Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(30), P. 16584 - 16596
Published: July 24, 2023
In
this
work,
we
have
fabricated
an
aryl
amino-substituted
graphitic
carbon
nitride
(g-C3N4)
catalyst
with
atomically
dispersed
Mn
capable
of
generating
hydrogen
peroxide
(H2O2)
directly
from
seawater.
This
new
exhibited
excellent
reactivity,
obtaining
up
to
2230
μM
H2O2
in
7
h
alkaline
water
and
1800
seawater
under
identical
conditions.
More
importantly,
the
was
quickly
recovered
for
subsequent
reuse
without
appreciable
loss
performance.
Interestingly,
unlike
usual
two-electron
oxygen
reduction
reaction
pathway,
generation
through
a
less
common
oxidation
(WOR)
process
which
both
direct
indirect
WOR
processes
occurred;
namely,
photoinduced
h+
oxidized
H2O
via
one-step
2e-
WOR,
first
hydroxide
(OH-)
ion
generate
hydroxy
radical
(•OH),
formed
indirectly
by
combination
two
•OH.
We
characterized
material,
at
catalytic
sites,
atomic
level
using
electron
paramagnetic
resonance,
X-ray
absorption
near
edge
structure,
extended
fine
high-resolution
transmission
microscopy,
photoelectron
spectroscopy,
magic-angle
spinning
solid-state
NMR
multiscale
molecular
modeling,
combining
classical
reactive
dynamics
simulations
quantum
chemistry
calculations.
Chemical Reviews,
Journal Year:
2018,
Volume and Issue:
119(4), P. 2192 - 2452
Published: Nov. 27, 2018
C–H
activation
has
surfaced
as
an
increasingly
powerful
tool
for
molecular
sciences,
with
notable
applications
to
material
crop
protection,
drug
discovery,
and
pharmaceutical
industries,
among
others.
Despite
major
advances,
the
vast
majority
of
these
functionalizations
required
precious
4d
or
5d
transition
metal
catalysts.
Given
cost-effective
sustainable
nature
earth-abundant
first
row
metals,
development
less
toxic,
inexpensive
3d
catalysts
gained
considerable
recent
momentum
a
significantly
more
environmentally-benign
economically-attractive
alternative.
Herein,
we
provide
comprehensive
overview
on
until
summer
2018.
Chemical Reviews,
Journal Year:
2018,
Volume and Issue:
119(4), P. 2681 - 2751
Published: Dec. 31, 2018
The
use
of
3d
metals
in
de/hydrogenation
catalysis
has
emerged
as
a
competitive
field
with
respect
to
"traditional"
precious
metal
catalyzed
transformations.
introduction
functional
pincer
ligands
that
can
store
protons
and/or
electrons
expressed
by
metal-ligand
cooperativity
and
ligand
redox-activity
strongly
stimulated
this
development
conceptual
starting
point
for
rational
catalyst
design.
This
review
aims
at
providing
comprehensive
picture
the
utilization
first-row
transition
hydrogenation
dehydrogenation
related
synthetic
concepts
relying
on
these
such
hydrogen
borrowing
methodology.
Particular
emphasis
is
put
implementation
relevance
cooperating
redox-active
within
mechanistic
scenarios.
Chemical Reviews,
Journal Year:
2018,
Volume and Issue:
119(4), P. 2524 - 2549
Published: Nov. 20, 2018
The
conservation
of
our
element
resources
is
a
fundamental
challenge
mankind.
development
alcohol
refunctionalization
reactions
possible
fossil
carbon
strategy
since
alcohols
can
be
obtained
from
indigestible
and
abundantly
available
biomass.
rare
noble
metals,
frequently
used
in
key
technologies
such
as
catalysis,
might
feasible
by
replacing
them
with
highly
abundant
metals.
alkylation
amines
related
C–C
coupling
are
early
examples
reactions.
These
follow
mostly
the
borrowing
hydrogen
or
autotransfer
catalysis
concept,
many
3d-metal
catalysts
have
been
disclosed
recent
years.
In
this
review,
we
summarize
progress
made
developing
Cu,
Ni,
Co,
Fe,
Mn
for
C–N
bond
formation
using
concept.
We
expect
that
findings
field
will
inspire
others
to
develop
new
efficient
selective
earth-abundant
metal
applications
novel
mediated
Chemical Reviews,
Journal Year:
2018,
Volume and Issue:
119(4), P. 2611 - 2680
Published: Dec. 5, 2018
The
reduction
of
nitro
compounds
to
the
corresponding
amines
is
one
most
utilized
catalytic
processes
in
fine
and
bulk
chemical
industry.
latest
development
catalysts
with
cheap
metals
like
Fe,
Co,
Ni,
Cu
has
led
their
tremendous
achievements
over
last
years
prompting
greater
application
as
"standard"
catalysts.
In
this
review,
we
will
comprehensively
discuss
use
homogeneous
heterogeneous
based
on
non-noble
3d-metals
for
using
various
reductants.
different
systems
be
revised
considering
both
performances
synthetic
aspects
highlighting
also
advantages
disadvantages.
