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Catalysts, Volume 8, Issue 9 (September 2018)

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Cover Story (view full-size image) Eliminative Azide–Olefin Cycloaddition (EAOC) Catalyzed by a Reusable IL/FeCl3 System to Synthesize [...] Read more.
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Open AccessReview Covalent Organic Frameworks: Promising Materials as Heterogeneous Catalysts for C-C Bond Formations
Catalysts 2018, 8(9), 404; https://doi.org/10.3390/catal8090404
Received: 28 August 2018 / Revised: 13 September 2018 / Accepted: 15 September 2018 / Published: 19 September 2018
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Abstract
Covalent organic frameworks (COFs) are defined as highly porous and crystalline polymers, constructed and connected via covalent bonds, extending in two- or three-dimension. Compared with other porous materials such as zeolite and active carbon, the versatile and alternative constituent elements, chemical bonding types
[...] Read more.
Covalent organic frameworks (COFs) are defined as highly porous and crystalline polymers, constructed and connected via covalent bonds, extending in two- or three-dimension. Compared with other porous materials such as zeolite and active carbon, the versatile and alternative constituent elements, chemical bonding types and characteristics of ordered skeleton and pore, enable the rising large family of COFs more available to diverse applications including gas separation and storage, optoelectronics, proton conduction, energy storage and in particular, catalysis. As the representative candidate of next-generation catalysis materials, because of their large surface area, accessible and size-tunable open nano-pores, COFs materials are suitable for incorporating external useful active ingredients such as ligands, complexes, even metal nanoparticles deposition and substrate diffusion. These advantages make it capable to catalyze a variety of useful organic reactions such as important C-C bond formations. By appropriate pore-engineering in COFs materials, even enantioselective asymmetric C-C bond formations could be realized with excellent yield and ee value in much shorter reaction time compared with their monomer and oligomer analogues. This review will mainly introduce and discuss the paragon examples of COFs materials for application in C-C bond formation reactions for the organic synthetic purpose. Full article
(This article belongs to the Special Issue Active Sites in Catalytic Reaction)
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Open AccessArticle Photooxidation of Cyclohexane by Visible and Near-UV Light Catalyzed by Tetraethylammonium Tetrachloroferrate
Catalysts 2018, 8(9), 403; https://doi.org/10.3390/catal8090403
Received: 2 August 2018 / Revised: 6 September 2018 / Accepted: 18 September 2018 / Published: 19 September 2018
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Abstract
Tetraethylammonium tetrachloroferrate catalyzes the photooxidation of cyclohexane heterogeneously, exhibiting significant photocatalysis even in the visible portion of the spectrum. The photoproducts, cyclohexanol and cyclohexanone, initially develop at constant rates, implying that the ketone and the alcohol are both primary products. The yield is
[...] Read more.
Tetraethylammonium tetrachloroferrate catalyzes the photooxidation of cyclohexane heterogeneously, exhibiting significant photocatalysis even in the visible portion of the spectrum. The photoproducts, cyclohexanol and cyclohexanone, initially develop at constant rates, implying that the ketone and the alcohol are both primary products. The yield is improved by the inclusion of 1% acetic acid in the cyclohexane. With small amounts of catalyst, the reaction rate increases with the amount of catalyst employed, but then passes through a maximum and decreases, due to increased reflection of the incident light. The reaction rate also passes through a maximum as the percentage of dioxygen above the sample is increased. This behavior is due to quenching by oxygen, which at the same time is a reactant. Under one set of reaction conditions, the photonic efficiency at 365 nm was 0.018 mol/Einstein. Compared to TiO2 as a catalyst, Et4N[FeCl4] generates lower yields at wavelengths below about 380 nm, but higher yields at longer wavelengths. Selectivity for cyclohexanol is considerably greater with Et4N[FeCl4], and oxidation does not proceed past cyclohexanone. Full article
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Open AccessArticle Synergistic Degradation of Dye Wastewaters Using Binary or Ternary Oxide Systems with Immobilized Laccase
Catalysts 2018, 8(9), 402; https://doi.org/10.3390/catal8090402
Received: 13 August 2018 / Revised: 8 September 2018 / Accepted: 15 September 2018 / Published: 18 September 2018
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Abstract
In recent years, groundwater contamination caused by dyes has become an important problem. They enter into wastewater as a result of the textile, automotive, or cosmetics industries. For this reason, new methods are being sought, which would aid at the removal of dye
[...] Read more.
In recent years, groundwater contamination caused by dyes has become an important problem. They enter into wastewater as a result of the textile, automotive, or cosmetics industries. For this reason, new methods are being sought, which would aid at the removal of dye impurities with high efficiency and also would be relatively cheap. In the presented study synthesized TiO2-ZrO2 (with TiO2:ZrO2 molar ratio of 8:2) and TiO2-ZrO2-SiO2 (with TiO2:ZrO2:SiO2 molar ratio of 8:1:1) oxide materials were used as supports for enzyme immobilization. Effective synthesis of the carriers was confirmed by results of scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), low-temperature nitrogen sorption and Fourier transform infrared spectroscopy (FTIR). The materials achieve high immobilization efficiency of the laccases from Trametes versicolor (83% and 96% for TiO2-ZrO2-laccase and TiO2-ZrO2-SiO2-laccase, respectively). The effect of selected dye concentrations, pH, temperature, and reusability were also tested. The obtained results showed that after removal of textile dyes, such as Alizarin Red S (ARS), Remazol Brilliant Blue R (RBBR), and Reactive Black 5 (RB5), under optimal process conditions, which were pH 5 and 25 °C, from dye solution of 5 mg/L degradation efficiency reached 100%, 91%, and 77%, respectively, suggesting synergistic mechanism of degradation by simultaneous sorption and catalytic action. Finally, reduction of chemical oxygen demand (COD) of the solution after treatment indicated lower mixture toxicity and effective dye degradation. Full article
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Open AccessArticle Immobilization of Chitosanases onto Magnetic Nanoparticles to Enhance Enzyme Performance
Catalysts 2018, 8(9), 401; https://doi.org/10.3390/catal8090401
Received: 7 September 2018 / Revised: 16 September 2018 / Accepted: 17 September 2018 / Published: 18 September 2018
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Abstract
In this study, chitosanase cloning from Streptomyces albolongus was fermented and purified by a Ni-NTA column. Fe3O4-SiO2 magnetite nanoparticles (MNPs) were synthesized by the co-precipitation method coating with silica via a sol-gel reaction and were then amino functioned
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In this study, chitosanase cloning from Streptomyces albolongus was fermented and purified by a Ni-NTA column. Fe3O4-SiO2 magnetite nanoparticles (MNPs) were synthesized by the co-precipitation method coating with silica via a sol-gel reaction and were then amino functioned by treating with 3-aminopropyltriethoxysilane. Chitosanases were immobilized onto the surface of MNPs by covalent bonding (MNPs@chitosanase). Transmission electron microscopy (TEM), Fourier transform infrared spectrometer (FT–IR), and magnetic measurements were used to illustrate the MNPs and immobilized chitosanase. The optimal conditions of immobilization were studied. The thermal, pH, and stabilities of immobilized chitosanase were tested and the results showed that the stabilities were significantly enhanced compared with free chitosanase. After being recycled 10 times, the residual activity of the immobilized chitosanase was 43.7% of the initial activity. Full article
(This article belongs to the Special Issue Biocatalysis for Industrial Applications)
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Open AccessArticle Biosynthesis of Nylon 12 Monomer, ω-Aminododecanoic Acid Using Artificial Self-Sufficient P450, AlkJ and ω-TA
Catalysts 2018, 8(9), 400; https://doi.org/10.3390/catal8090400
Received: 25 August 2018 / Revised: 14 September 2018 / Accepted: 15 September 2018 / Published: 18 September 2018
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Abstract
ω-Aminododecanoic acid is considered as one of the potential monomers of Nylon 12, a high-performance member of the bioplastic family. The biosynthesis of ω-aminododecanoic acid from renewable sources is an attractive process in the polymer industry. Here, we constructed three artificial self-sufficient P450s
[...] Read more.
