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[NH2-MIL-53(Fe)] Fe-Based MOFs for Photocatalytic CO2 Reduction
Summary:
The authors from the Research Institute of Photocatalysis, Fuzhou University, China, developed a series of Fe-based metal-organic frameworks (MOFs) with coordination unsaturated sites, achieving significant results in photocatalytic CO2 reduction under visible light.
Background:
1. To address the problem of global warming and energy shortage, previous researchers developed various photocatalysts for CO2 reduction, achieving success with inorganic semiconductors and noble-metal complexes. However, these materials either lack visible light activity or rely on expensive metals, limiting their practical application.
2. The authors proposed using earth-abundant Fe-based MOFs with coordination unsaturated sites and dual excitation pathways, obtaining enhanced photocatalytic performance for CO2 reduction.
Research Content:
1. Synthesis:
The authors synthesized MIL-101(Fe), MIL-53(Fe), and MIL-88B(Fe) using hydrothermal methods. Their amino-functionalized derivatives (NH2-MIL-101(Fe), NH2-MIL-53(Fe), and NH2-MIL-88B(Fe)) were prepared by replacing the linker with 2-aminoterephthalic acid.
2. Characterizations:
1) BET surface area measurements showed high porosity for all MOFs.
2) SEM/TEM tests revealed particle sizes ranging from nanometers to micrometers.
3) UV-vis spectra indicated strong absorption in the visible light region, while XRD patterns confirmed the crystalline structures.
3. Application:
The Fe-based MOFs were tested for photocatalytic CO2 reduction under visible light. MIL-101(Fe) showed the highest activity, producing 59 μmol of formate in 8 hours. Amino-functionalized MOFs exhibited enhanced performance, with NH2-MIL-101(Fe) achieving a 3-fold increase in formate production.
4. Mechanism:
The direct excitation of Fe−O clusters and subsequent electron transfer from O2− to Fe3+ were identified as the primary mechanism. Amino-functionalized MOFs exhibited dual excitation pathways, enhancing photocatalytic performance through synergistic effects.
Outlook:
This research provides a novel approach to designing visible-light-responsive photocatalysts using earth-abundant metals, significantly contributing to sustainable CO2 reduction and energy conversion.
Fe-Based MOFs for Photocatalytic CO2 Reduction: Role of Coordination Unsaturated Sites and Dual Excitation Pathways
Authors: Dengke Wang, Renkun Huang, Wenjun Liu, Dengrong Sun, Zhaohui Li
DOI: 10.1021/cs501169t
Link: https://pubs.acs.org/doi/10.1021/cs501169t
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