- Title
- Catalytic coupling of CH₄ with CHF₃ for the synthesis of VDF over LaOF catalyst
- Creator
- Cheng, Yimin; Wang, Jinchao; Stockenhuber, Michael; Kennedy, Eric M.; Han, Wenfeng; Song, Yanyan; Liu, Wucan; Yang, Luteng; Wang, Shucheng; Wu, Zhixing; Tang, Haodong; Zhang, Jianjun
- Relation
- Greenhouse Gasses: science and technology Vol. 8, Issue 3, p. 587-602
- Publisher Link
- http://dx.doi.org/10.1002/ghg.1769
- Publisher
- John Wiley & Sons
- Resource Type
- journal article
- Date
- 2018
- Description
- The oxidative coupling of methane (OCM) with CHF₃ facilitates the synthesis of vinylidene fluoride (VDF). The aim is to utilize CHF₃, which is otherwise considered a waste with a very high global warming potential. This study focuses on the effect of a LaOF catalyst on OCM occurring in the presence of CHF₃, which engenders a promoting effect of O₂ on CH₄ activation. It examines the structural and phase changes of the lanthanum catalyst during the reaction and then speculates on the reaction mechanism. In combining OCM with CHF₃, both the conversion of CH₄ and the formation rate of VDF are almost tripled at 700°C. However, at higher temperatures, gas‐phase reactions play a dominating role in the conversion of CH₄ and LaOF catalyst plays a very minor role in the reaction system at elevated temperatures. Irrespective of the reaction temperature, VDF is produced via the gas‐phase coupling of CH₃ radicals with CF₂. During pretreatment or during the reaction itself, La₂O₃ is fluorinated by CHF₃ and HF, yielding the formation of surface LaOF and LaF₃ species. LaF₃ is a relatively inactive catalyst for CH₄ conversion, whereas, in comparison LaOF appears to play a very important role in the activation of CH₄ at low temperatures. The activation mechanism of CH₄ at relatively low temperatures is similar with that postulated to occur during the OCM.
- Subject
- trifluoromethane; La₂O₃; vinylidene fluoride; pyrolysis
- Identifier
- http://hdl.handle.net/1959.13/1405460
- Identifier
- uon:35492
- Identifier
- ISSN:2152-3878
- Language
- eng
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