Sapsford, Joshua SJoshua SSapsfordCsókás, DánielDánielCsókásScott, Daniel JDaniel JScottTurnell-Ritson, Roland CRoland CTurnell-RitsonPiascik, Adam DAdam DPiascikPápai, ImreImrePápaiAshley, Andrew EAndrew EAshley2020-07-152021-06-082020-06-08ACS Catalysis, 2020, 10, pp.7573-75832155-5435http://hdl.handle.net/10044/1/80661Cationic Lewis acids (LAs) are gaining interest as targets for frustrated Lewis pair (FLP)-mediated catalysis. Unlike neutral boranes, which are the most prevalent LAs for FLP hydrogenations, the Lewis acidity of cations can be tuned through modulation of the counteranion; however, detailed studies on such anion effects are currently lacking in the literature. Herein, we present experimental and computational studies which probe the mechanism of H2 activation using iPr3SnOTf (1-OTf) in conjunction with a coordinating (quinuclidine; qui) and noncoordinating (2,4,6-collidine; col) base and compare its reactivity with {iPr3Sn·base}{Al[OC(CF3)3]4} (base = qui/col) systems which lack a coordinating anion to investigate the active species responsible for H2 activation and hence resolve any mechanistic roles for OTf– in the iPr3SnOTf-mediated pathway.© 2020 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acscatal.0c020230302 Inorganic Chemistry0305 Organic Chemistry0904 Chemical EngineeringJournal Articlehttps://www.dx.doi.org/10.1021/acscatal.0c02023https://pubs.acs.org/doi/10.1021/acscatal.0c020232155-5435