The dinitroxide bis(TEMPO) bisketal (bTbk) was shown to crystallize into open frameworks whose structures were determined by single-crystal X-ray diffraction. We show that bTbk can be used as a supramolecular building block for the hosting of a plethora of guests inside the 1D channels of its paramagnetic framework, including other radicals such as TEMPO or 2-azaadamantane-N-oxyl. C60 and C70 were also found to be easily included in this open framework during its crystallization. This resulted in well-defined, nanostructured assemblies of composite radical crystals (bTbk/toluene/C60 or C70) or (bTbk/toluene/TEMPO) by a very simple dissolution/crystallization process with tunable guest content. Selective C60 extraction was also demonstrated directly from fullerene soot.
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