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Catalysts, Volume 8, Issue 5 (May 2018)

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Open AccessArticle Selective Reduction of Ketones and Aldehydes in Continuous-Flow Microreactor—Kinetic Studies
Catalysts 2018, 8(5), 221; https://doi.org/10.3390/catal8050221
Received: 24 April 2018 / Revised: 14 May 2018 / Accepted: 18 May 2018 / Published: 22 May 2018
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Abstract
In this work, the kinetics of Meerwein–Ponndorf–Verley chemoselective reduction of carbonyl compounds was studied in monolithic continuous-flow microreactors. To the best of our knowledge, this is the first report on the MPV reaction kinetics performed in a flow process. The microreactors are a
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In this work, the kinetics of Meerwein–Ponndorf–Verley chemoselective reduction of carbonyl compounds was studied in monolithic continuous-flow microreactors. To the best of our knowledge, this is the first report on the MPV reaction kinetics performed in a flow process. The microreactors are a very attractive alternative to the batch reactors conventionally used in this process. The proposed micro-flow system for synthesis of unsaturated secondary alcohols proved to be very efficient and easily controlled. The microreactors had reactive cores made of zirconium-functionalized silica monoliths of excellent catalytic properties and flow characteristics. The catalytic experiments were carried out with the use of 2-butanol as a hydrogen donor. Herein, we present the kinetic parameters of cyclohexanone reduction in a flow reactor and data on the reaction rate for several important ketones and aldehydes. The lack of diffusion constraints in the microreactors was demonstrated. Our results were compared with those from other authors and demonstrate the great potential of microreactor applications in fine chemical and complex intermediate manufacturing. Full article
(This article belongs to the Special Issue Catalytic Methods in Flow Chemistry)
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Open AccessArticle Effects of Synthesis on the Structural Properties and Methane Partial Oxidation Activity of Ni/CeO2 Catalyst
Catalysts 2018, 8(5), 220; https://doi.org/10.3390/catal8050220
Received: 10 April 2018 / Revised: 10 May 2018 / Accepted: 10 May 2018 / Published: 21 May 2018
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Abstract
Nickel catalysts supported on homemade CeO2 oxide were prepared by two procedures intending to achieve different degree of metal-support interaction. One method consisted of a co-precipitation that was assisted by microwave; the other method was based on a modified wetness impregnation in
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Nickel catalysts supported on homemade CeO2 oxide were prepared by two procedures intending to achieve different degree of metal-support interaction. One method consisted of a co-precipitation that was assisted by microwave; the other method was based on a modified wetness impregnation in the presence of the organic complexing ligand, nitrilotriacetic acid (NTA). The support and catalysts were characterized by temperature programmed reduction (TPR), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) techniques. Significant differences in the structure, in redox properties and in the elemental surface composition emerged. The catalytic behavior in the partial oxidation of methane was tested at atmospheric pressure, in a range of temperature between 400–800 °C, using diluted feed gas mixture with CH4/O2 = 2 and GHSV= 60,000 mL g−1 h−1. Moreover, the effect of the catalyst reduction pretreatment was investigated. The better catalytic performance of the microwave-assisted sample as compared to the NTA prepared sample was attributed to the stronger interaction of nickel with CeO2. Indeed, according to the structural and reducibility results, an adequate electronic contact between the metal and the support favors the formation of oxygen vacancies of ceria and inhibits the sintering of the catalyst active species, with an improvement of the catalytic performance. Full article
(This article belongs to the Special Issue Structure–Activity Relationships in Catalysis)
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Open AccessArticle Catalytic Ozonation by Iron Coated Pumice for the Degradation of Natural Organic Matters
