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author:

Zhang, Mingyuan (Zhang, Mingyuan.) [1] | Luo, Yongjin (Luo, Yongjin.) [2] | Peng, Xuanbei (Peng, Xuanbei.) [3] | Zhang, Shiyong (Zhang, Shiyong.) [4] | Zhang, Lei (Zhang, Lei.) [5] | Xu, Cong-Qiao (Xu, Cong-Qiao.) [6] | Zhou, Yanliang (Zhou, Yanliang.) [7] (Scholars:周岩良) | Zheng, Lirong (Zheng, Lirong.) [8] | Ni, Jun (Ni, Jun.) [9] | Wang, Xiuyun (Wang, Xiuyun.) [10] | Jiang, Lilong (Jiang, Lilong.) [11] (Scholars:江莉龙) | Li, Jun (Li, Jun.) [12]

Indexed by:

EI Scopus SCIE

Abstract:

Ammonia (NH3) plays an important role in the development and evolution of Earth's life system. The extremely high bond energy (941 kJ mol(-1)) of N-2 hinder the conversion of N-2 to NH3 under mild conditions. Meanwhile, clearly identifying the distribution of intermediates for NH3 synthesis remains a huge challenge in the experiment. Herein, we anchored carbon clusters (C-60 or C-70) onto Ru catalysts supported on rare earth oxides, forming a class of Ru-carbon cluster co-catalysts that exhibit strong electronic metal-carbon cluster interaction (EMCI). Carbon clusters function as an electron buffer that induced electron uptake from metallic Ru sites and concurrently provides electron feedback to Ru delta+ in a reversible manner, achieving a flexible balance of electron density at the Ru active sites. Moreover, H-affinitive carbon clusters serve as the site for the adsorption, activation and migration of hydrogen. With Ru and carbon clusters synergistically bridged by hydrogen spillover, the Ru-C-60 co-catalyst exhibits an exceptionally high NH3 synthesis rate and remarkable stability. Experimental provides direct evidence of the distribution and evolution of *N2Hx (x = 1 similar to 3) intermediates, with the hydrogenation of *NH2 to form *NH3 identified as the rate-determining step. This work paves the way for utilizing carbon clusters in important chemical reactions.

Keyword:

ammonia synthesis carbon clusters electron buffer N-2 activation reaction mechanism

Community:

  • [ 1 ] [Zhang, Mingyuan]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 2 ] [Peng, Xuanbei]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 3 ] [Zhang, Shiyong]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 4 ] [Zhang, Lei]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 5 ] [Zhou, Yanliang]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 6 ] [Ni, Jun]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 7 ] [Wang, Xiuyun]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 8 ] [Jiang, Lilong]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China
  • [ 9 ] [Zhang, Mingyuan]Qingyuan Innovat Lab, Quanzhou 362801, Fujian, Peoples R China
  • [ 10 ] [Peng, Xuanbei]Qingyuan Innovat Lab, Quanzhou 362801, Fujian, Peoples R China
  • [ 11 ] [Wang, Xiuyun]Qingyuan Innovat Lab, Quanzhou 362801, Fujian, Peoples R China
  • [ 12 ] [Jiang, Lilong]Qingyuan Innovat Lab, Quanzhou 362801, Fujian, Peoples R China
  • [ 13 ] [Luo, Yongjin]Fujian Normal Univ, Coll Environm & Resource Sci, Coll Carbon Neutral Modern Ind, Fuzhou 350007, Peoples R China
  • [ 14 ] [Xu, Cong-Qiao]Southern Univ Sci & Technol, Dept Chem, Guangdong Prov Key Lab Catalyt Chem, Shenzhen 518055, Peoples R China
  • [ 15 ] [Zheng, Lirong]Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China
  • [ 16 ] [Li, Jun]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 17 ] [Li, Jun]Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Minist Educ, Beijing 100084, Peoples R China

Reprint 's Address:

  • 王秀云

    [Wang, Xiuyun]Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China;;[Wang, Xiuyun]Qingyuan Innovat Lab, Quanzhou 362801, Fujian, Peoples R China;;[Xu, Cong-Qiao]Southern Univ Sci & Technol, Dept Chem, Guangdong Prov Key Lab Catalyt Chem, Shenzhen 518055, Peoples R China

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Source :

ADVANCED FUNCTIONAL MATERIALS

ISSN: 1616-301X

Year: 2024

Issue: 8

Volume: 35

1 8 . 5 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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