Three novel cicada-like nickel(II) clusters, formulated as [Ni6(bdped)2(mba)6(Hdmpz)2(NO3)2(H2O)2]•4MeCN (SD/Ni6b), [Ni5(bdped)2(tca)6(Hdmpz)(MeOH)2(H2O)]•MeOH (SD/Ni5a) and [Ni4(Hbdped)2(ba)4(Hdmpz)2]•2NO3•2MeCN (SD/Ni4a), were obtained by tuning the auxiliary carboxylic acids while H2bdped = 1,2-bis-(3,5-dimethylpyrazol-1-yl)-ethane-1,2-diol; Hmba = 2-methylbenzoic acid;...

Silica‐supported ionic liquid Si–[SbSipim][PF6] as a catalyst was used first in the synthesis of polyhydroquinolines. The catalyst exhibits high catalytic activity in the reaction, and can be easily recovered and reused without significant loss of its activity for six runs. This green method offers several advantages, including high yield, short reaction time, simple work‐up procedure, ease of separation, and recyclability of the catalyst.