Mechanism of Efficient Viologen Radical Generation by Ultrafast Electron Transfer from CdS Quantum Dots

Autor: Ke-Li Han, Tianquan Lian, Feng-Jiao Zhao, Qiuyang Li
Rok vydání: 2018
Předmět:
Zdroj: The Journal of Physical Chemistry C. 122:17136-17142
ISSN: 1932-7455
1932-7447
DOI: 10.1021/acs.jpcc.8b06551
Popis: Artificial photosynthetic systems consisted of nanocrystal light absorbers, molecular redox mediators, and catalysts are one of the most promising and flexible approaches for solar fuel generation because their constituents can be independently tuned. In this work, we investigate the photoreduction of three viologen derivatives, one of the most widely investigated molecular redox mediators, of different redox potentials, 7,8-dihydro-6H-dipyrido[1,2-a:2′,1′-c][1,4]diazepinediium (PDQ2+), methyl viologen (MV2+), and benzyl viologen (BV2+), using CdS quantum dots (QDs) as the light absorber and mercaptopropionic acid as a sacrificial electron donor in aqueous (pH = 7) solution. Under continuous 405 nm light-emitting diode illumination, the steady-state radical generation quantum yield (QY) follows the order of PDQ•+ (15.99%) > MV•+ (12.61%) > BV•+ (6.56%). Transient absorption spectroscopy studies show that while the rates of initial electron transfer (ET) from the excited QD conduction band to the mediators...
Databáze: OpenAIRE