Tuesday, April 1, 2008 - 2:40 PM

Status of Hydrogen Separation Membrane Development

U. (Balu) Balachandran, Tae H. Lee, Ling Chen, and Stephen E. Dorris. Argonne National Laboratory

The Office of Fossil Energy (FE) at the U.S. Department of Energy (DOE) sponsors a wide range of research, development, and demonstration programs to maximize the use of vast domestic fossil resources and to ensure a fuel-diverse energy sector while responding to global environmental concerns.  Cost-effective, membrane-based reactor and separation technologies are of considerable interest to DOE’s FE program to develop advanced technologies for hydrogen production from fossil resources.  Supported by DOE’s FE, Argonne National Laboratory is developing dense cermet (i.e., ceramic-metal composite) hydrogen transport membranes (HTMs) for separating hydrogen from mixed gases, particularly product streams generated during coal gasification and/or methane reforming.  Hydrogen separation with these membranes is nongalvanic (i.e., it does not use electrodes or an external power supply to drive the separation) and requires no additional post-separation purification steps because the hydrogen separated from the feed stream is of high purity.

Cermet membranes were prepared by conventional ceramic processing and fabrication techniques.  Using several feed gas mixtures, we measured the nongalvanic hydrogen permeation rate, or flux, for the cermet membranes in the temperature range of 500-900°C. This rate varied linearly with the inverse of membrane thickness and reached ≈33 cm3[STP]/min-cm2 at 900°C for an ≈15-micron-thick membrane on a porous support structure when 100% H2 at ambient pressure was used as the feed gas. Good chemical stability is a critical requirement for membranes separating hydrogen from the product streams of coal gasification and/or methane reforming.  When cermet membranes were tested in a gas mixture that contained high concentrations of CH4, CO, and CO2 for times that approached ≈500 h, performance did not degrade.  Because HTMs will encounter H2S, we also tested the cermet membranes in gas mixtures containing H2, CH4, CO2, CO, and H2S.  Hydrogen flux measurements showed that  the cermet membranes are stable at 900°C for up to 1200 h in gases that contain 400 ppm H2S.  The cermet membranes are found to be stable in the temperature range of 500 - 800°C in simulated synthesis gas mixtures containing ≈21% steam. To be practical, HTMs must have good mechanical integrity at high temperature (≈900°C) and high pressure (>300 psig).  We have recently constructed a reactor that allows the hydrogen flux of membranes to be measured at temperatures up to 900°C and pressures up to 300 psig. The present status of membrane development at Argonne and the challenges involved in bringing this technology to fruition will be presented in this talk.

Work supported by the U.S. Department of Energy, Office of Fossil Energy, National Energy Technology Laboratory’s Hydrogen and Syngas Technology Program, under Contract DE-AC02-06CH11357.