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author:

Zhang, Shiyong (Zhang, Shiyong.) [1] | Zhang, Mingyuan (Zhang, Mingyuan.) [2] | Zhang, Tianhua (Zhang, Tianhua.) [3] | Sun, Jizhen (Sun, Jizhen.) [4] | Li, Jiaxin (Li, Jiaxin.) [5] | Su, Kailin (Su, Kailin.) [6] | Mao, Ruishao (Mao, Ruishao.) [7] | Zhou, Yanliang (Zhou, Yanliang.) [8] (Scholars:周岩良) | Peng, Xuanbei (Peng, Xuanbei.) [9] | Zhang, Yangyu (Zhang, Yangyu.) [10] | Ni, Jun (Ni, Jun.) [11] | Lin, Bingyu (Lin, Bingyu.) [12] (Scholars:林炳裕) | Wang, Xiuyun (Wang, Xiuyun.) [13] | Jiang, Lilong (Jiang, Lilong.) [14] (Scholars:江莉龙)

Indexed by:

EI Scopus SCIE

Abstract:

Achieving green ammonia (NH3) synthesis requires developing effective catalysts under mild conditions. However, the competitive adsorption of N-2 and H-2, as well as the strong binding of N-containing intermediates on the catalyst, greatly inhibits the active sites for efficient NH3 synthesis. Here, we constructed a series of ZrH2-modified Fe catalysts with dual active sites to address these issues and realized efficient NH3 synthesis under mild conditions. Our study shows that ZrH2 can not only provide active sites for H-2 activation but also transfer electrons to Fe sites for accelerating N-2 activation. The interaction between Fe and ZrH2 over 40ZrH(2)-Fe leads to a decrease in work function and a downward shift of the d-band center, which is conducive to N-2 activation and NH3 desorption, respectively. The utilization of distinct sites for activating different reactants can avoid the competitive adsorption of N-2 and H-2, leading to excellent NH3 synthesis activity of the 40 wt.% ZrH2-mediated Fe catalyst. As a result, 40ZrH(2)-Fe exhibits a high NH3 synthesis rate of 23.3 mmol g(cat)(-1) h(-1) at 400 degrees C and 1 MPa and robust stability during 100 h time-on-stream.

Keyword:

ammonia synthesis competitive adsorption dual-site catalyst N-2 activation synergistic effect

Community:

  • [ 1 ] [Zhang, Shiyong]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 2 ] [Zhang, Mingyuan]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 3 ] [Zhang, Tianhua]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 4 ] [Sun, Jizhen]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 5 ] [Li, Jiaxin]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 6 ] [Su, Kailin]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 7 ] [Mao, Ruishao]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 8 ] [Zhou, Yanliang]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 9 ] [Peng, Xuanbei]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 10 ] [Zhang, Yangyu]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 11 ] [Ni, Jun]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 12 ] [Lin, Bingyu]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 13 ] [Wang, Xiuyun]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 14 ] [Jiang, Lilong]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China
  • [ 15 ] [Peng, Xuanbei]Qingyuan Innovat Lab, Quanzhou 362801, Peoples R China
  • [ 16 ] [Wang, Xiuyun]Qingyuan Innovat Lab, Quanzhou 362801, Peoples R China
  • [ 17 ] [Jiang, Lilong]Qingyuan Innovat Lab, Quanzhou 362801, Peoples R China

Reprint 's Address:

  • [Zhou, Yanliang]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China;;[Wang, Xiuyun]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China;;[Jiang, Lilong]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Peoples R China;;[Wang, Xiuyun]Qingyuan Innovat Lab, Quanzhou 362801, Peoples R China;;[Jiang, Lilong]Qingyuan Innovat Lab, Quanzhou 362801, Peoples R China;;

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Source :

SCIENCE CHINA-CHEMISTRY

ISSN: 1674-7291

Year: 2025

Issue: 4

Volume: 68

Page: 1576-1584

1 0 . 4 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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