Influence of Cation Substitutions Based on ABO3 Perovskite Materials, Sr1-xYxTi1-yRuyO3-δ, on Ammonia Dehydrogenation

Hyunmi Doh, Hyo Young Kim, Ghun Sik Kim, Junyoung Cha, Hyun S. Park, Hyung Chul Ham, Sung Pil Yoon, Jonghee Han, SukWoo Nam, Kwang Ho Song, Chang Won Yoon

Research output: Contribution to journalArticle

7 Citations (Scopus)

Abstract

In order to screen potential catalytic materials for synthesis and decomposition of ammonia, a series of ABO3 perovskite materials, Sr1-xYxTi1-yRuyO3-δ (x = 0, 0.08, and 0.16; y = 0, 0.04, 0.07, 0.12, 0.17, and 0.26) were synthesized and tested for ammonia dehydrogenation. The influence of A or B site substitution on the catalytic ammonia dehydrogenation activity was determined by varying the quantity of either A or B site cation, producing Sr1-xYxTi0.92Ru0.08O3-δ and Sr0.92Y0.08Ti1-yRuyO3-δ, respectively. Characterizations of the as-synthesized materials using different analytical techniques indicated that a new perovskite phase of SrRuO3 was produced upon addition of large amounts of Ru (≥12 mol %), and the surface Ru0 species were formed simultaneously to ultimately yield Ruz(surface)/Sr0.92Y0.08Ti1-yRuy-zO3-δ and/or Ruz-w(surface)/SrwRuwO3/Sr0.92-wY0.08Ti1-yRuy-zO3-δ. The newly generated surface Ru0 species at the perovskite surfaces accelerated ammonia dehydrogenation under different conditions, and Sr0.84Y0.16Ti0.92Ru0.08O3-δ exhibited a NH3 conversion of ca. 96% at 500 °C with a gas hourly space velocity (GHSV) of 10 000 mL gcat -1 h-1. In addition, Sr0.84Y0.16Ti0.92Ru0.08O3-δ further proved to be highly active and stable toward ammonia decomposition at different reaction temperatures and GHSVs for >275 h.

Original languageEnglish
Pages (from-to)9370-9379
Number of pages10
JournalACS Sustainable Chemistry and Engineering
Volume5
Issue number10
DOIs
Publication statusPublished - 2017 Oct 2

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perovskite
Dehydrogenation
Ammonia
Perovskite
Cations
substitution
Substitution reactions
ammonia
cation
Positive ions
decomposition
Decomposition
analytical method
Thermodynamic properties
Gases
material
gas
temperature
Temperature

Keywords

  • Ammonia dehydrogenation
  • Ammonia synthesis
  • Hydrogen production
  • Perovskite
  • Ruthenium

ASJC Scopus subject areas

  • Chemistry(all)
  • Environmental Chemistry
  • Chemical Engineering(all)
  • Renewable Energy, Sustainability and the Environment

Cite this

Influence of Cation Substitutions Based on ABO3 Perovskite Materials, Sr1-xYxTi1-yRuyO3-δ, on Ammonia Dehydrogenation. / Doh, Hyunmi; Kim, Hyo Young; Kim, Ghun Sik; Cha, Junyoung; Park, Hyun S.; Ham, Hyung Chul; Yoon, Sung Pil; Han, Jonghee; Nam, SukWoo; Song, Kwang Ho; Yoon, Chang Won.

In: ACS Sustainable Chemistry and Engineering, Vol. 5, No. 10, 02.10.2017, p. 9370-9379.

