Plasma-Enhanced Chemical Looping Oxidative Coupling of Methane through Synergy between Metal-Loaded Dielectric Particles and Non-Thermal Plasma
A plasma–catalyst hybrid system has been developed for the direct conversion of methane to C<sub>2+</sub> hydrocarbons in dielectric barrier discharge (DBD) plasma. TiO<sub>2</sub> presented the highest C<sub>2+</sub> yield of 11.63% among different dielectric mat...
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MDPI AG
2023-03-01
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| Series: | Catalysts |
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| Online Access: | https://www.mdpi.com/2073-4344/13/3/557 |
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| author | Shunshun Kang Jinlin Deng Xiaobo Wang Kun Zhao Min Zheng Da Song Zhen Huang Yan Lin Anqi Liu Anqing Zheng Zengli Zhao |
| author_facet | Shunshun Kang Jinlin Deng Xiaobo Wang Kun Zhao Min Zheng Da Song Zhen Huang Yan Lin Anqi Liu Anqing Zheng Zengli Zhao |
| author_sort | Shunshun Kang |
| collection | DOAJ |
| description | A plasma–catalyst hybrid system has been developed for the direct conversion of methane to C<sub>2+</sub> hydrocarbons in dielectric barrier discharge (DBD) plasma. TiO<sub>2</sub> presented the highest C<sub>2+</sub> yield of 11.63% among different dielectric materials when integrated with DBD plasma, which made us concentrate on the TiO<sub>2</sub>-based catalyst. It was demonstrated that MnTi catalyst showed the best methane coupling performance of 27.29% C<sub>2+</sub> yield with 150 V applied voltage, without additional thermal input. The catalytic performance of MnTi catalyst under various operation parameters was further carried out, and different techniques, such as X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and H<sub>2</sub>-temperature-programmed reduction were used to explore the effect of Mn loading on methane oxidative coupling (OCM) performance. The results showed that applied voltage and flow rate had a significant effect on methane activation. The dielectric particles of TiO<sub>2</sub> loaded with Mn not only synergistically affected the coupling reaction, but also facilitated charge deposition to generate a strong local electric field to activate methane. The synergy effects boosted the OCM performance and the C<sub>2+</sub> yield became 1.25 times higher than that of the undoped TiO<sub>2</sub> under identical operating conditions in plasma, which was almost impossible to occur even at 850 °C on the MnTi catalyst in the absence of plasma. Moreover, the reaction activity of the catalyst was fully recovered by plasma regeneration at 300 °C and maintained its stability in for at least 30 consecutive cyclic redox tests. This work presents a new opportunity for efficient methane conversion to produce C<sub>2+</sub> at low temperatures by plasma assistance. |
| first_indexed | 2024-03-11T06:47:44Z |
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| id | doaj.art-864de4c193704742bb85c4790fec78be |
| institution | Directory Open Access Journal |
| issn | 2073-4344 |
| language | English |
| last_indexed | 2024-03-11T06:47:44Z |
| publishDate | 2023-03-01 |
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| series | Catalysts |
| spelling | doaj.art-864de4c193704742bb85c4790fec78be2023-11-17T10:11:07ZengMDPI AGCatalysts2073-43442023-03-0113355710.3390/catal13030557Plasma-Enhanced Chemical Looping Oxidative Coupling of Methane through Synergy between Metal-Loaded Dielectric Particles and Non-Thermal PlasmaShunshun Kang0Jinlin Deng1Xiaobo Wang2Kun Zhao3Min Zheng4Da Song5Zhen Huang6Yan Lin7Anqi Liu8Anqing Zheng9Zengli Zhao10Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, ChinaGuangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, ChinaGuangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, ChinaGuangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, ChinaState Key Laboratory of Complex Metal Resources Clean Utilization, Kunming University of Science and Technology, Kunming 650031, ChinaGuangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, ChinaGuangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, ChinaGuangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, ChinaGuangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, ChinaGuangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, ChinaGuangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, ChinaA plasma–catalyst hybrid system has been developed for the direct conversion of methane to C<sub>2+</sub> hydrocarbons in dielectric barrier discharge (DBD) plasma. TiO<sub>2</sub> presented the highest C<sub>2+</sub> yield of 11.63% among different dielectric materials when integrated with DBD plasma, which made us concentrate on the TiO<sub>2</sub>-based catalyst. It was demonstrated that MnTi catalyst showed the best methane coupling performance of 27.29% C<sub>2+</sub> yield with 150 V applied voltage, without additional thermal input. The catalytic performance of MnTi catalyst under various operation parameters was further carried out, and different techniques, such as X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and H<sub>2</sub>-temperature-programmed reduction were used to explore the effect of Mn loading on methane oxidative coupling (OCM) performance. The results showed that applied voltage and flow rate had a significant effect on methane activation. The dielectric particles of TiO<sub>2</sub> loaded with Mn not only synergistically affected the coupling reaction, but also facilitated charge deposition to generate a strong local electric field to activate methane. The synergy effects boosted the OCM performance and the C<sub>2+</sub> yield became 1.25 times higher than that of the undoped TiO<sub>2</sub> under identical operating conditions in plasma, which was almost impossible to occur even at 850 °C on the MnTi catalyst in the absence of plasma. Moreover, the reaction activity of the catalyst was fully recovered by plasma regeneration at 300 °C and maintained its stability in for at least 30 consecutive cyclic redox tests. This work presents a new opportunity for efficient methane conversion to produce C<sub>2+</sub> at low temperatures by plasma assistance.https://www.mdpi.com/2073-4344/13/3/557oxidative coupling of methanechemical loopingsynergy effectsplasma enhancement |
| spellingShingle | Shunshun Kang Jinlin Deng Xiaobo Wang Kun Zhao Min Zheng Da Song Zhen Huang Yan Lin Anqi Liu Anqing Zheng Zengli Zhao Plasma-Enhanced Chemical Looping Oxidative Coupling of Methane through Synergy between Metal-Loaded Dielectric Particles and Non-Thermal Plasma Catalysts oxidative coupling of methane chemical looping synergy effects plasma enhancement |
| title | Plasma-Enhanced Chemical Looping Oxidative Coupling of Methane through Synergy between Metal-Loaded Dielectric Particles and Non-Thermal Plasma |
| title_full | Plasma-Enhanced Chemical Looping Oxidative Coupling of Methane through Synergy between Metal-Loaded Dielectric Particles and Non-Thermal Plasma |
| title_fullStr | Plasma-Enhanced Chemical Looping Oxidative Coupling of Methane through Synergy between Metal-Loaded Dielectric Particles and Non-Thermal Plasma |
| title_full_unstemmed | Plasma-Enhanced Chemical Looping Oxidative Coupling of Methane through Synergy between Metal-Loaded Dielectric Particles and Non-Thermal Plasma |
| title_short | Plasma-Enhanced Chemical Looping Oxidative Coupling of Methane through Synergy between Metal-Loaded Dielectric Particles and Non-Thermal Plasma |
| title_sort | plasma enhanced chemical looping oxidative coupling of methane through synergy between metal loaded dielectric particles and non thermal plasma |
| topic | oxidative coupling of methane chemical looping synergy effects plasma enhancement |
| url | https://www.mdpi.com/2073-4344/13/3/557 |
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