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作者:

Ding, Jia (Ding, Jia.) | Wang, Lizhuo (Wang, Lizhuo.) | Wu, Ping (Wu, Ping.) | Li, Ang (Li, Ang.) (学者:李昂) | Li, Wei (Li, Wei.) | Stampfl, Catherine (Stampfl, Catherine.) | Liao, Xiaozhou (Liao, Xiaozhou.) | Haynes, Brian S. (Haynes, Brian S..) | Han, Xiaodong (Han, Xiaodong.) (学者:韩晓东) | Huang, Jun (Huang, Jun.)

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EI Scopus SCIE

摘要:

Ammonia is an important feedstock for producing fertilizer and chemicals as well as is also a potential energy carrier. Generally, MgO is considered as an electronic promoter for Ru catalysts in ammonia synthesis. In this research, it was found for the first time that surface atoms of Ru particles are stabilized by MgO modification at high temperature and reaction atmosphere, which contained more highly active B5-sites for ammonia synthesis. Ex situ HRTEM images show similar Ru nanoparticles containing steps with or without promoters. Under reaction temperatures and gas environment, in situ environmental transmission electron microscopy (ETEM) observe that Ru particles without MgO promoter suffer from dynamic change and lost the B5-sites on Ru steps, which results in the poor ammonia yield obtained by both the continuing-flow reaction system. While MgO modification can stabilize the Ru surface structure and keep B5-sites there, which contributes to the much higher ammonia yield. Density functional theory calculations show that B5-site is a catalytic active center for ammonia synthesis and the N-2 dissociation barrier on B5-site containing step is lower than B5-site-free step on Ru nanoparticles. The finding provides a new explanation for the high activity of MgO modified Ru catalysts. Moreover, adding CsOx with MgO will contribute electron donation to stabilized Ru surface and accelerate the ammonia synthesis with five-fold higher than MgO-Ru/MS at 500 degrees C. A better fundamental understanding of the dynamics of Ru catalysts and its reaction mechanism in this research is vital for optimizing the design of catalysts for ammonia synthesis.

关键词:

in&#8197 Ru catalyst MgO ammonia synthesis structure confinement situ transmission electron microscopy

作者机构:

  • [ 1 ] [Ding, Jia]Univ Sydney, Sydney Nano Inst, Sch Chem & Biomol Engn, Sydney, NSW 2006, Australia
  • [ 2 ] [Wang, Lizhuo]Univ Sydney, Sydney Nano Inst, Sch Chem & Biomol Engn, Sydney, NSW 2006, Australia
  • [ 3 ] [Wu, Ping]Univ Sydney, Sydney Nano Inst, Sch Chem & Biomol Engn, Sydney, NSW 2006, Australia
  • [ 4 ] [Haynes, Brian S.]Univ Sydney, Sydney Nano Inst, Sch Chem & Biomol Engn, Sydney, NSW 2006, Australia
  • [ 5 ] [Huang, Jun]Univ Sydney, Sydney Nano Inst, Sch Chem & Biomol Engn, Sydney, NSW 2006, Australia
  • [ 6 ] [Li, Ang]Beijing Univ Technol, Beijing Key Lab Microstruct & Property Adv Mat, Beijing 100024, Peoples R China
  • [ 7 ] [Li, Wei]Beijing Univ Technol, Beijing Key Lab Microstruct & Property Adv Mat, Beijing 100024, Peoples R China
  • [ 8 ] [Han, Xiaodong]Beijing Univ Technol, Beijing Key Lab Microstruct & Property Adv Mat, Beijing 100024, Peoples R China
  • [ 9 ] [Wu, Ping]Univ Sydney, Sch Phys, Sydney Nano Inst, Sydney, NSW 2006, Australia
  • [ 10 ] [Stampfl, Catherine]Univ Sydney, Sch Phys, Sydney Nano Inst, Sydney, NSW 2006, Australia
  • [ 11 ] [Liao, Xiaozhou]Univ Sydney, Sydney Nano Inst, Mech & Mechatron Engn, Sydney, NSW 2006, Australia

通讯作者信息:

  • 李昂 韩晓东

    [Huang, Jun]Univ Sydney, Sydney Nano Inst, Sch Chem & Biomol Engn, Sydney, NSW 2006, Australia;;[Li, Ang]Beijing Univ Technol, Beijing Key Lab Microstruct & Property Adv Mat, Beijing 100024, Peoples R China;;[Han, Xiaodong]Beijing Univ Technol, Beijing Key Lab Microstruct & Property Adv Mat, Beijing 100024, Peoples R China

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来源 :

CHEMCATCHEM

ISSN: 1867-3880

年份: 2020

期: 2

卷: 13

页码: 534-538

4 . 5 0 0

JCR@2022

ESI学科: CHEMISTRY;

ESI高被引阀值:139

被引次数:

WoS核心集被引频次: 10

SCOPUS被引频次: 11

ESI高被引论文在榜: 0 展开所有

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中文被引频次:

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