Issue 3, 2022

Identification of the active site during CF4 hydrolytic decomposition over γ-Al2O3

Abstract

Aluminum production processes emit carbon tetrafluoride (CF4) directly into the atmosphere, which is a powerful greenhouse gas (with a greenhouse warming potential 6500 times that of CO2) with serious potential to exacerbate global warming. As the most feasible method of eliminating CF4, the hydrolytic decomposition of CF4 at moderate temperatures is still challenging due to the active site remaining elusive. Herein, we demonstrated that three-coordinated Al (AlIII) on the γ-Al2O3 (110) surface is the dominant active site during the hydrolytic decomposition of CF4. DFT calculations present the strong adsorption of CF4 on the AlIII site. γ-Al2O3 nano-slices with exposed (110) crystal planes with different AlIII occupation levels were synthesized. The amounts of AlIII in the catalysts were quantified via27Al MAS NMR and the number of AlIII sites directly affects the catalytic activity. In situ FTIR spectra show that the AlIII sites could be activated and that they had a stable presence under the given reaction conditions.

Graphical abstract: Identification of the active site during CF4 hydrolytic decomposition over γ-Al2O3

Supplementary files

Article information

Article type
Paper
Submitted
28 déc. 2021
Accepted
29 janv. 2022
First published
31 janv. 2022

Environ. Sci.: Nano, 2022,9, 954-963

Identification of the active site during CF4 hydrolytic decomposition over γ-Al2O3

H. Zhang, T. Luo, Y. Long, Y. Chen, J. Fu, H. Liu, J. Hu, Z. Lin, L. Chai and M. Liu, Environ. Sci.: Nano, 2022, 9, 954 DOI: 10.1039/D1EN01202A

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