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author:

Wang, S. (Wang, S..) [1] | Zhuang, Z. (Zhuang, Z..) [2] | Chen, X. (Chen, X..) [3] | Wang, Y. (Wang, Y..) [4] | Li, X. (Li, X..) [5] | Yang, M. (Yang, M..) [6] | Wu, Y. (Wu, Y..) [7] | Peng, Q. (Peng, Q..) [8] | Chen, C. (Chen, C..) [9] | Li, Y. (Li, Y..) [10]

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Scopus

Abstract:

γ-valerolactone (GVL) is a key value-added chemical catalytically produced from levulinic acid (LA), an important biomass derivative platform chemical. Here an ultra-efficient 3D Ru catalyst generated by in situ reduction of RuZnOx nanoboxes is reported; the catalyst features a well-defined structure of highly dispersed in situ oxide-derived Ru (IOD-Ru) clusters (≈1 nm in size) spatially confined within the 3D nanocages with rich mesopores, which guarantees a maximized atom utilization with a high exposure of Ru active sites as well as a 3D accessibility for substrate molecules. The IOD-Ru exhibits ultrahigh performance for the hydrogenation of LA into GVL with a record-breaking turnover frequency (TOF) up to 59400 h−1, 14 times higher than that of the ex situ reduction of RuZnOx nanoboxes catalyst. Structural characterizations and theoretical calculations collectively indicate that the defect-rich and coordination-unsaturated IOD-Ru sites can boost the activation of the carbonyl group in LA with a significantly lowered energy barrier of hydrogenation. © 2023 Wiley-VCH GmbH.

Keyword:

in situ reduction levulinic acid Ru clusters RuZnOx nanoboxes γ-valerolactone

Community:

  • [ 1 ] [Wang S.]Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084, China
  • [ 2 ] [Zhuang Z.]Department of Chemistry, Tsinghua University, Beijing, 100084, China
  • [ 3 ] [Zhuang Z.]College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 4 ] [Chen X.]Beijing Advanced Innovation Center for Materials Genome Engineering, Institute of Solid State Chemistry, University of Science and Technology Beijing, Beijing, 100083, China
  • [ 5 ] [Wang Y.]Department of Chemistry, Tsinghua University, Beijing, 100084, China
  • [ 6 ] [Li X.]Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084, China
  • [ 7 ] [Yang M.]Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084, China
  • [ 8 ] [Wu Y.]Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084, China
  • [ 9 ] [Peng Q.]Department of Chemistry, Tsinghua University, Beijing, 100084, China
  • [ 10 ] [Chen C.]Department of Chemistry, Tsinghua University, Beijing, 100084, China
  • [ 11 ] [Li Y.]Department of Chemistry, Tsinghua University, Beijing, 100084, China

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Small

ISSN: 1613-6810

Year: 2023

Issue: 7

Volume: 20

1 3 . 0

JCR@2023

1 3 . 0 0 0

JCR@2023

JCR Journal Grade:1

CAS Journal Grade:1

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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