Electrocatalytic N–C–N coupling over a hierarchically ordered open single-atom superstructure toward organonitrogen synthesis
Nature Communications,
Journal Year:
2025,
Volume and Issue:
16(1)
Published: April 15, 2025
Electrochemically
constructing
C-N
and
N-C-N
bonds
provides
an
economical
sustainable
alternative
to
conventional
chemosynthesis.
Herein,
a
hierarchically
ordered
open
superstructure
of
N-doped
carbon
isolated
with
accessible
three-coordinated
Zn
single-atom
sites
is
explored
for
efficient
electrocatalytic
coupling.
Benefiting
from
the
distinctive
structural
merits,
this
catalyst
enables
preparation
bonded
compounds
methanol
amines.
Notably,
Faradaic
efficiency
selectivity
N,N,N',N'-tetramethyldiaminomethane
reach
up
77%
96%
at
0.8
V,
respectively.
Further
integrating
aminoalkylation
reaction,
electro-thermo
cascade
synthesis
electrochemically
obtained
serving
as
unique
reagent,
leading
specific
set
organonitrogen
(dimethylamino)methyl
substituent,
including
topotecan
hydrochloride,
anti-tumor
drug,
high
yield
95%.
Furthermore,
in
situ
spectroscopic
characterization
calculations
unveil
that
under-coordinated
Zn-N3
play
pivotal
role
stabilizing
key
*CH2O
intermediate,
thereby
facilitating
subsequent
nucleophilic
addition
Language: Английский
In a search of the single-atom electrocatalysts for hydrogen production: the first sulfur-free mono- and diphenanthrenyl-terminated iron and cobalt(II) clathrochelates versus their thioanalogs
Process Safety and Environmental Protection,
Journal Year:
2024,
Volume and Issue:
192, P. 285 - 299
Published: Oct. 16, 2024
Language: Английский