选择性化多不和脂肪酸甲基在双功能基修饰Pd/MIL-101(Cr) 催化剂上的选择性化
Phuwadon Khenkhom1,2, Chonlada Ritvirulh1, Kittisak Choojun1,2
1Department of Chemistry, School of Science, King Mongkut's Institute of Technology Ladkrabang, Chalongkrung Road, Ladkrabang, Bangkok 10520, Thailand.
这项研究在MIL-101 (Cr) 框架内引入了纳米颗粒 (PdNP) 的双功能连接体,增强了脂肪酸甲基 (FAME) 的选择性化. 量身定制的配体提高了催化剂的稳定性和可重复使用性,为单不和FAME产生了高选择性.
科学领域:
- 材料科学和纳米技术
- 催化剂是一种催化剂.
- 绿色化学 绿色化学
背景情况:
- 像MIL-101 (Cr) 这样的金属有机框架 (MOF) 提供可调节的多孔结构来支持催化剂.
- 纳米粒子 (Pd NPs) 是化反应的关键催化剂.
- 用特定的连接体功能化MOF可以控制纳米粒子分散和催化活性.
研究的目的:
- 为了合成和描述MIL-101 (((Cr) 框架的功能,与各种双功能的配体用于Pd NP的整合.
- 为了研究不同连接体功能对Pd特异,分散和FAME化中的催化性能的影响.
- 评估开发的催化系统的稳定性,可重复使用性和选择性.
主要方法:
- 将含有氨基和碳酸的配体 (en, DET, AN, ABA, AVA, GA, AA) 移植到MIL-101上.
- 将0.5%重量的纳米颗粒 (PdNP) 纳入功能化框架.
- 使用光谱和结构分析进行表征 (例如,确认带-Cr和带-Pd协调).
- 多不和脂肪酸甲基 (FAMEs) 的液相化,以评估催化活性和选择性.
- 热过和可回收性测试,以确定催化剂的稳定性和泄.
主要成果:
- 证实了对Cr节点和Pd物种的带协调.
- 用ABA,AVA和GA联体功能化的催化剂显示了高度分散的PdNP (<1 nm) 与Pd0的特异化.
- 这些催化剂实现了高周转频率 (高达~15,400小时-1) 和对单不和FAMEs的>94%选择性.
- 相反,En和DET移植材料中强大的Pd-N相互作用阻碍了Pd0的形成和减少活性.
- 在可回收性测试中观察到高催化剂稳定性和可以忽略的Pd出.
结论:
- 在MIL-101 ((Cr) 中的双功能联体架构有效调整了FAME化过程中的Pd特种化和催化活性.
- 像ABA,AVA和GA这样的配体促进最佳的Pd0分散,导致高活性和选择性.
- 开发的催化系统提供了一个强大的,可重复使用的平台,用于选择性化FAME,与绿色化学原则保持一致.
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