Frustrated Lewis pairs on pentacoordinated Al 3+ -enriched Al 2 O 3 promote heterolytic hydrogen activation and hydrogenation

was activated by surface FLPs in a heterolytic pathway, leading to the hydrogenation of styrene in a stepwise process. This work paves the way for the exploration of more underlying heterogeneous FLPs catalysts and further understanding of accurate active sites and catalytic mechanisms of heterogeneous FLPs at the molecular level.