Research output: Contribution to journalArticle

Doh, Hyunmi ; Kim, Hyo Young ; Kim, Ghun Sik ; Cha, Junyoung ; Park, Hyun S. ; Ham, Hyung Chul ; Yoon, Sung Pil ; Han, Jonghee ; Nam, SukWoo ; Song, Kwang Ho ; Yoon, Chang Won. / Influence of Cation Substitutions Based on ABO3 Perovskite Materials, Sr1-xYxTi1-yRuyO3-δ, on Ammonia Dehydrogenation. In: ACS Sustainable Chemistry and Engineering. 2017 ; Vol. 5, No. 10. pp. 9370-9379.
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abstract = "In order to screen potential catalytic materials for synthesis and decomposition of ammonia, a series of ABO3 perovskite materials, Sr1-xYxTi1-yRuyO3-δ (x = 0, 0.08, and 0.16; y = 0, 0.04, 0.07, 0.12, 0.17, and 0.26) were synthesized and tested for ammonia dehydrogenation. The influence of A or B site substitution on the catalytic ammonia dehydrogenation activity was determined by varying the quantity of either A or B site cation, producing Sr1-xYxTi0.92Ru0.08O3-δ and Sr0.92Y0.08Ti1-yRuyO3-δ, respectively. Characterizations of the as-synthesized materials using different analytical techniques indicated that a new perovskite phase of SrRuO3 was produced upon addition of large amounts of Ru (≥12 mol {\%}), and the surface Ru0 species were formed simultaneously to ultimately yield Ruz(surface)/Sr0.92Y0.08Ti1-yRuy-zO3-δ and/or Ruz-w(surface)/SrwRuwO3/Sr0.92-wY0.08Ti1-yRuy-zO3-δ. The newly generated surface Ru0 species at the perovskite surfaces accelerated ammonia dehydrogenation under different conditions, and Sr0.84Y0.16Ti0.92Ru0.08O3-δ exhibited a NH3 conversion of ca. 96{\%} at 500 °C with a gas hourly space velocity (GHSV) of 10 000 mL gcat -1 h-1. In addition, Sr0.84Y0.16Ti0.92Ru0.08O3-δ further proved to be highly active and stable toward ammonia decomposition at different reaction temperatures and GHSVs for >275 h.",
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AU - Kim, Hyo Young

AU - Kim, Ghun Sik

AU - Cha, Junyoung

AU - Park, Hyun S.

AU - Ham, Hyung Chul

AU - Yoon, Sung Pil

AU - Han, Jonghee

AU - Nam, SukWoo

AU - Song, Kwang Ho

AU - Yoon, Chang Won

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AB - In order to screen potential catalytic materials for synthesis and decomposition of ammonia, a series of ABO3 perovskite materials, Sr1-xYxTi1-yRuyO3-δ (x = 0, 0.08, and 0.16; y = 0, 0.04, 0.07, 0.12, 0.17, and 0.26) were synthesized and tested for ammonia dehydrogenation. The influence of A or B site substitution on the catalytic ammonia dehydrogenation activity was determined by varying the quantity of either A or B site cation, producing Sr1-xYxTi0.92Ru0.08O3-δ and Sr0.92Y0.08Ti1-yRuyO3-δ, respectively. Characterizations of the as-synthesized materials using different analytical techniques indicated that a new perovskite phase of SrRuO3 was produced upon addition of large amounts of Ru (≥12 mol %), and the surface Ru0 species were formed simultaneously to ultimately yield Ruz(surface)/Sr0.92Y0.08Ti1-yRuy-zO3-δ and/or Ruz-w(surface)/SrwRuwO3/Sr0.92-wY0.08Ti1-yRuy-zO3-δ. The newly generated surface Ru0 species at the perovskite surfaces accelerated ammonia dehydrogenation under different conditions, and Sr0.84Y0.16Ti0.92Ru0.08O3-δ exhibited a NH3 conversion of ca. 96% at 500 °C with a gas hourly space velocity (GHSV) of 10 000 mL gcat -1 h-1. In addition, Sr0.84Y0.16Ti0.92Ru0.08O3-δ further proved to be highly active and stable toward ammonia decomposition at different reaction temperatures and GHSVs for >275 h.

KW - Ammonia dehydrogenation

KW - Ammonia synthesis

KW - Hydrogen production

KW - Perovskite

KW - Ruthenium

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