单晶Au表面和Au/TiO2(110)模型催化剂表面CO氧化反应机理和活性位

doi:10.1016/S1872-2067(16)62516-0

催化学报 ›› 2016, Vol. 37 ›› Issue (10): 1676-1683.DOI: 10.1016/S1872-2067(16)62516-0

单晶Au表面和Au/TiO₂(110)模型催化剂表面CO氧化反应机理和活性位

Tadahiro Fujitani, Isao Nakamura

日本国立产业技术综合研究所, 筑波305-8565, 日本

收稿日期:2016-04-08 修回日期:2016-07-27 出版日期:2016-10-21 发布日期:2016-10-22
通讯作者: Tadahiro Fujitani

Mechanism and active sites of CO oxidation over single-crystal Au surfaces and a Au/TiO₂(110) model surface

Tadahiro Fujitani, Isao Nakamura

National Institute of Advanced Industrial Science and Technology(AIST), 1-1-1 Higashi, Tsukuba 305-8565, Japan

Received:2016-04-08 Revised:2016-07-27 Online:2016-10-21 Published:2016-10-22
Contact: Tadahiro Fujitani
Supported by:
This work was financially supported by JST-CREST.

摘要/Abstract

摘要：

在分子尺度上介绍了Au/TiO₂（110）模型催化剂表面和单晶Au表面CO氧化反应机理和活性位、以及H₂O的作用.在低温（<320 K），H₂O起着促进CO氧化的作用，CO氧化的活性位位于金纳米颗粒与TiO₂载体界面（Au^δ+-O^δ--Ti）的周边.O₂和H₂O在金纳米颗粒与TiO₂载体界面边缘处反应形成OOH，而形成的OOH使O-O键活化，随后OOH与CO反应生成CO₂.300 K时CO₂的形成速率受限于O₂压力与该反应机理相印证.相反，在高温（>320 K）下，因暴露于CO中而导致催化剂表面重组，在表面形成低配位金原子.低配位的金原子吸附O₂，随后O₂解离，并在金属金表面氧化CO.

关键词: 金, 模型催化剂, 一氧化碳氧化, 反应机理, 活性位

Abstract:

We describe the reaction mechanism and active sites for CO oxidation over a Au/TiO₂(110) model surface and Au single-crystal surfaces, along with the role of H₂O, on a molecular scale. At low temperature (<320 K), H₂O played an essential role in promoting CO oxidation, and the active site for CO oxidation was the perimeter of the interface between the gold nanoparticles and the TiO₂ support (Au^δ+-O^δ--Ti). We believe that the O-O bond was activated by the formation of OOH, which was produced directly from O₂ and H₂O at the perimeter of the interface between the gold nanoparticles and the TiO₂ support, and consequently OOH reacted with CO to form CO₂. This reaction mechanism explains the dependence of the CO₂ formation rate on O₂ pressure at 300 K. In contrast, at high temperature (>320 K), low-coordinated gold atoms built up on the surface as a result of surface reconstruction due to exposure to CO. The low-coordinated gold atoms adsorbed O₂, which then dissociated and oxidized CO on the metallic gold surface.

Key words: Gold, Model catalyst, CO oxidation, Reaction mechanism, Active sites

Tadahiro Fujitani, Isao Nakamura. 单晶Au表面和Au/TiO₂(110)模型催化剂表面CO氧化反应机理和活性位[J]. 催化学报, 2016, 37(10): 1676-1683.

Tadahiro Fujitani, Isao Nakamura. Mechanism and active sites of CO oxidation over single-crystal Au surfaces and a Au/TiO₂(110) model surface[J]. Chinese Journal of Catalysis, 2016, 37(10): 1676-1683.

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单晶Au表面和Au/TiO₂(110)模型催化剂表面CO氧化反应机理和活性位

Mechanism and active sites of CO oxidation over single-crystal Au surfaces and a Au/TiO₂(110) model surface

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