title: Design of Polymer Networks Involving a Photoinduced Electronic Transmission Circuit toward Artificial Photosynthesis.
abstract: Many strategies have been explored to achieve artificial photosynthesis utilizing mediums such as liposomes and supramolecules. Because the photochemical reaction is composed of multiple functional molecules, the surrounding microenvironment is expected to be rationally integrated as observed during photosynthesis in chloroplasts. In this study, photoinduced electronic transmission surrounding the microenvironment of Ru(bpy)3(2+) in a polymer network was investigated using poly(N-isopropylacrylamide-co-Ru(bpy)3), poly(acrylamide-co-Ru(bpy)3), and Ru(bpy)3-conjugated microtubules. Photoinduced energy conversion was evaluated by investigating the effects of (i) Ru(bpy)3(2+) immobilization, (ii) polymer type, (iii) thermal energy, and (iv) cross-linking. The microenvironment surrounding copolymerized Ru(bpy)3(2+) in poly(N-isopropylacrylamide) suppressed quenching and had a higher radiative process energy than others. This finding is related to the nonradiative process, i.e., photoinduced H2 generation with significantly higher overall quantum efficiency (13%) than for the bulk solution. We envision that useful molecules will be generated by photoinduced electronic transmission in polymer networks, resulting in the development of a wide range of biomimetic functions with applications for a sustainable society.
authors.affiliation: School of Materials Science, Japan Advanced Institute of Science and Technology , 1-1 Asahidai, Nomi-shi, Ishikawa 923-1292, Japan.
authors.forename: Kosuke
authors.initials: K
authors.lastname: Okeyoshi
authors.affiliation: Department of Chemistry, Faculty of Science, Saitama University , 225 Shimo-okubo, Sakura-ku, Saitama 338-8570, Japan.
authors.forename: Ryuzo
authors.initials: R
authors.lastname: Kawamura
authors.affiliation: Department of Materials Engineering, Graduate School of Engineering, The University of Tokyo , 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.
authors.forename: Ryo
authors.initials: R
authors.lastname: Yoshida
authors.affiliation: RIKEN, 2-1 Hirosawa, Wako-shi, Saitama 351-0198, Japan.
authors.forename: Yoshihito
authors.initials: Y
authors.lastname: Osada
mesh_terms: D015082:2,2'-Dipyridyl / Q000031:analogs & derivatives* / Q000737:chemistry; D000180:Acrylic Resins / Q000737:chemistry*; D040761:Biomimetic Materials / Q000737:chemistry*; D056831:Coordination Complexes; D004583:Electrons; D006859:Hydrogen / Q000737:chemistry; D008027:Light; D008870:Microtubules / Q000737:chemistry; D010777:Photochemistry / Q000379:methods; D010788:Photosynthesis / Q000502:physiology; D013816:Thermodynamics; D000099166:Polyacrylamides; D017975:Ruthenium Compounds
chemical_list: D015082:2,2'-Dipyridyl; D000180:Acrylic Resins; D056831:Coordination Complexes; D006859:Hydrogen; D000099166:Polyacrylamides; C547232:tris(2,2-bipyridine)-ruthenium(II); D017975:Ruthenium Compounds; C052970:poly-N-isopropylacrylamide