Atomic Layer Deposition-Confined Nonstoichiometric TiO2 Nanocrystals with Tunneling Effects for Solar Driven Hydrogen Evolution

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• 作者：Peng Zhang ; Takashi Tachikawa ; Mamoru Fujitsuka ; Tetsuro Majima
• 刊名：The Journal of Physical Chemistry Letters
• 出版年：2016
• 出版时间：April 7, 2016
• 年：2016
• 卷：7
• 期：7
• 页码：1173-1179
• 全文大小：528K
• ISSN：1948-7185

文摘

Ti³⁺ self-doped TiO₂ nanocrystals (TNCs) confined with controllable atomic layer deposition (ALD) amorphous layers were developed to provide a novel model of metal–insulator–semiconductor (MIS) photocatalysts for hydrogen generation in the ultraviolet to near-infrared region. Photoexcitation of optimized MIS nanostructures consisting of a metal cocatalyst (Pt), electron tunneling layer (ALD TiO₂), and photoactive nonstoichiometric core (Ti³⁺-doped TNC) exhibited efficient hydrogen generation (52 μmol h^–1·g^–1), good reusability (16 h), and long-term stability (>7 d). The charge-transfer dynamics were examined using transient absorption spectroscopy to clarify the relationship between the photocatalytic activity and the tunneling effect. Our strategies highlight defect engineering in fabricating MIS photocatalysts with improved charge separation and tailored solar energy conversion properties.