Hydrogen production via natural gas steam reforming in a Pd-Au membrane reactor. Comparison between methane and natural gas steam reforming reactions
Hydrogen production via natural gas steam reforming in a Pd-Au membrane reactor. Comparison between methane and natural gas steam reforming reactions
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DOI：
10.1016/j.memsci.2018.09.054
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发表时间：
2018-12
影响因子：
9.5
通讯作者：
Bryce H. Anzelmo;J. Wilcox;S. Liguori
中科院分区：
文献类型：
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作者：
Bryce H. Anzelmo;J. Wilcox;S. Liguori
在填充有市售Ni基催化剂的Pd-Au复合膜反应器中，在温和的操作条件下进行天然气水蒸气重整，制备直接供给质子交换膜燃料电池的高纯氢气。通过使用无电和电镀技术在多孔不锈钢支撑体上分别沉积存款Pd和Au层，制备了厚度约为12 μm的Pd-Au复合膜。退火后，该膜在450 °C下的氢渗透率为1.30 × 10− 3 mol/s-m2-Pa0.5，在低于300 kPa的压力和低于400 °C的温度下，H2/Ar的理想选择性接近无限。天然气重整反应在450 °C下以3.5的蒸汽/甲烷比和2600 h-1的气时空速在100 kPa至300 kPa的不同操作压力下进行。作为对比，在相同的操作条件下进行了甲烷水蒸气重整反应，天然气重整反应表现出比甲烷水蒸气重整反应更好的性能，在450 °C和300 kPa下，高级烃转化率达到80%以上，氢气回收率接近65%。在所有的实验测试中获得了高纯度的氢气。没有观察到焦炭形成。通过扫描电子显微镜和能量色散X射线能谱仪讨论了膜的反应后分析。
High-purity hydrogen to be fed directly to a PEMFC was produced by carrying out natural gas steam reforming under moderate operating conditions in a Pd-Au composite membrane reactor packed with a commercial Ni-based catalyst. The Pd-Au composite membrane with a thickness of approximately 12 µm was fabricated by using both electroless and electroplating techniques to deposit Pd and Au layers, respectively, over a porous stainless-steel support. After annealing, the membrane showed a hydrogen permeance of 1.30 × 10−3mol/s-m2-Pa0.5at 450 °C, and near-infinite ideal selectivity of H2/Ar at pressures lower than 300 kPa and at temperatures lower than 400 °C. The natural gas reforming reaction was performed at 450 °C with a steam-to-methane ratio of 3.5 and gas hourly space velocity of 2600 h−1at different operating pressures varying from 100 kPa to 300 kPa. As a comparison, the steam methane reforming reaction was also carried out at the same operating conditions.The natural gas reforming reaction showed better performance than the steam methane reforming reaction and reached > 80% conversion of the higher hydrocarbons and almost 65% of hydrogen recovery at 450 °C and 300 kPa. High-purity hydrogen was obtained in all the experimental tests. No coke formation was observed. Post-reaction analysis of the membrane is discussed via scanning electron microscope and energy-dispersive X-ray spectroscopy.