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Reactions between PhSiH3 and alkali‐metal diamidoalkylmagnesiates ([M{N(SiMe3)2}2MgBu], M=Li, Na, K) provide either selective alkyl metathesis or the formation of polyhydride aggregates contingent upon the identity of the Group 1 metal. In the case of [M{N(SiMe3)2}2MgBu], this reactivity results in a structurally unprecedented dodecametallic decahydride cluster species.
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