用氧化物支持的单原子催化剂的合理设计:在Ceria上原子分散黄金
Jin-Cheng Liu1, Yang-Gang Wang1, Jun Li1
1Department of Chemistry and Key Laboratory of Organic Optoelectronics & Molecular Engineering of Ministry of Education, Tsinghua University , Beijing 100084, China.
Journal of the American Chemical Society
|April 14, 2017
概括
这项研究揭示了氧化物支上的单原子催化剂 (SAC) 如何设计为稳定性和反应性. 这项研究强调了单个原子在黄金纳米催化中的关键作用.
科学领域:
- 材料科学
- 物理化学
- 催化剂
背景情况:
- 单原子催化剂 (SAC) 提供高原子效率,但它们的稳定性和反应性是复杂的.
- 对于催化剂设计来说,了解单个原子 (SA) 和金属纳米粒子 (NP) 之间的相互作用至关重要.
研究的目的:
- 开发化学潜力的一般热力学模型,以指导SAC的合理设计.
- 在氧化物支上研究金属SAC的动态,反应和运动方面,使用黄金在Ceria作为模型系统.
主要方法:
- 一开始的电子结构计算
- 分子动力学模拟
- 动力蒙特卡洛分析
- 化学潜力的热力学建模
主要成果:
- 级位上的单个金原子 (SAs) 在高达700K时是稳定的,并且对CO氧化具有高度反应性.
- 环境因素 (温度,压力,颗粒大小,支可减少性) 显著影响SAC的稳定性和反应性.
- 在小型AuNP的接口上动态创建AuSA解释了黄金催化中的尺寸效应.
结论:
- 开发的模型为设计稳定和反应性SAC提供了一个框架.
- 单原子金种在金纳米催化中起着关键的,往往未被认可的作用.
- 这项工作提供了在氧化物支上设计金属SAC的一般方法.
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