低温氧化乙到氧化物通过氧气通过聚变催化剂
1Beijing National Laboratory for Molecular Engineering, College of Chemistry and Molecular Engineering and College of Engineering, BIC-ESAT , Peking University , Beijing 100871 , P. R. China.
Journal of the American Chemical Society
|October 25, 2019
概括
研究人员在纳米钻石上开发了催化剂,用于选择性乙氧化到酸. 一氧化碳对于在温和条件下保持催化剂活性和选择性至关重要.
科学领域:
- 催化剂
- 材料科学
- 化学工程
背景情况:
- 在温和条件下选择性氧化轻,如乙到有价值的化学物质是一个重要的工业和学术挑战.
- 现有的方法通常需要严格的条件或缺乏足够的选择性,从而限制了它们的实际应用.
- 开发直接功能化的有效催化剂是可持续化学合成的关键.
研究的目的:
- 在纳米钻石上制造和评估氧化乙聚合物和原子分散的催化剂.
- 在温和反应条件下研究催化性能,包括活性和选择性.
- 阐明一氧化碳在增强催化剂稳定性和性能方面的作用.
主要方法:
- 使用纳米钻石作为支材料合成团和原子分散的催化剂.
- 在100°C使用氧气对乙选择性氧化的试验.
- 使用X射线光电子光谱 (XPS) 鉴定催化剂以了解物种的氧化状态.
- 在现场回收实验以评估多个周期的催化剂耐用性和性能.
主要成果:
- 经过五次现场回收,聚合催化剂的初始活性高 (7.5mol/mol/h),对酸的选择性优异 (>70%).
- 在反应料中发现一氧化碳 (CO) 的存在对于实现高性能至关重要.
- XPS分析表明,CO在催化循环期间在维持活性物种的金属状态方面发挥着至关重要的作用,防止失活.
结论:
- 纳米钻石支持的催化剂,特别是集群形式的催化剂,在温和的条件下对乙进行选择性氧化非常有效.
- 一氧化碳对于稳定活性金属物种至关重要,确保持续的高活性和选择性.
- 这项研究提出了一种有前途的催化系统,用于直接利用轻,解决化学合成中的一个关键挑战.
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