title: Zeolite membrane-based artificial photosynthetic assembly for long-lived charge separation.
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)(2)Ru(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, 3DQ(2+)). 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 3DQ(2+) 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.
authors.affiliation: Department of Chemistry, The Ohio State University, 120 West 18th Avenue, Columbus, Ohio 43210, USA.
authors.forename: Yanghee
authors.initials: Y
authors.lastname: Kim
authors.forename: Amitava
authors.initials: A
authors.lastname: Das
authors.forename: Haoyu
authors.initials: H
authors.lastname: Zhang
authors.forename: Prabir K
authors.initials: PK
authors.lastname: Dutta