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Low‐density, solid‐state, porous supramolecular organic frameworks are constructed using pillarenes. The frameworks have a honeycomb‐like structure, permanent porosity, high thermal stability, and selective and reversible sorption properties toward CO2. The exceptionally selective CO2‐sorption properties (375/1, 339/1) of one framework over N2 and CH4 indicate potential applications in CO2‐capture...
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