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Fluidised bed membrane reactor for ultrapure hydrogen production via methane steam reforming: Experimental demonstration and model validation

机译：通过甲烷蒸汽重整生产超纯氢的流化床膜反应器：实验演示和模型验证

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Hydrogen is emerging as a future alternative for mobile and stationary energy carriers in addition to its use in chemical and petrochemical applications. A novel multifunctional reactor concept has been developed for the production of ultrapure hydrogen (<10 ppm CO) from light hydrocarbons such as methane for online use in downstream polymer electrolyte membrane fuel cells. A high degree of process intensification can be achieved by integrating perm-selective hydrogen membranes for selective hydrogen removal to shift the methane steam reforming and water-gas-shift equilibriums in the favourable direction and perm-selective oxygen membranes for selective oxygen addition to supply the required reaction energy via partial oxidation of part of the methane feed and enable pure CO2 capture without costly post-treatment. This can be achieved in a proposed novel multifunctional bi-membrane bi-section fluidised bed reactor [Patil, C.S., van Sint Annaland, M., Kuipers. J.A.M., 2005. Design of a novel autothermal membrane assisted fluidized bed reactor for the production of ultrapure hydrogen from methane. Industrial and Engineering Chemistry Research 44, 9502-9512]. In this paper, an experimental proof of principle for the steam reforming/water-gas-shift section of the proposed novel fluidised bed membrane reactor is presented. A fluidised bed membrane reactor for steam reforming of methane/water-gas-shift on a commercial noble metal-based catalyst has been designed and constructed using 10 H-2 perm-selective Pd membranes for a fuel cell power output in the range of 50-100W. It has been experimentally demonstrated that by the insertion of the membranes in the fluidised bed, the thermodynamic equilibrium constraints can indeed be overcome, i.e., increased CH4 conversion, decreased CO selectivity and higher product yield (H-2 produced/CH4 reacted). Experiments at different superficial gas velocities and also at different temperatures and pressures (carried out in the regime without kinetic limitations) revealed enhanced reactor performance at higher temperatures (650 degrees C) and pressures (3-4 bar). With a phenomenological two-phase reactor model for the fluidised bed membrane reactor, incorporating a separately developed lumped flux expression for the H-2 permeation rate through the used Pd-based membranes, the measured data from the fluidised bed membrane reactor could be well described, provided that axial gas back-mixing in the membrane-assisted fluidised bed reactor is negligible. This indicates that the membrane reactor behaviour approached that of an ideal isothermal plug flow reactor with maximum H-2 permeation. (C) 2007 Elsevier Ltd. All rights reserved.
机译：除了在化学和石化应用中使用氢以外，氢正在成为移动和固定式能源载体的未来替代品。已经开发了一种新颖的多功能反应器概念，用于从轻烃（例如甲烷）生产超纯氢（<10 ppm CO），用于下游聚合物电解质膜燃料电池的在线使用。通过集成用于选择性除氢的渗透选择性氢膜以使甲烷蒸汽重整和水煤气转换平衡朝有利方向移动，以及用于选择性添加氧气的渗透选择性氧膜来提供较高的工艺强度，可以实现高度的工艺强化。通过部分甲烷进料的部分氧化来消耗所需的反应能量，并且无需昂贵的后处理即可捕集纯CO2。这可以在提出的新型多功能双膜两段流化床反应器中实现[Patil，C.S.，van Sint Annaland，M.，Kuipers。 J.A.M.，2005年。一种新型自热膜辅助流化床反应器的设计，该反应器用于从甲烷生产超纯氢。工业与工程化学研究44，9502-9512]。本文提出了所提出的新型流化床膜反应器的蒸汽重整/水煤气变换段原理的实验证明。已经设计并构造了一种流化床膜反应器，用于在市售贵金属基催化剂上进行甲烷/水煤气变换的蒸汽重整，并使用10 H-2渗透选择性Pd膜进行了设计和构造，以使燃料电池的输出功率达到50 -100W。实验证明，通过将膜插入流化床中，确实可以克服热力学平衡的限制，即增加CH4转化率，降低CO选择性和提高产物收率（产生H-2 / CH4反应）。在不同的表观气体速度以及不同的温度和压力（在没有动力学限制的情况下进行）下进行的实验表明，在较高温度（650摄氏度）和压力（3-4巴）下，反应器性能得到了提高。利用流化床膜反应器的现象学两相反应器模型，结合单独开发的通过使用过的基于Pd的膜的H-2渗透率集总通量表达式，可以很好地描述流化床膜反应器的测量数据只要在膜辅助流化床反应器中轴向气体回混可以忽略不计。这表明膜反应器的性能接近具有最大H-2渗透率的理想等温活塞流反应器的性能。 （C）2007 Elsevier Ltd.保留所有权利。

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