A family of isomorphous three-dimensional metal-organic frameworks based on bimetallic (FeCo, FeNi, and CoNi) chains with random metal sites have been prepared and magnetically characterized. The solid-solution-type bimetallic materials inherit intrachain ferromagnetic interactions and single-chain-magnet (SCM) behaviors from the homometallic parent materials. Interestingly, different composition dependence of magnetic behaviors has been found. The Fe Ni series (0≤x≤1) show an innocent composition dependence, where the blocking temperature of slow relaxation decreases monotonically as Fe is replaced by less anisotropic Ni . The Fe Co series show an unexpected antagonistic blending effect on slow relaxation: blending Fe and Co tends to depress the spin dynamics, and the bimetallic materials with intermediate composition show significantly lower blocking temperature than both Fe and Co materials. This is quite the opposite of what happens in the Co Ni series, where Co and Ni seem to have a synergetic effect so that slow relaxation in bimetallic systems can be promoted to higher temperature than both Co and Ni materials.
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