High Permeability Ternary Palladium Alloy Membranes with Improved Sulfur and Halide Tolerances

摘要

The project team consisting of Southwest Research Institute(reg sign) (SwRI(reg sign)), Georgia Institute of Technology (GT), the Colorado School of Mines (CSM), TDA Research, and IdaTech LLC was focused on developing a robust, poison-tolerant, hydrogen selective free standing membrane to produce clean hydrogen. The project completed on schedule and on budget with SwRI, GT, CSM, TDA and IdaTech all operating independently and concurrently. GT has developed a robust platform for performing extensive DFT calculations for H in bulk palladium (Pd), binary alloys, and ternary alloys of Pd. Binary alloys investigated included Pd96M4 where M = Li, Na, Mg, Al, Si, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Ga, Y, Zr, Nb, Mo, Tc, Ru, Rh, Ag, Cd, In, Sn, Sb, Te, Hf, Ta, W, Re, Os, Ir, Pt, Au, Tl, Pb, Bi, Ce, Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu. SwRI deposited and released over 160 foils of binary and ternary Pd alloys. There was considerable work on characterizing and improving the durability of the deposited foils using new alloy compositions, post annealing and ion bombardment. The 10 and 25 (micro)m thick films were sent to CSM, TDA and IdaTech for characterization and permeation testing. CSM conducted over 60 pure gas permeation tests with SwRI binary and ternary alloy membranes. To date the PdAu and PdAuPt membranes have exhibited the best performance at temperatures in the range of 423-773 C and their performance correlates well with the predictions from GT. TDA completed testing under the Department of Energy (DOE) WGS conditions on over 16 membranes. Of particular interest are the PdAuPt alloys that exhibited only a 20% drop in flux when sulfur was added to the gas mixture and the flux was completely recovered when the sulfur flow was stopped. IdaTech tested binary and ternary membranes on a simulated flue gas stream and experienced significant difficulty in mounting and testing the sputter deposited membranes. IdaTech was able to successfully test PdAu and PdAuPt membranes and saw similar sulfur tolerance to what TDA found. The Program met all the deliverables on schedule and on budget. Over ten presentations at national and international conferences were made, four papers were published (two in progress) in technical journals, and three students (2 at GT and 1 at CSM) completed their doctorates using results generated during the course of the program.