PALLADIUM/COPPER ALLOY COMPOSITE MEMBRANES FOR HIGH TEMPERATURE HYDROGEN SEPARATION FROM COAL-DERIVED GAS STREAMS

Way, J. Douglas

Colorado School of Mines (United States)

关键词: 08 Hydrogen;    30 Direct Energy Conversion;    Alloys;    Hydrogen Embrittlement;    01 Coal, Lignite, And Peat;   

DOI  :  10.2172/811445
RP-ID  :  NONE
RP-ID  :  FG26-99FT40585
RP-ID  :  811445

美国|英语

来源: UNT Digital Library

【 摘 要 】

For hydrogen from coal gasification to be used economically, processing approaches that produce a high purity gas must be developed. Palladium and its alloys, nickel, platinum and the metals in Groups 3 to 5 of the Periodic Table are all permeable to hydrogen. Hydrogen permeable metal membranes made of palladium and its alloys are the most widely studied due to their high hydrogen permeability, chemical compatibility with many hydrocarbon containing gas streams, and infinite hydrogen selectivity. Our Pd composite membranes have demonstrated stable operation at 450 C for over 70 days. Coal derived synthesis gas will contain up to 15000 ppm H{sub 2}S as well as CO, CO{sub 2}, N{sub 2} and other gases. Highly selectivity membranes are necessary to reduce the H{sub 2}S concentration to acceptable levels for solid oxide and other fuel cell systems. Pure Pd-membranes are poisoned by sulfur, and suffer from mechanical problems caused by thermal cycling and hydrogen embrittlement. Recent advances have shown that Pd-Cu composite membranes are not susceptible to the mechanical, embrittlement, and poisoning problems that have prevented widespread industrial use of Pd for high temperature H{sub 2} separation. These membranes consist of a thin ({le} 5 {micro}m) film of metal deposited on the inner surface of a porous metal or ceramic tube. With support from this DOE Grant, we have fabricated thin, high flux Pd-Cu alloy composite membranes using a sequential electroless plating approach. Thin, Pd{sub 60}Cu{sub 40} films exhibit a hydrogen flux more than ten times larger than commercial polymer membranes for H{sub 2} separation, resist poisoning by H{sub 2}S and other sulfur compounds typical of coal gas, and exceed the DOE Fossil Energy target hydrogen flux of 80 ml/cm{sup 2} {center_dot} min = 0.6 mol/m{sup 2} {center_dot} s for a feed pressure of 40 psig. Similar Pd-membranes have been operated at temperatures as high as 750 C. We have developed practical electroless plating procedures for fabrication of thin Pd-Cu composite membranes at any scale.