Nafion-Assisted Noncovalent Assembly of Molecular Sensitizers and Catalysts for Sustained Photoreduction of CO2 to COClick to copy article linkArticle link copied!
- Shinbi LeeShinbi LeeDepartment of Chemical Engineering/Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), 77, Cheongam-ro, Pohang, Gyeongsangbuk-do 37673, KoreaMore by Shinbi Lee
- Sujeong KimSujeong KimDepartment of Chemical Engineering/Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), 77, Cheongam-ro, Pohang, Gyeongsangbuk-do 37673, KoreaMore by Sujeong Kim
- Cheolwoo ParkCheolwoo ParkDepartment of Chemical and Biological Engineering, College of Engineering, Sookmyung Women’s University, 99, Cheongpa-ro 47-gil, Seoul 04310, KoreaDepartment of Energy Science, Sungkyunkwan University, 2066, Seobu-ro, Suwon, Gyeonggi-do 16419, KoreaMore by Cheolwoo Park
- Gun-hee MoonGun-hee MoonDepartment of Chemical Engineering/Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), 77, Cheongam-ro, Pohang, Gyeongsangbuk-do 37673, KoreaMore by Gun-hee Moon
- Ho-Jin SonHo-Jin SonDepartment of Advanced Materials Chemistry, Korea University, 2511, Sejong-ro, Sejong 30019, KoreaMore by Ho-Jin Son
- Jin-Ook BaegJin-Ook BaegKorea Research Institute of Chemical Technology, 141, Gajeong-ro, Yuseong, Daejeon 34114, KoreaMore by Jin-Ook Baeg
- Wooyul Kim*Wooyul Kim*Email: [email protected]. Phone: +82-2-2077-7441 (W.K.).Department of Chemical and Biological Engineering, College of Engineering, Sookmyung Women’s University, 99, Cheongpa-ro 47-gil, Seoul 04310, KoreaMore by Wooyul Kim
- Wonyong Choi*Wonyong Choi*Email: [email protected]. Phone: +82-54-279-2283 (W.C.).Department of Chemical Engineering/Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), 77, Cheongam-ro, Pohang, Gyeongsangbuk-do 37673, KoreaMore by Wonyong Choi
Abstract
The efficient coupling of light absorbers with catalysts is the most critical step in the multielectron transfer process for CO2 conversion. Here a heterogenized photoconversion system consisting of noncovalent assembly is tested and proposed. Nafion (Nf) polymer is employed as a simple and robust platform that couples the light absorber (Ru-(bpy)32+: RuL) and the catalyst (fac-Re(bpy)(CO)3Cl: Re(I)) without making any chemical linkage between them to drive the reductive conversion of CO2 to CO. The results clearly show that the ternary Re(I)-RuL-Nf system exhibits higher photoconversion of CO2 and higher photostability than those of the homogeneous Re(I)-RuL system without Nf. Nf polymer backbone provides sulfonate ionic exchange sites that tightly bind cationic RuL through electrostatic attraction. The Nf-bound RuL sensitizers hinder the destructive self-sensitized reaction but enhance the chance of bimolecular electron transfer from the excited RuL to Re(I), which was confirmed by time-resolved spectroscopic analysis. The total turnover number (TON) of produced CO after 20 h reached 454 in the Re(I)-RuL-Nf system (vs TON 110 in Re(I)-RuL), which demonstrated the essential role of Nf in the photoconversion process.
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