32a Defect-Free Composite Pd Membranes with High Temperature Long-Term Stability

M. Engin Ayturk, Dept. of Chemical Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA 01609 and Yi Hua Ma, Worcester Polytechnique Institute, Chemical Enginering, Worcester, MA 01609.

The membrane selectivity is among the key determinants that affect the overall H2 separation efficiency and the long-term stability of the composite Pd and Pd/alloy membranes. To mitigate high temperature leak growth and to improve the long-term stability of the membrane selectivity, a novel synthesis procedure was implemented during the preparation of the composite Pd membrane supported on a media-grade 0.1 µm Inconel support, which was oxidized at 800°C for 12 hours to generate the intermetallic diffusion barrier. The successful synthesis of the 7.6 µm thick pure-Pd/Inconel membrane with a special emphasis on the formation of leak resistant deposition layers and saturated (stable) grain boundaries, led to an excellent long-term stability at 450°C with essentially infinite H2/He ideal selectivity. At 450°C and at a ΔP of 35 psi (PHigh=50 psia & PLow=15 psia), the He leak of the membrane was undetectable and the membrane maintained an excellent H2/He selectivity stability over a period of ~845 hours with numerous H2/He cyclings. Upon the completion of the long-term H2 permeation characterization (~1250 hours within 300-450°C), the high pressure testing of the 7.6 µm Pd /Inconel membrane was conducted at a feed side pressure as high as 116 psia (7.9 bara). At 400°C and a ΔP of 101 psi (PHigh=116 psia & PLow=15 psia), the stable H2 flux for the 7.6 µm Pd/Inconel membrane was as high as 150 scfh/ft2, exceeding the 2007 DOE target under similar operating conditions. Furthermore, the He leak after the high-pressure testing remained undetectable. The long-term selectivity stability is a significant achievement towards the successful utilization of Pd- and/or Pd/alloy-based catalytic membrane reactors for the production of high-purity H2 suitable for fuel cell applications in industrial steam reformers and/or high temperature water-gas shift reactors integrated into the downstream of the industrial coal gasification units.