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The super acidity of the unsolvated Al(C6F5)3 enabled isolation of the elusive silane–alane complex [SiH⋅⋅⋅Al], which was structurally characterized by spectroscopic and X‐ray diffraction methods. The Janus‐like nature of this adduct, coupled with strong silane activation, effects multifaceted frustrated‐Lewis‐pair‐type catalysis. When compared with the silane–borane system, the silane–alane system...
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