Selective removal of ethylene, a deposit precursor, from a "dirty" synthesis gas stream via gas-phase partial oxidation.
Selective removal of ethylene, a deposit precursor, from a "dirty" synthesis gas stream via gas-phase partial oxidation.
复制标题
通过气相部分氧化从“脏”合成气流中选择性去除乙烯（沉积物前体）。
DOI：
10.1021/jp102049c
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发表时间：
2010
期刊：
影响因子：
--
通讯作者：
A. Dean
中科院分区：
文献类型：
--
作者：
Stephanie M. Villano;J. Hoffmann;H. Carstensen;A. Dean
生物质气化中的一个基本问题是，除了所需的合成气产物（H（2）和CO的混合物）之外，气化器流出物还含有其他不需要的产物，这些产物需要在任何进一步的下游加工可以发生之前除去。这项工作评估了通过气相部分氧化从合成气流中选择性去除烃类的潜力。具体地，已经使用管式流动反应器在环境压力下在760-910 ℃的温度范围内和在0.4 - 2.4秒的停留时间范围内研究了甲烷掺杂、乙烯掺杂和甲烷/乙烯掺杂的模型合成气混合物的部分氧化。对于含有甲烷或乙烯的合成气混合物，氧的加入显著降低了烃浓度，而仅观察到氢浓度的小的降低。对于掺杂有甲烷和乙烯的合成气混合物，氧的添加优先除去乙烯，而甲烷和氢气的浓度保持相对不受影响。这些结果进行了比较，使用的反应机制，旨在描述小烃类的热解和部分氧化的活塞流模型的预测。实验观察和模型预测之间的协议是相当不错的，使我们能够探索潜在的化学，导致碳氢化合物的选择性氧化。这些结果的影响进行了简要讨论，在使用合成气生产液体燃料和电力通过固体氧化物燃料电池。
A fundamental issue in the gasification of biomass is that in addition to the desired synthesis gas product (a mixture of H(2) and CO), the gasifier effluent contains other undesirable products that need to be removed before any further downstream processing can occur. This work assesses the potential to selectively remove hydrocarbons from a synthesis gas stream via gas-phase partial oxidation. Specifically, the partial oxidation of methane-doped, ethylene-doped, and methane/ethylene-doped model synthesis gas mixtures has been investigated at ambient pressures over a temperature range of 760-910 degrees C and at residence times ranging from 0.4 to 2.4 s using a tubular flow reactor. For the synthesis gas mixtures that contain either methane or ethylene, the addition of oxygen substantially reduces the hydrocarbon concentration while only a small reduction in the hydrogen concentration is observed. For the synthesis gas mixtures doped with both methane and ethylene, the addition of oxygen preferentially removes ethylene while the concentrations of methane and hydrogen remain relatively unaffected. These results are compared to the predictions of a plug flow model using a reaction mechanism that is designed to describe the pyrolysis and partial oxidation of small hydrocarbon species. The agreement between the experimental observations and the model predictions is quite good, allowing us to explore the underlying chemistry that leads to the hydrocarbon selective oxidation. The implications of these results are briefly discussed in terms of using synthesis gas to produce liquid fuels and electrical power via a solid oxide fuel cell.