The Lewis acids Ga(C₆F₅)₃, In(C₆F₅)₃ and Ga(C₆Cl₅)₃ are prepared and their Lewis acidity has been probed experimentally and computationally. The species Ga(C₆F₅)₃ and In(C₆F₅)₃ in conjunction with phosphine donors are shown to heterolytically split H₂ and catalyse the hydrogenation of an imine. In addition, frustrated Lewis pairs (FLPs) derived from Ga(C₆F₅)₃ and In(C₆F₅)₃ and phosphines react with diphenyldisulfide to phosphoniumgallates or indates of the form [tBu₃PSPh][PhSE(C₆F₅)₃] and [tBu₃PSPh][(μ-SPh)(E(C₆F₅)₃)₂] (E = Ga, In). The potential of the FLPs based on Ga(C₆F₅)₃, In(C₆F₅)₃ and Ga(C₆Cl₅)₃ and phosphines is also shown in reactions with phenylacetylene to give pure or mixtures of the products [tBu₃PH][PhCCE(C₆X₅)₃] and R₃P(Ph)C=C(H)E(C₆X₅)₃ A number of these species are crystallographically characterized. The implications for the use of these species in FLP chemistry are considered.This article is part of the themed issue 'Frustrated Lewis pair chemistry'.

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