Journal of the Korean institute of surface engineering (한국표면공학회지)

The Korean Institute of Surface Engineering (한국표면공학회)
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Hydrogen Perm-Selectivity Properties of the Pd-Ni-Ag Alloy Hydrogen Separation Membranes with Various Surface Nickel Composition

표면 니켈 조성에 따른 팔라듐-니켈-은 합금 수소분리막의 수소투과선택 특성

  • Lim, Da-Sol (Department of Advanced Materials Engineering, Kyonggi University) ;
  • Kim, Se-Hong (Department of Advanced Materials Engineering, Kyonggi University) ;
  • Kim, Do-Hui (Department of Advanced Materials Engineering, Kyonggi University) ;
  • Cho, Seo-Hyun (Industry-Academia Collaboration Foundation, Kyonggi University) ;
  • Kim, Dong-Won (Department of Advanced Materials Engineering, Kyonggi University)
  • 임다솔 (경기대학교 신소재공학과) ;
  • 김세홍 (경기대학교 신소재공학과) ;
  • 김도희 (경기대학교 신소재공학과) ;
  • 조서현 (경기대학교 산학협력단) ;
  • 김동원 (경기대학교 신소재공학과)
  • Received : 2018.08.10
  • Accepted : 2018.10.02
  • Published : 2018.10.31
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Abstract

In this study, Pd-Ni-Ag alloy hydrogen separation membranes were fabricated by Pd/Ag/Pd/Ni/Pd multi-layer sputter deposition on the modified MIM(Metal Injection Molding)-PSS(Porous Stainless Steel) support and followed heat treatment. Nickel, used as an alloying element in Pd alloy membranes, is inexpensive and stable material in a hydrogen isotope environment at high temperature up to 1123 K. Hydrogen perm-selectivity of Pd-Ni-Ag alloy membranes is affected not only by composition of membrane films but also by other factors such as surface properties of PSS support, microstructure of membrane films and inter-diffused impurities from PSS support. In order to clarify the effect of surface Ni composition on hydrogen perm-selectivity of Pd-Ni-Ag alloy membranes, the other effects were significantly minimized by the formation of dense and homogeneous Pd-Ni-Ag alloy membranes. Hydrogen permeation test showed that hydrogen permeability decreased from $7.6{\times}10^{-09}$ to $1.02{\times}10^{-09}mol/m{\cdot}s{\cdot}Pa^{0.5}$ as Ni composition increased from 0 to 16 wt% and the selectivity for $H_2/N_2$ was infinite.

Keywords

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Fig. 1. Schematic diagram of experiment processes for Pd-Ni-Ag alloy hydrogen separation membrane.

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Fig. 2. FE-SEM images, CLSM images and apparent porosity of porous stainless steel supports : (a) HP PSS (b) MIM PSS.

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Fig. 3. FE-SEM images and CLSM images of porous stainless steel supports after surface treatment : (a) HP PSS (b) MIM PSS.

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Fig. 4. FE-SEM images of sputtered Pd films on the modified MIM PSS at various working pressure and DC power.

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Fig. 5. FE-SEM images of sputtered Pd, Ag and Ni films on the modified MIM PSS : (a) Pd, (b) Ag, (c) Ni.

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Fig. 6. FE-SEM images, XRD patterns and EDS profiles of Pd-Ni-Ag hydrogen separation membrane : (a) sputter as-deposition, (b) after heat treatment.

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Fig. 7. Schematic illustration of Pd/Ag sputter multi-deposition diffusion barrier for preventing intermetallic diffusion in PSS : (a) FE-SEM images of Pd alloy films with dense and homogeneous microstructure, (b) Fe-Ag phase diagram, (c) Fe-Pd phase diagram, (d) cross-sectional EDS composition line scan profiles.

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Fig. 8. FE-SEM images and surface composition of Pd alloy as a function of thickness ratio between Pd and Ni films after heat treatment for 1h at 923 K : (a) Pd/Ni layer on Si wafer, (b) Pd/Ni/Pd/Ag/Pd layer on modified MIM PSS.

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Fig. 9. Hydrogen perm-selectivity of Pd-Ni-Ag alloy hydrogen separation membranes as a function of surface Ni composition at various pressure difference.

Table 1. Comparison of different Pd-based membranes.

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