Photoinduced Desorption of Sulfur from Nobel Metal Nanoparticles Loaded on Semiconductors

半导体上负载的诺贝尔金属纳米颗粒中硫的光诱导解吸

• 批准号: 16550169
• 负责人: TADA Hiroaki
• 金额: $ 2.05万
• 依托单位: Kinki University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (C)
• 财政年份: 2004
• 资助国家: 日本
• 起止时间: 2004 至 2005
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-16550169/
• 关键词: Semiconductor; Gold; Nanoparticle; Sulfur; Catalyst; 金ナノ粒子; 白金ナノ粒子; 硫黄被毒; 光クリーニング; 光触媒; 酸化チタン; 金ナノ微粒子; 白金ナノ微粒子

Kinetic analysis of the photoinduced desorption of sulfur from gold nanoparticles loaded on TiO_2 particles in water has revealed a rate constant increase with increasing pH. Our photoelectrochemical measurements and density functional theoretical (DFT) calculations have led us to the conclusion that this reaction results from an upward shift in the Fermi energy of gold nanoparticles with irradiation. Anatase-type TiO_2 films were formed on SiO_2 film-coated glass substrates by a sol-gel method. Nanometer-sized gold particles were highly dispersed on the surfaces of the TiO_2 film (Au/TiO_2-TF) and TiO_2 particles (Au/TiO_2-P) using a deposition-precipitation method. X-ray photoelectron spectra of Au/TiO_2-TF adsorbed with sulfur from S_8 molecules indicated that the sulfurs are selectively adsorbed on the Au surfaces with the two kinds of chemisorption modes, atomic and molecular adsorption (S-Au/TiO_2-TF). Light-irradiation (λ_<ex> > 300 nm) to S-Au/TiO_2-TF and S-Au/TiO_2-P in water at 298 K gave rise to desorption of the sulfur with the Au particle size almost maintained. Kinetic analysis showed that the rate constant for the sulfur desorption from S-Au/TiO_2-TF in an opened reaction system is larger than that from S-Au/TiO_2-P in a closed reaction system by a factor of ca. 3.6.

水中载金纳米颗粒光诱导脱附硫的动力学分析表明，随着pH值的升高，速率常数增大。我们的光电化学测量和密度泛函理论(DFT)计算得出的结论是，该反应是由于金纳米粒子的费米能随辐照而向上移动的结果。采用溶胶-凝胶法在镀膜玻璃衬底上制备了锐钛矿型二氧化钛薄膜。采用沉积-沉淀法将纳米金粒子高度分散在二氧化钛薄膜(Au/TiO2Tf)和二氧化钛颗粒(Au/TiO2P)表面。X-射线光电子能谱表明，硫以原子吸附和分子吸附(S-Au/TiO2Tf)两种化学吸附方式选择性地吸附在Au表面。298K时，S-Au/TiO_2-Tf和S-Au/TiO_2-P经λ_&lt；ex&gt；&gt；300 nm光照射后，硫被解吸，而金的粒径基本保持不变。动力学分析表明，在开放式反应体系中，S-Au/TiO_2-Tf体系的硫脱附速率常数比闭合反应体系中S-Au/TiO_2-P体系的速率常数大3.6倍。

项目成果

Photo-induced Dissolution and Redeposition of the Au Nanoparticles Supported on TiO_2

TiO_2负载Au纳米粒子的光诱导溶解和再沉积

• 发表时间: 2005
• 期刊: J. Colloid Interface Sci. 286
• 作者: T.Kawahara;T.Soejima;T.Mitsui;K.Kiyonaga;H.Tada;S.Ito
• 通讯作者: S.Ito

Kinetic and DFT Studies on the Photoinduced Desorption of Sulfur from Gold Nanoparticles Loaded on Titanium Dioxide

二氧化钛负载金纳米粒子光诱导硫脱附的动力学和密度泛函研究

• 发表时间: 2005
• 期刊: ChemPhysChem 6
• 作者: T.Kiyonaga;T.Mitsui;T.Soejima;S.Ito;H.Tada;T.Kawahara;T.Akita;K.Tanaka;H.Kobayashi
• 通讯作者: H.Kobayashi

Kinetic and DFT Studies on the Photoinduced Desorption of Sulfur from Gold Nanoparticles Loaded on Titanium Dioxide,

二氧化钛负载金纳米颗粒光诱导硫脱附的动力学和 DFT 研究，

• 发表时间: 2005
• 期刊: ChemPhysChem 6
• 作者: Tomokazu Kiyonaga;Tomohiro Mitsui;Tetsuro Soejima;Seishiro Ito;Hiroaki Tada;Tetsuro Kawahara;Tomoki Akita;Koji Tanaka;Hisayoshi Kobayashi
• 通讯作者: Hisayoshi Kobayashi

Low-Temperature Photocleaning of Sulfur-Poisoned Au Nanoparticles on Titanium Dioxide Film

• DOI: 10.1149/1.2164549
• 发表时间: 2006-03
• 期刊: Electrochemical and Solid State Letters
• 作者: T. Kiyonaga;T. Kawahara;H. Tada

Photoinduced Desorption of Sulfur from Gold Nanaoparticles Loaded on Metal Oxide Surfaces

金属氧化物表面负载的金纳米粒子光诱导硫脱附

• 发表时间: 2004
• 期刊: J Am. Chem. Soc. 126
• 作者: H.Tada;T.Soejima;S.Ito;H.Kobayashi
• 通讯作者: H.Kobayashi