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Published on: April 30, 2023
1,2-Dichloroethane Deep Oxidation over Bifunctional Ru/Ce Al Catalysts
Yufeng Gu1, Xingxing Jiang1, Wei Sun1
1Lab for Advanced Materials, Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, PR China.
Ruthenium on ceria-alumina catalysts efficiently oxidize 1,2-dichloroethane (1,2-DCE) with high CO2 selectivity. These catalysts exhibit enhanced reducibility and acidity, crucial for effective 1,2-DCE combustion and stability.
Area of Science:
- Materials Science
- Catalysis
- Environmental Chemistry
Background:
- 1,2-dichloroethane (1,2-DCE) is a persistent environmental pollutant requiring effective degradation methods.
- Ceria-alumina (Ce-Al) supports offer tunable properties for catalytic applications.
- Ruthenium (Ru) is a noble metal catalyst with potential for oxidation reactions.
Purpose of the Study:
- To synthesize and characterize Ru/Ce-Al catalysts for 1,2-DCE oxidation.
- To investigate the influence of ceria content on catalyst properties and activity.
- To elucidate the reaction mechanism and assess catalyst stability.
Main Methods:
- Catalyst synthesis via impregnation of RuCl3 onto Ce-Al supports.
- Characterization using X-ray diffraction (XRD), Raman spectroscopy, temperature-programmed desorption (TPD) of NH3 and CO2, X-ray photoelectron spectroscopy (XPS), and H2-temperature-programmed reduction (H2-TPR).
- Evaluation of catalytic activity and selectivity for 1,2-DCE oxidation, including in situ Fourier transform infrared spectroscopy (FTIR).
Main Results:
- CeO2 exhibited a face-centered cubic fluorite structure, with Ru species' state and structure dependent on Ce content.
- Catalyst reducibility and acidity increased with the Ce/Ce+Al ratio, peaking at a Ce/Ce+Al range of 0-0.25.
- Ru/Ce-Al catalysts showed high activity for 1,2-DCE combustion, with turnover frequency (TOF) correlating with strong acidity and reducibility. Ru addition significantly reduced chlorination byproducts.
- Ru/Ce10Al90 demonstrated excellent stability at 280 °C for over 25 hours, achieving >99% CO2 selectivity.
- In situ FTIR revealed a ClCH2-CH2O- intermediate species, leading to CH3CHO and CH2=CHCl, with CH3CHO facilitating deep oxidation.
Conclusions:
- Ru/Ce-Al catalysts are effective for 1,2-DCE oxidation, with synergistic effects between Ru reducibility and support acidity.
- Optimized ceria content enhances catalytic performance and stability, minimizing undesirable chlorination.
- The study provides insights into the reaction pathway, highlighting the role of specific intermediates in the deep oxidation of 1,2-DCE.
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