Green Chemistry,
Journal Year:
2024,
Volume and Issue:
26(13), P. 7891 - 7901
Published: Jan. 1, 2024
Here,
we
propose
and
demonstrate
an
air/metal
hydride
battery
with
the
function
of
both
treating
acid–base
wastewaters
gathering
waste
heat
energy
in
form
electricity.
Ni-PyH-catalyzed
regioselective
synthesis
of
α-benzyl
substituted
β-hydroxy
ketones
is
reported
via
a
Fenton
free-radical
reaction.
Protocol
enables
facile
access
to
products
in
good
excellent
yields
toluene
at
room
temperature
100
°C.
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 11, 2025
Replacing
the
oxygen
evolution
reaction
(OER)
in
CO2
electrolysis
with
an
energetically
and
economically
favorable
alternative
is
very
promising.
Yet,
understanding
paired
organic
oxidation
environment
for
reduction
particularly
challenging,
as
monitoring
multiple
side
reactions
problematic.
Herein,
we
examined
of
ethylene
glycol
(EG),
one
simplest
polyols,
a
model
on
series
nickel
oxyhydroxide
catalysts
(β-NiMxOOH,
M
=
Ni,
Co,
Fe,
Cu).
Using
situ
techniques,
including
surface-enhanced
infrared
absorption
spectroscopy
(SEIRAS)
differential
electrochemical
mass
spectrometry
(DEMS),
together
various
ex
approaches,
obtained
potential-resolved
quantitative
information
comprising
OER,
overoxidation
to
CO/CO2,
catalyst
dissolution,
from
electrolyte
decarbonation.
Many
factors
impurity
cations,
pH,
potential
can
substantially
influence
product
distribution
reactions.
Such
influences
are
nearly
identical
both
electrocatalytic
chemical-electrochemical
pathways.
The
optimized
system
achieve
stable
high
Faradaic
efficiencies
formate
(∼100%),
glycolaldehyde
(∼86%),
glycolate
(∼66%),
respectively.
Importantly,
easily
suffer
higher
energy
consumption
than
conventional
counterpart,
provided
unregulated.
Yet
modulated
consumed
21.1%
less
even
when
separation
was
considered.
This
work
reveals
unique
electrolysis,
opening
up
opportunities
designing
efficient
systems
real-life
applications.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(11), P. 8922 - 8929
Published: May 27, 2024
Transition
metals,
such
as
nickel
(Ni),
cobalt
(Co),
and
iron
(Fe),
exhibit
catalytic
activity
for
electrochemical
oxidation
under
basic
conditions.
In
this
study,
we
demonstrate
the
highly
selective
of
primary
alcohols
to
aldehydes
using
Ni,
Co,
Fe
catalysts
in
an
anion-exchange
membrane
(AEM)
reactor.
Our
findings
indicate
that
non-noble
metal
can
be
utilized
electrocatalytic
by
leveraging
conditions
do
not
corrode
these
metals.
addition,
prepared
binary
alloys
oxide
investigated
their
abilities
alcohol
oxidation.
The
results
controlling
oxygen
evolution
reaction
potential
through
composition
ratio
catalyst
avoiding
interference
with
desired
are
crucial
increasing
yield
products.
Furthermore,
despite
nature
sites,
selectively
yielded
corresponding
aldehydes,
which
was
attributed
unique
triple-phase
interfacial
sites
AEM
Biodiesel
plays
a
key
role
in
achieving
economy-wide
decarbonization
but
its
production
discharges
significant
amounts
of
CO2
and
glycerol-laden
wastewater.
Given
the
increasing
abundance
biodiesel
wastewater
low
redox
potential
glycerol,
coupling
glycerol
oxidation
reaction
(GOR)
with
electrolysis
has
emerged
as
an
attractive
strategy
to
achieve
sustainable
management,
utilization,
green
chemical
synthesis
single
unit
process.
Despite
need
for
highly
stable
catalysts,
few
studies
have
examined
electrocatalyst
deactivation
environmental
waste
streams.
Here,
we
present
first-of-a-kind
diagnostic
study
that
investigates
nickel
(Ni)
catalyst
stability
during
GOR
synthetic
wastewaters.
A
current
decline
99.7%
was
observed
within
24
h
operation.
This
coincided
80%
decrease
surface
active
Ni(II)/Ni(III)
concentrations,
190-fold
increases
interfacial
impedance,
appearance
electrode
C-bonds
suggested
coverage
by
reactants
intermediates
likely
main
contributor
loss
catalytic
activity.
Analyses
more
complex
electrolytes
containing
methanol
oleate
emergence
distinct
mechanisms
through
restricted
NiOOH
formation.
Altogether,
this
details
several
previously
unreported
mechanisms.
These
findings
can
ultimately
help
inform
future
design
toward
practical
valorization.
The Journal of Physical Chemistry C,
Journal Year:
2024,
Volume and Issue:
128(23), P. 9556 - 9565
Published: June 1, 2024
Redox-active
metal
oxides
are
prevalent
in
the
fields
of
thermal,
photo-,
and
electrocatalysis.
Thermodynamics
proton-coupled
electron
transfer
(PCET)
reactions
at
their
surfaces
critical,
as
they
scale
with
activity
a
catalyst.
The
free
energy
H
atom
binding
on
catalyst
surface
is
employed
catalytic
descriptor
for
H2,
O2,
many
others.
structural
heterogeneity
ambiguity
sites
have
largely
precluded
understanding
exact
redox-active
sites,
challenging
chemists
to
design
structure
down
atomic
level.
Here,
we
report
electrochemically
determined
stoichiometry
thermodynamics
PCET
cerium-based
metal–organic
framework
(MOF),
Ce-MOF-808.
Cyclic
voltammograms
(CVs)
MOF-deposited
electrodes
aqueous
buffers
various
pHs
revealed
Faradaic
couple
that
can
be
ascribed
Ce4+/3+
redox.
Plotting
half-wave
potential
(E1/2)
against
electrolyte
pH
resulted
Pourbaix
diagram
slope
65
±
9
mV/pH,
suggesting
1H+/1e–
stoichiometry.
Using
thermochemical
analogy
between
one
(H•),
hexanuclear
Ce6
node,
Ce3+O–H
bond
dissociation
(BDFE),
was
calculated
78
2
kcal
mol–1.
In-silico
calculations
quantitatively
corroborated
our
BDFE
measurements.
Furthermore,
multiple
proton
topologies
were
computationally
elucidated
exhibit
BDFEs
similar
experimental
values,
agreeing
wide
features
all
CVs,
implicating
system
has
substantial
distribution.
To
best
understanding,
this
first
measurement
MOF-liquid
interface.
Implications
presented
measurements
catalysis
using
MOFs
discussed.
Journal of Materials Chemistry A,
Journal Year:
2023,
Volume and Issue:
11(32), P. 17237 - 17245
Published: Jan. 1, 2023
Using
differential
electrochemical
mass
spectrometry
(DEMS),
carbon
oxidation
monitoring
in
alkaline
media
with
sensitive
detection
of
CO
2
is
enabled
and
a
simple
strategy
to
suppress
corrosion
offered.