Encapsulation of H4SiW12O40 into an Amide-Functionalized MOF: A Highly Efficient Nanocomposite Catalyst for Oxidative Desulfurization of Diesel Fuel
Mingyuzhi Sun,
Reza Abazari,
Jing Chen
et al.
Abstract:Production of hydrocarbon fuels containing sulfur in ultralow levels is in high demand and requires the development of novel catalytic systems for oxidative desulfurization (ODS). Herein, a new nanocomposite SiW 12 @ZSTU-10 catalyst containing H 4 SiW 12 O 40 (SiW 12 ) encapsulated into a zinc(II) 3D metal−organic framework (MOF) (ZSTU-10) was assembled and characterized. The intricate structure and porosity of ZSTU-10 permit efficient encapsulation of the catalytically active SiW 12 cages. The impact of diffe… Show more
“…The FT-IR spectra of bimetallic ZnV-MOFs contain the same characteristic absorption bands as those observed for the initial Zn-MOF material (Figure b). The samples share a broad band at 3145–3720 cm –1 , attributed to the stretching vibrations of O–H groups. , At a wavenumber of 3110 cm –1 , a band derived from N–H stretching vibration was detected. , The low-intensity bands at wavenumbers in the 2283–2963 cm –1 range, corresponding to the −CH 3 /–CH 2 – stretching vibrations, were also registered. In addition, the FT-IR spectra revealed bands at 1589 and 1465 cm –1 assigned to the asymmetric and symmetric vibrations of the carboxylic groups, respectively. , Each MOF sample exhibited a band at ∼1380 cm –1 , derived from the stretching vibrations of the C–H bonds.…”
Urea oxidation reaction (UOR) is one of the potential routes in which urea-rich wastewater is used as a source of energy for hydrogen production. Metal−organic frameworks (MOFs) have promising applications in electrocatalytic processes, although there are still challenges in identifying the MOFs' molecular regulation and obtaining practical catalytic systems. The current study sought to synthesize [Zn 6 (IDC) 4 (OH) 2 (Hprz) 2 ] n (Zn-MOF) with three symmetrically independent Zn(II) cations connected via linear N-donor piperazine (Hprz), rigid planar imidazole-4,5-dicarboxylate (IDC 3− ), and −OH ligands, revealing the 3,4T1 topology. The optimized noblemetal-free Zn 0.33 V 0.66 -MOF/NF electrocatalysts show higher robustness and performance compared to those of the parent Zn monometallic MOF/NF electrode and other bimetallic MOFs with different Zn−V molar ratios. The low potential of 1.42 V (vs RHE) at 50 mA cm −2 in 1.0 M KOH with 0.33 M urea required by the developed Zn 0.33 V 0.66 -MOF electrode makes its application in the UOR more feasible. The availability of more exposed active sites, ion diffusion path, and higher conductivity result from the distinctive configuration of the synthesized electrocatalyst, which is highly stable and capable of synergistic effects, consequently enhancing the desired reaction. The current research contributes to introducing a practical, cost-effective, and sustainable solution to decompose urea-rich wastewater and produce hydrogen.
