A Highly Stable Zeotype Mesoporous Zirconium Metal–Organic Framework with Ultralarge Pores

Abstract 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 cm 3 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 different functional moieties. Through facile internal surface modification, the interaction between PCN‐777 and different guests can be varied to realize efficient immobilization.