金纳米颗粒在等离子体共振光催化剂中的作用机理研究

doi:10.7517/j.issn.1674-0475.2015.05.394

影像科学与光化学 ›› 2015, Vol. 33 ›› Issue (5): 394-402.DOI: 10.7517/j.issn.1674-0475.2015.05.394

金纳米颗粒在等离子体共振光催化剂中的作用机理研究

曹寅虎^1,2, 曹溢涛^1,2, 吴骊珠¹, 佟振合¹, 张铁锐¹

1. 中国科学院理化技术研究所, 北京 100190;
2. 中国科学院大学, 北京 100049

收稿日期:2015-03-19 修回日期:2015-03-26 出版日期:2015-09-16 发布日期:2015-09-16
通讯作者: 张铁锐
基金资助:
国家自然科学基金项目(21401206, 51322213, 21301183, 51172245, 91127005, 21401207)、国家重点基础研究发展计划(2014CB239402, 2013CB834505)、中国科学院重点部署项目(KGZD-EW-T05)、北京市自然科学基金项目 (2152033, 2122054, 2154058)、中组部"万人计划"-首批"青年拔尖人才支持计划"和中国科学院"百人计划"资助

Mechanism Study of Au Nanoparticle Functionalized Plasmonic Photocatalyst

CAO Yinhu^1,2, CAO Yitao^1,2, WU Lizhu¹, TONG Zhenhe¹, ZHANG Tierui¹

1. Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China;
2. University of Chinese Academy of Sciences, Beijing 100049, P. R. China

Received:2015-03-19 Revised:2015-03-26 Online:2015-09-16 Published:2015-09-16

摘要/Abstract

摘要：

金纳米颗粒在等离子体共振光催化剂中具有多种不同的作用机理。本文采用溶胶-凝胶法合成了氮/碳共掺杂超薄二氧化钛(D-TiO₂)包覆的SiO₂/Au/D-TiO₂三明治型及SiO₂/D-TiO₂核壳纳米结构材料,对金纳米颗粒在含有可见光响应型半导体的等离子体共振光催化剂光催化分解水制氢反应中的作用机理进行了探索。研究结果表明,在该等离子体共振光催化剂的光催化反应过程中,金纳米颗粒同时体现出肖特基效应和等离子体共振效应作用机理,且作用机理与光生载流子的多少以及金纳米颗粒的负载量有关。负载量较低时,金纳米颗粒的作用机理与光生载流子的多少有关。而在高负载量条件下,金纳米颗粒在可见光照射下主要表现出肖特基效应对光催化活性的影响。

关键词: 金纳米颗粒, 等离子体共振光催化剂, 光催化制氢, 作用机理

Abstract:

Au nanoparticles function in many different ways in plasmonic photocatalysts. Herein, N and C co-doped TiO₂(D-TiO₂) ultrathin layer coated SiO₂/Au/D-TiO₂sandwich core-shell nanostructures and SiO₂/D-TiO₂core-shell nanostructures were designed and synthesized by sol-gel method to reveal the functional mechanism of Au nanoparticles in the photocatalytic water-splitting under visible light irradiation. Our results demonstrated that Au nanoparticles exhibited the coexistence of the Schottky effect and plasmonic effect for gas generation. The distinct mechanisms depended on charge amount generated together with the loading amount of Au nanoparticles. In the condition of a low loading amount of Au nanoparticles, the functional mechanisms showed their relationship with the amount of photogenerated charges. At a high loading level, Au nanoparticles mainly exhibited the Schottky effect under the visible light irradiation.

Key words: Au nanoparticles, plasmonic photocatalysts, photocatalytic H₂evolution, functional mechanism

曹寅虎, 曹溢涛, 吴骊珠, 佟振合, 张铁锐. 金纳米颗粒在等离子体共振光催化剂中的作用机理研究[J]. 影像科学与光化学, 2015, 33(5): 394-402.

CAO Yinhu, CAO Yitao, WU Lizhu, TONG Zhenhe, ZHANG Tierui. Mechanism Study of Au Nanoparticle Functionalized Plasmonic Photocatalyst[J]. Imaging Science and Photochemistry, 2015, 33(5): 394-402.

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金纳米颗粒在等离子体共振光催化剂中的作用机理研究

Mechanism Study of Au Nanoparticle Functionalized Plasmonic Photocatalyst

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