ω-Aminododecanoic acid is considered as one of the potential monomers of Nylon 12, a high-performance member of the bioplastic family. The biosynthesis of ω-aminododecanoic acid from renewable sources is an attractive process in the polymer industry. Here, we constructed three artificial self-sufficient P450s (ArtssP450s) using CYP153A13 from Alcanivorax borkumensis and cytochrome P450 reductase (CPR) domains of natural self-sufficient P450s (CYP102A1, CYP102A5, and 102D1). Among them, artificial self-sufficient P450 (CYP153A13BM3CPR) with CYP102A1 CPR showed the highest catalytically activity for dodecanoic acid (DDA) substrate. This form of ArtssP450 was further co-expressed with ω-TA from Silicobacter pomeroyi and AlkJ from Pseudomonas putida GPo1. This single-cell system was used for the biotransformation of dodecanoic acid (DDA) to ω-aminododecanoic acid (ω-AmDDA), wherein we could successfully biosynthesize 1.48 mM ω-AmDDA from 10 mM DDA substrate in a one-pot reaction. The productivity achieved in the present study was five times higher than that achieved in our previously reported multistep biosynthesis method (0.3 mM). Full article
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Open AccessArticle Performance of Mn-Fe-Ce/GO-x for Catalytic Oxidation of Hg0 and Selective Catalytic Reduction of NOx in the Same Temperature Range
Catalysts 2018, 8(9), 399; https://doi.org/10.3390/catal8090399
Received: 28 July 2018 / Revised: 10 September 2018 / Accepted: 11 September 2018 / Published: 18 September 2018
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Abstract
A series of composites of Mn-Fe-Ce/GO-x have been synthesized by a hydrothermal method. Their performance in simultaneously performing the catalytic oxidation of Hg0 and the selective catalytic reduction of nitrogen oxides (NOx) in the same temperature range were investigated. In
[...] Read more.
A series of composites of Mn-Fe-Ce/GO-x have been synthesized by a hydrothermal method. Their performance in simultaneously performing the catalytic oxidation of Hg0 and the selective catalytic reduction of nitrogen oxides (NOx) in the same temperature range were investigated. In order to investigate the physicochemical properties and surface reaction, basic tests, including Brunauer-Emmett-Teller (BET), XRD, scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS) were selected. The results indicate that the active components deposited on graphene play an important role in the removal of mercury and NOx, with different valences. Especially, the catalyst of Mn-Fe-Ce/GO-20% possesses an excellent efficiency in the temperature range of 170 to 250 °C. Graphene has a huge specific surface area and good mechanical property; thus, the active components of the Mn-Fe-Ce catalyst can be highly dispersed on the surface of graphene oxide. In addition, the effects of O2, H2O, NO and SO2 on the removal efficiency of Hg0 were examined in flue gas. Furthermore, the regeneration experiments conducted by thermal methods proved to be promising methods. Full article
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Open AccessEditorial Catalytic Transformation of Lignocellulosic Platform Chemicals
Catalysts 2018, 8(9), 398; https://doi.org/10.3390/catal8090398
Received: 5 September 2018 / Revised: 11 September 2018 / Accepted: 11 September 2018 / Published: 16 September 2018
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(This article belongs to the Special Issue Catalytic Transformation of Lignocellulosic Platform Chemicals)
Open AccessArticle Hydrotreating of Light Cycle Oil over Supported on Porous Aromatic Framework Catalysts
Catalysts 2018, 8(9), 397; https://doi.org/10.3390/catal8090397
Received: 21 August 2018 / Revised: 12 September 2018 / Accepted: 12 September 2018 / Published: 14 September 2018
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Abstract
The hydroprocessing of substituted naphthalenes and light cycle oil (LCO) over bimetallic Ni-W-S and Ni-Mo-S catalysts that were obtained by decomposition of [N(n-Bu)4]2[Ni(MeS4)2] (Me = W, Mo) complexes in situ in the pores of mesoporous
[...] Read more.
