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Deprotonation of [Et3NH][C5(CN)5] with metal bases provides a very simple approach to coordination compounds containing the pentacyanocyclopentadienide anion [C5(CN)5]− (1). The three‐dimensional polymer [Na(thf)1.5(1)]∞ and the molecular dimer [{(tmeda)2Na(1)}2] are obtained by reaction of this precursor with NaH in the presence of thf or tmeda (Me2NCH2CH2NMe2). Their single‐crystal X‐ray structures...
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