Journal Article

FZJ-2020-04036

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Tuning regioselective oxidation toward phenol via atomically dispersed iron sites on carbon

Ding, Y. (Corresponding author) ; Zhang, P. ; Xiong, H. ; Sun, X. ; Klyushin, A. ; Zhang, B. ; Liu, Z.FZJ* ; Zhang, J. ; Zhu, H. ; Qiao, Z.-A. ; Heumann, S. ; Dai, S. (Corresponding author)

2020
RSC Cambridge

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Please use a persistent id in citations: http://hdl.handle.net/2128/25905  doi:10.1039/D0GC01717E

Abstract: The development of environmentally benign catalysts for highly regioselective hydroxylation of phenol remains an unsolved challenge in both industry and academia because the electrophilic substitution of phenol simultaneously occurs on both ortho- and para-positions. Herein, we report a designed atomically dispersed iron-based heterogeneous catalyst, in which the iron species is coordinated by a functionalized ionic liquid monolayer on carbon nanotubes. The catalyst exhibits an unprecedented level of regioselectivity (>99%) towards the hydroxylation of phenol and displays a much better activity (TOF towards catechol productivity, 1.79 s−1) compared to the homogeneous free ion system (TOF towards catechol productivity, 0.44 s−1). Both experimental and theoretical investigations confirm that the catalytic oxidation with hydroperoxide undergoes a non-radical addition process and substitutes only the ortho-positions of phenol. This finding provides not only a quite active and selective catalyst for industrially very important reactions, but also a promising methodology of designing biomimetic iron-based heterogeneous catalysts at the atomic level.

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Contributing Institute(s):

1. Grundlagen der Elektrochemie (IEK-9)

Research Program(s):

1. 131 - Electrochemical Storage (POF3-131) (POF3-131)

Appears in the scientific report 2020

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Database coverage:
; ; ; Allianz-Lizenz / DFG ; Chemical Reactions ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 5 ; JCR ; NCBI Molecular Biology Database ; National-Konsortium ; Nationallizenz ; SCOPUS ; Science Citation Index ; Science Citation Index Expanded ; Web of Science Core Collection

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