Modulation of crystal growth and structure within cerium-based metal–organic frameworks,CrystEngComm

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Modulation of crystal growth and structure within cerium-based metal–organic frameworks
CrystEngComm ( IF 2.6 ) Pub Date : 2020-11-25 , DOI: 10.1039/d0ce01223h
Megan C. Wasson _{1,

2,

3,

4} , Ken-ichi Otake _{1,

2,

3,

4} , Xinyi Gong _{1,

2,

3,

4} , Annabella R. Strathman _{1,

2,

3,

4} , Timur Islamoglu _{1,

2,

3,

4} , Nathan C. Gianneschi _{1,

2,

3,

4} , Omar K. Farha _{1,

2,

3,

4}

Affiliation

The intriguing catalytic properties of cerium-based materials have motivated the development of Ce-based metal–organic frameworks (MOFs). However, the controlled crystallization of Ce MOFs remains nascent due to complications with the high reduction potential of Ce⁴⁺ species. Modulators offer a route in other well-studied coordination networks to slow down crystallization processes to allow for corrective, uniform crystal growth. Herein, we report an investigation of modulator identity and concentration on the synthesis of a Ce-UiO-type MOF with 2,6-naphthalenedicarboxylic acid (NDC) as a linker. At low concentrations using both benzoic acid and trifluoroacetic acid, we observed a mononuclear Ce³⁺ MOF (NU-350) through single-crystal X-ray diffraction studies. Higher modulator concentrations yielded pure-phase Ce-UiO-NDC, with uniform particle sizes observed with utilizing benzoic acid as a modulator. Moreover, we demonstrated the transferability of this synthesis through the pure-phase synthesis of Ce-UiO-66 with benzoic acid as a modulator. High-resolution transmission electron microscopy showed a single crystalline domain within Ce-UiO-NDC.

中文翻译：

铈基金属有机框架内晶体生长和结构的调控

铈基材料令人着迷的催化性能推动了铈基金属有机骨架（MOF）的发展。然而，由于具有Ce ⁴⁺物种的高还原潜力的并发症，Ce MOF的受控结晶仍处于新生阶段。调节剂在其他经过充分研究的配位网络中提供了一条途径，可以减慢结晶过程，从而实现校正性均匀晶体的生长。在本文中，我们报告了在以2，6-萘二甲酸（NDC）为连接基的Ce-UiO型MOF合成中对调节剂同一性和浓度的研究。在使用苯甲酸和三氟乙酸的低浓度条件下，我们观察到单核Ce ³⁺MOF（NU-350）通过单晶X射线衍射研究。较高的调节剂浓度可生成纯相Ce-UiO-NDC，使用苯甲酸作为调节剂可观察到均匀的粒径。而且，我们证明了通过以苯甲酸为调节剂的Ce-UiO-66的纯相合成，该合成的可转移性。高分辨率透射电子显微镜显示Ce-UiO-NDC中有一个单晶域。

更新日期：2020-11-25

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