C1 oxidative coupling via bromine activation and tandem catalytic condensation and neutralization over CaO/zeolite composites: II. Product distribution variation and full bromine confinement
C1 oxidative coupling via bromine activation and tandem catalytic condensation and neutralization over CaO/zeolite composites: II. Product distribution variation and full bromine confinement
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DOI：
10.1016/j.cattod.2004.09.013
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发表时间：
2004-12
期刊：
影响因子：
5.3
通讯作者：
I. Lorkovic;M. Noy;Walter A. Schenck;Craig A. Belon;M. Weiss;Shouli Sun;J. Sherman;E. McFarland
中科院分区：
文献类型：
--
作者：
I. Lorkovic;M. Noy;Walter A. Schenck;Craig A. Belon;M. Weiss;Shouli Sun;J. Sherman;E. McFarland
我们描述了一个以O2为氧化剂的三步溴催化甲烷氧化偶联反应过程。在第一步中，负载型金属溴化物与O2反应生成Br2和负载型金属氧化物。这样形成的Br2与过量的CH4反应，得到CH4、溴甲烷和HBr的混合物。这种混合物通过CaO/沸石复合材料，使溴碳100%转化为产物，并中和HBr以重整金属溴。生成的产品含有更高的碳氢化合物、过量的CH4和水。一旦CaO的HBR中和能力耗尽，负载型CaBr2/ZSM-5也可以作为甲基溴偶联的催化剂。讨论了温度、压力和反应时间对中间体甲烷溴化反应的影响以及对部分氧化产物分布的影响。描述了将该方案并入仅向其进料甲烷和O2的反应器中。
We describe a three-step bromine-mediated process for oxidative coupling of methane using O2as oxidant. In the first step, a supported metal bromide solid is treated with O2to generate Br2and supported metal oxide. The Br2thus formed reacts with excess CH4, giving a mixture of CH4, bromomethanes, and HBr. This mixture is passed over a CaO/zeolite composite which condenses bromocarbons with 100% conversion to products, and neutralizes HBr to reform the metal bromide. The resulting product contains higher hydrocarbons, excess CH4, and water. Once the HBr neutralizing capacity of the CaO is spent, the supported CaBr2/ZSM-5 may also serve as catalyst for methyl bromide coupling. The effect of temperature, pressure, and reaction time on the intermediate methane bromination as well as on the overall partial oxidation product distribution is discussed. Incorporation of this scheme into a reactor into which only methane and O2are fed is described.