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Integration of Methane Steam Reforming and Water Gas Shift Reaction in a Pd/Au/Pd-Based Catalytic Membrane Reactor for Process Intensification

机译:基于Pd / Au / Pd的催化膜反应器中甲烷蒸汽重整和水煤气变换反应的集成以增强工艺

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摘要

Palladium-based catalytic membrane reactors (CMRs) effectively remove H2 to induce higher conversions in methane steam reforming (MSR) and water-gas-shift reactions (WGS). Within such a context, this work evaluates the technical performance of a novel CMR, which utilizes two catalysts in series, rather than one. In the process system under consideration, the first catalyst, confined within the shell side of the reactor, reforms methane with water yielding H2, CO and CO2. After reforming is completed, a second catalyst, positioned in series, reacts with CO and water through the WGS reaction yielding pure H2O, CO2 and H2. A tubular composite asymmetric Pd/Au/Pd membrane is situated throughout the reactor to continuously remove the produced H2 and induce higher methane and CO conversions while yielding ultrapure H2 and compressed CO2 ready for dehydration. Experimental results involving (i) a conventional packed bed reactor packed (PBR) for MSR, (ii) a PBR with five layers of two catalysts in series and (iii) a CMR with two layers of two catalysts in series are comparatively assessed and thoroughly characterized. Furthermore, a comprehensive 2D computational fluid dynamics (CFD) model was developed to explore further the features of the proposed configuration. The reaction was studied at different process intensification-relevant conditions, such as space velocities, temperatures, pressures and initial feed gas composition. Finally, it is demonstrated that the above CMR module, which was operated for 600 h, displays quite high H2 permeance and purity, high CH4 conversion levels and reduced CO yields.
机译:钯基催化膜反应器(CMR)可有效除去H2,以在甲烷蒸汽重整(MSR)和水煤气变换反应(WGS)中引起更高的转化率。在这样的背景下,这项工作评估了一种新型CMR的技术性能,该新型CMR采用了串联的两种催化剂,而不是一种。在所考虑的工艺系统中,限制在反应器壳侧的第一催化剂用水重整甲烷,生成H2,CO和CO2。重整完成后,串联放置的第二种催化剂通过WGS反应与CO和水反应,生成纯净的H2O,CO2和H2。管状复合不对称Pd / Au / Pd膜遍布整个反应器,以连续除去产生的H2并诱导更高的甲烷和CO转化率,同时产生超纯H2和压缩的CO2,可供脱水。相对评估并彻底评估了涉及(i)用于MSR的常规填充床反应器填充(PBR),(ii)具有五层两个串联催化剂的PBR和(iii)具有两层两个串联催化剂的CMR的实验结果表征。此外,开发了全面的二维计算流体动力学(CFD)模型,以进一步探索所提出配置的功能。在与工艺强度相关的不同条件下研究了反应,例如空速,温度,压力和初始进料气组成。最后,证明了运行600 h的上述CMR模块显示出相当高的H2渗透率和纯度,高CH4转化水平和降低的CO收率。

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