Two dicopper(II)-paddlewheel-based metal–organic frameworks (PCN-81 and -82) have been synthesized by using tetratopic ligands featuring 90°-carbazole–dicarboxylate moieties. Both adopt 12-connected tfb topology with nanoscopic octahedra as building units. The freeze-dried PCN-82 shows Brunauer–Emmett–Teller (BET) and Langmuir surface areas as high as 4488 and 4859 m2 g−1, respectively. It also exhibits high H2-adsorption capacity at low pressure (300 cm3 g−1 or 2.6 wt% at 77 K and 1 bar), which can be attributed to its high surface area, microporosity, and open metal sites.
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