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author:

Zhang, Tianhua (Zhang, Tianhua.) [1] | Hu, Haihui (Hu, Haihui.) [2] | Li, Jiaxin (Li, Jiaxin.) [3] | Gao, Yinglong (Gao, Yinglong.) [4] | Li, Lingling (Li, Lingling.) [5] | Zhang, Mingyuan (Zhang, Mingyuan.) [6] | Peng, Xuanbei (Peng, Xuanbei.) [7] | Zhou, Yanliang (Zhou, Yanliang.) [8] | Ni, Jun (Ni, Jun.) [9] (Scholars:倪军) | Lin, Bingyu (Lin, Bingyu.) [10] (Scholars:林炳裕) | Lin, Jianxin (Lin, Jianxin.) [11] (Scholars:林建新) | Zhu, Bing (Zhu, Bing.) [12] | Wu, Dongshuang (Wu, Dongshuang.) [13] | Zhang, Linjie (Zhang, Linjie.) [14] | Han, Lili (Han, Lili.) [15] | Zheng, Lirong (Zheng, Lirong.) [16] | Wang, Xiuyun (Wang, Xiuyun.) [17] | Jiang, Lilong (Jiang, Lilong.) [18] (Scholars:江莉龙)

Indexed by:

EI Scopus SCIE CSCD

Abstract:

Ammonia (NH3) is an excellent candidate for hydrogen storage and transport. However, producing NH3 under mild conditions is a long-term, arduous task. Atomic cluster catalysts (ACCs) have been shown to be effective for catalytic N2-to-NH3 conversion, opening the door to the development of efficient catalysts under mild conditions. Still, ACC formation with thermally stable catalytic sites remains a challenge because of their high surface free energy. Herein, we report anchoring Ba and/or Ce onto Ru ACCs (2 wt% Ru atomic clusters supported on N-doped carbon) to form so-called clusters-metal oxide promoters electronic interaction (CMEI) to stabilize the Ru atomic clusters. The resulting Ba/Ce/Ru ACCs significantly boost the NH3 synthesis rate to 56.2 mmolNH3 gcat-1 h-1 at 400 degrees C and 1 MPa, which is 7.5-fold higher than that of Ru ACC. The strengthened CMEI between the Ba/Ce and Ru atomic clusters across the Ba/Ce/Ru ACC enables electron transfer from Ba and/or Ce to Ru atomic clusters. As such, the electron-enriched Ru atom could facilitate electron transfer to N equivalent to N bond pi* orbitals, which would weaken the N equivalent to N bond and drive the eventual conversion of N2 to NH3. This study offers insight into the role of CMEI in Ru ACCs and provides an effective approach for designing stable atomic cluster catalysts for NH3 synthesis.

Keyword:

Ammonia synthesis Atomic cluster Electronic interaction N 2 activation Promoter

Community:

  • [ 1 ] [Zhang, Tianhua]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 2 ] [Li, Jiaxin]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 3 ] [Gao, Yinglong]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 4 ] [Li, Lingling]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 5 ] [Zhang, Mingyuan]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 6 ] [Peng, Xuanbei]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 7 ] [Zhou, Yanliang]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 8 ] [Ni, Jun]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 9 ] [Lin, Bingyu]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 10 ] [Lin, Jianxin]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 11 ] [Wang, Xiuyun]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 12 ] [Jiang, Lilong]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 13 ] [Hu, Haihui]Fuzhou Univ, Coll Chem, Fuzhou 350002, Fujian, Peoples R China
  • [ 14 ] [Zhu, Bing]Nanyang Technol Univ, Coll Engn, Sch Mat Sci & Engn MSE, Nanyang Ave, Singapore 639798, Singapore
  • [ 15 ] [Wu, Dongshuang]Nanyang Technol Univ, Coll Engn, Sch Mat Sci & Engn MSE, Nanyang Ave, Singapore 639798, Singapore
  • [ 16 ] [Zhang, Linjie]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
  • [ 17 ] [Han, Lili]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
  • [ 18 ] [Zheng, Lirong]Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China

Reprint 's Address:

  • [Li, Lingling]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China;;[Wang, Xiuyun]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China;;[Jiang, Lilong]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China;;

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Source :

CHINESE JOURNAL OF CATALYSIS

ISSN: 0253-9837

Year: 2024

Volume: 60

Page: 209-218

1 5 . 7 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: 1

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