Catalysts 2018, 8(5), 219; https://doi.org/10.3390/catal8050219
Received: 5 April 2018 / Revised: 14 May 2018 / Accepted: 15 May 2018 / Published: 21 May 2018
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Abstract
The use of iron-coated pumice (ICP) in heterogeneous catalytic ozonation significantly enhanced the removal efficiency of natural organic matters (NOMs) in water, due to the synergistic effect of hybrid processes when compared to sole ozonation and adsorption. Multiple characterization analyses (BET, TEM, XRD,
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The use of iron-coated pumice (ICP) in heterogeneous catalytic ozonation significantly enhanced the removal efficiency of natural organic matters (NOMs) in water, due to the synergistic effect of hybrid processes when compared to sole ozonation and adsorption. Multiple characterization analyses (BET, TEM, XRD, DLS, FT-IR, and pHPZC) were employed for a systematic investigation of the catalyst surface properties. This analysis indicated that the ICP crystal structure was α-FeOOH, the surface hydroxyl group of ICP was significantly increased after coating, the particle size of ICP was about 200–250 nm, the BET surface area of ICP was about 10.56 m2 g−1, the pHPZC value of ICP was about 7.13, and that enhancement by iron loading was observed in the FT-IR spectra. The contribution of surface adsorption, hydroxyl radicals, and sole ozonation to catalytic ozonation was determined as 21.29%, 66.22%, and 12.49%, respectively. The reaction kinetic analysis with tert-Butyl alcohol (TBA) was used as a radical scavenger, confirming that surface ferrous iron loading promoted the role of the hydroxyl radicals. The phosphate was used as an inorganic probe, and significantly inhibited the removal efficiency of catalytic NOM ozonation. This is an indication that the reactions which occur are more dominant in the solution phase. Full article
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Open AccessArticle Activation of Persulfate Using an Industrial Iron-Rich Sludge as an Efficient Nanocatalyst for Landfill Leachate Treatment
Catalysts 2018, 8(5), 218; https://doi.org/10.3390/catal8050218
Received: 3 April 2018 / Revised: 12 May 2018 / Accepted: 16 May 2018 / Published: 20 May 2018
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Abstract
In this research, the performance of nanomaterials obtained from the converter sludge (CS) of Esfahan Steel Company, Iran was investigated for the activation of persulfate (PS). The experiments were conducted on real and synthetic leachates. CS showed high catalytic activity for removal of
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In this research, the performance of nanomaterials obtained from the converter sludge (CS) of Esfahan Steel Company, Iran was investigated for the activation of persulfate (PS). The experiments were conducted on real and synthetic leachates. CS showed high catalytic activity for removal of chemical oxygen demand COD and NH3 because of its high iron oxide content. The effects of pH, CS dosage, and PS/COD ratio, temperature, and reaction time on the removal of COD and NH3 were evaluated to optimize operational conditions (pH 2, CS dosage: 1.2 g L−1, PS/COD: 4, and reaction time: 60 min). Maximum COD and NH3 removal efficiencies were 73.56 and 63.87%, respectively. Finally, the optimized process was applied for treatment of a real leachate sample. Although the treated leachate was not suitable to discharge into the environment, an increase in the 5-day biochemical oxygen demand (BOD5) and biodegradability (BOD5/COD) of leachate after treatment indicated that the effluent can be biologically treated. As a consequence, it can be combined with sewage or can be returned to the landfill. Full article
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Open AccessFeature PaperArticle Deep Eutectic Mixtures as Reaction Media for the Enantioselective Organocatalyzed α-Amination of 1,3-Dicarbonyl Compounds
Catalysts 2018, 8(5), 217; https://doi.org/10.3390/catal8050217
Received: 27 April 2018 / Revised: 15 May 2018 / Accepted: 16 May 2018 / Published: 18 May 2018
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Abstract
The enantioselective α-amination of 1,3-dicarbonyl compounds has been performed using deep eutectic solvents (DES) as a reaction media and chiral 2-amino benzimidazole-derived compounds as a catalytic system. With this procedure, the use of toxic volatile organic compounds (VOCs) as reaction media is avoided.
