The synthesis of various commodity chemicals like cyclic urea,
urethanes, and carbamates via effective utilization of CO2 has proved to be highly advantageous. Production of the chemicals
mentioned above from CO2 requires a complicated catalyst
design and stringent reaction conditions. A simple catalyst possessing
suitable sites that can effectively adsorb and activate CO2 is required to synthesize these valuable chemicals. The catalyst
should also have optimum acidity for amine adsorption to facilitate
these reactions. This study demonstrates the synthesis of a highly
efficient catalyst, Ce-BTC MOF-derived CeO2, for CO2 activation. Ce-BTC-MOF is synthesized and calcined to obtain
Ce-BTC MOF-derived CeO2. The presence of various facets
and the oxygen vacancy required for CO2 activation and
adsorption is confirmed using Raman spectroscopy, X-ray photoelectron
spectroscopy (XPS), and high-resolution transmission electron microscopy
(HRTEM). CO2 adsorption efficiency is evaluated using the
adsorption experiments. The acidity and basicity of the catalyst are
evaluated using the temperature-programmed desorption (TPD) analysis.
Cyclic urea is produced by the reaction of diamine and CO2 at low CO2 pressure, while the CO2 and amino
alcohol reaction produce cyclic urethane. The reaction between CO2 and primary amine produces carbamate. The calcination of
Ce-BTC MOF at 573 K generates a CeO2 catalyst, which offers
an excellent activity for producing these chemicals. Ce-BTC MOF-derived
CeO2 exhibits efficient recyclability and stability. The
developed ecofriendly and robust catalyst will be of significant scientific
interest because it can be industrially deployed in producing these
commercial synthetic intermediates.
The catalytic transformation of the lignocellulosic biomass to different platform chemicals has paved the way to reduce global fossil fuel dependence. Biorefineries largely rely on utilizing acid catalysts and hydrogenation/oxidation...
2-Methylfuran obtained via the hydrogenation of furfural is an important biomass-derived liquid fuel. However, the large-scale production of 2-methylfuran from furfural requires cost-effective, active, and selective heterogeneous catalysts. Herein, we...
The insertion of CO produces useful chemicals such as urethanes, cyclic carbonates, and cyclic urea using CO2 or urea as a sacrificial source. Synthesis of these chemicals using CO2 as...
The development of an economical transition metalbased catalyst for photocatalytic carbon−carbon coupling reactions is aspiring. Herein, a Cu−Ce metal−organic framework (MOF) was synthesized and carbonized to produce bimetallic Cu 2 O−CeO 2 /C, which was utilized in the Sonogashira cross-coupling reaction. The defects and oxygen vacancies in the catalyst were characterized by Xray photoelectron spectroscopy and Raman spectroscopy, while the nature of Cu was characterized by H 2 -TPR analysis. The defectinduced MOF-derived Cu−Ce heterojunction created more oxygen vacancies (O V ) in CeO 2 , revealing the high photocatalytic activity. The Cu−Ce heterojunction (Cu 2 O−CeO 2 /C) formed a Cu(I)− phenylacetylide active complex and exhibited higher catalytic activity for the visible light-induced Sonogashira cross-coupling reaction. 25% Cu 2 O−CeO 2 /C offered 93.8% phenylacetylene conversion with a 94.2% Sonogashira product selectivity by using household light-emitting diodes. No discernible activity loss was observed from the recycling of the catalyst. Based on catalytic activity, control reactions, and physicochemical and optoelectronic characterization, the structure−activity relationship was established and a reaction mechanism was proposed. Replacement of the costly Pd metal-based catalyst with a cheap Cu 2 O−CeO 2 -based catalyst for the synthesis of commercially important compounds with a sustainable visible light-induced catalytic process will be highly attractive to chemists and industrialists.
The hydrogenation of lignin-derived phenolics to produce
valuable
chemicals is a promising but challenging task. This study successfully
demonstrates the use of sustainable transition metal-based catalysts
to hydrogenate lignin-derived phenolics. A defect-induced oxygen vacancy
containing H-NbO
x
prepared from commercial
Nb2O5 was employed as a catalyst. H-NbO
x
exhibited higher oxygen vacancies (158.21
μmol/g) than commercial Nb2O5 (39.01 μmol/g),
evaluated from O2-TPD. Upon supporting 10 wt % Ni, a Ni/NiO
interface was formed over H-NbO
x
, which
was intrinsically active for the hydrogenation of phenolics. 10Ni/H-NbO
x
exhibited a two-fold increase in activity
than 10Ni/Nb2O5, achieving >99% eugenol conversion
and affording ∼94% 4-propyl cyclohexanol selectivity, wherein
∼63% eugenol conversion and ∼73% 4-propyl cyclohexanol
selectivity were obtained over 10Ni/Nb2O5. The
Ni/NiO formation was confirmed by X-ray photoelectron spectroscopy,
HR-TEM, and H2-TPR analysis, while the oxygen vacancies
were verified by Raman spectroscopy and O2-TPD analysis.
The resulting interface enhanced the synergy between Ni and H-NbO
x
and facilitated hydrogen dissociation, confirmed
by H2-TPD. Remarkably, 10Ni/H-NbO
x
maintained its catalytic activity for five tested cycles and
demonstrated exceptional activity with various phenolics. Our findings
highlight the potential of a sustainable transition metal catalyst
for the hydrogenation of lignin-derived phenolic compounds, which
could pave the path to producing valuable chemicals in an environmentally
friendly manner.
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