Photoinduced Electron Transfer from Nitrogen-Doped Tantalum Oxide to Adsorbed Ruthenium Complex

Autor: Shunsuke Sato, Tsutomu Kajino, Takeshi Morikawa, Masayo Iwaki, Ken-ichi Yamanaka
Rok vydání: 2011
Předmět:
Zdroj: The Journal of Physical Chemistry C. 115:18348-18353
ISSN: 1932-7455
1932-7447
DOI: 10.1021/jp205223k
Popis: To understand the photoinduced electron-transfer process and the reaction mechanism of semiconductor/metal-complex hybrid CO2-reducing photocatalysts, the excited-state dynamics of nitrogen-doped Ta2O5 (N–Ta2O5) and that adsorbed with Ru complexes (Ru/N–Ta2O5) were investigated. Upon adsorption of the Ru complex ([Ru(dcbpy)2(CO)2]2+) on N–Ta2O5 powder, one of the CO ligands was exchanged to COOH ([Ru(dcbpy)2(CO)(COOH)]+), which resulted in absorption spectral changes in UV/visible and infrared regions (dcbpy: 4,4′-dicarboxy-2,2′-bipyridine). A detailed analysis of time-resolved emission measurements after excitation at 400 nm (Ta 4f ← N 2p transition) revealed a fast trapping process from shallow defect sites to deep defect sites with a time constant of 24 ± 1 ps in N–Ta2O5 powder. In Ru/N–Ta2O5, ultrafast electron transfer from the shallow defect sites of N–Ta2O5 to the adsorbed Ru complex occurred with a time constant of 12 ± 1 ps. The values of rate constant (ket) and quantum yield (Φet) of the electro...
Databáze: OpenAIRE