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Title: Nanoporous, Metal Carbide, Surface Diffusion Membranes for High Temperature Hydrogen Separations

Technical Report ·
DOI:https://doi.org/10.2172/1121750· OSTI ID:1121750
 [1];  [2]
  1. Colorado School of Mines, Golden, CO (United States). Dept. of Chemical and Biological Engineering
  2. Colorado School of Mines, Golden, CO (United States)

Colorado School of Mines (CSM) developed high temperature, hydrogen permeable membranes that contain no platinum group metals with the goal of separating hydrogen from gas mixtures representative of gasification of carbon feedstocks such as coal or biomass in order to meet DOE NETL 2015 hydrogen membrane performance targets. We employed a dual synthesis strategy centered on transition metal carbides. In the first approach, novel, high temperature, surface diffusion membranes based on nanoporous Mo2C were fabricated on ceramic supports. These were produced in a two step process that consisted of molybdenum oxide deposition followed by thermal carburization. Our best Mo2C surface diffusion membrane achieved a pure hydrogen flux of 367 SCFH/ft2 at a feed pressure of only 20 psig. The highest H2/N2 selectivity obtained with this approach was 4.9. A transport model using “dusty gas” theory was derived to describe the hydrogen transport in the Mo2C coated, surface diffusion membranes. The second class of membranes developed were dense metal foils of BCC metals such as vanadium coated with thin (< 60 nm) Mo2C catalyst layers. We have fabricated a Mo2C/V composite membrane that in pure gas testing delivered a H2 flux of 238 SCFH/ft2 at 600 °C and 100 psig, with no detectable He permeance. This exceeds the 2010 DOE Target flux. This flux is 2.8 times that of pure Pd at the same membrane thickness and test conditions and over 79% of the 2015 flux target. In mixed gas testing we achieved a permeate purity of ≥99.99%, satisfying the permeate purity milestone, but the hydrogen permeance was low, ~0.2 SCFH/ft2.psi. However, during testing of a Mo2C coated Pd alloy membrane with DOE 1 feed gas mixture a hydrogen permeance of >2 SCFH/ft2.psi was obtained which was stable during the entire test, meeting the permeance associated with the 2010 DOE target flux. Lastly, the Mo2C/V composite membranes were shown to be stable for at least 168 hours = one week, including cycling at high temperature and alternating He/H2 exposure.

Research Organization:
Trustees of the Colorado School of Mines, Golden, CO (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
FE0001009
OSTI ID:
1121750
Country of Publication:
United States
Language:
English