Spallina Vincenzo, Melchiori Tommaso, Gallucci Fausto, van Sint Annaland Martin
Chemical Process Intensification, Chemical Engineering and Chemistry, Eindhoven University of Technology, 5600MB Eindhoven, The Netherlands.
Molecules. 2015 Mar 18;20(3):4998-5023. doi: 10.3390/molecules20034998.
The integration of mixed ionic electronic conducting (MIEC) membranes for air separation in a small-to-medium scale unit for H2 production (in the range of 650-850 Nm3/h) via auto-thermal reforming of methane has been investigated in the present study. Membranes based on mixed ionic electronic conducting oxides such as Ba0.5Sr0.5Co0.8Fe0.2O3-δ (BSCF) give sufficiently high oxygen fluxes at temperatures above 800 °C with high purity (higher than 99%). Experimental results of membrane permeation tests are presented and used for the reactor design with a detailed reactor model. The assessment of the H2 plant has been carried out for different operating conditions and reactor geometry and an energy analysis has been carried out with the flowsheeting software Aspen Plus, including also the turbomachines required for a proper thermal integration. A micro-gas turbine is integrated in the system in order to supply part of the electricity required in the system. The analysis of the system shows that the reforming efficiency is in the range of 62%-70% in the case where the temperature at the auto-thermal reforming membrane reactor (ATR-MR) is equal to 900 °C. When the electric consumption and the thermal export are included the efficiency of the plant approaches 74%-78%. The design of the reactor has been carried out using a reactor model linked to the Aspen flowsheet and the results show that with a larger reactor volume the performance of the system can be improved, especially because of the reduced electric consumption. From this analysis it has been found that for a production of about 790 Nm3/h pure H2, a reactor with a diameter of 1 m and length of 1.8 m with about 1500 membranes of 2 cm diameter is required.
本研究对混合离子电子导体（MIEC）膜在中、小规模装置中用于空气分离以通过甲烷自热重整制氢（制氢规模为650 - 850 Nm³/h）进行了研究。基于混合离子电子导电氧化物（如Ba₀.₅Sr₀.₅Co₀.₈Fe₀.₂O₃₋δ（BSCF））的膜在800℃以上温度下能提供足够高的氧通量且纯度较高（高于99%）。给出了膜渗透测试的实验结果，并将其用于带有详细反应器模型的反应器设计。针对不同的操作条件和反应器几何形状对制氢装置进行了评估，并使用流程模拟软件Aspen Plus进行了能量分析，其中还包括实现适当热集成所需的涡轮机。系统中集成了一台微型燃气轮机，以提供系统所需的部分电力。系统分析表明，在自热重整膜反应器（ATR - MR）温度为900℃的情况下，重整效率在62% - 70%范围内。当计入电耗和热输出时，装置效率接近74% - 78%。利用与Aspen流程相关联的反应器模型进行了反应器设计，结果表明，增大反应器体积可提高系统性能，特别是能降低电耗。通过该分析发现，要生产约790 Nm³/h的纯氢，需要一个直径1 m、长度1.8 m的反应器，其中约有1500个直径为2 cm的膜。
