通过单原子合金催化剂调节不和化物的化选择性
Hio Tong Ngan1, Philippe Sautet1,2,3
1Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, California 90095, United States.
Journal of the American Chemical Society
|January 22, 2024
概括
在铜上的单原子合金催化剂可选择性地将不和化物化为酒精. 铜中的 (Cu) 提供最佳的结合,并防止不必要的副作用,增强催化选择性.
科学领域:
- 催化剂
- 材料科学
- 表面化学
背景情况:
- 选择性化α,β不和化成不和醇是催化的一个关键挑战.
- 控制CO和CC键化之间的选择性对于高效合成至关重要.
研究的目的:
- 在铜上探索单原子合金 (SAA) 催化剂,用于选择性CO化不和化物.
- 了解Cu中的不同过渡金属如何影响吸附和化途径.
主要方法:
- 使用第一原理模拟来研究各种过渡金属的电子和吸附性质.
- 使用动力模拟来评估醇形成的选择性.
主要成果:
- 早期的过渡金属 (Ti,Zr,Hf) 在Cu上有利于CO结合,但导致过度化.
- 晚期过渡金属在Cu上有利于CC结合,产生不必要的和化物.
- 由于中度结合和高迁移障碍,中度过渡金属 (Cr,Mn) 在Cu111上表现出最佳的CO选择性.
结论:
- 单原子合金可以调整催化中间体和过渡状态的结合强度.
- 在不和化中,SAA催化剂,特别是Cr in Cu,为控制催化活性和选择性提供了有希望的策略.
- 防止从CO迁移到CC结合模式是实现不和醇高选择性的关键.
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