在UiO-66的支持下,乙烯在-硫复合体上进行化
Maryam Mansoori Kermani1,2, Matthew Neurock1,3,2, Donald G Truhlar1,2
1Department of Chemistry, Chemical Theory Center, and Minnesota Supercomputing Institute, University of Minnesota, 55455-0431, USA. truhlar@umn.edu.
这项研究探讨了用于乙烯化的一种金属有机框架上的-硫催化剂. 单硫联体复合体显示了更有利的转移热力学,推进了具有成本效益的催化剂设计.
科学领域:
- 催化剂是一种催化剂.
- 材料科学 材料科学 材料科学
- 计算化学计算化学
背景情况:
- 支持的单站点催化剂对于具有成本效益的选择性化至关重要.
- 金属硫化物复合物为设计定制的催化性能提供了潜力.
研究的目的:
- 研究涉及金属硫化物在金属有机框架 (MOFs) 上的催化循环的热力学.
- 作为一个模型反应,检查UIO-66上的-硫复合物以乙烯化.
主要方法:
- 使用密度函数理论 (DFT) 的计算.
- 对乙烯化催化路径进行了热力学分析.
- 研究了UiO-66上具有一个或两个硫连接体的-硫复合体.
主要成果:
- 含有两个以上硫联结体的复合物对乙烯吸附不利.
- 化物第一和质子第一机制都涉及两种状态的反应性.
- 具有较低氧化状态的MoS单硫联体复合物为第一个转移产生了更有利的中间体.
结论:
- 在MOF上的单位硫催化剂显示出选择性化的前景.
- 催化剂的设计可以通过控制硫配体和氧化状态的数量来优化.
- DFT计算提供了对催化过程的详细机械洞察.
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