Palladium/Copper Alloy Composite Membranes for High Temperature Hydrogen Separation

Abstract

This report summarizes progress made during the a three year University Coal Research grant (DEFG26-03NT41792) at the Colorado School of Mines. The period of performance was September 1, 2003 through August of 2006. We made excellent progress toward our goal of contributing to the development of high productivity, sulfur tolerant composite metal membranes for hydrogen production and membrane reactors. Composite Pd and Pd alloy metal membranes with thin metal films (1-7 {micro}m) were prepared on porous stainless steel and ceramic supports that meet or exceed the DOE 2010 and 2015 pure hydrogen flux targets at differential pressure of only 20 psi. For example, a 2 {micro}m pure Pd membrane on a Pall AccuSep{reg_sign} substrate achieved an ideal H{sub 2}/N{sub 2} separation factor of over 6000, with a pure hydrogen flux of 210 SCFH/ft{sup 2} at only 20 psig feed pressure. Similar performance was achieved with a Pd{sub 80}Au{sub 20} composite membrane on a similar stainless steel substrate. Extrapolating the pure hydrogen flux of this PdAu membrane to the DOE Fossil Energy target conditions of 150 psia feed pressure and 50 psia permeate pressure gives a value of 508 SCFH/ft{sup 2}, exceeding the 2015 target. At these thicknesses, it is the support cost that will dominate the cost of a large scale module. In a direct comparison of FCC phase PdCu and PdAu alloys on identical supports, we showed that a Pd{sub 85}Au{sub 15} (mass %) alloy membrane is not inhibited by CO, CO{sub 2}, or steam present in a water-gas shift feed mixture at 400 C, has better resistance to sulfur than a Pd{sub 94}Cu{sub 6} membrane, and has over twice the hydrogen permeance.