The hydroprocessing of substituted naphthalenes and light cycle oil (LCO) over bimetallic Ni-W-S and Ni-Mo-S catalysts that were obtained by decomposition of [N(n-Bu)4]2[Ni(MeS4)2] (Me = W, Mo) complexes in situ in the pores of mesoporous aromatic frameworks (PAFs) during the reaction, was studied. The promotion of acid-catalyzed processes by PAF-AlCl3, synthesized by impregnation of a PAF with AlCl3 from its toluene solution, was investigated. It has been found that Ni-W-S catalytic systems were more active in the hydrodearomatization reactions, while Ni-Mo-S catalytic systems were more active in hydrodesulfurization and hydrocracking reactions. The introduction of sulfur into the reaction medium enhanced the activity of the catalysts and the presence of PAF-AlCl3 led to an acceleration of the hydrocracking processes. Full article
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Open AccessArticle Wetting Fraction in a Tubular Reactor with Solid Foam Packing and Gas/Liquid Co-Current Downflow
Catalysts 2018, 8(9), 396; https://doi.org/10.3390/catal8090396
Received: 5 August 2018 / Revised: 7 September 2018 / Accepted: 12 September 2018 / Published: 14 September 2018
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Abstract
The performance of fixed-bed reactors with structured catalysts depends heavily on the gas–liquid–solid contacting pattern. For a broad range of flow conditions, the liquid phase does not cover the solid surface of the packing homogeneously; this is known as partial wetting. The wetting
[...] Read more.
The performance of fixed-bed reactors with structured catalysts depends heavily on the gas–liquid–solid contacting pattern. For a broad range of flow conditions, the liquid phase does not cover the solid surface of the packing homogeneously; this is known as partial wetting. The wetting fraction in solid foams was obtained using a modified electrochemical measurement method with adaption of the limiting-current technique in different pre-wetting scenarios. The external wetting fraction, which is defined as fraction of the external solid-foam area covered by the liquid phase to the total external solid-foam area, is directly linked to the overall rate of reaction through the overall liquid mass transfer rate. The wetting fraction decreased with an increase in foam density, a process which was related to decreasing the strut thickness, increasing foam surface area, and consequently, decreasing the wetted area. Additionally, the results indicate that a better distribution of liquid and an increased wetting fraction occurred when a spray nozzle distributor was applied. A new wetting correlation for solid foams is proposed to estimate the wetting fraction with consideration of foam morphology and flow regime. Full article
(This article belongs to the Special Issue Structured Catalysts for Catalytic Processes Intensification)
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Open AccessReview Microemulsion-Based One-Step Electrochemical Fabrication of Mesoporous Catalysts
Catalysts 2018, 8(9), 395; https://doi.org/10.3390/catal8090395
Received: 1 September 2018 / Revised: 11 September 2018 / Accepted: 11 September 2018 / Published: 14 September 2018
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Abstract
Electrochemical technology has been proposed as an alternative or complementary method to classical inorganic synthesis for the fabrication of effective metallic solid catalysts. Microemulsion-based electrodeposition is a novel, fast, and one-step procedure to obtain mesoporous catalysts with extraordinarily effective areas, which can be
[...] Read more.
Electrochemical technology has been proposed as an alternative or complementary method to classical inorganic synthesis for the fabrication of effective metallic solid catalysts. Microemulsion-based electrodeposition is a novel, fast, and one-step procedure to obtain mesoporous catalysts with extraordinarily effective areas, which can be used in heterogeneous catalysis for degradation of pollutants and clean energy production. The fabrication process involves conducting microemulsions containing ionic species (dissolved in aqueous solutions) as precursors of the metallic catalysts. The presence of nanometric droplets of organic or ionic-liquid components in the microemulsion defines the mesoporosity of the catalysts during a one-step electrodeposition process. This method also allows the fabrication of metal catalysts as supported mesoporous films or mesoporous nanowires with very high effective areas. Additionally, reactants have excellent accessibility to the overall surface of the catalysts. The different catalysts fabricated with the help of this technology have been tested for competitive degradation of organic pollutants and anodes' materials for fuel cell devices. Full article
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Open AccessCommunication Synthesis of Stable Hierarchical MIL-101(Cr) with Enhanced Catalytic Activity in the Oxidation of Indene
Catalysts 2018, 8(9), 394; https://doi.org/10.3390/catal8090394
Received: 18 August 2018 / Revised: 4 September 2018 / Accepted: 11 September 2018 / Published: 13 September 2018
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Abstract
Nowadays, the controllable synthesis of stable hierarchical metal–organic frameworks (MOFs) is very important for practical applications, especially in catalysis. Herein, a well-known chromium–benzenedicarboxylate metal–organic framework, MIL-101(Cr), with a stable hierarchical structure, was produced by using phenylphosphonic acid (PPOA) as a modulator via the
[...] Read more.
Nowadays, the controllable synthesis of stable hierarchical metal–organic frameworks (MOFs) is very important for practical applications, especially in catalysis. Herein, a well-known chromium–benzenedicarboxylate metal–organic framework, MIL-101(Cr), with a stable hierarchical structure, was produced by using phenylphosphonic acid (PPOA) as a modulator via the hydrothermal method. The presence of phenylphosphonic acid could create structural defects and generate larger mesopores. The synthesized hierarchical MIL-101(Cr) possesses relatively good porosity, and the larger mesopores had widths of 4–10 nm. The hierarchical MIL-101(Cr) showed significant improvement for catalytic activity in the oxidation of indene. Further, the presence of a hierarchical structure could largely enhance large dye molecule uptake properties by impregnating. Full article
(This article belongs to the Special Issue Catalysis by Metal-Organic Frameworks)
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Open AccessCommunication A Zn-MOF-Catalyzed Terpolymerization of Propylene Oxide, CO2, and β-butyrolactone
Catalysts 2018, 8(9), 393; https://doi.org/10.3390/catal8090393
Received: 22 August 2018 / Revised: 5 September 2018 / Accepted: 11 September 2018 / Published: 13 September 2018
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Abstract
The terpolymerization of propylene oxide (PO), CO2, and a lactone is one of the prominent sustainable procedures for synthesizing thermoplastic materials at an industrial scale. Herein, the one-pot terpolymerization of PO, CO2, and β-butyrolactone (BBL) was achieved for the
[...] Read more.
