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This work demonstrates a feasible strategy for the synthesis of new zeolite-like framework materials. With the strategy of using two different supertetrahedral clusters as secondary building units, two new heterometallic zeolite-like frameworks with isomeric structures but tunable topologies were first made. Besides, the porous nature and the proton conduction performance of the new materials were further studied.

Graphical abstract: Designed assembly of heterometallic zeolite-like framework materials from two different supertetrahedral metal clusters

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