建模的单原子位Pt催化剂,具有对水化反应的定义良好的协调结构
Mengge Lu1, Xuxin Kang2, Changjin Qian3
1State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing, 100029, China.
合成了一种具有定义结构的新单原子位点 (SAS) 催化剂. 这种高度选择性的催化剂通过反马尔科夫尼科夫的水化有效地转化基,为机械学研究提供了一个模型.
科学领域:
- 不同质的催化剂.
- 一个原子位点 (SAS) 催化剂
- 有机金属化学 有机金属化学
背景情况:
- 单原子位 (SAS) 催化剂具有高活性,非常适合机理学研究.
- 通过热解合成的SAS催化剂的协调环境和分布的控制是具有挑战性的.
- 开发具有明确协调结构的模型催化剂至关重要,但很困难.
研究的目的:
- 合成具有精确定义的协调结构的单原子位点 (SAS) 催化剂.
- 为了利用这种模型催化剂对抗马尔科夫尼科夫的烯水化机制的研究.
- 为了建立SAS催化剂的结构-活动关系.
主要方法:
- 对于SAS催化剂合成的现场减少组装策略.
- 单晶X射线衍射和X射线吸收光谱学用于结构确认.
- 密度函数理论 (DFT) 计算来研究反应机制.
主要成果:
- 一个Pt1C48H61P2Cl SAS催化剂与一个确认的Pt-P2C1Cl1协调结构被合成.
- 催化剂在1小时内在无溶剂条件下实现了98%的转化和99%以上的选择性,在抗马尔科夫尼科夫基因水化中.
- 与Pt (111) 相比,DFT的计算显示,SAS催化剂上的水化能障碍较小.
结论:
- 合成的Pt-SAS催化剂作为研究SAS催化剂的有效模型.
- 精确定义的协调环境增强了催化活动和选择性.
- 催化剂的性能归因于氧化添加阶段的较弱相互作用,促进产品脱离.
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