Membrane reactor performance of steam reforming of methane using hydrogen-permselective catalytic SiO2 membranes
Membrane reactor performance of steam reforming of methane using hydrogen-permselective catalytic SiO2 membranes
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DOI：
10.1016/j.memsci.2007.10.057
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发表时间：
2008-05
影响因子：
9.5
通讯作者：
T. Tsuru;T. Morita;H. Shintani;Tomohisa Yoshioka;M. Asaeda
中科院分区：
文献类型：
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作者：
T. Tsuru;T. Morita;H. Shintani;Tomohisa Yoshioka;M. Asaeda
对膜催化反应器中甲烷水蒸气重整制氢进行了模拟和实验研究。膜反应器的模拟，使用等温和活塞流模型与选择性渗透从反应物流渗透流，进行评估的渗透选择性对膜反应器的性能的影响-如甲烷转化率和氢气产率-在高达1000 kPa的压力。以甲烷转化率为0.8为目标的模拟研究表明，如果氢气与氮气的渗透比（α（H2/N2））大于100，H2与H2O的渗透比大于15，则氢气产率和产率对操作条件（如反应压力）的依赖性大致相同。制备了由微孔Ni掺杂SiO2顶层和催化剂载体组成的催化膜反应器，并在500°C下进行了甲烷水蒸气重整实验。为了提高膜催化活性，制备了一种双峰催化剂载体，该载体允许金属催化剂的大扩散性和高分散性。考察了H2渗透率在2-5×10− 6 m3 m −2s− 1 kPa −1范围内、H2/N2为2 - 5 -500和H2/H2O为6-15的催化膜用于甲烷水蒸气重整反应。实验结果表明，随着反应侧压力的增加（高达500 kPa），反应器的产氢性能得到了提高，这与理论模拟结果一致。
Hydrogen production by steam reforming of methane using catalytic membrane reactors was investigated first by simulation, then by experimentation. The membrane reactor simulation, using an isothermal and plug-flow model with selective permeation from reactant stream to permeate stream, was conducted to evaluate the effect of permselectivity on membrane reactor performance – such as methane conversion and hydrogen yield – at pressures as high as 1000kPa. The simulation study, with a target for methane conversion of 0.8, showed that hydrogen yield and production rate have approximately the same dependency on operating conditions, such as reaction pressure, if the permeance ratio of hydrogen over nitrogen (α(H2/N2)) is larger than 100 and of H2over H2O is larger than 15. Catalytic membrane reactors, consisting of a microporous Ni-doped SiO2top layer and a catalytic support, were prepared and applied experimentally for steam reforming of methane at 500°C. A bimodal catalytic support, which allows large diffusivity and high dispersion of the metal catalyst, was prepared for the enhancement of membrane catalytic activity. Catalytic membranes having H2permeances in the range of 2–5×10−6m3m−2s−1kPa−1, with H2/N2of 25–500 and H2/H2O of 6–15, were examined for steam reforming of methane. Increased performance for the production of hydrogen was experimentally obtained with an increase in reaction-side pressure (as high as 500kPa), which agreed with the theoretical simulation with no fitting parameters.