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Metal Variance in Multivariate Metal-Organic Frameworks for Boosting Catalytic Conversion of CO2
Xu Chen1, Jing-Yi Song1, Ji Zheng1
1College of Chemistry and Materials Science, and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou 510632, China.
Journal of the American Chemical Society
|July 1, 2024
Summary
Developing efficient metal-organic framework (MOF) catalysts for carbon dioxide (CO2) conversion is crucial. This study introduces novel multivariate MOFs (MTV-MOFs) with tunable Ag/Cu ratios, showing significantly enhanced catalytic activity for CO2 utilization.
Area of Science:
- Materials Science
- Catalysis
- Green Chemistry
Background:
- Developing efficient, low-cost catalysts for carbon dioxide (CO2) conversion under mild conditions is a significant challenge.
- Metal-organic frameworks (MOFs) offer tunable structures for catalytic applications.
- Heterogeneous catalysis for CO2 utilization is key to sustainable chemical processes.
Purpose of the Study:
- To design and synthesize novel two-dimensional (2D) multivariate metal-organic frameworks (MTV-MOFs) for efficient CO2 conversion.
- To investigate the effect of silver (Ag) and copper (Cu) ratios within the MOF structure on catalytic performance.
- To explore the potential of these MTV-MOFs as reusable heterogeneous catalysts for the cyclization of propargylamine with CO2.
Main Methods:
- Synthesis of isostructural 2D MTV-MOFs incorporating copper- and/or silver-based cyclic trinuclear complexes (Cu-CTC and Ag-CTC).
- Catalytic testing of MTV-MOFs for the cyclization of propargylamine with CO2 under varying Ag/Cu ratios.
- Evaluation of catalytic activity using turnover frequency (TOF) and testing with simulated flue gas.
- Mechanistic studies employing Nuclear Magnetic Resonance (NMR) monitoring and Density Functional Theory (DFT) calculations.
Main Results:
- The synthesized MTV-MOFs demonstrated efficient and reusable heterogeneous catalytic activity for CO2 conversion.
- Fine-tuning the Ag/Cu ratio in the MTV-MOFs significantly impacted catalytic performance.
- A bimetallic MOF with 10% Ag exhibited a 20-fold increase in catalytic efficiency (TOF = 243 h-1) compared to the 100% Cu-based MOF (TOF = 10.8 h-1).
- The bimetallic MOF maintained high catalytic activity even with a low CO2 concentration (10%) representative of simulated flue gas.
Conclusions:
- MTV-MOFs with tunable Ag/Cu ratios are highly effective heterogeneous catalysts for CO2 conversion.
- The strategic incorporation of silver enhances the catalytic performance of copper-based MOFs for CO2 cyclization.
- These findings present a promising pathway for developing advanced catalysts for CO2 utilization, even from low-concentration sources like flue gas.
