Prediction of hydrogen flux through sulfur-tolerant binary alloy membranes
Prediction of hydrogen flux through sulfur-tolerant binary alloy membranes
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DOI：
10.1126/science.1107041
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发表时间：
2005-01-28
期刊：
影响因子：
56.9
通讯作者：
Sholl, DS
中科院分区：
文献类型：
--
作者：
Kamakoti, P;Morreale, BD;Sholl, DS
金属膜在氢净化中起着至关重要的作用。无缺陷膜可以表现出有效的无限选择性，但也必须提供高通量、抗中毒、长使用寿命和低成本。合金化为改进基于纯金属（如钯）的膜提供了一条途径。我们展示了从头计算和粗粒度建模如何能够准确预测通过二元合金膜的氢通量，作为合金成分，温度和压力的函数。我们的方法，不需要实验输入，除了大块晶体结构的知识，证明了钯铜合金，由于面心立方和体心立方晶体结构的存在，表现出非凡的行为，并具有抗硫中毒的潜力。通过与在高温下使用厚箔的大量实验的比较，检验了我们方法的准确性。我们的实验也证明了这些膜抵抗硫化氢中毒的能力。
Metal membranes play a vital rote in hydrogen purification. Defect-free membranes can exhibit effectively infinite selectivity but must also provide high fluxes, resistance to poisoning, long operational lifetimes, and low cost. Alloying offers one route to improve on membranes based on pure metals such as palladium. We show how ab initio calculations and coarse-grained modeling can accurately predict hydrogen fluxes through binary alloy membranes as functions of alloy composition, temperature, and pressure. Our approach, which requires no experimental input apart from knowledge of bulk crystal structures, is demonstrated for palladium-copper alloys, which show nontrivial behavior due to the existence of face-centered cubic and body-centered cubic crystal structures and have the potential to resist sulfur poisoning. The accuracy of our approach is examined by a comparison with extensive experiments using thick foils at elevated temperatures. Our experiments also demonstrate the ability of these membranes to resist poisoning by hydrogen sulfide.