PdCuAu ternary alloy membranes. Hydrogen permeation properties in the presence of H2S

Tarditi, Ana M.; Imhoff, Carolina; Braun, Fernando; Miller, James B.; Gellman, Andrew J.; Cornaglia, Laura

doi:10.1016/j.memsci.2014.12.030

Title: PdCuAu ternary alloy membranes. Hydrogen permeation properties in the presence of H₂S

Journal Article · Tue Dec 30 00:00:00 EST 2014 · Journal of Membrane Science

DOI:https://doi.org/10.1016/j.memsci.2014.12.030· OSTI ID:1225783

Tarditi, Ana M. ^[1]; Imhoff, Carolina ^[1]; Braun, Fernando ^[1]; Miller, James B. ^[2]; Gellman, Andrew J. ^[2]; Cornaglia, Laura ^[1]

Instituto de Investigaciones en Catalisis y Petroquimica (FIQ, UL-CONICET), Santa Fe (Argentina)
Carnegie Mellon Univ., Pittsburgh, PA (United States); National Energy Technology Lab. (NETL), Pittsburgh, PA (United States)

PdCuAu ternary alloy membranes with different component compositions were synthesized by sequential electroless deposition of components onto porous stainless steel substrates. The ternary with the highest Au content, Pd₆₉Cu₁₄Au₁₇, exhibited the highest hydrogen permeation flux, comparable to that of a Pd₉₁Au₉ membrane. Upon exposure to 100 ppm H₂S/H₂ at 673 K for 24 h, all PdCuAu membranes experienced flux reductions of ~55%, followed by recovery to ~80% of the initial hydrogen flux upon reintroduction of pure hydrogen at 400 °C. Complete flux recovery after H₂S exposure required hydrogen treatment at 500 °C. X-ray diffraction (XRD) analysis of the H₂S-exposed PdCuAu membranes revealed fcc alloy structure with no evidence of bulk sulfide formation. In agreement with the XRD results, sulfur was not detected in the bulk of H₂S-exposed samples by energy dispersive spectroscopy (EDS). However, analysis of H₂S-exposed PdCuAu alloys by X-ray photoelectron spectroscopy (XPS) depth profiling revealed low, but measureable, amounts of sulfur in the near-surface region, about 10 nm in depth. The depth profiles of samples after hydrogen recovery treatment showed significantly reduced sulfur content. Furthermore, these results indicate that H₂S exposure causes flux loss in PdCuAu alloys through a surface-poisoning mechanism, and that the surface sulfide can be removed—and flux recovered—by high temperature treatment in hydrogen.

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Research Organization:: National Energy Technology Lab. (NETL), Albany, OR (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: CBET1033804

OSTI ID:: 1225783

Report Number(s):: A-UNIV-PUB-136

Journal Information:: Journal of Membrane Science, Vol. 479, Issue C; ISSN 0376-7388

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

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