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钯复合膜表面缺陷修饰材料的研究

作者：徐天莹，俞佳枫，张继新，徐恒泳

单位：中科院大连化学物理研究所，大连，116023

关键词：金属钯复合膜；透氢性能；分子筛；氧化铝；缺陷

DOI号：

分类号： 0643

出版年,卷(期):页码： 2015,35(2):30-35

摘要：

利用钯膜分离氢是高纯或超纯氢气生产的主要方式，然而，钯膜表面缺陷是影响氢分离纯度的主要因素。本文选择NaA分子筛和γ-Al2O3两种缺陷填充材料对初镀后的钯膜表面缺陷进行修饰，发现两种材料修饰后钯膜透氮量分别下降了57和2倍，NaA分子筛材料修饰后钯膜的透氮量为未修饰钯膜的1/2500。经过补镀和活化后，在相同钯膜厚度（2.5µm）条件下，三种钯膜透氮量分别为1.91×10-2、6.12×10-3和4.89×10-3 m3/h·m2·bar[改成标准单位mPa]。不同修饰材料修饰的钯膜的氢氮分离因子顺序为NaA分子筛 > γ-Al2O3 > 无修饰，说明通过修饰钯膜缺陷的方法可提高钯膜的氢分离选择性，且用NaA分子筛材料要优于γ-Al2O3材料，因为NaA分子筛在缺陷中可根据缺陷形状原位生长，更能有效填补缺陷。NaA分子筛材料修饰后的钯膜经过20次300-400℃以及0.1-1.0MPa的温度和压力循环仍保持性能不变，具有较高的稳定性。

were used to modify the defects of palladium membrane. The performances of unmodified ultra-thin palladium membrane and those modified by NaA zeolite and γ-Al2O3 were investigated. The results showed that, the nitrogen permeations decreased 57 and 2 times after modified by NaA zeolite and γ-Al2O3, respectively. After second electroless plating and activation, the nitrogen permeations of palladium membrane with the same thickness modified by NaA zeolite was 1/2500 of the unmodified membrane. The nitrogen permeations of these three palladium membranes were 1.9108×10-2 , 6.115×10-3 and 4.892×10-3m3/h·m2·bar. The H2/N2 selectivity of palladium membranes followed the order of NaA zeolite-modified > γ-Al2O3-modified > unmodified. It was indicated that the performance of palladium membrane can be improved by modification. And the performances of palladium membrane modified by NaA zeolite were better than γ-Al2O3. In the stability tests of NaA zeolite modified palladium membrane, the purity of hydrogen remained stable during 20 cycles of temperature and pressure changes in the range of 300-400°C and 0.1-1.0 MPa.

基金项目：

国家自然科学基金，分子筛限域原位生长法制备超薄金属钯复合膜的研究，项目批准号：21306183.

作者简介：

徐天莹（1988-），女，黑龙江省哈尔滨人，硕士，从事钯膜制备及钯膜性能评价研究.

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