介质阻挡放电等离子体中氧化铈负载单原子铂催化剂上甲烷的非氧化偶联
Nonoxidative Coupling of Methane over Ceria-Supported Single-Atom Pt Catalysts in DBD Plasma.
作者信息
Liu Lina, Das Sonali, Zhang Zhikun, Kawi Sibudjing
机构信息
Department of Chemical & Biomolecular Engineering, National University of Singapore, Singapore 117585.
MOE Key Laboratory of Pollution Processes and Environmental Criteria, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.
出版信息
ACS Appl Mater Interfaces. 2022 Feb 2;14(4):5363-5375. doi: 10.1021/acsami.1c21550. Epub 2022 Jan 24.
Plasma-catalytic direct nonoxidative coupling of methane (NCM) into C hydrocarbons was investigated over ceria-supported atomically dispersed Pt (Pt/CeO-SAC) and nanoparticle Pt (Pt/CeO-NP) catalysts in dielectric barrier discharge (DBD) plasma. Nonthermal plasma facilitated C-H bond dissociation in CH at low temperatures (<150 °C) and atmospheric pressure. The presence of Pt/CeO catalysts in plasma further enhanced CH conversion and C hydrocarbon selectivity by enabling the conversion of vibrationally excited methane species with high internal energy on active Pt sites. Noticeably, the Pt/CeO-SAC catalyst displayed a more remarkable performance, with a CH conversion of 39% and a C selectivity of 54% at 54 W. The enhanced CH conversion was attributed to abundant coordinatively unsaturated Pt sites in Pt/CeO-SAC, which were more active for C-H bond scission. Meanwhile, isolated Pt atoms in Pt/CeO-SAC promoted C hydrocarbon formation by hindering the unselective formation of coke from deep dehydrogenation of CH intermediates and higher hydrocarbons from oligomerization reactions.
在介质阻挡放电（DBD）等离子体中，研究了在二氧化铈负载的原子分散铂（Pt/CeO-SAC）和纳米颗粒铂（Pt/CeO-NP）催化剂上，甲烷（NCM）的等离子体催化直接非氧化偶联生成碳氢化合物。非热等离子体在低温（<150°C）和大气压下促进了甲烷中C-H键的解离。等离子体中Pt/CeO催化剂的存在通过使具有高内能的振动激发甲烷物种在活性Pt位点上转化，进一步提高了甲烷转化率和碳氢化合物选择性。值得注意的是，Pt/CeO-SAC催化剂表现出更显著的性能，在54 W时甲烷转化率为39%，碳选择性为54%。甲烷转化率的提高归因于Pt/CeO-SAC中大量的配位不饱和Pt位点，这些位点对C-H键断裂更具活性。同时，Pt/CeO-SAC中孤立的Pt原子通过阻碍甲烷中间体深度脱氢形成焦炭以及齐聚反应形成高级烃的非选择性反应，促进了碳氢化合物的形成。
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