Unraveling the size-dependent effect of Ru-based catalysts on Ammonia synthesis at mild conditions

Yanliang Zhou; Junjie Wang; Lili Liang; Qianjin Sai; Jun Ni; Chak tong Au; Xingyi Lin; Xiuyun Wang; Ying Zheng; Lirong Zheng; Lilong Jiang

doi:10.1016/j.jcat.2021.10.024

Unraveling the size-dependent effect of Ru-based catalysts on Ammonia synthesis at mild conditions

Yanliang Zhou, Junjie Wang, Lili Liang, Qianjin Sai, Jun Ni, Chak tong Au, Xingyi Lin, Xiuyun Wang, Ying Zheng, Lirong Zheng, Lilong Jiang

School of Materials Sience and Engineering

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

30 Scopus citations

Abstract

Identifying optimal Ru size in NH₃ synthesis can improve reaction activity and maximize the utilization of Ru to reduce catalyst cost. However, previous researches are focused on large Ru particle size (≥2 nm) while that below 2 nm in NH₃ synthesis is unclear. Here we synthesized a series of Rux/BaCeO₃ with different Ru sizes (x = 1.1–3.0 nm) through size-controlled Ru colloid. With the decrease of Ru size, NH₃ synthesis rate over Ru1.1/BaCeO₃ increases to 19.4 mmol g_cat⁻¹h⁻¹ at 400 °C and 1 MPa, which is 5.7 times that of Ru3.0/BaCeO₃ and superior to most of Ru-based catalysts previously reported. It reveals that the reduction of Ru size enhances the generation of Ce³⁺ and oxygen vacancies in BaCeO₃, which can donate electron to Ru centers and promote N₂ dissociation. Moreover, the small Ru size enhances hydrogen spillover from Ru to BaCeO₃ to alleviate hydrogen poisoning, resulting in efficient NH₃ synthesis.

Original language	English
Pages (from-to)	501-511
Number of pages	11
Journal	Journal of Catalysis
Volume	404
DOIs	https://doi.org/10.1016/j.jcat.2021.10.024
State	Published - Dec 2021

Keywords

Ammonia synthesis
Ce and oxygen vacancies
Electron transfer
Hydrogen spillover
Size-dependent

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10.1016/j.jcat.2021.10.024

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title = "Unraveling the size-dependent effect of Ru-based catalysts on Ammonia synthesis at mild conditions",

abstract = "Identifying optimal Ru size in NH3 synthesis can improve reaction activity and maximize the utilization of Ru to reduce catalyst cost. However, previous researches are focused on large Ru particle size (≥2 nm) while that below 2 nm in NH3 synthesis is unclear. Here we synthesized a series of Rux/BaCeO3 with different Ru sizes (x = 1.1–3.0 nm) through size-controlled Ru colloid. With the decrease of Ru size, NH3 synthesis rate over Ru1.1/BaCeO3 increases to 19.4 mmol gcat−1h−1 at 400 °C and 1 MPa, which is 5.7 times that of Ru3.0/BaCeO3 and superior to most of Ru-based catalysts previously reported. It reveals that the reduction of Ru size enhances the generation of Ce3+ and oxygen vacancies in BaCeO3, which can donate electron to Ru centers and promote N2 dissociation. Moreover, the small Ru size enhances hydrogen spillover from Ru to BaCeO3 to alleviate hydrogen poisoning, resulting in efficient NH3 synthesis.",

keywords = "Ammonia synthesis, Ce and oxygen vacancies, Electron transfer, Hydrogen spillover, Size-dependent",

author = "Yanliang Zhou and Junjie Wang and Lili Liang and Qianjin Sai and Jun Ni and Au, {Chak tong} and Xingyi Lin and Xiuyun Wang and Ying Zheng and Lirong Zheng and Lilong Jiang",

note = "Publisher Copyright: {\textcopyright} 2021 Elsevier Inc.",

year = "2021",

month = dec,

doi = "10.1016/j.jcat.2021.10.024",

language = "英语",

volume = "404",

pages = "501--511",

journal = "Journal of Catalysis",

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T1 - Unraveling the size-dependent effect of Ru-based catalysts on Ammonia synthesis at mild conditions

AU - Zhou, Yanliang

AU - Wang, Junjie

AU - Liang, Lili

AU - Sai, Qianjin

AU - Ni, Jun

AU - Au, Chak tong

AU - Lin, Xingyi

AU - Wang, Xiuyun

AU - Zheng, Ying

AU - Zheng, Lirong

AU - Jiang, Lilong

PY - 2021/12

Y1 - 2021/12

N2 - Identifying optimal Ru size in NH3 synthesis can improve reaction activity and maximize the utilization of Ru to reduce catalyst cost. However, previous researches are focused on large Ru particle size (≥2 nm) while that below 2 nm in NH3 synthesis is unclear. Here we synthesized a series of Rux/BaCeO3 with different Ru sizes (x = 1.1–3.0 nm) through size-controlled Ru colloid. With the decrease of Ru size, NH3 synthesis rate over Ru1.1/BaCeO3 increases to 19.4 mmol gcat−1h−1 at 400 °C and 1 MPa, which is 5.7 times that of Ru3.0/BaCeO3 and superior to most of Ru-based catalysts previously reported. It reveals that the reduction of Ru size enhances the generation of Ce3+ and oxygen vacancies in BaCeO3, which can donate electron to Ru centers and promote N2 dissociation. Moreover, the small Ru size enhances hydrogen spillover from Ru to BaCeO3 to alleviate hydrogen poisoning, resulting in efficient NH3 synthesis.

AB - Identifying optimal Ru size in NH3 synthesis can improve reaction activity and maximize the utilization of Ru to reduce catalyst cost. However, previous researches are focused on large Ru particle size (≥2 nm) while that below 2 nm in NH3 synthesis is unclear. Here we synthesized a series of Rux/BaCeO3 with different Ru sizes (x = 1.1–3.0 nm) through size-controlled Ru colloid. With the decrease of Ru size, NH3 synthesis rate over Ru1.1/BaCeO3 increases to 19.4 mmol gcat−1h−1 at 400 °C and 1 MPa, which is 5.7 times that of Ru3.0/BaCeO3 and superior to most of Ru-based catalysts previously reported. It reveals that the reduction of Ru size enhances the generation of Ce3+ and oxygen vacancies in BaCeO3, which can donate electron to Ru centers and promote N2 dissociation. Moreover, the small Ru size enhances hydrogen spillover from Ru to BaCeO3 to alleviate hydrogen poisoning, resulting in efficient NH3 synthesis.

KW - Ammonia synthesis

KW - Ce and oxygen vacancies

KW - Electron transfer

KW - Hydrogen spillover

KW - Size-dependent

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DO - 10.1016/j.jcat.2021.10.024

M3 - 文章

AN - SCOPUS:85118925793

SN - 0021-9517

VL - 404

SP - 501

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JO - Journal of Catalysis

JF - Journal of Catalysis

ER -

Unraveling the size-dependent effect of Ru-based catalysts on Ammonia synthesis at mild conditions

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Keywords

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