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The enantioselective α-amination of 1,3-dicarbonyl compounds has been performed using deep eutectic solvents (DES) as a reaction media and chiral 2-amino benzimidazole-derived compounds as a catalytic system. With this procedure, the use of toxic volatile organic compounds (VOCs) as reaction media is avoided. Furthermore, highly functionalized chiral molecules, which are important intermediates for the natural product synthesis, are synthetized by an efficient and stereoselective protocol. Moreover, the reaction can be done on a preparative scale, with the recycling of the catalytic system being possible for at least five consecutive reaction runs. This procedure represents a cheap, simple, clean, and scalable method that meets most of the principles to be considered a green and sustainable process. Full article
(This article belongs to the Special Issue Catalyzed Synthesis of Natural Products)
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Open AccessEditorial Biocatalysis and Biotransformations
Catalysts 2018, 8(5), 216; https://doi.org/10.3390/catal8050216
Received: 14 May 2018 / Revised: 14 May 2018 / Accepted: 17 May 2018 / Published: 17 May 2018
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(This article belongs to the Special Issue Biocatalysis and Biotransformations)
Open AccessArticle The Pros and Cons of Polydopamine-Sensitized Titanium Oxide for the Photoreduction of CO2
Catalysts 2018, 8(5), 215; https://doi.org/10.3390/catal8050215
Received: 17 April 2018 / Revised: 11 May 2018 / Accepted: 15 May 2018 / Published: 17 May 2018
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Abstract
Photocatalytic reduction of CO2 into fuels is a promising route to reduce greenhouse gas emission, and it demands high-performance photocatalysts that can use visible light in the solar spectrum. Due to its broadband light adsorption, polydopamine (PDA) is considered as a promising
[...] Read more.
Photocatalytic reduction of CO2 into fuels is a promising route to reduce greenhouse gas emission, and it demands high-performance photocatalysts that can use visible light in the solar spectrum. Due to its broadband light adsorption, polydopamine (PDA) is considered as a promising photo-sensitization material for semiconductor photocatalysts. In this work, titanium oxides have been coated with PDA through an in-situ oxidation polymerization method to pursue CO2 reduction under visible light. We have shown that the surface coated PDA with a thickness of around 1 nm can enhance the photocatalytic performance of anatase under visible light to reduce CO2 into CO. Assisted with additional UV-vis adsorption and photoluminescence characterizations, we confirmed the sensitization effect of PDA on anatase. Furthermore, our study shows that thicker PDA coating might not be favorable, as PDA could decompose under both visible and UV-vis light irradiations. 13C solid-state nuclear magnetic resonance showed structural differences between thin and thick PDA coatings and revealed compositional changes of PDA after light irradiation. Full article
(This article belongs to the Special Issue Nanomaterials for Environmental Purification and Energy Conversion)
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Open AccessReview Host-Guest Engineering of Layered Double Hydroxides towards Efficient Oxygen Evolution Reaction: Recent Advances and Perspectives
Catalysts 2018, 8(5), 214; https://doi.org/10.3390/catal8050214
Received: 29 March 2018 / Revised: 17 April 2018 / Accepted: 25 April 2018 / Published: 17 May 2018
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Abstract
Electrochemical water splitting has great potential in the storage of intermittent energy from the sun, wind, or other renewable sources for sustainable clean energy applications. However, the anodic oxygen evolution reaction (OER) usually determines the efficiency of practical water electrolysis due to its
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Electrochemical water splitting has great potential in the storage of intermittent energy from the sun, wind, or other renewable sources for sustainable clean energy applications. However, the anodic oxygen evolution reaction (OER) usually determines the efficiency of practical water electrolysis due to its sluggish four-electron process. Layered double hydroxides (LDHs) have attracted increasing attention as one of the ideal and promising electrocatalysts for water oxidation due to their excellent activity, high stability in basic conditions, as well as their earth-abundant compositions. In this review, we discuss the recent progress on LDH-based OER electrocatalysts in terms of active sites, host-guest engineering, and catalytic performances. Moreover, further developments and challenges in developing promising electrocatalysts based on LDHs are discussed from the viewpoint of molecular design and engineering. Full article