The terpolymerization of propylene oxide (PO), CO2, and a lactone is one of the prominent sustainable procedures for synthesizing thermoplastic materials at an industrial scale. Herein, the one-pot terpolymerization of PO, CO2, and β-butyrolactone (BBL) was achieved for the first time using a heterogeneous nano-sized catalyst: zinc glutarate (ZnGA-20). The reactivity of both PO and BBL increased with the CO2 pressure, and the polyester content of the terpolymer poly (carbonate-co-ester) could be tuned by controlling the infeed ratio of PO to BBL. When the polyester content increased, the thermal stability of the polymers increased, whereas the glass transition temperature (Tg) decreased. Full article
(This article belongs to the Special Issue Catalysis by Metal-Organic Frameworks)
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Open AccessArticle A Facile Synthesis of Visible-Light Driven Rod-on-Rod like α-FeOOH/α-AgVO3 Nanocomposite as Greatly Enhanced Photocatalyst for Degradation of Rhodamine B
Catalysts 2018, 8(9), 392; https://doi.org/10.3390/catal8090392
Received: 22 August 2018 / Revised: 6 September 2018 / Accepted: 7 September 2018 / Published: 12 September 2018
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Abstract
In this work, we have synthesized the rod-on-rod–like α-FeOOH/α-AgVO3 nanocomposite photocatalysts with the different amounts of solvothermally synthesized α-FeOOH nanorods via a simple co-precipitation method. The as-synthesized photocatalysts were characterized by X-ray diffraction (XRD), Fourier-transform infrared (FT-IR) spectroscopy, UV−Visible diffuse reflectance spectroscopy,
[...] Read more.
In this work, we have synthesized the rod-on-rod–like α-FeOOH/α-AgVO3 nanocomposite photocatalysts with the different amounts of solvothermally synthesized α-FeOOH nanorods via a simple co-precipitation method. The as-synthesized photocatalysts were characterized by X-ray diffraction (XRD), Fourier-transform infrared (FT-IR) spectroscopy, UV−Visible diffuse reflectance spectroscopy, scanning electron microscopy (SEM), element mapping, high-resolution transmission electron microscopy (HR-TEM) and X-ray photoelectron spectroscopy (XPS) analysis. The observed SEM images show that both α-AgVO3 and α-FeOOH exhibits the rod-shaped morphology with nano size. Furthermore, the photocatalytic activities of the obtained photocatalysts were evaluated towards the degradation of Rhodamine B (RhB) under visible-light irradiation. It is demonstrated that the 3 mg α-FeOOH added to the α-FeOOH/α-AgVO3 nanocomposite exhibited an enhanced photocatalytic performance as compared with the pure α-AgVO3 and α-FeOOH. This significant improvement can be attributed to the increased photo-excited electron-hole pair separation efficiency, large portion of visible-light absorption ability and the reduced recombination of the electron-hole pair. The recycling test revealed that the optimized nanocomposite exhibited good photostability and reusability properties. In addition, the believable photodegradation mechanism of RhB using α-FeOOH/α-AgVO3 nanocomposite is proposed. Hence, the developed α-FeOOH/α-AgVO3 nanocomposite is a promising material for the degradation of organic pollutants in an aqueous environment. Full article
(This article belongs to the Special Issue Hybrid Catalysis)
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Open AccessFeature PaperCommunication Bio-Glycidol Conversion to Solketal over Acid Heterogeneous Catalysts: Synthesis and Theoretical Approach
Catalysts 2018, 8(9), 391; https://doi.org/10.3390/catal8090391
Received: 29 August 2018 / Revised: 7 September 2018 / Accepted: 7 September 2018 / Published: 11 September 2018
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Abstract
The present work deals with the novel use of heterogeneous catalysts for the preparation of solketal from bio-glycidol. Sustainable feedstocks and mild reaction conditions are considered to enhance the greenness of the proposed process. Nafion NR50 promotes the quantitative and selective acetalization of
[...] Read more.
The present work deals with the novel use of heterogeneous catalysts for the preparation of solketal from bio-glycidol. Sustainable feedstocks and mild reaction conditions are considered to enhance the greenness of the proposed process. Nafion NR50 promotes the quantitative and selective acetalization of glycidol with acetone. DFT calculations demonstrate that the favored mechanism consists in the nucleophilic attack of acetone to glycidol concerted with the ring opening assisted by the acidic groups on the catalyst and in the following closure of the five member ring of the solketal. Full article
(This article belongs to the Special Issue Catalytic Processes for The Valorisation of Biomass Derived Molecules)
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Open AccessArticle Enhanced Catalytic Dechlorination of 1,2-Dichlorobenzene Using Ni/Pd Bimetallic Nanoparticles Prepared by a Pulsed Laser Ablation in Liquid
Catalysts 2018, 8(9), 390; https://doi.org/10.3390/catal8090390
Received: 11 August 2018 / Revised: 4 September 2018 / Accepted: 7 September 2018 / Published: 10 September 2018
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Abstract
Bimetallic nanoparticles (NPs) exhibit advantageous electrical, optical, and catalytic properties. Among the various NP synthesis methods, pulsed laser ablation in liquid (PLAL) is currently attracting much attention because of its simplicity and versatility. In this study, a pulsed laser was used to produce
[...] Read more.
Bimetallic nanoparticles (NPs) exhibit advantageous electrical, optical, and catalytic properties. Among the various NP synthesis methods, pulsed laser ablation in liquid (PLAL) is currently attracting much attention because of its simplicity and versatility. In this study, a pulsed laser was used to produce nickel/palladium (Ni/Pd) bimetallic NPs in methanol and deionized water. The morphological and optical properties of the resulting Ni/Pd bimetallic NPs were characterized. The synthesized Ni/Pd bimetallic NPs were used for the dechlorination of 1,2-dichlorobenzene (1,2-DCB) under various conditions. The dechlorination rates of 1,2-DCB while using single (Ni and Pd) and bimetallic (Ni powder/Pd and Ni/Pd) NPs were investigated. The results showed that the Ni/Pd bimetallic NPs with 19.16 wt.% Pd exhibited much enhanced degradation efficiency for 1,2-DCB (100% degradation after 30 min). Accordingly, the results of enhanced the degradation of 1,2-DCB provide plausible mechanism insights into the catalytic reaction. Full article
(This article belongs to the Section Catalytic Materials)
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Open AccessArticle A Hybrid Reactor System Comprised of Non-Thermal Plasma and Mn/Natural Zeolite for the Removal of Acetaldehyde from Food Waste
Catalysts 2018, 8(9), 389; https://doi.org/10.3390/catal8090389
Received: 3 August 2018 / Revised: 30 August 2018 / Accepted: 8 September 2018 / Published: 10 September 2018
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Abstract
The degradation of low concentrations of acetaldehyde while using a non-thermal plasma (NTP)/catalyst hybrid reactor system was investigated while using humidified air at ambient temperature. A series of highly active manganese-impregnated natural zeolite (Mn/NZ) catalysts were synthesized by the incipient wetness method using
[...] Read more.
