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Title: Role of metal components in Pd?Cu bimetallic catalysts supported on CeO2 for the oxygen-enhanced water gas shift

Journal Article · · Applied Catalysis. B, Environmental
; ; ;  [1]
  1. Chemical Sciences and Engineering Division

Catalytic hydrogen production and CO removal in a post-reforming process are critical for low-temperature fuel cell applications. The present study aims at clarifying the role of metal components in bimetallic catalysts for oxygen-enhanced water gas shift (OWGS), wherein a small amount of O{sub 2} is added to H{sub 2}-rich reformate gas to enhance CO shift. Among CeO{sub 2}-supported bimetallic catalysts, Pd-Cu and Pt-Cu combinations were found to show strong synergetic promoting effect in OWGS, which leads to much higher CO conversion and higher H{sub 2} yield than WGS at low temperature around 250 C. Temperature programmed reduction (TPR) showed strong interaction between Pd and Cu in Pd-Cu/CeO{sub 2} by a single reduction peak in contrast to multiple peaks on monometallic Cu/CeO{sub 2}. Extended X-ray absorption fine structure (EXAFS) analysis revealed that such bimetallic Pd-Cu and Pt-Cu form alloy nanoparticles, where noble metal is mainly surrounded by Cu atoms. Oxygen storage capacity (OSC) measurements point to higher resistance of Pd-Cu to oxidation indicating that Pd keeps Cu in reduced state in air pulse condition. From kinetic study, Pd in Pd-Cu was found to promote CO shift, rather than CO oxidation by increasing the number of active sites and by suppressing H{sub 2} activation (that is inherent to monometallic Pd), which minimizes both the inhibition effect of H{sub 2} and the loss of H{sub 2} by oxidation in OWGS. Transient response technique revealed that Cu in Pd-Cu enhances desorption of strongly chemisorbed CO{sub 2} on catalyst surface in contrast to very slow CO{sub 2} desorption from surface of monometallic Pd. Thus, the excellent OWGS activity of Pd-Cu catalyst has been attributed to the complementary roles of the two metals for enhancing CO shift, which is realized by its alloy structure and the accompanying strong interaction between metal components.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC); ONR; Penn State Univ.
DOE Contract Number:
DE-AC02-06CH11357
OSTI ID:
1047441
Report Number(s):
ANL/CSE/JA-67258; ACBEE3; TRN: US201216%%289
Journal Information:
Applied Catalysis. B, Environmental, Vol. 105, Issue 3-4; ISSN 0926-3373
Country of Publication:
United States
Language:
ENGLISH