ACS Catalysis,
Journal Year:
2018,
Volume and Issue:
8(12), P. 11435 - 11469
Published: Oct. 16, 2018
Homogeneous
catalysis
of
organic
transformations
by
metal
complexes
has
been
mostly
based
on
noble
metals.
In
recent
years,
tremendous
progress
made
in
the
field
base-metal
catalysis,
with
pincer-type
complexes,
such
as
iron,
cobalt,
nickel,
and
manganese
pincer
systems.
Particularly
impressive
is
explosive
growth
Mn-based
first
being
reported
recently
2016.
This
review
covers
homogeneously
catalyzed
reactions
using
cobalt
manganese.
Various
are
described,
including
acceptorless
dehydrogenation,
hydrogenation,
dehydrogenative
coupling,
hydrogen
borrowing,
transfer,
H–X
additions,
C–C
alkene
polymerization
N2
fixation,
their
scope
brief
mechanistic
comments.
Chemical Reviews,
Journal Year:
2021,
Volume and Issue:
122(1), P. 385 - 441
Published: Nov. 2, 2021
As
the
world
pledges
to
significantly
cut
carbon
emissions,
demand
for
sustainable
and
clean
energy
has
now
become
more
important
than
ever.
This
includes
both
production
storage
of
carriers,
a
majority
which
involve
catalytic
reactions.
article
reviews
recent
developments
homogeneous
catalysts
in
emerging
applications
energy.
The
most
focus
been
on
hydrogen
as
several
efficient
have
reported
recently
(de)hydrogenative
transformations
promising
economy.
Another
direction
that
extensively
covered
this
review
is
methanol
Homogeneous
investigated
from
CO
Chemical Reviews,
Journal Year:
2018,
Volume and Issue:
119(4), P. 2876 - 2953
Published: Dec. 19, 2018
Cobalt
has
become
increasingly
attractive
in
homogeneous
catalysis
because
of
its
unique
characteristics
and
outstanding
catalytic
performance
addition
to
being
cheap
earth-abundant.
Hydride
transfer
processes
are
involved
a
broad
range
organic
transformations
that
allow
the
facile
preparation
various
useful
chemicals
synthetic
building
blocks.
These
reactions
have
continuously
received
great
attention
both
from
academia
industry.
In
this
perspective,
we
review
cobalt-catalyzed
hydride
according
classified
reaction
types
provide
comprehensive
overview
design,
synthesis,
reactivity
cobalt
catalysts,
their
applications,
mechanisms.
Chemical Reviews,
Journal Year:
2018,
Volume and Issue:
119(4), P. 2453 - 2523
Published: Oct. 30, 2018
Computational
chemistry
provides
a
versatile
toolbox
for
studying
mechanistic
details
of
catalytic
reactions
and
holds
promise
to
deliver
practical
strategies
enable
the
rational
in
silico
catalyst
design.
The
reactivity
nontrivial
electronic
structure
effects,
common
systems
based
on
3d
transition
metals,
introduce
additional
complexity
that
may
represent
particular
challenge
standard
computational
strategies.
In
this
review,
we
discuss
challenges
capabilities
modern
methods
reaction
mechanisms
promoted
by
metal
molecular
catalysts.
Particular
focus
will
be
placed
ways
addressing
multiconfigurational
problem
calculations
role
expert
bias
utilization
available
methods.
development
density
functionals
designed
address
metals
is
also
discussed.
Special
emphasis
account
solvation
effects
multicomponent
nature
systems.
This
followed
an
overview
recent
studies
processes
catalysts
metals.
Cases
involve
noninnocent
ligands,
systems,
metal-ligand
metal-metal
cooperativity,
as
well
modeling
complex
such
metal-organic
frameworks
are
presented.
Conventionally,
heavily
dependent
chemical
intuition
input
researcher.
Recent
developments
advanced
automated
path
analysis
hold
eliminating
human-bias
from
catalysis
studies.
A
brief
these
approaches
presented
final
section
review.
paper
closed
with
general
concluding
remarks.
Organic & Biomolecular Chemistry,
Journal Year:
2018,
Volume and Issue:
17(7), P. 1595 - 1607
Published: Sept. 17, 2018
The
review
highlights
the
recent
advances
(2013-present)
in
use
of
earth-abundant
first
row
transition
metals
homogeneous
borrowing
hydrogen
catalysis.
utility
catalysts
based
on
Mn,
Fe,
Co,
Ni
and
Cu
to
promote
a
diverse
array
important
C-C
C-N
bond
forming
reactions
is
described,
including
discussion
reaction
mechanisms,
scope
limitations,
future
challenges
this
burgeoning
area
sustainable
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(1), P. 243 - 472
Published: Jan. 1, 2021
The
promising
aspects
of
iron
in
synthetic
chemistry
are
being
explored
for
three-four
decades
as
a
green
and
eco-friendly
alternative
to
late
transition
metals.
This
present
review
unveils
these
rich
iron-chemistry
towards
different
transformations.
