American Chemical Society
ja0c02053_si_001.pdf (1.66 MB)

An Artificial Z‑Scheme Constructed from Dye-Sensitized Metal Oxide Nanosheets for Visible Light-Driven Overall Water Splitting

Download (1.66 MB)
journal contribution
posted on 2020-04-27, 14:34 authored by Takayoshi Oshima, Shunta Nishioka, Yuka Kikuchi, Shota Hirai, Kei-ichi Yanagisawa, Miharu Eguchi, Yugo Miseki, Toshiyuki Yokoi, Tatsuto Yui, Koji Kimoto, Kazuhiro Sayama, Osamu Ishitani, Thomas E. Mallouk, Kazuhiko Maeda
Sensitization of a wide-gap oxide semiconductor with a visible-light-absorbing dye has been studied for decades as a means of producing H2 from water. However, efficient overall water splitting using a dye-sensitized oxide photocatalyst has remained an unmet challenge. Here we demonstrate visible-light-driven overall water splitting into H2 and O2 using HCa2Nb3O10 nanosheets sensitized by a Ru­(II) tris-diimine type photosensitizer, in combination with a WO3-based water oxidation photocatalyst and a triiodide/iodide redox couple. With the use of Pt-intercalated HCa2Nb3O10 nanosheets further modified with amorphous Al2O3 clusters as the H2 evolution component, the dye-based turnover number and frequency for H2 evolution reached 4580 and 1960 h–1, respectively. The apparent quantum yield for overall water splitting using 420 nm light was 2.4%, by far the highest among dye-sensitized overall water splitting systems reported to date. The present work clearly shows that a carefully designed dye/oxide hybrid has great potential for photocatalytic H2 production, and represents a significant leap forward in the development of solar-driven water splitting systems.