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Tuning the Cerium-Based Metal-Organic Framework Formation by Template Effect and Precursor Selection.
Dimitry Grebenyuk1,2, Maria Shaulskaya1, Artem Shevchenko3,1
1Lomonosov Moscow State University, Moscow 119991, Russia.
ACS Omega
|December 25, 2023
Summary
A novel metal-organic framework, Ce-MOF, was synthesized using a solvothermal method with dimethylamine acting as a templating agent. This Ce-MOF exhibits catalytic activity in CO oxidation after transformation into cerium dioxide (CeO2).
Area of Science:
- Materials Science
- Inorganic Chemistry
- Nanotechnology
Background:
- Metal-organic frameworks (MOFs) offer tunable properties for various applications.
- Cerium-based MOFs are of interest due to cerium's redox properties.
- Controlling MOF synthesis is crucial for achieving desired structures and functionalities.
Purpose of the Study:
- To synthesize and characterize a novel cerium-based metal-organic framework (Ce-MOF).
- To investigate the templating effect of dimethylamine on Ce-MOF formation.
- To explore the thermal stability and transformation of Ce-MOF.
- To evaluate the catalytic activity of MOF-derived cerium dioxide (CeO2) in CO oxidation.
Main Methods:
- Solvothermal synthesis method.
- Powder X-ray diffraction (PXRD) for structural analysis.
- Thermogravimetric analysis (TGA), Differential Thermal Analysis (DTA), and Mass Spectrometry (MS) for thermal decomposition studies.
- Total X-ray scattering with pair distribution function (PDF) analysis for local structure determination.
- CO oxidation reaction to assess catalytic activity.
Main Results:
- A novel 3D bcu-type Ce-MOF, [(CH3)2NH2]2[Ce2(bdc)4(DMF)2]·2H2O, was successfully synthesized.
- Dimethylamine demonstrated a crucial templating role in the reproducible formation of Ce-MOF.
- Ce-MOF exhibits distinct thermal decomposition stages, yielding [Ce2(bdc)3(H2bdc)] and subsequently Ce2(bdc)3.
- Combustion in an oxidative atmosphere at 390 °C produces CeO2.
- MOF-derived CeO2 from Ce-MOF, Ce5, and CeO2@Ce5 showed catalytic activity in CO oxidation.
Conclusions:
- Dimethylamine is essential for the controlled synthesis of the novel Ce-MOF.
- The thermal behavior of Ce-MOF involves the staged removal of guest molecules and framework modification.
- Ce-MOF serves as a precursor for catalytically active CeO2 nanoparticles.
- The study highlights the potential of MOFs as platforms for generating functional nanomaterials for catalysis.
