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Monolayer Bi
2
MoO
6
nanosheets doped with F atoms (F-BMO-NSs) were developed as catalysts for the one-pot alkylation of nitrobenzene with benzyl alcohol. 95.88% conversion of nitrobenzene coupled with 99.98% selectivity of
n
-benzylideneaniline was achieved over the F
0.04
-BMO-NSs under visible light irradiation and 1 atm N
2
at room temperature. XPS and EPR results suggested that F doping not only produced enhanced Lewis acid sites (Bi
3+
and Mo
6+
), but also generated Lewis base sites (Mo
5+
).
In situ
FTIR spectra revealed that benzyl alcohol would be selectively adsorbed on the enhanced Lewis acid sites
via
Bi
3+
(Mo
6+
) OH-C- interface coordination, resulting in the activation of HO-C-. Moreover, nitrobenzene would be chemisorbed on the Mo
5+
basic sites
via
Mo
5+
NO
2
coordination, inducing charge transfer from Mo
5+
to -NO
2
. Under visible light irradiation, hydrogen transfer takes place from the chemisorbed benzyl alcohol to nitrobenzene generating benzaldehyde and aniline, finally coupling to form the imine. Based on these surface cooperated functional sites, a synergistic mechanism has been proposed to elucidate the accurate structure-performance relationship. This work provides a new perspective for the design of high activity, high selectivity and high stability photocatalysts for the precise synthesis of imines.
Selective chemisorption and activation of benzyl alcohol and nitrobenzene on F
0.04
-BMO-NSs
via
interface coordination Bi
3+
(Mo
6+
) OH-C- and Mo
5+
O
2
N. Hydrogen transfer takes place from the alcohol to nitrobenzene precisely forming
N
-benzylideneaniline.
Sprache
–
Identifikatoren
ISSN: 2044-4753
eISSN: 2044-4761
DOI: 10.1039/d3cy00528c
Titel-ID: cdi_rsc_primary_d3cy00528c
Format
–
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