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Tuning Stability of Ce/Zr-MOFs (UiO-66, MOF-808)
Summary:
The authors from Christian-Albrechts-Universität zu Kiel developed a series of bimetallic Ce/Zr-MOFs (UiO-66 and MOF-808 structures) with tunable Ce⁴⁺/Zr⁴⁺ ratios, achieving enhanced thermal and chemical stability while maintaining redox activity for potential catalytic applications.
Background:
1. To address the poor stability of Ce-based MOFs and the redox inertness of Zr-MOFs, previous researchers attempted post-synthetic metal substitution or doping, achieving limited success in balancing stability and functionality.
2. The authors proposed a one-pot modulated synthesis strategy to construct solid-solution Ce/Zr-MOFs, achieving synergistic integration of redox-active Ce⁴⁺ and stable Zr⁴⁺ within a single framework.
Research Content:
1. Synthesis:
The authors synthesized Ce/Zr-MOFs via a rapid (15–20 min) modulated solvothermal method using Ce(IV) ammonium nitrate, Zr(IV) salts, and organic linkers (H₂BDC or H₃BTC) in DMF with formic acid as modulator.
2. Characterizations:
1) BET surface areas ranged from 1146–1443 m²/g; micropore volumes ~0.45–0.62 cm³/g.
2) SEM/DLS showed particle sizes from 150–410 nm depending on Ce content.
3) VT-PXRD and TGA confirmed thermal stability up to 350°C for Ce-poor samples; acid resistance (pH = 0) was demonstrated for Ce ≤ 17.9 at%.
3. Application:
While not directly tested in applications, the materials exhibit tunable redox behavior and high stability, suggesting potential in catalysis, sensing, or adsorption.
4. Mechanism:
The linear correlation of lattice parameters with Ce content (Vegard’s law) confirms homogeneous metal distribution. Zr-rich frameworks enhance stability via strong Zr–O bonding, while Ce introduces redox-active sites.
Outlook:
This work demonstrates a scalable route to engineer stable, redox-active MOFs by tuning Ce/Zr ratios, offering a platform for designing functional materials in catalysis and environmental applications.
Tuning the stability of bimetallic Ce(IV)/Zr(IV)-based MOFs with UiO-66 and MOF-808 structures
Authors: M. Lammert, C. Glißmann, N. Stock
DOI: 10.1039/c7dt00259a
Link: https://pubs.rsc.org/en/content/articlelanding/2017/dt/c7dt00259a
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