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; Suk Woo Nam; Kwang Ho Song; Chang Won Yoon

doi:10.1021/acssuschemeng.7b02402

Influence of Cation Substitutions Based on ABO₃ Perovskite Materials, Sr_1-xY_xTi_1-yRu_yO_3-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, Suk Woo Nam, Kwang Ho Song, Chang Won Yoon

Research output: Contribution to journal › Article › peer-review

32 Scopus citations

Abstract

In order to screen potential catalytic materials for synthesis and decomposition of ammonia, a series of ABO₃ perovskite materials, Sr_1-xY_xTi_1-yRu_yO_3-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 Sr_1-xY_xTi_0.92Ru_0.08O_3-δ and Sr_0.92Y_0.08Ti_1-yRu_yO_3-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 Ru_z(surface)/Sr_0.92Y_0.08Ti_1-yRu_y-zO_3-δ and/or Ru_z-w(surface)/Sr_wRu_wO₃/Sr_0.92-wY_0.08Ti_1-yRu_y-zO_3-δ. The newly generated surface Ru⁰ species at the perovskite surfaces accelerated ammonia dehydrogenation under different conditions, and Sr_0.84Y_0.16Ti_0.92Ru_0.08O_3-δ exhibited a NH₃ conversion of ca. 96% at 500 °C with a gas hourly space velocity (GHSV) of 10 000 mL g_cat^-1 h^-1. In addition, Sr_0.84Y_0.16Ti_0.92Ru_0.08O_3-δ further proved to be highly active and stable toward ammonia decomposition at different reaction temperatures and GHSVs for >275 h.

Original language	English
Pages (from-to)	9370-9379
Number of pages	10
Journal	ACS Sustainable Chemistry and Engineering
Volume	5
Issue number	10
DOIs	https://doi.org/10.1021/acssuschemeng.7b02402
State	Published - 2 Oct 2017
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2017 American Chemical Society.

Keywords

Ammonia dehydrogenation
Ammonia synthesis
Hydrogen production
Perovskite
Ruthenium

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10.1021/acssuschemeng.7b02402

Cite this

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

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.",

keywords = "Ammonia dehydrogenation, Ammonia synthesis, Hydrogen production, Perovskite, Ruthenium",

author = "Hyunmi Doh and Kim, {Hyo Young} and Kim, {Ghun Sik} and Junyoung Cha and Park, {Hyun S.} and Ham, {Hyung Chul} and Yoon, {Sung Pil} and Jonghee Han and Nam, {Suk Woo} and Song, {Kwang Ho} and Yoon, {Chang Won}",

note = "Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

year = "2017",

month = oct,

day = "2",

doi = "10.1021/acssuschemeng.7b02402",

language = "English",

volume = "5",

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T1 - Influence of Cation Substitutions Based on ABO3 Perovskite Materials, Sr1-xYxTi1-yRuyO3-δ, on Ammonia Dehydrogenation

AU - Doh, Hyunmi

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, Suk Woo

AU - Song, Kwang Ho

AU - Yoon, Chang Won

PY - 2017/10/2

Y1 - 2017/10/2

N2 - 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.

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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DO - 10.1021/acssuschemeng.7b02402

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