Chemical Reviews,
Journal Year:
2021,
Volume and Issue:
121(11), P. 6522 - 6587
Published: May 11, 2021
The
large
carbon
footprint
of
the
Haber–Bosch
process,
which
provides
ammonia
for
fertilizers
but
also
feedstock
all
nitrogenous
commercial
products,
has
fueled
quest
alternative
synthetic
strategies
to
nitrogen
fixation.
Owing
extraordinarily
strong
N≡N
triple
bond,
key
step
reaction,
i.e.,
dissociative
adsorption
N2,
requires
high
temperatures.
Since
first
report
in
1995,
a
wide
variety
molecular
transition
metal
and
f-block
compounds
have
been
reported
that
can
fully
cleave
N2
at
ambient
conditions
form
well-defined
nitrido
complexes.
We
here
provide
comprehensive
survey
current
state
splitting
reactions
solution
follow-up
transfer
reactivity.
Particular
emphasis
is
put
on
electronic
structure
requirements
formation
suitable
precursors
their
N–N
scission
prospects
synthesis
containing
products
will
be
discussed,
ranging
from
heterocumulenes
organic
amines,
amides
or
nitriles
via
proton
coupled
electron
transfer,
carbonylation,
electrophilic
functionalization
derived
Accomplishments
challenges
fixation
are
presented
offer
guidelines
development
catalytic
platforms.
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(21), P. 12070 - 12097
Published: Jan. 1, 2021
Incorporation
of
LSPR
features
into
electrocatalysis
shows
unprecedented
activities.
This
review
summarizes
the
mechanisms,
preparation
and
characterization
strategies,
as
well
recent
exciting
progress
in
LSPR-mediated
electrocatalysis.
ACS Nano,
Journal Year:
2022,
Volume and Issue:
16(5), P. 7915 - 7925
Published: April 22, 2022
Electrocatalytic
nitrogen
reduction
reaction
(NRR)
is
a
promising
approach
for
renewable
NH3
production,
while
developing
the
NRR
electrocatalysis
systems
with
both
high
activity
and
selectivity
remains
significant
challenge.
Herein,
we
combine
catalyst
electrolyte
engineering
to
achieve
high-efficiency
enabled
by
Se-vacancy-rich
WSe2-x
in
water-in-salt
(WISE).
Extensive
characterizations,
theoretical
calculations,
situ
X-ray
photoelectron/Raman
spectroscopy
reveal
that
WISE
ensures
suppressed
H2
evolution,
improved
N2
affinity
on
surface,
as
well
an
enhanced
π-back-donation
ability
of
active
sites,
thereby
promoting
NRR.
As
result,
excellent
faradaic
efficiency
62.5%
yield
181.3
μg
h-1
mg-1
achieved
12
m
LiClO4,
which
among
highest
performances
reported
date.
Chemical Reviews,
Journal Year:
2021,
Volume and Issue:
121(11), P. 6522 - 6587
Published: May 11, 2021
The
large
carbon
footprint
of
the
Haber–Bosch
process,
which
provides
ammonia
for
fertilizers
but
also
feedstock
all
nitrogenous
commercial
products,
has
fueled
quest
alternative
synthetic
strategies
to
nitrogen
fixation.
Owing
extraordinarily
strong
N≡N
triple
bond,
key
step
reaction,
i.e.,
dissociative
adsorption
N2,
requires
high
temperatures.
Since
first
report
in
1995,
a
wide
variety
molecular
transition
metal
and
f-block
compounds
have
been
reported
that
can
fully
cleave
N2
at
ambient
conditions
form
well-defined
nitrido
complexes.
We
here
provide
comprehensive
survey
current
state
splitting
reactions
solution
follow-up
transfer
reactivity.
Particular
emphasis
is
put
on
electronic
structure
requirements
formation
suitable
precursors
their
N–N
scission
prospects
synthesis
containing
products
will
be
discussed,
ranging
from
heterocumulenes
organic
amines,
amides
or
nitriles
via
proton
coupled
electron
transfer,
carbonylation,
electrophilic
functionalization
derived
Accomplishments
challenges
fixation
are
presented
offer
guidelines
development
catalytic
platforms.