The degradation of low concentrations of acetaldehyde while using a non-thermal plasma (NTP)/catalyst hybrid reactor system was investigated while using humidified air at ambient temperature. A series of highly active manganese-impregnated natural zeolite (Mn/NZ) catalysts were synthesized by the incipient wetness method using sonication. The Mn/NZ catalysts were analyzed by Brunauer-Emmett-Teller surface area measurements and X-ray photoelectron spectroscopy. The Mn/NZ catalyst located at the downstream of a dc corona was used for the decomposition of ozone and acetaldehyde. The decomposition efficiency of ozone and acetaldehyde was increased significantly using the Mn/NZ catalyst with NTP. Among the various types of Mn/NZ catalysts with different Mn contents, the 10 wt.% Mn/NZ catalyst under the NTP resulted the highest ozone and acetaldehyde removal efficiency, almost 100% within 5 min. Moreover, this high efficiency was maintained for 15 h. The main reason for the high catalytic activity and stability was attributed to the high dispersion of Mn on the NZ made by the appropriate impregnation method using sonication. This system is expected to be efficient to decompose a wide range of volatile organic compounds with low concentrations. Full article
(This article belongs to the Special Issue Synthesis and Application of Zeolite Catalysts)
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Open AccessFeature PaperArticle Rational Design of High Surface Area Mesoporous Ni/CeO2 for Partial Oxidation of Propane
Catalysts 2018, 8(9), 388; https://doi.org/10.3390/catal8090388
Received: 4 August 2018 / Revised: 2 September 2018 / Accepted: 2 September 2018 / Published: 10 September 2018
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Abstract
A Ni loaded catalyst on mesoporous ceria, with a large surface area, prepared through the surfactant-assisted precipitation and impregnation method was investigated as an efficient catalyst for propane partial oxidation to produce synthesis gas. The results show that 2.5 wt% Ni/CeO2 had
[...] Read more.
A Ni loaded catalyst on mesoporous ceria, with a large surface area, prepared through the surfactant-assisted precipitation and impregnation method was investigated as an efficient catalyst for propane partial oxidation to produce synthesis gas. The results show that 2.5 wt% Ni/CeO2 had the optimum Ni loading, exhibiting the highest catalytic propane conversion. It also showed excellent stability, with no obvious activity drop after a 10 h time-on-stream reaction and slightly decreased in H2 and CO yields. The investigation of the reactant composition effect on carbon formation showed that by decreasing the C/O2 ratio the content of accumulated carbon decreased and propane conversion increased. The good activity of the Ni/CeO2 can be ascribed to the high surface area and rich surface defects of the ceria support and a high dispersion of active sites (Ni nanoparticles). Full article
(This article belongs to the Section Catalytic Materials)
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Open AccessArticle Production of New Isoflavone Glucosides from Glycosylation of 8-Hydroxydaidzein by Glycosyltransferase from Bacillus subtilis ATCC 6633
Catalysts 2018, 8(9), 387; https://doi.org/10.3390/catal8090387
Received: 24 August 2018 / Revised: 4 September 2018 / Accepted: 7 September 2018 / Published: 10 September 2018
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Abstract
8-Hydroxydaidzein (8-OHDe) has been proven to possess some important bioactivities; however, the low aqueous solubility and stability of 8-OHDe limit its pharmaceutical and cosmeceutical applications. The present study focuses on glycosylation of 8-OHDe to improve its drawbacks in solubility and stability. According to
[...] Read more.
8-Hydroxydaidzein (8-OHDe) has been proven to possess some important bioactivities; however, the low aqueous solubility and stability of 8-OHDe limit its pharmaceutical and cosmeceutical applications. The present study focuses on glycosylation of 8-OHDe to improve its drawbacks in solubility and stability. According to the results of phylogenetic analysis with several identified flavonoid-catalyzing glycosyltransferases (GTs), three glycosyltransferase genes (BsGT110, BsGT292 and BsGT296) from the genome of the Bacillus subtilis ATCC 6633 strain were cloned and expressed in Escherichia coli. The three BsGTs were then purified and the glycosylation activity determined toward 8-OHDe. The results showed that only BsGT110 possesses glycosylation activity. The glycosylated metabolites were then isolated with preparative high-performance liquid chromatography and identified as two new isoflavone glucosides, 8-OHDe-7-O-β-glucoside and8-OHDe-8-O-β-glucoside, whose identity was confirmed by mass spectrometry and nuclear magnetic resonance spectroscopy. The aqueous solubility of 8-OHDe-7-O-β-glucoside and 8-OHDe-8-O-β-glucoside is 9.0- and 4.9-fold, respectively, higher than that of 8-OHDe. Moreover, more than 90% of the initial concentration of the two 8-OHDe glucoside derivatives remained after 96 h of incubation in 50 mM of Tris buffer at pH 8.0. In contrast, the concentration of 8-OHDe decreased to 0.8% of the initial concentration after 96 h of incubation. The two new isoflavone glucosides might have potential in pharmaceutical and cosmeceutical applications. Full article
(This article belongs to the Special Issue Biocatalysis: Chemical Biosynthesis)
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Open AccessEditorial Immobilized Biocatalysts
Catalysts 2018, 8(9), 386; https://doi.org/10.3390/catal8090386
Received: 28 August 2018 / Accepted: 4 September 2018 / Published: 9 September 2018
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(This article belongs to the Special Issue Immobilized Biocatalysts) Printed Edition available
Open AccessArticle Toward the Sustainable Synthesis of Propanols from Renewable Glycerol over MoO3-Al2O3 Supported Palladium Catalysts
Catalysts 2018, 8(9), 385; https://doi.org/10.3390/catal8090385
Received: 17 August 2018 / Revised: 6 September 2018 / Accepted: 6 September 2018 / Published: 9 September 2018
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Abstract
The catalytic conversion of glycerol to value-added propanols is a promising synthetic route that holds the potential to overcome the glycerol oversupply from the biodiesel industry. In this study, selective hydrogenolysis of 10 wt% aqueous bio-glycerol to 1-propanol and 2-propanol was performed in
