Abstract
Self-assembly has proven to be a widely successful synthetic strategy for functional materials, especially for metal–organic materials (MOMs), an emerging class of porous materials consisting of metal–organic frameworks (MOFs) and metal–organic polyhedra (MOPs). However, there are areas in MOM synthesis in which such self-assembly has not been fully utilized, such as controlling the interior of MOM crystals. Here we demonstrate sequential self-assembly strategy for synthesizing various forms of MOM crystals, including double-shell hollow MOMs, based on single-crystal to single-crystal transformation from MOP to MOF. Moreover, this synthetic strategy also yields other forms, such as solid, core-shell, double and triple matryoshka, and single-shell hollow MOMs, thereby exhibiting form evolution in MOMs. We anticipate that this synthetic approach might open up a new direction for the development of diverse forms in MOMs, with highly advanced areas such as sequential drug delivery/release and heterogeneous cascade catalysis targeted in the foreseeable future.
Highlights
Self-assembly has proven to be a widely successful synthetic strategy for functional materials, especially for metal–organic materials (MOMs), an emerging class of porous materials consisting of metal–organic frameworks (MOFs) and metal–organic polyhedra (MOPs)
The sequential steps involved in creating double-shell hollow MOF are shown in Fig. 2: (1) single-crystal to single-crystal transformation from MOP to MOF through postsynthetic linker insertion (I-a), (2) epitaxial growth of MOP on the MOF surface (I-b), (3) insertion of another linker to form double to triplematryoshka metal–organic materials (MOMs) (I-c), and (4) elimination of MOP by chemical etching (I-d)
In summary, we successfully demonstrated the first example of double-shell hollow MOF, UMOM-1-d, via sequential self-assembly, followed by self-disassembly
Summary
Self-assembly has proven to be a widely successful synthetic strategy for functional materials, especially for metal–organic materials (MOMs), an emerging class of porous materials consisting of metal–organic frameworks (MOFs) and metal–organic polyhedra (MOPs). The sequential steps involved in creating double-shell hollow MOF are shown in Fig. 2: (1) single-crystal to single-crystal transformation from MOP to MOF through postsynthetic linker insertion (I-a), (2) epitaxial growth of MOP on the MOF surface (I-b), (3) insertion of another linker to form double to triplematryoshka metal–organic materials (MOMs) (I-c), and (4) elimination of MOP by chemical etching (I-d). Through this stepwise synthetic procedure, we successfully complete form evolution from a parent MOP to various MOMs, including solid, core-shell, double and triple matryoshka, and hollow single- and double-shell structures
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