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  Methanol steam reforming catalysts derived by reduction of perovskite-type oxides LaCo1-x-yPdxZnyO3 +/-delta

Kuc, J., Neumann, M., Armbrüster, M., Yoon, S., Zhang, Y., Erni, R., et al. (2016). Methanol steam reforming catalysts derived by reduction of perovskite-type oxides LaCo1-x-yPdxZnyO3 +/-delta. Catalysis Science & Technology, 6(5), 1455-1468. doi:10.1039/c5cy01410g.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002A-3145-D Version Permalink: http://hdl.handle.net/21.11116/0000-0001-2646-6
Genre: Journal Article

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 Creators:
Kuc, Jagoda1, Author
Neumann, Matthias2, Author              
Armbrüster, Marc1, Author
Yoon, Songhak1, Author
Zhang, Yucheng1, Author
Erni, Rolf1, Author
Weidenkaff, Anke1, Author
Matam, Santhosh Kumar1, Author
Affiliations:
1External Organizations, ou_persistent22              
2Chemical Metal Science, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863405              

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 Abstract: Methanol steam reforming (MSR) catalysts are derived from perovskite-type oxides LaCo1-x-yPdxZnyO3 +/-delta by reductive pretreatment. The unsubstituted LaCoO3 +/-delta (LCO) and LaCo1-x-yPdxZnyO3 +/-delta (Co substituted with Pd and/or Zn) are synthesized by a citrate method and characterized by different techniques. The perovskite-type oxides exhibit a rhombohedral crystal structure and a comparable surface area (approximate to 8.5 (+/- 2) m(2) g(-1)). The temperature-programmed reduction (TPR) shows low (100 degrees C < T < 450 degrees C) and high (T > 450 degrees C) temperature reduction events that correspond to partial and complete reduction of the non-rareearth metal ions, respectively. At high temperatures, Pd-Zn alloy nanoparticles are formed exclusively on Pd-and Zn-containing LaCo1-x-yPdxZnyO3 +/-delta, as evident from high angular annular dark-field scanning transmission electron microscopy (HAADF-STEM). The CO2-selective MSR performance of the catalysts strongly depends on the reductive pretreatment temperature, catalyst composition (i.e., the Pd : Zn molar ratio and the degree of Co substitution) and reaction temperature. Only LaCo1-x-yPdxZnyO3 +/-delta catalysts show a low-temperature CO2 selectivity maximum between 225 and 250 degrees C, while all catalysts present similar high-temperature selectivity maxima at T > 400 degrees C. The former is missing on LCO, LaCo1-xPdxO3 +/-delta or LaCo1-yZnyO3 +/-delta. Pd-Zn nanoparticles facilitate Zn(OH)(2) and Co(OH)(2) formation exclusively on LaCo1-x-yPdxZnyO3 +/-delta, as evident from in situ XRD under steam atmosphere. This indicates the important role of Pd-Zn nanoparticles in the low-temperature CO2 selectivity, which is improved from 0 to 76% at 225 degrees C on LCO and LaCo0.75Pd0.125Zn0.125O3 +/-delta, respectively. The high-temperature CO2 selectivity is governed by the bulk catalyst composition and the occurrence of reverse water gas shift reaction.

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Language(s): eng - English
 Dates: 2016-02-252016-02-25
 Publication Status: Published in print
 Pages: -
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 Table of Contents: -
 Rev. Method: -
 Identifiers: ISI: 000371607600021
DOI: 10.1039/c5cy01410g
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Title: Catalysis Science & Technology
  Other : Catal. Sci. Technol.
Source Genre: Journal
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Publ. Info: Cambridge : Royal Society of Chemistry
Pages: - Volume / Issue: 6 (5) Sequence Number: - Start / End Page: 1455 - 1468 Identifier: Other: 2044-4753
CoNE: /journals/resource/2044-4753