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The catalytic conversion of glycerol to value-added propanols is a promising synthetic route that holds the potential to overcome the glycerol oversupply from the biodiesel industry. In this study, selective hydrogenolysis of 10 wt% aqueous bio-glycerol to 1-propanol and 2-propanol was performed in the vapor phase, fixed-bed reactor by using environmentally friendly bifunctional Pd/MoO3-Al2O3 catalysts prepared by wetness impregnation method. The physicochemical properties of these catalysts were derived from various techniques such as X-ray diffraction, NH3-temperature programmed desorption, scanning electron microscopy, 27Al NMR spectroscopy, surface area analysis, and thermogravimetric analysis. The catalytic activity results depicted that a high catalytic activity (>80%) with very high selectivity (>90%) to 1-propanol and 2-propanol was obtained over all the catalysts evaluated in a continuously fed, fixed-bed reactor. However, among all others, 2 wt% Pd/MoO3-Al2O3 catalyst was the most active and selective to propanols. The synergic interaction between the palladium and MoO3 on Al2O3 support and high strength weak to moderate acid sites of the catalyst were solely responsible for the high catalytic activity. The maximum glycerol conversion of 88.4% with 91.3% selectivity to propanols was achieved at an optimum reaction condition of 210 C and 1 bar pressure after 3 h of glycerol hydrogenolysis reaction. Full article
(This article belongs to the Special Issue Catalysis by Precious Metals, Past and Future)
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Open AccessArticle NOx Removal by Selective Catalytic Reduction with Ammonia over a Hydrotalcite-Derived NiFe Mixed Oxide
Catalysts 2018, 8(9), 384; https://doi.org/10.3390/catal8090384
Received: 24 July 2018 / Revised: 5 September 2018 / Accepted: 6 September 2018 / Published: 8 September 2018
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Abstract
A series of NiFe mixed oxide catalysts were prepared via calcining hydrotalcite-like precursors for the selective catalytic reduction of nitrogen oxides (NOx) with NH3 (NH3-SCR). Multiple characterizations revealed that catalytic performance was highly dependent on the phase composition,
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A series of NiFe mixed oxide catalysts were prepared via calcining hydrotalcite-like precursors for the selective catalytic reduction of nitrogen oxides (NOx) with NH3 (NH3-SCR). Multiple characterizations revealed that catalytic performance was highly dependent on the phase composition, which was vulnerable to the calcination temperature. The MOx phase (M = Ni or Fe) formed at a lower calcination temperature would induce more favorable contents of Fe2+ and Ni3+ and as a result contribute to the better redox capacity and low-temperature activity. In comparison, NiFe2O4 phase emerged at a higher calcination temperature, which was expected to generate more Fe species on the surface and lead to a stable structure, better high-temperature activity, preferable SO2 resistance, and catalytic stability. The optimum NiFe-500 catalyst incorporated the above virtues and afforded excellent denitration (DeNOx) activity (over 85% NOx conversion with nearly 98% N2 selectivity in the region of 210–360 °C), superior SO2 resistance, and catalytic stability. Full article
(This article belongs to the Special Issue Ni-Containing Catalysts)
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Open AccessCommunication Two Possible Side Reaction Pathways during Furanic Etherification
Catalysts 2018, 8(9), 383; https://doi.org/10.3390/catal8090383
Received: 16 August 2018 / Revised: 6 September 2018 / Accepted: 6 September 2018 / Published: 8 September 2018
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Abstract
The revealing mechanism of side reactions is crucial for obtaining theoretical yield in industrialization when 2,5-bis(methoxymethyl)furan (BMMF) yield is above 95%. By-products catalyzed by the conventional ZSM-5 (C-ZSM-5) and hierarchical porous ZSM-5 (HP-ZSM-5) catalytic systems were different, and some key by-products were identified.
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The revealing mechanism of side reactions is crucial for obtaining theoretical yield in industrialization when 2,5-bis(methoxymethyl)furan (BMMF) yield is above 95%. By-products catalyzed by the conventional ZSM-5 (C-ZSM-5) and hierarchical porous ZSM-5 (HP-ZSM-5) catalytic systems were different, and some key by-products were identified. Thus, possible pathways were proposed, which helps to further improve BMMF selectivity. Additionally, HP-ZSM-5 exhibited quicker reaction rate, higher BMMF yield and selectivity, and slower deactivation process. The relatively weak acidity of HP-ZSM-5 suppresses the ring-opening reaction and subsequent side reactions, and introduction of mesopores improves mass transport and slightly increases hydration of 2,5-bis(hydroxymethyl)furan (BHMF). Full article
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Open AccessArticle Modeling the OEC with Two New Biomimetic Models: Preparations, Structural Characterization, and Water Photolysis Studies of a Ba–Mn Box Type Complex and a Mn4N6 Planar-Diamond Cluster
Catalysts 2018, 8(9), 382; https://doi.org/10.3390/catal8090382
Received: 28 July 2018 / Revised: 25 August 2018 / Accepted: 3 September 2018 / Published: 7 September 2018
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Abstract
The oxygen-evolving complex (OEC) is the native enzyme that catalyzes the oxidation of water in natural photosynthesis. Two new classes of manganese cluster complexes of formula Ba2Mn2L12(H3L1)2(CH3OH)4
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The oxygen-evolving complex (OEC) is the native enzyme that catalyzes the oxidation of water in natural photosynthesis. Two new classes of manganese cluster complexes of formula Ba2Mn2L12(H3L1)2(CH3OH)4 1 and Mn4L26Cl2 2 were prepared (H4L1 = N,N′-(ethane-1,2-diyl)bis(2-hydroxybenzamide); L2 = methyl picolinimidate) and characterized by standard techniques including microanalysis, IR spectroscopy, ESI spectrometry, and magnetic susceptibility measurements. X-ray diffraction studies of these complexes revealed (i) a box-type structure for 1 formed by two redox-active manganese(III) ions and two barium(II) ions connected by two bridging bisamido-bisphenoxy ligand molecules; and (ii) a planar-diamond array for Mn4N6 cluster 2 where the picolinimidates act as chelating ligands through the two nitrogen atoms. The ability of 1 and 2 to split water has been studied by means of water photolysis experiments. In these experiments, the oxygen evolution was measured in aqueous media in the presence of p-benzoquinone (acting as the hydrogen acceptor), the reduction of which was followed by UV-spectroscopy. The relevant photolytic activity found for 1 is in contrast to the inactivity of 2 in the photolytic experiments. This different behavior is discussed on the basis of the structure of the biomimetic models and the proposed reaction mechanism for this process supported by DFT calculations. Full article
(This article belongs to the Special Issue Photocatalytic Water Splitting)
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Open AccessArticle Theoretical Study on the Hydrogenation Mechanisms of Model Compounds of Heavy Oil in a Plasma-Driven Catalytic System
Catalysts 2018, 8(9), 381; https://doi.org/10.3390/catal8090381
