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We report a comparative study of the binding of I 2 (iodine) in a pair of redox-active metal-organic framework (MOF) materials, MFM-300(V III ) and its oxidized, deprotonated analogue, MFM-300(V IV ). Adsorption of I 2 in MFM-300(V III ) triggers a host-to-guest charge-transfer, accompanied by a partial (∼30%) oxidation of the V III centers in the host framework and formation of I 3  - species residing in the MOF channels. Importantly, this charge-transfer induces a significant enhancement in the electrical conductivity (Δ σ = 7) of I 2 @MFM-300(V III/IV ) in comparison to MFM-300(V III ). In contrast, no host-guest charge-transfer or apparent change in the conductivity was observed upon adsorption of I 2 in MFM-300(V IV ). High-resolution synchrotron X-ray diffraction of I 2 @MFM-300(V III/IV ) confirms the first example of self-aggregation of adsorbed iodine species (I 2 and I 3  - ) into infinite helical chains within a MOF.

Iodine Adsorption in a Redox-Active Metal–Organic Framework: Electrical Conductivity Induced by Host−Guest Charge-Transfer