Abstract
Although 2Dπ-d conjugated metal-organic frameworks (MOFs) exhibit high in-plane conductivity, the closely stacked layers result in low specific surface area and difficulty in mass transfer and diffusion. Hence, a conductive 3DMOF Fe3(HITP)2/bpm@Co (HITP = 2,3,6,7,10,11-hexaiminotriphenylene) is reported through inserting bpm (4,4'-bipyrimidine) ligands and Co2+ into the interlayers of 2D MOF Fe3(HITP)2. Compared to 2D Fe3(HITP)2 (37.23m2g-1), 3D Fe3(HITP)2/bpm@Co displays a huge improvement in the specific surface area (373.82m2g-1). Furthermore, the combined experimental and density functional theory (DFT) theoretical calculations demonstrate the metallic behavior of Fe3(HITP)2/bpm@Co, which will benefit to the electrocatalytic activity of it. Impressively, Fe3(HITP)2/bpm@Co exhibits prominent and stable oxygen evolution reaction (OER) performance (an overpotential of 299mV vs RHE at a current density of 10mAcm-2 and a Tafel slope of 37.14mVdec-1), which is superior to 2D Fe3(HITP)2 and comparable to commercial IrO2. DFT theoretical calculation reveals that the combined action of the Fe and Co sites in Fe3(HITP)2/bpm@Co is responsible for the enhanced electrocatalytic activity. This work provides an alternative approach to develop conductive 3D MOFs as efficient electrocatalysts.
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