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Electrically Conductive π-Intercalated Graphitic Metal–Organic Framework Containing Alternate π-Donor/Acceptor Stacks



Ashok Yadav, Shiyu Zhang, Paola Benavides, Wei Zhou, Sourav Saha


Electrical conductivity of metal-organic frameworks (MOFs) is a function of charge-carrier density and long-range charge transport capability. Although two-dimensional graphitic MOFs (GMOF) exhibit high intrinsic conductivity (σ ≥ 1 S/m) chiefly due to efficient through-bond charge movement within the hexagonal sheets consisting of metal-ligand coordination networks, less efficient out-of-plane charge movement through slipped-parallel stacked layers often creates large disparities between anisotropic conductivities in orthogonal directions and limits the bulk conductivity. Herein, we demonstrate a novel strategy to boost out-of-plane charge movement capacity and the bulk conductivity of GMOFs by developing the first π-intercalated GMOF (iGMOF-1) containing built-in alternating π-donar/acceptor stacks of π-donor 2,3,6,7,10.11-hexaminotriphenylene (HATP) ligands of Cu3(HATP)2 scaffold and non-coordinatively intercalated π-acidic hexacyanotriphenylene (HCTP) molecules. Since post-synthetic guest intercalation between closely π-stacked GMOF layers is not feasible, iGMOF-1 was prepared in a bottom-up fashion by introducing Cu2+ to preassembled supramolecular [HATP/HCTP]n array. iGMOF-1 pellets consistently displaced an order of magnitude higher electrical conductivity and notable smaller activation energy than Cud3^(HATP)2 pellets (σaverage = 25 vs. 2 S/m, Ea = 36 vs. 65 meV) prepared and measured under the same conditions, which can be attributed to improved out-of-plane charge movement through the alternating HATP/HCTP stacks present in the former, as both materials possessed similar in-plane through-bond charge transport pathways. This breakthrough clears the access to other iGMOFs containing built-in alternating π-donor/acceptor stacks of different redox-complementary ligands and intercalated guests that can precisely regulate the efficacy of out-of-plane charge movement, reduce the differences between anisotropic conductivity, and thereby boost their bulk conductivity.
Journal of American Chemical Society


Porous Material, Electrical Conductivity, Intercalation, Charge Transfer


Yadav, A. , Zhang, S. , Benavides, P. , Zhou, W. and Saha, S. (2023), Electrically Conductive π-Intercalated Graphitic Metal–Organic Framework Containing Alternate π-Donor/Acceptor Stacks, Journal of American Chemical Society, [online],, (Accessed April 23, 2024)
Created June 26, 2023, Updated March 15, 2024