Ancillary Ligand Effects on Heteroleptic Ir-III Dye in Dye-Sensitized Photocatalytic CO2 Reduction: Photoaccumulation of Charges on Arylated Bipyridine Ligand and Its Control on Catalytic Performance
- Authors
- Jo, Ju Hyoung; Choi, Sunghan; Cheong, Ha-Yeon; Shin, Jae Yoon; Kim, Chul Hoon; Cho, Dae Won; Son, Ho-Jin; Pac, Chyongjin; Kang, Sang Ook
- Issue Date
- 15-12월-2020
- Publisher
- WILEY-V C H VERLAG GMBH
- Keywords
- intraligand electron delocalization; iridium; photochemical CO2 reduction; photochemistry; sensitizer; supported catalysts
- Citation
- CHEMISTRY-A EUROPEAN JOURNAL, v.26, no.70, pp.16733 - 16754
- Indexed
- SCIE
SCOPUS
- Journal Title
- CHEMISTRY-A EUROPEAN JOURNAL
- Volume
- 26
- Number
- 70
- Start Page
- 16733
- End Page
- 16754
- URI
- https://scholar.korea.ac.kr/handle/2021.sw.korea/50788
- DOI
- 10.1002/chem.202002575
- ISSN
- 0947-6539
- Abstract
- Herein, we report the synthesis, and photochemical and -physical properties, as well as the catalytic performance, of a series of heteroleptic Ir-III photosensitizers (IrPSs), [Ir(C<^>N)(2)(N<^>N-Aryl)](+), possessing ancillary ligands that are varied with aryl-substituents on bipyridyl unit [C<^>N=(2-pyridyl)benzo[b]thiophen-3-yl (btp); N<^>N-Aryl=4,4 '-Y-2-bpy (Y=-Ph or -PhSi(Ph)(3)]. We found that the pi-extension of bipyridyl ligand by aryl-substitution put bipyridyl ligand in use as an electron relay unit that performed charge accumulation before delivering to the catalytic center, greatly improving the overall CO2-to-CO conversion activities. In a typical run, the aryl-substituted IrPS ((IrP)-Ir-tBu-Ph-Si)-sensitized homogeneous systems (IrPS+Re-I catalyst) gave a turnover number of 1340 (phi(CO)=24.2 %) at the early stage of photolysis (<5 h). This study demonstrates that the pi-character modulation on the ancillary bipyridyl ligand is critical for forthcoming catalytic performance.
- Files in This Item
- There are no files associated with this item.
- Appears in
Collections - Graduate School > Department of Advanced Materials Chemistry > 1. Journal Articles
Items in ScholarWorks are protected by copyright, with all rights reserved, unless otherwise indicated.