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author:

Zhang, Y. (Zhang, Y..) [1] | Peng, X. (Peng, X..) [2] | Tian, H.-R. (Tian, H.-R..) [3] | Yang, B. (Yang, B..) [4] | Chen, Z.-C. (Chen, Z.-C..) [5] | Li, J. (Li, J..) [6] | Zhang, T. (Zhang, T..) [7] | Zhang, M. (Zhang, M..) [8] | Liang, X. (Liang, X..) [9] | Yu, Z. (Yu, Z..) [10] | Zhou, Y. (Zhou, Y..) [11] | Zheng, L. (Zheng, L..) [12] | Wang, X. (Wang, X..) [13] | Zheng, J.-W. (Zheng, J.-W..) [14] | Tang, Y. (Tang, Y..) [15] | Au, C.-T. (Au, C.-T..) [16] | Jiang, L. (Jiang, L..) [17] | Xie, S.-Y. (Xie, S.-Y..) [18]

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Abstract:

Developing highly effective catalysts for ammonia (NH3) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH3 synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene (C60) onto non-iron transition metals yields cluster-matrix co-catalysts that are highly efficient for NH3 synthesis. Such co-catalysts feature separate catalytic active sites for hydrogen and nitrogen. The ‘electron buffer’ behaviour of C60 balances the electron density at catalytic transition metal sites and enables the synergistic activation of nitrogen on transition metals in addition to the activation and migration of hydrogen on C60 sites. As demonstrated in long-term, continuous runs, the C60-promoting transition metal co-catalysts exhibit higher NH3 synthesis rates than catalysts without C60. With the involvement of C60, the rate-determining step in the cluster-matrix co-catalysis is found to be the hydrogenation of *NH2. C60 incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts. (Figure presented.) © The Author(s), under exclusive licence to Springer Nature Limited 2024.

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  • [ 1 ] [Zhang Y.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, China
  • [ 2 ] [Peng X.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, China
  • [ 3 ] [Tian H.-R.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China
  • [ 4 ] [Yang B.]School of Physical Science and Technology, ShanghaiTech University, Shanghai, China
  • [ 5 ] [Chen Z.-C.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China
  • [ 6 ] [Li J.]School of Physical Science and Technology, ShanghaiTech University, Shanghai, China
  • [ 7 ] [Zhang T.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, China
  • [ 8 ] [Zhang M.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, China
  • [ 9 ] [Liang X.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, China
  • [ 10 ] [Yu Z.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, China
  • [ 11 ] [Zhou Y.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, China
  • [ 12 ] [Zheng L.]Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China
  • [ 13 ] [Wang X.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, China
  • [ 14 ] [Zheng J.-W.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China
  • [ 15 ] [Tang Y.]Institute of Molecular Catalysis and In Situ/Operando Studies, College of Chemistry, Fuzhou University, Fuzhou, China
  • [ 16 ] [Au C.-T.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, China
  • [ 17 ] [Jiang L.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, China
  • [ 18 ] [Xie S.-Y.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China

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Source :

Nature Chemistry

ISSN: 1755-4330

Year: 2024

Issue: 11

Volume: 16

Page: 1781-1787

1 9 . 2 0 0

JCR@2023

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ESI Highly Cited Papers on the List: 0 Unfold All

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