“…The FT-IR spectra of bimetallic ZnV-MOFs contain the same characteristic absorption bands as those observed for the initial Zn-MOF material (Figure b). The samples share a broad band at 3145–3720 cm –1 , attributed to the stretching vibrations of O–H groups. , At a wavenumber of 3110 cm –1 , a band derived from N–H stretching vibration was detected. , The low-intensity bands at wavenumbers in the 2283–2963 cm –1 range, corresponding to the −CH 3 /–CH 2 – stretching vibrations, were also registered. In addition, the FT-IR spectra revealed bands at 1589 and 1465 cm –1 assigned to the asymmetric and symmetric vibrations of the carboxylic groups, respectively. , Each MOF sample exhibited a band at ∼1380 cm –1 , derived from the stretching vibrations of the C–H bonds.…”
Urea oxidation reaction (UOR) is one of the potential routes in which urea-rich wastewater is used as a source of energy for hydrogen production. Metal−organic frameworks (MOFs) have promising applications in electrocatalytic processes, although there are still challenges in identifying the MOFs' molecular regulation and obtaining practical catalytic systems. The current study sought to synthesize [Zn 6 (IDC) 4 (OH) 2 (Hprz) 2 ] n (Zn-MOF) with three symmetrically independent Zn(II) cations connected via linear N-donor piperazine (Hprz), rigid planar imidazole-4,5-dicarboxylate (IDC 3− ), and −OH ligands, revealing the 3,4T1 topology. The optimized noblemetal-free Zn 0.33 V 0.66 -MOF/NF electrocatalysts show higher robustness and performance compared to those of the parent Zn monometallic MOF/NF electrode and other bimetallic MOFs with different Zn−V molar ratios. The low potential of 1.42 V (vs RHE) at 50 mA cm −2 in 1.0 M KOH with 0.33 M urea required by the developed Zn 0.33 V 0.66 -MOF electrode makes its application in the UOR more feasible. The availability of more exposed active sites, ion diffusion path, and higher conductivity result from the distinctive configuration of the synthesized electrocatalyst, which is highly stable and capable of synergistic effects, consequently enhancing the desired reaction. The current research contributes to introducing a practical, cost-effective, and sustainable solution to decompose urea-rich wastewater and produce hydrogen.
“…MOFs provide considerably large surface areas, consistent adjustable pore sizes, and significant pore volumes. At the same time, they can also perform various tasks as their metal nodes and ligands are easily modified, 68 making them suitable candidates as catalysts and electrode materials. 69–71 MOFs have evenly distributed catalytic sites, large surface areas, open channels for substrate diffusion to access the active sites, and highly recyclable structures (Fig.…”
Section: Structures and Characteristics Of Mofsmentioning
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“…Metal–organic frameworks (MOFs) represent a category of remarkably permeable and crystalline substances characterized by fascinating structures. These materials exhibit broad possibilities for utilization in gas storage and segregation, catalysis, and optical and sensing applications. − By the incorporation of emissive organic connectors or metal clusters, it is possible to produce porous MOF constructions that exhibit intriguing luminescent properties. These unique metal–organic frameworks, referred to as LMOFs, have attracted considerable attention in recent years due to their extensive photophysical features and immense potential for sensing applications in various areas. − Owing to the remarkable degree of precision in controlling both structure and composition by utilizing a wide range of organic linkers and metal clusters, energy transfer LMOFs are highly promising for numerous luminescence recognition applications.…”
In
this study, a stable and luminescent UiO-66-NH2 (UN) and its derivative Cu2+@UN were
prepared and utilized successfully as an Off–On luminescent
sensing platform for effective, selective, as well as rapid (5 min)
detection of l-Histidine (l-His). The UN reveals efficient quenching in the presence of Cu2+ ions
through photoinduced electron transition (PET) mechanism as a dynamic
quenching process (in the range of 0.01–1 mM) forming Cu2+@UN sensing platform. However, due to the remarkable
affinity between l-His and Cu2+, the luminescence
of Cu2+@UN is recovered in the presence of l-His indicating Turn-On behavior via a quencher detachment
mechanism (QD). A good linear relationship between the l-His
concentration and luminescence intensity was observed in the range
of 0.01–40 μM (R
2 = 0.9978)
with a detection limit of 7 nM for l-His sensing. The suggested
method was successfully utilized for l-His determination
in real samples with good recoveries and satisfying consequences.
Moreover, the result indicates that only l-His induces a
significant luminescence restoration of Cu2+@UN and that the signal is significantly greater than that of the other
amino acids. Also, the portable test paper based on bacterial cellulose
(BC) as the Cu2+@UNBC sensing platform was
developed to conveniently evaluate the effective detection of l-His.
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