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author:

Zhang, X. (Zhang, X..) [1] | Yan, P. (Yan, P..) [2] | Xu, J. (Xu, J..) [3] | Li, F. (Li, F..) [4] | Herold, F. (Herold, F..) [5] | Etzold, B.J.M. (Etzold, B.J.M..) [6] | Wang, P. (Wang, P..) [7] | Su, D.S. (Su, D.S..) [8] | Lin, S. (Lin, S..) [9] | Qi, W. (Qi, W..) [10] | Xie, Z. (Xie, Z..) [11]

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Scopus

Abstract:

Borocarbonitrides (BCNs) have emerged as highly selective catalysts for the oxidative dehydrogenation (ODH) reaction. However, there is a lack of in-depth understanding of the catalytic mechanism over BCN catalysts due to the complexity of the surface oxygen functional groups. Here, BCN nanotubes with multiple active sites are synthesized for oxygen-assisted methanol conversion reaction. The catalyst shows a notable activity improvement for methanol conversion (29%) with excellent selectivity to formaldehyde (54%). Kinetic measurements indicate that carboxylic acid groups on BCN are responsible for the formation of dimethyl ether, while the redox catalysis to formaldehyde occurs on both ketonic carbonyl and boron hydroxyl (B-OH) sites. The ODH reaction pathway on the B-OH site is further revealed by in situ infrared, x-ray absorption spectra, and density functional theory. The present work provides physical-chemical insights into the functional mechanism of BCN catalysts, paving the way for further development of the underexplored nonmetallic catalytic systems. Copyright © 2020 The Authors, some rights reserved.

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Community:

  • [ 1 ] [Zhang, X.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350016, China
  • [ 2 ] [Yan, P.]Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, China
  • [ 3 ] [Xu, J.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350016, China
  • [ 4 ] [Li, F.]Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, China
  • [ 5 ] [Herold, F.]Ernst-Berl-Institut für Technische und Makromolekulare Chemie, Technische Universität Darmstadt, Darmstadt, 64287, Germany
  • [ 6 ] [Etzold, B.J.M.]Ernst-Berl-Institut für Technische und Makromolekulare Chemie, Technische Universität Darmstadt, Darmstadt, 64287, Germany
  • [ 7 ] [Wang, P.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350016, China
  • [ 8 ] [Su, D.S.]Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, China
  • [ 9 ] [Su, D.S.]Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, Berlin, 14195, Germany
  • [ 10 ] [Lin, S.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350016, China
  • [ 11 ] [Qi, W.]Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, China
  • [ 12 ] [Xie, Z.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350016, China

Reprint 's Address:

  • [Lin, S.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou UniversityChina

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Source :

Science Advances

ISSN: 2375-2548

Year: 2020

Issue: 26

Volume: 6

1 4 . 1 3 6

JCR@2020

1 1 . 7 0 0

JCR@2023

ESI HC Threshold:420

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 40

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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