Surface activation inspires high performance of ultra-thin Pd membrane for hydrogen separation

Surface activation inspires high performance of ultra-thin Pd membrane for hydrogen separation
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表面活化激发超薄钯膜用于氢分离的高性能

DOI:
10.1016/j.memsci.2016.12.025
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发表时间:
2017-03
影响因子:
9.5
通讯作者:
Hui Li
Hui Li
中科院分区:
工程技术1区
文献类型:
--
作者:
Hengyong Xu;Dangsheng Su;Jian Zhang;Hui Li

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钯基膜在氢气提纯和小规模制氢领域起着关键作用。超薄Pd膜的微观结构和组成直接决定了其性能和稳定性,然而这是复杂和难以捉摸的。我们首次应用了一种新的技术,环境扫描电子显微镜(ESEM)与EDS分析的Pd复合膜下的气热处理的微观结构和组成的原位调查。它可以逐步分析演变过程,并通过在膜样品的完全相同位置进行分析,提供比非原位技术更细致的细节。在这里,我们观察到消除Pd微晶以及均匀化/扩散沿着整个膜表面以下的高T处理在惰性气体或H2气氛。由于α−β相变或暴露于O2或H2O中,Pd膜表面的微丘逐渐演化,H2处理可有效地“平滑”微丘。暴露于蒸汽中表现出温和的氧化作用,没有针孔形成,与空气/氧气处理相比,这似乎是一种更合适的表面清洁工艺。在H2/O2/H2O气氛中,Pd层与ZrO 2/Al 2 O3基体之间存在明显的层间扩散。
Pd-based membranes play a critical role in the field of hydrogen purification and small-scale hydrogen generation. The microstructure and composition of ultra-thin Pd membranes immediately determines their performance and stability, which are however complex and elusive. We applied for the first time a novel technique of environmental scanning electron microscopy (ESEM) together with EDS analysis for in-situ investigation of microstructure and composition of Pd composite membranes under gas-thermal treatment. It enables step by step analysis of the evolution process and offers more meticulous details compared to ex-situ technologies through analysis at exactly the same location of membrane samples. Here we observed the elimination of Pd crystallites as well as the homogenization/diffusion along the whole membrane surface following high T treatment under inert gas or H2atmosphere. Gradual evolution of microhillocks on Pd membrane surface was resulted due to α−β phase transition or exposure to either O2or H2O, which can be effectively “smoothened” out during H2treatment. The exposure to steam exhibited a mild oxidation effect without pinhole formations, which appears a more appropriate surface cleaning process compared to air/oxygen treatment. A significant interlayer diffusion was revealed between Pd layer and ZrO2/alumina substrate in H2/O2/H2O atmosphere.
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