- Title
- Synergistic catalysis of carbon-partitioned LaF3 -BaF2 composites for the coupling of CH4 with CHF3 to VDF
- Creator
- Wang, Jinchao; Han, Wenfeng; Wang, Shucheng; Tang, Haodong; Liu, Wucan; Li, Ying; Lu, Chunshan; Zhang, Jianjun; Kennedy, Eric M.; Li, Xiaonian
- Relation
- Catalysis Science and Technology Vol. 9, Issue 6, p. 1338-1348
- Publisher Link
- http://dx.doi.org/10.1039/c8cy02376j
- Publisher
- Royal Society of Chemistry
- Resource Type
- journal article
- Date
- 2019
- Description
- Catalytic coupling of CH4 with potent greenhouse gas CHF3 to vinylidene fluoride (VDF) was investigated over composite catalysts. Carbon-partitioned LaF3–BaF2 catalysts were prepared by PVDF (polyvinylidene fluoride)-mediated calcination. During catalyst preparation, PVDF functions as the fluorine source and carbon source. Compared with the catalysts prepared by the conventional HF co-precipitation method, the transformation of LaF3 and BaF2 to Ba1−xLaxF2+x solid solution is inhibited as Ba and La are separated by carbon layers derived from the decomposition of PVDF. The Ba1−xLaxF2+x phase is not favorable for the coupling of CH4 with CHF3 to VDF. In addition, PVDF-mediated calcination facilitates the formation of LaOF which is one of the key species for coupling of CH4 with CHF3 to VDF. O− species, which is the most active oxygen species for the activation of CH4, increases significantly following PVDF-mediated calcination due to the formation of LaOF. Consequently, the formation rate of VDF over the catalyst derived from PVDF-mediated calcination is 3.6 times higher than the HF co-precipitation catalyst at a reaction temperature of 700 °C. The formation rate of the HF co-precipitated catalyst declines to nearly half of the initial rate in a time-on-stream of 15 h. By contrast, only slight deactivation is observed over the catalyst prepared by PVDF-mediated calcination. The present work provides a promising strategy for the preparation of composite catalysts.
- Subject
- carbon-partitioned; catalyst preparation; coupling of CH4; CHF3; VDF
- Identifier
- http://hdl.handle.net/1959.13/1467069
- Identifier
- uon:47734
- Identifier
- ISSN:2044-4753
- Language
- eng
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