通过Al修改,为高效的乙烯回氧化提供支持的银催化剂中的电子金属支相互作用的定制
Hongling Yang1,2, Ganggang Li1, Qinggang Liu3
1National Engineering Laboratory for VOCs Pollution Control Material & Technology, Research Center for Environmental Material and Pollution Control Technology, University of the Chinese Academy of Sciences, Beijing, 101408, China.
Angewandte Chemie (International ed. in English)
|February 23, 2024
概括
在MnO2上对白银催化剂的改性增强了乙烯环氧化. 这种新的方法克服了活动选择性权衡,在温和条件下实现高乙烯转化和乙烯氧化物选择性.
科学领域:
- 不同质的催化剂.
- 材料科学 材料科学 材料科学
- 表面化学 表面化学
背景情况:
- 金属改性催化剂在异质催化中提供了增强的性能.
- 银 (Ag) 对于乙烯环氧化是活跃的,但通常面临着活性和对乙烯氧化物 (EO) 的选择性之间的权衡.
研究的目的:
- 为了克服使用 (Al) 修改Ag催化剂的乙烯环氧化中的活性-选择性权衡.
- 在温和条件下实现高乙烯转化和EO选择性.
主要方法:
- 在Al-修改的Ag和MnO2支之间利用强大的电子金属支相互作用 (EMSI).
- 使用结构特征和理论计算.
- 研究Ag的电子结构和反应物的吸附性质.
主要成果:
- 通过EMSI,Al修改量身定制了Ag的空置3d状态,将乙烯转化提高到~100%.
- 在温和条件下 (170°C,大气压) 达到90%的乙烯氧化物 (EO) 选择性.
- 乙烯和氧气的调节吸附,促进了EO脱附,并降低了EO形成的能量屏障.
结论:
- 强大的电子金属支相互作用对于设计高性能催化剂至关重要.
- 对Ag/MnO2的Al修饰为高效和选择性的乙烯环氧化提供了一个有希望的途径.
- 这一战略为开发用于选择性氧化反应的先进金属催化剂提供了新的途径.
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