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Open AccessArticle The Role of Pulse Voltage Amplitude on Chemical Processes Induced by Streamer Discharge at Water Surface
Catalysts 2018, 8(5), 213; https://doi.org/10.3390/catal8050213
Received: 29 March 2018 / Revised: 5 May 2018 / Accepted: 11 May 2018 / Published: 17 May 2018
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Abstract
The paper reports the effects of pulse voltage amplitude on streamer discharge propagation at water surface. The subsequent chemical processes in a reactor following the surface discharges with different voltages are presented. A pulsed power modulator (PPM) system equipped with a control unit
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The paper reports the effects of pulse voltage amplitude on streamer discharge propagation at water surface. The subsequent chemical processes in a reactor following the surface discharges with different voltages are presented. A pulsed power modulator (PPM) system equipped with a control unit was employed to generate 0–25 kV pulses at 500 Hz. A point-plane electrode configuration was used for experiments, with the point electrode placed with 1 mm gap from the water surface in atmospheric air, and plane ground submerged with 30 mm gap in water. The streamer length at water surface was significantly influenced by the pulse voltage amplitude. Colorimetric measurement of hydrogen peroxide (H2O2) and treatment of indigo carmine organic dye solution were carried out to elucidate the chemical processes produced at various pulse voltages. The experimental results reveal that the applied voltage is a factor that greatly affects water surface discharges and their chemical processes. Full article
(This article belongs to the Special Issue Catalytic Wet-Air Oxidation Processes)
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Open AccessReview Nanostructured Oxides Synthesised via scCO2-Assisted Sol-Gel Methods and Their Application in Catalysis
Catalysts 2018, 8(5), 212; https://doi.org/10.3390/catal8050212
Received: 2 April 2018 / Revised: 3 May 2018 / Accepted: 9 May 2018 / Published: 17 May 2018
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Abstract
Nanostructured metal oxides and silicates are increasingly applied in catalysis, either as supports or as active species in heterogeneous catalysts, owing to the physicochemical properties that typically distinguish them from bulk oxides, such as higher surface area and a larger fraction of coordinatively
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Nanostructured metal oxides and silicates are increasingly applied in catalysis, either as supports or as active species in heterogeneous catalysts, owing to the physicochemical properties that typically distinguish them from bulk oxides, such as higher surface area and a larger fraction of coordinatively unsaturated sites at their surface. Among the different synthetic routes for preparing these oxides, sol-gel is a relatively facile and efficient method. The use of supercritical CO2 (scCO2) in the sol-gel process can be functional to the formation of nanostructured materials. The physical properties of the scCO2 medium can be controlled by adjusting the processing temperature and the pressure of CO2, thus enabling the synthesis conditions to be tuned. This paper provides a review of the studies on the synthesis of oxide nanomaterials via scCO2-assisted sol-gel methods and their catalytic applications. The advantages brought about by scCO2 in the synthesis of oxides are described, and the performance of oxide-based catalysts prepared by scCO2 routes is compared to their counterparts prepared via non-scCO2-assisted methods. Full article
(This article belongs to the Special Issue Sol–Gel Chemistry: A Toolbox for Catalyst Preparation)
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Open AccessArticle Catalytic Ozonation of Toluene Using Chilean Natural Zeolite: The Key Role of Brønsted and Lewis Acid Sites
