Zeolite Membrane-Based Artificial Photosynthetic Assembly for Long-Lived Charge Separation

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Abstract
Photochemically generated long-lived charge separation is the key step in processes that aim for conversion of solar energy into chemical energy. In this study, we focus on a Ru polypyridyl complex [(bpy)2Ru(II)L, bpy = bipyridine, L = 1,2-bis[4-(4‘-2,2‘-bipyridyl) ethene] encapsulated on the surface of a pinhole-free zeolite membrane by quaternization of L and surrounded with intrazeolitic bipyridinium ions (N,N‘-trimethyl-2,2‘-bipyridinium ion, 3DQ2+). Visible-light irradiation of the Ru complex side of the membrane in the presence of a sacrificial electron donor led to formation of PVS-• on the other side. Pore-blocking disilazane-based chemistry allows for Na+ to migrate through the membrane to maintain charge balance, while keeping the 3DQ2+ entrapped in the zeolite. These results provide encouragement that the zeolite membrane based architecture has the necessary features for not only incorporating molecular assemblies with long-lived charge separation but also for ready exploitation of the spatially separated charges to store visible light energy in chemical species.

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