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Covalently functionalizing mechanical exfoliated mono‐ and bilayer graphenides with λ‐iodanes led to the discovery that the monolayers supported on a SiO 2  substrate are considerably more reactive than bilayers as demonstrated by statistical Raman spectroscopy/microscopy. Supported by DFT calculations we show that ditopic addend binding leads to much more stable products than the corresponding monotopic reactions as a result of the much lower lattice strain of the reactions products. The chemical nature of the substrate (graphene versus SiO 2 ) plays a crucial role.

Substrate‐Modulated Reductive Graphene Functionalization