孔环境对扩张Fe2的催化环氧化的影响
Dianne J Xiao, Julia Oktawiec, Phillip J Milner
1Materials Sciences Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
Journal of the American Chemical Society
|October 6, 2016
概括
研究人员修改了基于铁的金属有机框架以改善环素氧化. 增加毛孔疏水性提高了产品选择性和催化剂稳定性,证明了催化剂设计的新方法.
科学领域:
- 材料科学
- 催化剂
- 超分子化学
背景情况:
- 金属有机框架 (MOF) 可以精确地控制催化剂周围的化学环境.
- 不同质的催化对于工业化学转化至关重要.
研究的目的:
- 研究铁基MOF中的疏水孔环境在循环氧化过程中对产品选择性和催化剂稳定性的影响.
- 通过系统地修改孔径大小和疏水性来探索MOF中的结构属性关系.
主要方法:
- 合成具有不同孔径和疏水功能的铁基MOF类似物.
- 使用环素氧化作为模型反应的催化性能评估.
- 使用Mössbauer光谱,动态同位素效应研究和气体吸附测量进行了表征.
主要成果:
- 一系列基于铁的MOF,包括双和三衍生物,被合成和测试.
- 经过修改的MOF,酒精:基比增加了3倍,周转率增加了10倍.
- 疏水功能组和较大的孔径显著提高了产品的选择性和催化剂性能.
结论:
- 在环素氧化过程中,MOF孔环境的疏水性直接影响产品的选择性和催化剂的稳定性.
- 调整MOF孔径和结合非极性功能组是提高催化效率的有效策略.
- 环素的吸附度与A:K选择性相关,突出了范德瓦尔斯相互作用的作用.
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