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Screening of MgO- and CeO2-Based Catalysts for Carbon Dioxide Oxidative Coupling of Methane to C2+ Hydrocarbons

机译:甲烷氧化甲烷与C2 +烃的MgO-和CeO2基催化剂的筛选

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摘要

The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM)have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based solids with oxides from alkali (Li2O), alkaline earth (CaO), and transition metal groups (WO3 or MnO). The presence of the peroxide (O22-) active sites on the Li2O2, revealed by Raman spectroscopy, may be the key factor in the enhanced performance of some of the Li2O/MgO catalysts.The high reducibility of the CeO2 catalyst, an important factor in the CO2-OCM catalyst activity, may be enhanced by the presence of manganese oxide species. The manganese oxide species increases oxygen mobility and oxygen vacancies in the CeO2 catalyst. Raman and Fourier Transform Infra Red (FT-IR) spectroscopies revealed the presence of lattice vibrations of metal-oxygen bondings and active sites in which the peaks corresponding to the bulk crystalline structures of Li2O, CaO, WO3 and MnO are detected. The performance of 5%MnO/15%CaO/CeO2 catalyst is the most potential among the CeO2-based catalysts,although lower than the 2%Li2O/MgO catalyst. The 2%Li2O/MgO catalyst showed the most promising C2+ hydrocarbons selectivity and yield at 98.0% and 5.7%, respectively.
机译:已经在三元和二元金属氧化物催化剂上研究了用于甲烷的二氧化碳氧化偶联(CO2-OCM)的催化剂筛选试验。通过用基于碱金属(Li2O),碱土金属(CaO)和过渡金属基团(WO3或MnO)的氧化物掺杂MgO和CeO2固体,来制备催化剂。拉曼光谱显示,Li2O2上过氧化物(O22-)活性位点的存在可能是某些Li2O / MgO催化剂性能增强的关键因素.CeO2催化剂的高还原性是CO2-OCM催化剂的活性可以通过存在氧化锰来增强。氧化锰物质会增加CeO2催化剂中的氧迁移率和氧空位。拉曼光谱和傅立叶变换红外光谱(FT-IR)显示存在金属-氧键和活性位的晶格振动,其中检测到与Li2O,CaO,WO3和MnO的整体晶体结构相对应的峰。 5%MnO / 15%CaO / CeO2催化剂的性能是CeO2基催化剂中最有潜力的,尽管低于2%Li2O / MgO催化剂。 2%Li2O / MgO催化剂显示出最有希望的C2 +烃选择性和产率,分别为98.0%和5.7%。

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