Received: 6 August 2018 / Revised: 25 August 2018 / Accepted: 3 September 2018 / Published: 7 September 2018
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Abstract
Heavy oil will likely dominate the future energy market. Nevertheless, processing heavy oils using conventional technologies has to face the problems of high hydrogen partial pressure and catalyst deactivation. Our previous work reported a novel method to upgrade heavy oil using hydrogen non-thermal
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Heavy oil will likely dominate the future energy market. Nevertheless, processing heavy oils using conventional technologies has to face the problems of high hydrogen partial pressure and catalyst deactivation. Our previous work reported a novel method to upgrade heavy oil using hydrogen non-thermal plasma under atmospheric pressure without a catalyst. However, the plasma-driven catalytic hydrogenation mechanism is still ambiguous. In this work, we investigated the intrinsic mechanism of hydrogenating heavy oil in a plasma-driven catalytic system based on density functional theory (DFT) calculations. Two model compounds, toluene and 4-ethyltoluene have been chosen to represent heavy oil, respectively; a hydrogen atom and ethyl radical have been chosen to represent the high reactivity species generated by plasma, respectively. DFT study results indicate that toluene is easily hydrogenated by hydrogen atoms, but hard to hydrocrack into benzene and methane; small radicals, like ethyl radicals, are prone to attach to the carbon atoms in aromatic rings, which is interpreted as the reason for the increased substitution index of trap oil. The present work investigated the hydrogenation mechanism of heavy oil in a plasma-driven catalytic system, both thermodynamically and kinetically. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis for Energy Conversion)
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Open AccessArticle High Active and Selective Ni/CeO2–Al2O3 and Pd–Ni/CeO2–Al2O3 Catalysts for Oxy-Steam Reforming of Methanol
Catalysts 2018, 8(9), 380; https://doi.org/10.3390/catal8090380
Received: 2 August 2018 / Revised: 27 August 2018 / Accepted: 2 September 2018 / Published: 6 September 2018
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Abstract
Herein, we report monometallic Ni and bimetallic Pd–Ni catalysts supported on CeO2–Al2O3 binary oxide which are highly active and selective in oxy-steam reforming of methanol (OSRM). Monometallic and bimetallic supported catalysts were prepared by an impregnation method. The
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Herein, we report monometallic Ni and bimetallic Pd–Ni catalysts supported on CeO2–Al2O3 binary oxide which are highly active and selective in oxy-steam reforming of methanol (OSRM). Monometallic and bimetallic supported catalysts were prepared by an impregnation method. The physicochemical properties of the catalytic systems were investigated using a range of methods such as: Brunauer–Emmett–Teller (BET), X-ray Powder Diffraction (XRD), Temperature-programmed reduction (TPR–H2), Temperature-programmed desorption (TPD–NH3), X-ray photoelectron spectroscopy (XPS) and Scanning Electron Microscope equipped with an energy dispersive spectrometer (SEM–EDS). We demonstrate that the addition of palladium facilitates the reduction of nickel catalysts. The activity tests performed for all catalysts confirmed the promotion effect of palladium on the catalytic activity of nickel catalyst and their selectivity towards hydrogen production. Both nickel and bimetallic palladium–nickel supported catalysts showed excellent stability during the reaction. The reported catalytic systems are valuable to make advances in the field of fuel cell technology. Full article
(This article belongs to the Special Issue Catalysis in Steam Reforming)
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Open AccessReview Recent Advances in the Direct Synthesis of Hydrogen Peroxide Using Chemical Catalysis—A Review
Catalysts 2018, 8(9), 379; https://doi.org/10.3390/catal8090379
Received: 1 August 2018 / Revised: 26 August 2018 / Accepted: 28 August 2018 / Published: 5 September 2018
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Abstract
Hydrogen peroxide is an important chemical of increasing demand in today’s world. Currently, the anthraquinone autoxidation process dominates the industrial production of hydrogen peroxide. Herein, hydrogen and oxygen are reacted indirectly in the presence of quinones to yield hydrogen peroxide. Owing to the
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Hydrogen peroxide is an important chemical of increasing demand in today’s world. Currently, the anthraquinone autoxidation process dominates the industrial production of hydrogen peroxide. Herein, hydrogen and oxygen are reacted indirectly in the presence of quinones to yield hydrogen peroxide. Owing to the complexity and multi-step nature of the process, it is advantageous to replace the process with an easier and straightforward one. The direct synthesis of hydrogen peroxide from its constituent reagents is an effective and clean route to achieve this goal. Factors such as water formation due to thermodynamics, explosion risk, and the stability of the hydrogen peroxide produced hinder the applicability of this process at an industrial level. Currently, the catalysis for the direct synthesis reaction is palladium based and the research into finding an effective and active catalyst has been ongoing for more than a century now. Palladium in its pure form, or alloyed with certain metals, are some of the new generation of catalysts that are extensively researched. Additionally, to prevent the decomposition of hydrogen peroxide to water, the process is stabilized by adding certain promoters such as mineral acids and halides. A major part of today’s research in this field focusses on the reactor and the mode of operation required for synthesizing hydrogen peroxide. The emergence of microreactor technology has helped in setting up this synthesis in a continuous mode, which could possibly replace the anthraquinone process in the near future. This review will focus on the recent findings of the scientific community in terms of reaction engineering, catalyst and reactor design in the direct synthesis of hydrogen peroxide. Full article
(This article belongs to the Special Issue Direct Synthesis of Hydrogen Peroxide)
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Open AccessArticle The Preparation of Pd/Foam-Ni Electrode and Its Electrocatalytic Hydrodechlorination for Monochlorophenol Isomers
Catalysts 2018, 8(9), 378; https://doi.org/10.3390/catal8090378
Received: 21 August 2018 / Revised: 1 September 2018 / Accepted: 3 September 2018 / Published: 5 September 2018
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Abstract
