H2 Photogeneration Using a Phosphonate-Anchored Ni-PNP Catalyst on a Band-Edge-Modified p-Si(111)|AZO Construct
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- 作者：Hark Jin Kim ; Junhyeok Seo ; Michael J. Rose
- 刊名：ACS Applied Materials & Interfaces
- 出版年：2016
- 出版时间：January 20, 2016
- 年：2016
- 卷：8
- 期：2
- 页码：1061-1066
- 全文大小：389K
- ISSN：1944-8252
文摘
We report the fabrication of a {semiconductor}|{metal oxide}|{molecular catalyst} construct for the photogeneration of dihydrogen (H2) under illumination, including band-edge modulation of the semiconductor electrode depending on the identity of Si(111)–R and the metal oxide. Briefly, a synergistic band-edge modulation is observed upon (i) the introduction of a p-Si|n-AZO heterojunction and (ii) introduction of an organic dimethoxyphenyl (diMeOPh) group at the heterojunction interface; the AZO also serves as a transparent and conductive conduit, which was capped with an ultrathin layer (20 ?) of amorphous TiO2 for stability. A phosphonate-appended PNP ligand and its Ni complex were then adsorbed to the p/n heterojunction for photoelectrochemical H2 generation (figures of merit: Vonset ≈ + 0.03 V vs NHE, Jmax ≈ 8 mA cm–2 at 60 mM TsOH).