通过模板效应和前体选择调整基金属有机框架形成
Dimitry Grebenyuk1,2, Maria Shaulskaya1, Artem Shevchenko3,1
1Lomonosov Moscow State University, Moscow 119991, Russia.
ACS omega
|December 25, 2023
概括
一种新的金属有机框架,Ce-MOF,使用溶热方法合成,其中二甲基胺作为模板剂. 这种Ce-MOF在转化为二氧化 (CeO2) 后,在CO氧化过程中表现出催化活性.
科学领域:
- 材料科学 材料科学 材料科学
- 无机化学 无机化学
- 纳米技术纳米技术
背景情况:
- 金属有机框架 (MOF) 为各种应用提供可调节的特性.
- 基于的MOF由于的氧化还原特性引起了人们的兴趣.
- 控制MOF合成对于实现所需的结构和功能至关重要.
研究的目的:
- 合成和描述一种基于的新型金属有机框架 (Ce-MOF).
- 调查二甲基胺对Ce-MOF形成的模板效应.
- 探索Ce-MOF的热稳定性和转变.
- 评估MOF衍生的二氧化 (CeO2) 在CO氧化中的催化活性.
主要方法:
- 溶解热合成方法.
- 粉末X射线衍射 (PXRD) 用于结构分析.
- 热重力测量分析 (TGA),差分热分析 (DTA) 和质谱 (MS) 用于热分解研究.
- 总X射线散射与对分布函数 (PDF) 分析用于局部结构确定.
- CO氧化反应以评估催化活性.
主要成果:
- 一种新的3D bcu-type Ce-MOF, [(CH3) 2NH2]2[Ce2(bdc) 4(DMF) 2·2H2O,已成功合成.
- 甲基胺在Ce-MOF的可再生形成中发挥了关键的模板作用.
- Ce-MOF表现出不同的热分解阶段,产生[Ce2(bdc) 3(H2bdc) ],随后是Ce2(bdc) 3.
- 在390°C的氧化大气中燃烧产生CeO2.2.
- 来自Ce-MOF,Ce5和CeO2@Ce5的MOF衍生的CeO2在CO氧化过程中表现出催化活性.
结论:
- 甲基胺对于新型Ce-MOF的受控合成至关重要.
- Ce-MOF的热行为包括分阶段去除客分子和框架修改.
- Ce-MOF是催化活性CeO2纳米颗粒的前体.
- 该研究强调了MOF作为生成用于催化功能的功能纳米材料的平台的潜力.
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