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Title: Sulfur Tolerant Pd/Cu and Pd/Au Alloy Membranes for H2 Separation with High Pressure CO2 for Sequestration

Abstract

The effect of H{sub 2}S poisoning on Pd, Pd/Cu, and Pd/Au alloy composite membranes prepared by the electroless deposition method on porous Inconel supports was investigated to provide a fundamental understanding of the durability and preparation of sulfur tolerant membranes. X-ray photoelectron spectroscopy (XPS) studies showed that the exposure of pure Pd to 50 ppm H{sub 2}S/H{sub 2} mixtures caused bulk sulfide formation at lower temperatures and surface sulfide formation at higher temperatures. Lower temperatures, longer exposure times, and higher H{sub 2}S concentrations resulted in a higher degree of sulfidation. In a Pd membrane, the bulk sulfide formation caused a drastic irrecoverable H{sub 2} permeance decline and an irreparable loss in selectivity. Pd/Cu and Pd/Au alloy membranes exhibited permeance declines due to surface sulfide formation upon exposure to 50 ppm H{sub 2}S/H{sub 2} gas mixtures. However in contrast to the pure Pd membrane, the permeances of the Pd/Cu and Pd/Au alloy membranes were mostly recovered in pure H{sub 2} and the selectivity of the Pd alloy layers remained essentially intact throughout the characterization in H{sub 2}, He and H{sub 2}S/H{sub 2} mixtures which lasted several thousand hours. The amount of irreversible sulfur poisoning decreased with increasing temperature due to themore » exothermicity of H{sub 2}S adsorption. Longer exposure times increased the amount of irreversible poisoning of the Pd/Cu membrane but not the Pd/Au membrane. Pd/Au coupon studies of the galvanic displacement method showed that higher Au{sup 3+} concentrations, lower pH values, higher bath temperatures and stirring the bath at a rate of 200 rpm yielded faster displacement rates, more uniform depositions, and a higher Au content within the layers. While 400 C was found to be sufficient to form a Pd/Au alloy on the surface, high temperature X-ray diffraction (HTXRD) studies showed that even after annealing between 500-600 C, the Pd/Cu alloys could have part or all of the surface in the less sulfur resistant {beta} phase.« less

Authors:
; ;
Publication Date:
Research Org.:
Worcester Polytechnic Institute, MA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
952460
DOE Contract Number:  
FG26-04NT42194
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 54 ENVIRONMENTAL SCIENCES; MEMBRANES; PALLADIUM ALLOYS; COPPER ALLOYS; GOLD ALLOYS; HYDROGEN; SEPARATION PROCESSES; CARBON DIOXIDE; CARBON SEQUESTRATION; HYDROGEN SULFIDES; POISONING; FOULING; PERMEABILITY; SULFIDES; DEPOSITION

Citation Formats

Ma, Yi Hua, Pomerantz, Natalie, and Chen, Chao-Huang. Sulfur Tolerant Pd/Cu and Pd/Au Alloy Membranes for H2 Separation with High Pressure CO2 for Sequestration. United States: N. p., 2008. Web. doi:10.2172/952460.
Ma, Yi Hua, Pomerantz, Natalie, & Chen, Chao-Huang. Sulfur Tolerant Pd/Cu and Pd/Au Alloy Membranes for H2 Separation with High Pressure CO2 for Sequestration. United States. https://doi.org/10.2172/952460
Ma, Yi Hua, Pomerantz, Natalie, and Chen, Chao-Huang. 2008. "Sulfur Tolerant Pd/Cu and Pd/Au Alloy Membranes for H2 Separation with High Pressure CO2 for Sequestration". United States. https://doi.org/10.2172/952460. https://www.osti.gov/servlets/purl/952460.
@article{osti_952460,
title = {Sulfur Tolerant Pd/Cu and Pd/Au Alloy Membranes for H2 Separation with High Pressure CO2 for Sequestration},
author = {Ma, Yi Hua and Pomerantz, Natalie and Chen, Chao-Huang},
abstractNote = {The effect of H{sub 2}S poisoning on Pd, Pd/Cu, and Pd/Au alloy composite membranes prepared by the electroless deposition method on porous Inconel supports was investigated to provide a fundamental understanding of the durability and preparation of sulfur tolerant membranes. X-ray photoelectron spectroscopy (XPS) studies showed that the exposure of pure Pd to 50 ppm H{sub 2}S/H{sub 2} mixtures caused bulk sulfide formation at lower temperatures and surface sulfide formation at higher temperatures. Lower temperatures, longer exposure times, and higher H{sub 2}S concentrations resulted in a higher degree of sulfidation. In a Pd membrane, the bulk sulfide formation caused a drastic irrecoverable H{sub 2} permeance decline and an irreparable loss in selectivity. Pd/Cu and Pd/Au alloy membranes exhibited permeance declines due to surface sulfide formation upon exposure to 50 ppm H{sub 2}S/H{sub 2} gas mixtures. However in contrast to the pure Pd membrane, the permeances of the Pd/Cu and Pd/Au alloy membranes were mostly recovered in pure H{sub 2} and the selectivity of the Pd alloy layers remained essentially intact throughout the characterization in H{sub 2}, He and H{sub 2}S/H{sub 2} mixtures which lasted several thousand hours. The amount of irreversible sulfur poisoning decreased with increasing temperature due to the exothermicity of H{sub 2}S adsorption. Longer exposure times increased the amount of irreversible poisoning of the Pd/Cu membrane but not the Pd/Au membrane. Pd/Au coupon studies of the galvanic displacement method showed that higher Au{sup 3+} concentrations, lower pH values, higher bath temperatures and stirring the bath at a rate of 200 rpm yielded faster displacement rates, more uniform depositions, and a higher Au content within the layers. While 400 C was found to be sufficient to form a Pd/Au alloy on the surface, high temperature X-ray diffraction (HTXRD) studies showed that even after annealing between 500-600 C, the Pd/Cu alloys could have part or all of the surface in the less sulfur resistant {beta} phase.},
doi = {10.2172/952460},
url = {https://www.osti.gov/biblio/952460}, journal = {},
number = ,
volume = ,
place = {United States},
year = {Tue Sep 30 00:00:00 EDT 2008},
month = {Tue Sep 30 00:00:00 EDT 2008}
}