PdAgAu alloy with high resistance to corrosion by H2S

被引:45
|
作者
Braun, Fernando [1 ]
Miller, James B. [2 ,3 ]
Gellman, Andrew J. [2 ,3 ]
Tarditi, Ana M. [1 ]
Fleutot, Benoit [2 ]
Kondratyuk, Petro [2 ,3 ]
Cornaglia, Laura M. [1 ]
机构
[1] Inst Invest Catalisis & Petroquim FIQ UNL CONICET, RA-3000 Santa Fe, Argentina
[2] Carnegie Mellon Univ, Dept Chem Engn, Pittsburgh, PA 15213 USA
[3] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA
基金
美国国家科学基金会;
关键词
PdAgAu alloy; Sulfur tolerance; Ternary alloy; Hydrogen separation membrane; SURFACE SEGREGATION; HYDROGEN TRANSPORT; MEMBRANE REACTORS; PD; PERFORMANCE; ENERGY; DIFFRACTION; PERMEATION; PREDICTION; PHASE;
D O I
10.1016/j.ijhydene.2012.09.040
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
PdAgAu alloy films were prepared on porous stainless steel supports by sequential electroless deposition. Two specific compositions, Pd83Ag2Au15 and Pd74Ag14Au12, were studied for their sulfur tolerance. The alloys and a reference Pd foil were exposed to 1000H(2)S/H-2 at 623 K for periods of 3 and 30 h. The microstructure, morphology and bulk composition of both non-exposed and H2S-exposed samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS). XRD and SEM analysis revealed time-dependent growth of a bulk Pd4S phase on the Pd foil during H2S exposure. In contrast, the PdAgAu ternary alloys displayed the same FCC structure before and after H2S exposure. In agreement with the XRD and SEM results, sulfur was not detected in the bulk of either ternary alloy samples by EDS, even after 30 h of H2S exposure. X-ray photoelectron spectroscopy (XPS) depth profiles were acquired for both PdAgAu alloys after 3 and 30 h of exposure to characterize sulfur contamination near their surfaces. Very low S 2p and S 2s XPS signals were observed at the top-surfaces of the PdAgAu alloys, and those signals disappeared before the etch depth reached similar to 10 nm, even for samples exposed to H2S for 30 h. The depth profile analyses also revealed silver and gold segregation to the surface of the alloys; preferential location of Au on the alloys surface may be related to their resistance to bulk sulfide formation. In preliminary tests, a PdAgAu alloy membrane displayed higher initial H-2 permeability than a similarly prepared pure Pd sample and, consistent with resistance to bulk sulfide formation, lower permeability loss in H2S than pure Pd. Copyright (c) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:18547 / 18555
页数:9
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