Catalysts 2018, 8(5), 211; https://doi.org/10.3390/catal8050211
Received: 3 April 2018 / Revised: 24 April 2018 / Accepted: 2 May 2018 / Published: 17 May 2018
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Abstract
The influence of surface physical-chemical characteristics of Chilean natural zeolite on the catalytic ozonation of toluene is presented in this article. Surface characteristics of natural zeolite were modified by acid treatment with hydrochloric acid and ion-exchange with ammonium sulphate. Prior to catalytic ozonation
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The influence of surface physical-chemical characteristics of Chilean natural zeolite on the catalytic ozonation of toluene is presented in this article. Surface characteristics of natural zeolite were modified by acid treatment with hydrochloric acid and ion-exchange with ammonium sulphate. Prior to catalytic ozonation assays, natural and chemically modified zeolite samples were thermally treated at 623 and 823 K in order to enhance Brønsted and Lewis acid sites formation, respectively. Natural and modified zeolite samples were characterised by N2 adsorption at 77 K, elemental analysis, X-ray fluorescence, and Fourier transform infrared (FTIR) spectroscopy, using pyridine as a probe molecule. The highest values of the reaction rate of toluene oxidation were observed when NH4Z1 and 2NH4Z1 zeolite samples were used. Those samples registered the highest density values of Lewis acid sites compared to other samples used here. Results indicate that the presence of strong Lewis acid sites at the 2NH4Z1 zeolite surface causes an increase in the reaction rate of toluene oxidation, confirming the role of Lewis acid sites during the catalytic ozonation of toluene at room temperature. Lewis acid sites decompose gaseous ozone into atomic oxygen, which reacts with the adsorbed toluene at Brønsted acid sites. On the other hand, no significant contribution of Brønsted acid sites on the reaction rate was registered when NH4Z1 and 2NH4Z1 zeolite samples were used. Full article
(This article belongs to the Special Issue Catalytic Oxidation in Environmental Protection)
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Open AccessArticle Synthesis, Characterization of Nanosized ZnCr2O4 and Its Photocatalytic Performance in the Degradation of Humic Acid from Drinking Water
Catalysts 2018, 8(5), 210; https://doi.org/10.3390/catal8050210
Received: 31 March 2018 / Revised: 10 May 2018 / Accepted: 12 May 2018 / Published: 15 May 2018
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Abstract
Zinc chromite (ZnCr2O4) has been synthesized by the thermolysis of a new Zn(II)-Cr(III) oxalate coordination compound, namely [Cr2Zn(C2O4)4(OH2)6]·4H2O. The coordination compound has been characterized by
[...] Read more.
Zinc chromite (ZnCr2O4) has been synthesized by the thermolysis of a new Zn(II)-Cr(III) oxalate coordination compound, namely [Cr2Zn(C2O4)4(OH2)6]·4H2O. The coordination compound has been characterized by chemical analysis, infrared spectroscopy (IR), and thermal analysis. The zinc chromite obtained after a heating treatment of the coordination compound at 450 °C for 1 h has been investigated by XRD, FE-SEM, TEM/HR-TEM coupled with selected area electron diffraction (SAED) measurements. The photocatalytic performance of nanosized zinc chromite was assessed for the degradation and mineralization of humic acid (HA) from a drinking water source, envisaging the development of the advanced oxidation process for drinking water treatment technology. A mineralization efficiency of 60% was achieved after 180 min of 50 mg L−1 HA photocatalysis using zinc chromite under UV irradiation, in comparison with 7% efficiency reached by photolysis. Full article
(This article belongs to the Special Issue Nanomaterials for Environmental Purification and Energy Conversion)
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Open AccessArticle Improved CO-PROX Performance of CuO/CeO2 Catalysts by Using Nanometric Ceria as Support
Catalysts 2018, 8(5), 209; https://doi.org/10.3390/catal8050209
Received: 24 April 2018 / Revised: 11 May 2018 / Accepted: 11 May 2018 / Published: 15 May 2018
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Abstract
Despite of the huge number of papers about the catalytic preferential oxidation of CO (CO-PROX) for the purification of H2 streams, there is still a need for more effective catalysts in order to reduce the large required catalyst volume of CO-PROX unity.
