Kinetic Process Assessment of H2 Purification over Highly Porous Carbon Sorbents Under Multicomponent Feed Conditions

Kinetic Process Assessment of H2 Purification over Highly Porous Carbon Sorbents Under Multicomponent Feed Conditions
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DOI:
10.1016/j.seppur.2022.122695
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发表时间:
2022-11
影响因子:
8.6
通讯作者:
K. Baamran;Qasim Al-Naddaf;Shane Lawson;A. Ali Rownaghi;Fateme Rezaei
K. Baamran;Qasim Al-Naddaf;Shane Lawson;A. Ali Rownaghi;Fateme Rezaei
中科院分区:
工程技术1区
文献类型:
--
作者:
K. Baamran;Qasim Al-Naddaf;Shane Lawson;A. Ali Rownaghi;Fateme Rezaei

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作为一种通用的能量载体,由于其在石油化工精炼、金属还原和新兴燃料电池市场中的普遍作用,对纯H2的需求不断增加。甲烷蒸汽重整(SMR)制氢过程中通常含有CO2、CO和CH 4等杂质,要充分有效地筛选潜在的H2净化吸附剂,需要对多组分变压吸附(PSA)的热力学和动力学行为进行评价。因此,在这项研究中,我们评估了三种具有高表面积和孔体积的市售活性炭,用于从由H2/CO/CH 4/CO2(75/5/5/15体积%)组成的模拟SMR废气流中PSA提质H2。除了纯气体的高压吸附等温线,H2纯度和回收率,和H2生产率估计从循环PSA实验,而实际的(CO + CH 4 + CO2)/H2选择性值估计从突破实验。对于性能最好的材料,结果表明H2纯度和回收率分别为99.6%和55.3%,生产率为18.3molH2/kg.h,多组分(CO + CH 4 + CO2)/H2选择性为59.86%。不同吸附质对活性炭的亲合力从大到小依次为CO2> CH 4> CO> H2。这些碳基吸附剂上的H2纯化被发现是一个平衡控制的过程。
As a universal energy carrier, the need for pure H2is ever increasing due to its ubiquitous role in petrochemical refining, metal reduction, and the up-and-coming fuel cell market. Hydrogen produced from steam methane reforming (SMR) is typically laden with impurities such as CO2, CO, and CH4and a full efficiency screening for potential H2purification sorbents requires evaluating the thermodynamic and kinetic behaviors associated with multicomponent pressure swing adsorption (PSA). As such, in this study we assessed three commercially available activated carbons with high surface area and pore volume for the PSA upgrading of H2from simulated SMR off-gas stream consisting of H2/CO/CH4/CO2(75/5/5/15 vol%). In addition to high-pressure adsorption isotherms for pure gases, H2purity and recovery, and H2productivity were estimated from cyclic PSA experiments, while actual (CO + CH4+ CO2)/H2selectivity values were estimated from breakthrough experiments. For the best performing material, the results demonstrated H2purity and recovery of 99.6 and 55.3 %, respectively with a productivity of 18.3 molH2/kg.h and multicomponent (CO + CH4+ CO2)/H2selectivity of 59.86 %. Moreover, the affinity of the different adsorbates toward the activated carbons presented from the most adsorbed to the least adsorbed gas was in the order of CO2> CH4> CO ≫ H2. The H2purification over these carbon-based adsorbents was found to be an equilibrium-controlled process.