface of lithium manganese oxide (LixMn2O4) to yield single-sites of Ni2+ (Ni/LixMn2O4). Its activity for olefin hydrogenation was found to be a function of the redox state of the support material, with the most lithiated variant showing the most activity. X-ray absorption, X-ray photoelectron, solid-state nuclear magnetic resonance and electron paramagnetic resonance spectroscopies, and electron microscopy techniques established the nature of the nickel species on LixMn2O4. Catalyst control through support redox non-innocence was extended to an organotantalum complex on lithium titanium oxide (LixTiO2), demonstrating the generality of this phenomenon.