Photocatalytic Hydrogen Evolution Driven by a Heteroleptic Ruthenium(II) Bis(terpyridine) Complex

Autor: Elodie Rousset, Mira T. Rupp, Dirk G. Kurth, Gabriel M. Mercier, Garry S. Hanan, Valérie Marvaud, Thomas Auvray
Přispěvatelé: Université de Montréal (UdeM), Institut Parisien de Chimie Moléculaire (IPCM), Chimie Moléculaire de Paris Centre (FR 2769), Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)
Jazyk: angličtina
Rok vydání: 2019
Předmět:
Zdroj: Inorganic Chemistry
Inorganic Chemistry, American Chemical Society, 2019, 58 (14), pp.9127-9134. ⟨10.1021/acs.inorgchem.9b00698⟩
ISSN: 0020-1669
1520-510X
Popis: International audience; Since the initial report by Lehn et al. in 1979, ruthenium tris(bipyridine) ([Ru(bpy) 3 ] 2+) and its numerous derivatives were applied as photosensitizers (PSs) in a large panel of photocatalytic conditions while the bis(terpyridine) analogues were disregarded because of their low quantum yields and short excited-state lifetimes. In this study, we prepared a new terpyridine ligand, 4′-(4-bromophenyl)-4,4‴:4″,4‴′-dipyridinyl-2,2′:6′,2″-terpyridine (Bipytpy) and used it to prepare the heteroleptic complex [Ru(Tolyltpy)(Bipytpy)](PF 6) 2 (1; Tolyltpy = 4′-tolyl-2,2′:6′,2′-terpyridine). Complex 1 exhibits enhanced photophysical properties with a higher quantum yield (7.4 × 10-4) and a longer excited-state lifetime (3.8 ns) compared to those of [Ru(Tolyltpy) 2 ](PF 6) 2 (3 × 10-5 and 0.74 ns, respectively). These enhanced photophysical characteristics and the potential for PS-catalyst interaction through the peripheral pyridines led us to apply the complex for visible-light-driven hydrogen evolution. The photocatalytic system based on 1 as the PS, triethanolamine as a sacrificial donor, and cobaloxime as a catalyst exhibits sustained activity over more than 10 days under blue-light irradiation (light-emitting diode centered at 450 nm). A maximum turnover number of 764 was obtained after 12 days.
Databáze: OpenAIRE