CO2 activation by methane in a dual-bed configuration via methane cracking and iron oxide lattice oxygen transport – Concept and materials development
CO2 activation by methane in a dual-bed configuration via methane cracking and iron oxide lattice oxygen transport – Concept and materials development
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DOI：
10.1016/j.cej.2018.05.069
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发表时间：
2018-10
影响因子：
15.1
通讯作者：
M. Keller;Y. Matsuzaki;J. Otomo
中科院分区：
文献类型：
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作者：
M. Keller;Y. Matsuzaki;J. Otomo
在这项工作中，我们描述了一种新的工艺配置CO2活化成CO通过甲烷裂解。这在双反应器配置中通过在两个反应器之间循环具有沉积碳的负载型氧化铁/铁颗粒来实现。热力学平衡计算表明，具有逆流气-固流动的反应器配置能够实现产物气体中的高CO产率和浓度。在两个反应器在850 °C下逆流流动的情况下，潜在可实现的CO产量估计在吸热操作中为3.7 mol CO/mol CH 4，纯度为84%，在自热操作中为2.7 mol CO/mol CH 4，纯度为88%。Fe/载体复合材料是为这一应用而开发的，以实现两个反应器之间的氧传输功能，并作为固体碳形成的基底。Fe/BaZr0.9Y0.1O3−δ（BZY）复合材料表现出与H2的快速还原动力学，我们将其归因于BZY载体的原位铁掺杂所赋予的混合离子-电子传导。此外，该载体的高质子传导性导致高CH 4分解速率以形成固体碳和氢，这可能是由于加速了从其表面上的甲基基团中提取氢。因此，这种混合的导电性导致独特的性能，可以在这样的CH 4分解过程配置中利用。
In this work we describe a novel process configuration for CO2activation into CO via methane cracking. This is achieved in a two-reactor configuration by circulating supported iron oxide/iron particles with deposited carbon between the two reactors. Thermodynamic equilibrium calculations indicate that reactor configurations with counter-current gas-solids flow enable a high CO yield and concentration in the product gas. With both reactors in counter-current flow at 850 °C the potentially achievable production of CO is estimated at 3.7 mol CO per mol of CH4with 84% purity in endothermal operation and 2.7 mol CO per mol of CH4with 88% purity in autothermal operation. Fe/support composite materials are developed for this application to fulfill the function of oxygen transport between the two reactors and serve as a substrate for solid carbon formation. Fe/BaZr0.9Y0.1O3−δ(BZY) composites exhibit rapid reduction kinetics with H2that we ascribe to mixed-ionic-electronic conduction imparted by in-situ iron doping of the BZY support. In addition, the high proton conductivity of this support results in high CH4decomposition rates to form solid carbon and hydrogen, likely due to the acceleration of hydrogen abstraction from the methyl group on its surface. This mixed conductivity thus results in unique properties that can be exploited in such CH4decomposition process configurations.