Syntheses, crystal structures and magnetic properties of three new molecular magnets by self-assembly of bis(maleonitriledithiolate)nickel(III) anion and substituted N,N′-dibenzylpiperidinium

Three new molecular magnets [DiFBzPid][Ni(mnt)2]·0.5CH3COCH3(1), [DiBrBzPid][Ni(mnt)2](2) and [DiNO2BzPid][Ni(mnt)2](3)(mnt2−=maleonitriledithiolate) anion and [DiRBzPid]+ ([DiRBzPid]+=N,N′-diRbenzylpiperidinium; R=F, Br, NO2) have been investigated. The differences in the stacking mode of the anions and the cations result in the differences in magnetic coupling properties, both 1 and 3 show characteristic of spin-gap, while 2 exhibits an antiferromagnetic coupling feature.