Magnetism of layered magnets depends on the inter-layer through-space magnetic interactions ( ). Using guest sorption to address inter-layer pores in bulk-layered magnets is an efficient approach to magnetism control because the guest-delicate inter-layer distance ( ) is a variable parameter for modulating . Herein, we demonstrated magnetic changes induced by the adsorption of CO, N, and O gases in various isostructural layered magnets with a π-stacked pillared-layer framework, , (M = Co, 1, Fe, 2, Cr, 3; Cp* = η-CMe; 2,3,5,6-FPhCO = 2,3,5,6-tetrafluorobenzoate; TCNQ = 7,7,8,8-tetracyano--quinodimethane).
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