在模型 Al2O3 和 TiO2 支持的金纳米粒子上进行水气转移催化作用的尺寸和支效应
Mayank Shekhar1, Jun Wang, Wen-Sheng Lee
1School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States.
Journal of the American Chemical Society
|February 10, 2012
概括
黄金纳米粒子大小显著影响水气转移反应速率和动力学. 低协调的黄金矿床被确定为最活跃的,支持互动对水激活至关重要.
科学领域:
- 不同质的催化剂.
- 纳米粒子科学是一个科学领域.
- 表面化学 表面化学
背景情况:
- 水气转移 (WGS) 反应对于的生产和一氧化碳的去除至关重要.
- 在金属氧化物上支的黄金 (Au) 催化剂对WGS反应具有活性,但粒子大小和支的作用尚未完全理解.
- 了解催化剂结构,活性和反应机制之间的关系对于设计高效的WGS催化剂至关重要.
研究的目的:
- 研究金 (Au) 颗粒大小对水气转移 (WGS) 反应对Au/Al(2) O(3) 和Au/TiO(2) 催化剂的活性和动力学的影响.
- 确定活跃点的性质并阐明反应机制,包括支持的作用.
- 为了将催化性能与催化剂结构和表面特性相关联.
主要方法:
- 合成和表征Au/Al(2) O(3) 和Au/TiO(2) 催化剂,控制Au颗粒大小.
- 传输电子显微镜 (TEM) 用于精确确定Au粒子的大小分布和形状.
- 扩散反射红外光谱学 (DRIFTS) 和操作的里埃变换红外光谱学 (FTIR) 用于研究吸附的CO和活性站点的性质.
- 动力学研究以确定明显的反应顺序和激活能量.
主要成果:
- WGS反应速度因Au颗粒大小而有所变化,如Au/Al(2) O ((3) 的d(-2.2) 和Au/TiO ((2) 的d(-2.7).
- 低协调的角落Au站点被确定为主导的活跃站点,比周边站点活跃得多.
- 与Au/TiO2催化剂相比,Au/Al2O3催化剂表现出较高的表面H2O序列和较低的激活能量,这表明反应机制不同.
- 经营FTIR证实了活跃的Au网站的金属性质.
结论:
- 在WGS反应中,Au/Al2O3和Au/TiO2的催化性能强烈依赖于Au粒子的大小和支物的性质.
- 低协调的AU网站是主要的活跃中心,他们的活动受到支持材料的影响.
- 与TiO2相比,Al2O3支直接参与激活H2O分子,导致不同的反应动力学和较低的激活能量.
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