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

Coulter, K.

Southwest Research Institute Incorporated

关键词: Magnetrons;    Tolerance;    Alloys;    Halides;    08 Hydrogen;   

DOI  :  10.2172/1013344
RP-ID  :  FC26-07NT43056
RP-ID  :  1013344

美国|英语

来源: UNT Digital Library

【 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. They have also performed a series of calculations on Pd{sub 70}Cu{sub 26}Ag{sub 4}, Pd{sub 70}Cu{sub 26}Au{sub 4}, Pd{sub 70}Cu{sub 26}Ni{sub 4}, Pd{sub 70}Cu{sub 26}Pt{sub 4}, and Pd{sub 70}Cu{sub 26}Y{sub 4}. 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. The three major findings of program were; (1) the DFT modeling was verified as a predictive tool for the permeability of Pd based ternary alloys, (2) while magnetron sputtering is useful in precisely fabricating binary and ternary alloys, the mechanical durability of membranes fabricated using this technique are inferior compared to cold rolled membranes and this preparation method is currently not ready for industrial environments, (3) based on both modeling and experimental verification in pure gas and mixed gas environments PdAu and PdAuPt alloys were found to have the combination of the highest permeability and tolerance to sulfur.