对于尺寸控制的纳米颗粒,在固体/液体和固体/气体接口的催化性异醇氧化过程中,其动力学和机制显著不同
Hailiang Wang1, Andras Sapi, Christopher M Thompson
1Department of Chemistry, University of California , Berkeley, California 94720, United States.
Journal of the American Chemical Society
|July 4, 2014
概括
纳米颗粒催化剂在液体和气体阶段显示出异醇氧化活性增加,其颗粒大小在液体和气体阶段更大. 在这两个阶段之间,反应机制显著不同.
科学领域:
- 不同质的催化剂.
- 纳米材料科学 纳米材料科学
- 表面化学 表面化学
背景情况:
- 纳米粒子 (Pt NPs) 是重要的催化剂.
- 了解尺寸依赖的催化活性是关键.
- 异醇氧化是研究催化机制的一个模型反应.
研究的目的:
- 为了研究纳米颗粒大小对异醇氧化的影响.
- 为了比较液体和气体相中的催化性能.
- 用动力学和光谱学方法阐明反应机制.
主要方法:
- 控制尺寸 (2-8 nm) 的纳米颗粒的合成.
- 在60°C的液体和气体阶段对异醇氧化反应的研究.
- 总频率生成振动光谱 (SFG-VS) 和计算计算.
主要成果:
- 在两个阶段,随着Pt NP大小的增加,催化活性也会增加.
- 气相反应的速度是液相反应的100倍.
- 气相激活能量随着NP大小而减少;液相对大小不敏感.
- 水促进了液相反应,但抑制了气相反应.
结论:
- 液体和气体相存在不同的反应机制.
- 机制与不同的吸附异醇方向相关.
- Pt NP的大小和阶段显著影响异醇氧化效率和机制.
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