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Despite of the huge number of papers about the catalytic preferential oxidation of CO (CO-PROX) for the purification of H2 streams, there is still a need for more effective catalysts in order to reduce the large required catalyst volume of CO-PROX unity. In this work, large surface area nanometric ceria was used as support for CuO/CeO2 catalysts with CuO load up to 10 wt % easily dispersed by wet impregnation. Catalysts were characterized by ICP-MS, XRD, SEM/EDS, N2 physisorption, H2 temperature programmed reduction (TPR), and CO2 temperature programmed desorption (TPD) and tested under different reaction conditions (including under feed containing inhibiting species such as CO2 and H2O). Catalytic tests revealed that our samples show high activity and selectivity even under stringent reaction conditions; moreover, they result among the most active catalysts when compared to those reported in the scientific literature. The high activity can be related to the enhanced amount of highly dispersed copper sites in strong interaction with ceria related to the nature of the nanometric support, as evidenced by the characterization techniques. Despite the high concentration of active copper sites, catalytic performance is limited by CO2 desorption from ceria in the neighborhood of copper sites, which prevents a further improvement. This suggests that new catalyst formulations should also provide a lower affinity towards CO2. Full article
(This article belongs to the Special Issue Catalysts for Hydrogen Purification for Fuel Cell Applications)
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Open AccessArticle Cross-Linked Enzyme Aggregates of Feruloyl Esterase Preparations from Thermothelomyces thermophila and Talaromyces wortmannii
Catalysts 2018, 8(5), 208; https://doi.org/10.3390/catal8050208
Received: 18 April 2018 / Revised: 10 May 2018 / Accepted: 10 May 2018 / Published: 15 May 2018
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Abstract
Cross-linked enzyme aggregates (CLEA®) technology is a well-established method in the current literature for the low-cost and effective immobilization of several enzymes. The main advantage of this particular method is the simplicity of the process, since it consists of only two
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Cross-linked enzyme aggregates (CLEA®) technology is a well-established method in the current literature for the low-cost and effective immobilization of several enzymes. The main advantage of this particular method is the simplicity of the process, since it consists of only two steps. However, CLEA immobilization must be carefully designed for each desired enzyme, since the optimum conditions for enzymes can vary significantly, according to their physicochemical properties. In the present study, an investigation of the optimum CLEA immobilization conditions was carried out for eight feruloyl esterase preparations. Feruloyl esterases are a very important enzyme group in the valorization of lignocellulosic biomass, since they act in a synergistic way with other enzymes for the breakdown of plant biomass. Specifically, we investigated the type and concentration of precipitant and the crosslinker concentration, for retaining optimal activity. FAE68 was found to be the most promising enzyme for CLEA immobilization, since in this case, the maximum retained activity, over 98%, was observed. Subsequently, we examined the operational stability and the stability in organic solvents for the obtained CLEA preparations, as well as their structure. Overall, our results support that the maximum activity retaining and the stability properties of the final CLEAs can vary greatly in different FAE preparations. Nevertheless, some of the examined FAEs show a significant potential for further applications in harsh industrial conditions. Full article
(This article belongs to the Special Issue Novel Enzyme and Whole-Cell Biocatalysis)
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Open AccessArticle Fe Oxides Loaded on Carbon Cloth by Hydrothermal Process as an Effective and Reusable Heterogenous Fenton Catalyst
Catalysts 2018, 8(5), 207; https://doi.org/10.3390/catal8050207
Received: 27 April 2018 / Revised: 9 May 2018 / Accepted: 10 May 2018 / Published: 15 May 2018
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Abstract
Iron based heterogeneous Fenton catalysts are attracting much attention for its economic and environmental friendly characteristics. In this study, iron oxides loaded carbon cloth (assigned as Fe@CC) was prepared using hydrothermal hydrolysis of Fe(NO3)3. The specific surface area of
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Iron based heterogeneous Fenton catalysts are attracting much attention for its economic and environmental friendly characteristics. In this study, iron oxides loaded carbon cloth (assigned as Fe@CC) was prepared using hydrothermal hydrolysis of Fe(NO3)3. The specific surface area of Fe@CC determined by N2 adsorption–desorption Brunauer–Emmett–Teller method was up to 1325.5 m2/g, which increased by 81.8% compared with that of native carbon cloth mainly due to the loading of iron oxide. XPS (X-ray photoelectron spectroscopy) spectra confirmed that the iron oxide on the carbon surface included mainly FeOOH. Its heterogeneous Fenton-like activity was determined using Acid Red G as a model substrate for degradation. Fe@CC maintained high and relatively stable activity during 11 tests, and it showed high COD (Chemical Oxygen Demand) removal efficiency and high apparent H2O2 utilization efficiency. The homogeneous Fenton reaction using the amount of leached Fe(III) suggested that the surficial reaction on Fe@CC was dominant. The stability and the mechanism for gradual decrease of activity during the first 4 tests were also discussed. Full article
(This article belongs to the Special Issue Catalytic Oxidation in Environmental Protection)
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