对UIO-66缺陷的局部结构分析:固态核磁共振和X射线吸收细结构的洞察
Jiabin Xu1,2, Kun Feng2, Wanli Zhang1
1Department of Chemistry, The University of Western Ontario, London, Ontario N6A 5B7, Canada.
Journal of the American Chemical Society
|November 18, 2025
概括
基于的金属有机框架 (MOF) 的缺陷工程增强了催化活性. 在UiO-66中引入缺陷可以提高演化反应中集成纳米颗粒的性能.
科学领域:
- 材料科学
- 催化剂
- 纳米技术
背景情况:
- 金属有机框架 (MOF) 的缺陷工程是调整材料属性的关键策略.
- 基于的MOF,如UiO-66,是各种应用的有希望的材料.
- 可控引入缺陷可以显著改变MOF的功能.
研究的目的:
- 描述UiO-66 MOF中缺陷的原子级局部结构.
- 研究工程缺陷对集成纳米颗粒 (Pt NPs) 催化性能的影响.
- 探索有缺陷的UiO-66作为增强催化剂的支持.
主要方法:
- 使用多核固态NMR光谱 (SSNMR) 和X射线吸收细结构 (XAFS) 进行缺陷表征.
- 在Zr K边缘进行现场加热XAFS分析以监测结构变化.
- 使用各种多核SSNMR技术 (1H, 13C, 19F, 35/37Cl, 17O) 来识别与缺陷相关的物种.
主要成果:
- 在现场XAFS显示了Zr局部结构的变化,包括三酸 (TFA) 移除后Zr- O协调的降低和Zr- Zr距离的改变.
- 在MOF结构中确定了SSNMR的上限和缺陷相关物种.
- 与无缺陷的对应物相比,缺陷工程的Pt-UiO-66具有显著增强的演变反应 (HER) 活性和稳定性.
结论:
- 使用SSNMR和XAFS的组合,可以实现UiO-66缺陷的原子级特征.
- 在UiO-66中的工程缺陷有效地提高了集成PtNP的催化性能.
- 缺陷的UiO-66作为一种先进的催化支持材料,
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