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Through topological rationalization, a zeotype mesoporous Zr‐containing metal–organic framework (MOF), namely PCN‐777, has been designed and synthesized. PCN‐777 exhibits the largest cage size of 3.8 nm and the highest pore volume of 2.8 cm3 g−1 among reported Zr‐MOFs. Moreover, PCN‐777 shows excellent stability in aqueous environments, which makes it an ideal candidate as a support to incorporate...
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