Iran) and his MS degree in Inorganic Chemistry at Zanjan University (Iran). He obtained his PhD (2003) and started his independentc areer at Tarbiat Modares University,w here he has been aProfessor in the Department of Chemistry since 2012. In recent years he has spent sabbaticalsa t Northwestern University (with J. Hupp and O. Farha), UC-Berkeley (with O. Farha), and Düsseldorf University (with C. Janiak). His research interestsf ocus on coordination polymers and metal-organic frameworks.Scheme 2. Charge storage mechanisms in EDLCs, PCs and battery-like electrodes.
Electrochemical water splitting is a mature technology for hydrogen generation. Numerous studies have focused on the development of highly efficiency electrocatalysts to produce hydrogen and oxygen from water electrolysis through...
Carbon dioxide (CO2) fixation
to generate chemicals
and fuels is of high current importance, especially toward finding
mild and efficient strategies for catalytic CO2 transformation
to value added products. Herein, we report a novel Lewis acid–base
bifunctional amine-functionalized dysprosium(III) metal–organic
framework [Dy3(data)3·2DMF]·DMF (2,5-data:
2,5-diamino-terephthalate), NH2-TMU-73. This compound was
fully characterized and its crystal structure reveals a 3D metal–organic
framework (MOF) with micropores and free NH2 groups capable
of promoting the chemical fixation of CO2 to cyclic carbonates.
NH2-TMU-73 is built from the Dy(III) centers and data2– blocks, which are arranged into an intricate underlying
net with a rare type of xah topology. After activation,
NH2-TMU-73 and its terephthalate-based analogue (TMU-73)
were applied for CO2-to-epoxide coupling reactions to produce
cyclic carbonates. Important features of this catalytic process concern
high efficiency and activity in the absence of cocatalyst, use of
solvent-free medium, atmospheric CO2 pressure, and ambient
temperature conditions. Also, NH2-TMU-73 features high
structural stability and can be recycled and reused in subsequent
catalytic tests. An important role of free amino groups and open metal
sites in the MOF catalyst was highlighted when suggesting a possible
reaction mechanism.
This study proposes an approach for
improving catalysis of oxidative
desulfurization (ODS) of diesel fuel under mild reaction conditions
and enhancing supercapacitor (SC) properties for storage of a high
amount of charge. Our approach takes advantage of a novel dual-purpose
cobalt(II)-based metal–organic framework (MOF), [Co(2-ATA)2(4-bpdb)4]
n
(2-ATA:
2-aminoterephthalic acid and 4-bpdb: N,N-bis-pyridin-4-ylmethylene-hydrazine as the pillar spacer), which
is called NH2-TMU-53. Due to the stability of the used
compound, we decided to evaluate the capability of this compound as
a novel electrode material for storing energy in supercapacitors,
and also to investigate its catalytic capabilities. It is demonstrated
that the addition of H2O2 as an oxidant enhances
the efficiency of sulfur removal, which indicates that NH2-TMU-53 can efficiently catalyze the ODS reaction. According to the
kinetics results, the catalyzed process follows pseudo-first-order
kinetics and exhibits 15.57 kJ mol–1 activation
energy. Moreover, with respect to the radical scavenging evaluations,
the process is governed by direct catalytic oxidation rather than
indirect oxidative attack of radicals. Furthermore, NH2-TMU-53 was applied as an electrode material for energy storage in
SCs. This material is used in the three-electrode system and shows
a specific capacitance of 325 F g–1 at 5 A g–1 current density. The asymmetric supercapacitor of
NH2-TMU-53//activated carbon evaluates the further electrochemical
activity in real applications, delivers the high power density (2.31
kW kg–1), high energy density (50.30 Wh kg–1), and long cycle life after 6000 cycles (90.7%). Also, the asymmetric
supercapacitor practical application was demonstrated by a glowing
red light-emitting diode and driving a mini-rotating motor. These
results demonstrate that the fabricated device presents a good capacity
for energy storage without pyrolyzing the MOF structures. These findings
can guide the development of high-performance SCs toward a new direction
to improve their practical applications and motivate application of
MOFs without pyrolysis or calcination.
In this work, a new 3D metal–organic framework
(MOF) {[Co3(μ4-tpa)3(μ-dapz)(DMF)2]·2DMF}
n
(Co(II)-TMU-63;
H2tpa = terephthalic acid, dapz = pyrazine-2,5-diamine,
DMF = dimethylformamide) containing low-cost and readily available
ligands was generated, fully characterized, and used as an electrode
material in supercapacitors without the need for a calcination process.
Thus, the synthesis of this material represents an economical and
cost-effective method in the energy field. The crystal structure of
Co(II)-TMU-63 is assembled from two types of organic building blocks
(μ4-tpa2– and μ-dapz ligands),
which arrange the cobalt nodes into a complex layer-pillared net with
an unreported 4,4,4,6T14 topology. The presence of open sites in this
MOF is promising for studying electrochemical activity and other types
of applications. In fact, Co(II)-TMU-63 as a novel electrode material
when comparing with pristine MOFs shows great cycling stability, large
capacity, and high energy density and so acts as an excellent supercapacitor
(384 F g–1 at 6 A g–1). In addition,
there was a stable cycling performance (90% capacitance) following
6000 cycles at 12 A g–1 current density. Also, the
Co(II)-TMU-63//activated carbon (AC) asymmetric supercapacitor acted
in a broad potential window of 1.7 V (0–1.7 V), exhibiting
a high performance with 4.42 kW kg–1 power density
(PD) and 24.13 Whkg–1 energy density (ED). These
results show that the pristine MOFs have great potential toward improving
different high-performance electrochemical energy storage devices,
without requiring the pyrolysis or calcination stages. Hence, such
materials are very promising for future advancement of the energy
field.
IIn the presence of fossil fuels, several environmental concerns e.g. energy shortage, environmental pollution, and global warming may occur in the present century. In this respect, supercapacitors have been introduced...
The universal pollution of diverse water bodies and declined water quality represent very important environmental problems. The development of new and efficient photocatalytic water treatment systems based on the Z-scheme mechanisms can contribute to tackling such problems. This study reports the preparation, full characterization, and detailed sonophotocatalytic activity of a new series of hybrid NU@ZIS nanocomposites, which comprise a p−n heterojunction of 3D Zr(IV) metal−organic framework nanorods (NU-1000) and photoactive ZnIn 2 S 4 (ZIS) nanostars. Among the obtained materials with varying content of ZIS (5, 10, 20, and 30%) on the surface of NU-1000, the NU@ ZIS20 nanocomposite revealed an ultrahigh catalytic performance and recyclability in a quick visible-light-induced degradation of the tetracycline antibiotic in water under sonophotocatalytic conditions. Moreover, increased activity of NU@ZIS20 can be ascribed to the formation of a p−n heterojunction between NU-1000 and ZIS, and a synergistic effect of these components, leading to a high level of radical production, facilitating a Z-scheme charge carrier transfer and reducing the recombination of charge carriers. The radical trapping tests revealed that • OH, • O 2 − , and h + are the major active species in the sonophotocatalytic degradation of tetracycline. Possible mechanism and mineralization pathways were introduced. Cytotoxicity of NU@ZIS20 and aquatic toxicity of water samples after tetracycline degradation were also assessed, showing good biocompatibility of the catalyst and efficacy of sonophotocatalytic protocols to produce water that does not affect the growth of bacteria. Finally, the obtained nanocomposites and developed photocatalytic processes can represent an interesting approach toward diverse environmental applications in water remediation and the elimination of other types of organic pollutants.
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