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New insights and reaction mechanisms on ZrO2 (110) surface enhanced catalytic hydrolysis of CFC-12: a density functional theory study

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Abstract

Context

Freon, a greenhouse gas that contributes to the depletion of the ozone layer, has been the subject of investigation in this study. The catalytic hydrolysis enhancement of CFC-12 by ZrO2 was examined using a density functional theory approach. A detailed reaction mechanism and a new reaction pathway were proposed. The study found that CFC-12 is more likely to be adsorbed on the ZrO2 surface in the CFC-12-TO(F) configuration, while H2O is more likely to be adsorbed on the ZrO2 surface in the H2O-TO(H) configuration. Additionally, H2O replaces CFC-12 on the surface of ZrO2. The hydrolysis of CFC-12 is primarily determined by the first dechlorination process, while the defluorination process is comparatively easier. ZrO2 has a catalytic effect on both dechlorination and defluorination processes, with a more pronounced effect on the former. The production of C–OH bonds is inhibited, which facilitates the dechlorination and defluoridation processes.

Methods

This work was carried out in the Dmol3 program in the Material Studio 2017, including the geometric structure optimization and energy calculations. The GGA/PBE method was used in this work, along with the DNP basis, spin-polarized set, and DFT-D correction. The possible TSs were guessed based on the linear synchronous transit/quadratic synchronous transit/conjugate gradient (LST/QST/CG) method, and they were further confirmed and reoptimized to ensure that the only one imaginary frequency exists in the TSs.

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Data availability

No datasets were generated or analysed during the current study.

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Funding

This work was supported by the National Natural Science Foundation of China [22006058].

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Authors and Affiliations

  1. Department of Building Engineering, Zibo Vocational Institute, Zibo, 255300, China

    Dalong Zheng

  2. Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, 650500, China

    **n Song

  3. **xiang Huaxing Environmental Protection Engineering Technology Co., Ltd, **xiang, 337022, China

    **n Song

Authors
  1. Dalong Zheng
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  2. **n Song
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Contributions

**n Song contributed to the study conception and design. Calculation, data collection and analysis were performed by **n Song and Dalong Zheng. Dalong Zheng wrote the main manuscript text. All authors read and approved the final manuscript.

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Correspondence to **n Song.

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Zheng, D., Song, X. New insights and reaction mechanisms on ZrO2 (110) surface enhanced catalytic hydrolysis of CFC-12: a density functional theory study. J Mol Model 30, 204 (2024). https://doi.org/10.1007/s00894-024-06008-w

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