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Seven new metal–organic frameworks (MOFs) have been synthesized using different organic amines as templates: [Cd(HBTC) 2]·2(HDETA)·4(H 2O) ( 1) (BTC = 1,3,5-benzenetricarboxylate and DETA = diethylenetriamine), [Cd 2(BTC) 2(H 2O) 2]·2(HCHA)·2(EtOH)·2(H 2O) (CHA = cyclohexylamine) ( 2), [Cd 5(BTC) 4Cl 4]·4(HTEA)·2(H 3O) (TEA = triethylamine) ( 3), [Cd 3(BTC) 3(H 2O)]·(HTEA)·2(H 3O) ( 4), [Zn(BTC)(H 2O)]·(HTPA)·(H 2O) (TPA = tri- n-propylamine) ( 5), [Cd(BTC)]·(HTPA)·(H 2O) ( 6), and [Cd 2(BTC)(HBTC)]·(HTBA)·(H 2O) (TBA = tri- n-butylamine) ( 7). Topologically, the polymer 1exhibits a two-dimensional (2D) Cd-HBTC network with (4 4) topology, which is a sql structure; the polymer 2possesses a three-dimensional (3D) porous Cd-BTC framework with (4·6 2) 2(4 2·6 10·8 3) topology, which is a contorted rutile structure; polymer 3exhibits a 3D open Cd-BTC architecture with (6 2·8 2·10 2) 2(6 2·8 4)(6 3) 4topology; polymer 4is a 3D porous Cd-BTC network with new (4·6 2) 2(4 2·6 4·8 6·10 3)(6·8 2) 2(6 2·8 4)(6 2·8 4) 2(6 2·8) 2topology; similar to 1, polymer 5is a 2D Zn-BTC framework with (4·8 2) topology; interestingly, polymer 6possesses a 3D porous Cd-BTC architecture with the same topology as 2; polymer 7shows a 3D open Cd-BTC framework with (6 3)(6 5·10) topology. In addition to the structures of polymers 1– 7, their thermal stabilities, ion exchange properties, and nonbonding interaction energies, including H-bonding and van der Waals, have also been studied. Remarkably, those organic amine cations reside in the interlayer or channel space, playing important roles such as templating, space-filling, and charge-balancing agents. These studies would facilitate the exploration of novel MOFs with charming molecular topologies and multifunctional properties. [ABSTRACT FROM AUTHOR]