Noble metal palladium modified foamed nickel electrode (Pd/foam-Ni) was prepared by electrodeposition method. The fabricated electrode showed better catalytic performance than the Pd/foam-Ni prepared by conventional electroless deposition. The catalysts were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy
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Noble metal palladium modified foamed nickel electrode (Pd/foam-Ni) was prepared by electrodeposition method. The fabricated electrode showed better catalytic performance than the Pd/foam-Ni prepared by conventional electroless deposition. The catalysts were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). Electrocatalytic activity of the Pd/Ni was studied for the hydrodechlorination of monochlorophenol isomers. The Pd/Ni exhibited good catalytic activity for 3-chlorophenol (3-CP). Complete decomposition of chlorophenol isomers could be achieved within 2 h, and the hydrodechlorination process conformed to the pseudo-first-order kinetic model. It showed a supreme stability after recycling for 5 times. The Pd/Ni exhibited a promising application prospect with high effectiveness and low Pd loading. Full article
(This article belongs to the Special Issue Platinum-Free Electrocatalysts)
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Open AccessFeature PaperArticle Optimization and Tunability of 2D Graphene and 1D Carbon Nanotube Electrocatalysts Structure for PEM Fuel Cells
Catalysts 2018, 8(9), 377; https://doi.org/10.3390/catal8090377
Received: 3 August 2018 / Revised: 21 August 2018 / Accepted: 25 August 2018 / Published: 5 September 2018
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Abstract
In this work, N-doped Multi-Walled Carbon Nanotubes (MWCNTs) and Few Graphene Layers (FGLs) have been functionalized with platinum nanoparticles using two methods starting with hexachloroplatinic acid as precursor: (i) ethylene glycol (EG) reduction and (ii) impregnation followed by reduction in hydrogen atmosphere. Morphological
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In this work, N-doped Multi-Walled Carbon Nanotubes (MWCNTs) and Few Graphene Layers (FGLs) have been functionalized with platinum nanoparticles using two methods starting with hexachloroplatinic acid as precursor: (i) ethylene glycol (EG) reduction and (ii) impregnation followed by reduction in hydrogen atmosphere. Morphological scanning transmission electron microscopy (STEM) analyses showed a homogenous dispersion of metal particles with narrow-size distribution onto both carbon supports (Pt/C loadings between 30 wt % and 40 wt %). Electrocatalytic properties of the as-synthetized catalysts toward the Oxygen Reduction Reaction (ORR) was evaluated in aqueous electrolyte using a three electrodes electrochemical cell by cyclic voltammetry (CV) in rotating disk electrode (RDE). It is shown that a mixture of Pt supported on MWCNT and FGLs allows to enhance both the electrochemical surface area and the activity of the catalyst layer. Ageing tests performed on that optimized active layer showed higher stability than conventional Pt/C. Full article
(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)
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Open AccessArticle Synthesis of High Crystalline TiO2 Nanoparticles on a Polymer Membrane to Degrade Pollutants from Water
Catalysts 2018, 8(9), 376; https://doi.org/10.3390/catal8090376
Received: 27 July 2018 / Revised: 22 August 2018 / Accepted: 3 September 2018 / Published: 5 September 2018
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Abstract
Titanium dioxide (TiO2) is described as an established material to remove pollutants from water. However, TiO2 is still not applied on a large scale due to issues concerning, for example, the form of use or low photocatalytic activity. We present
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Titanium dioxide (TiO2) is described as an established material to remove pollutants from water. However, TiO2 is still not applied on a large scale due to issues concerning, for example, the form of use or low photocatalytic activity. We present an easily upscalable method to synthesize high active TiO2 nanoparticles on a polyethersulfone microfiltration membrane to remove pollutants in a continuous way. For this purpose, titanium(IV) isopropoxide was mixed with water and hydrochloric acid and treated up to 210 °C. After cooling, the membrane was simply dip-coated into the TiO2 nanoparticle dispersion. Standard characterization was undertaken (i.e., X-ray powder diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, water permeance, contact angle). Degradation of carbamazepine and methylene blue was executed. By increasing synthesis temperature crystallinity and photocatalytic activity elevates. Both ultrasound modification of nanoparticles and membrane pre-modification with carboxyl groups led to fine distribution of nanoparticles. The ultrasound-treated nanoparticles gave the highest photocatalytic activity in degrading carbamazepine and showed no decrease in degradation after nine times of repetition. The TiO2 nanoparticles were strongly bound to the membrane. Photocatalytic TiO2 nanoparticles with high activity were synthesized. The innovative method enables a fast and easy nanoparticle production, which could enable the use in large-scale water cleaning. Full article
(This article belongs to the Special Issue Photocatalytic Membrane Reactors)
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Open AccessArticle Ce and Zr Modified WO3-TiO2 Catalysts for Selective Catalytic Reduction of NOx by NH3
Catalysts 2018, 8(9), 375; https://doi.org/10.3390/catal8090375
Received: 21 August 2018 / Revised: 25 August 2018 / Accepted: 3 September 2018 / Published: 5 September 2018
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Abstract
A series of Ce and/or Zr modified WO3-TiO2 catalysts were synthesized by the impregnation method, which were employed for NH3-SCR reaction. The T50 contour lines of NOx were used to quickly optimize catalyst composition, the Ce20Zr12.5WTi
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A series of Ce and/or Zr modified WO3-TiO2 catalysts were synthesized by the impregnation method, which were employed for NH3-SCR reaction. The T50 contour lines of NOx were used to quickly optimize catalyst composition, the Ce20Zr12.5WTi catalyst was considered to be the optimization result, and also exhibited excellent NH3-SCR activity and thermal stability with broad operation temperature window, which is a very promising catalyst for NOx abatement from diesel engine exhaust. The excellent catalytic performance is associated with the formation of Ce-Zr solid solution. The introduction of Zr to CeWTi catalyst facilitated the redox of Ce4+/Ce3+ and the formation of more acid sites, more Ce3+ ions, more oxygen vacancies, larger quantities of surface adsorbed oxygen species and NH3, which were beneficial for the excellent selective catalytic reduction (SCR) performance. Full article
(This article belongs to the Special Issue Catalytic Applications of CeO2-Based Materials)
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