Electronic Control of Spin Coupling in Keplerate‐Type Polyoxomolybdates

Redox-controlled magnetism: The partial reduction of polyoxomolybdate building blocks in Keplerate cluster structures allows the magnetic superexchange mediated by these diamagnetic blocks to be altered. The isolation of a 16-fold reduced {MoV/VI72FeIII30} species illustrates how Raman-monitored synthesis can result in such clusters comprising a well-defined assembly of spin centers.