Since the industrial revolution, burning fossil fuels has thrown our planet into an energy and environmental crisis. It is our long-range goal to precisely control both distance and orientation of two organic catalysts, which are used for the hydrogen evolution reaction to produce a cleaner fuel, within a single framework structure and evaluate its catalytic performance. Artificial photosynthesis has been extensively studied to mimic plants ability to store, convert, and utilize sustainable solar energy. As emerging nanoporous materials, metal-organic frameworks (MOFs) can serve as photocatalysts to efficiently convert solar energy into chemical fuels due to their high surface area and porous characteristics. Our lab has synthesized and characterized NPF-210, a MOF composed of Zr6O8 clusters and a tetratopic ligand, with scu topology. Interestingly, secondary ligands of varying lengths can be inserted into NPF-210. In this, we aim to selectively incorporate a photosensitizer (PS) and a metal-comlex based catalyst (MC, a diiron complex based catalyst for hydrogen evolution reaction, HER) as secondary linkers within NPF-210 and to test its catalytic activity. This study will reveal the relationship between MOF structure and photocatalytic activity. We expect that, with successful insertion of the PS and MC ligands, NPF-210 could exhibit good hydrogen evolution catalytic activities upon optimization of the angle and distance of the two ligands. First, the primary tetratopic linker will be synthesized and used to connect with the octahedral Zr6O8 cluster and form NPF-210. Next, we will synthesize both PS and MC linkers and insert them into NPF-210 after characterizing them using 1H NMR spectroscopy. Lastly, the completed MOF, with both ligands inserted, will be characterized by powder X-ray diffraction, BET surface area measurement and single crystal X-ray diffraction. Our collaborators will test the HER performance and conduct the mechanistic studies.

Installing biomimetic diiron complex in metal-organic framework for photocatalytic hydrogen evolution

255th National Meeting (2018)

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