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Catalysts, Volume 7, Issue 4 (April 2017)

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Cover Story (view full-size image) The increasing demand for highly efficient, visible-light-active photocatalysts can be addressed by [...] Read more.
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Open AccessArticle Preparation of Rh/Ni Bimetallic Nanoparticles and Their Catalytic Activities for Hydrogen Generation from Hydrolysis of KBH4
Catalysts 2017, 7(4), 125; https://doi.org/10.3390/catal7040125
Received: 20 March 2017 / Revised: 16 April 2017 / Accepted: 18 April 2017 / Published: 23 April 2017
Cited by 4 | PDF Full-text (5358 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
ISOBAM-104 protected Rh/Ni bimetallic nanoparticles (BNPs) of 3.1 nm in diameter were synthesized by a co-reduction method with a rapid injection of KBH4 solution. The catalytic activities of as-prepared BNPs for hydrogen generation from hydrolysis of a basic KBH4 solution were
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ISOBAM-104 protected Rh/Ni bimetallic nanoparticles (BNPs) of 3.1 nm in diameter were synthesized by a co-reduction method with a rapid injection of KBH4 solution. The catalytic activities of as-prepared BNPs for hydrogen generation from hydrolysis of a basic KBH4 solution were evaluated. Ultraviolet-visible spectrophotometry (UV-Vis), transmission electron microscopy (TEM), and high-resolution transmission electron microscopy (HRTEM) were employed to characterize the structure, particle size, and chemical composition of the resultant BNPs. Catalytic activities for hydrolysis of KBH4 and catalytic kinetics of prepared BNPs were also investigated. It was shown that Rh/Ni BNPs displayed much higher catalytic activities than that of Rh or Ni monometallic nanoparticles (MNPs), and the prepared Rh10Ni90 BNPs possessed the highest catalytic activities with a value of 11580 mol-H2·h−1·mol-Rh−1. The high catalytic activities of Rh/Ni BNPs could be attributed to the electron transfer effect between Rh and Ni atoms, which was confirmed by a density functional theory (DFT) calculation. The apparent activation energy for hydrogen generation of the prepared Rh10Ni90 BNPs was about 47.2 ± 2.1 kJ/mol according to a kinetic study. Full article
(This article belongs to the Special Issue Small Molecule Activation and Catalysis)
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Open AccessArticle In Search of Governing Gas Flow Mechanism through Metal Solid Foams
Catalysts 2017, 7(4), 124; https://doi.org/10.3390/catal7040124
Received: 9 February 2017 / Revised: 11 April 2017 / Accepted: 17 April 2017 / Published: 21 April 2017
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Abstract
Solid foams have been intensely studied as promising structured catalytic internals. However, mechanisms governing flow and transport phenomena within the foam structures have not been properly addressed in the literature. The aim of this study was to consider such flow mechanisms based on
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Solid foams have been intensely studied as promising structured catalytic internals. However, mechanisms governing flow and transport phenomena within the foam structures have not been properly addressed in the literature. The aim of this study was to consider such flow mechanisms based on our experimental results on flow resistance. Two mechanisms were considered: developing laminar flow in a short capillary channel (flow-through model), and flow around an immersed solid body, either a cylinder or sphere (flow-around model). Flow resistance experiments were performed on three aluminum foams of 10, 20, and 40 PPI (pores per inch), using a 57 mm ID test column filled with the foams studied. The foam morphology was examined using microtomography and optical microscopy to derive the geometric parameters applied in the model equations. The flow-through model provided an accuracy of 25% for the experiments. The model channel diameter was the foam cell diameter, and the channel length was the strut thickness. The accuracy of the flow-around model was only slightly worse (35%). It was difficult to establish the geometry of the immersed solid body (sphere or cylinder) because experiment characteristics tended to change from sphere to cylinder with increasing PPI value. Full article
(This article belongs to the Special Issue Structured and Micro-Structured Catalysts and Reactors)
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Open AccessArticle A Simple and Efficient Process for Large Scale Glycerol Oligomerization by Microwave Irradiation
Catalysts 2017, 7(4), 123; https://doi.org/10.3390/catal7040123
Received: 28 February 2017 / Revised: 29 March 2017 / Accepted: 11 April 2017 / Published: 19 April 2017
Cited by 1 | PDF Full-text (1491 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
Herein, an optimized method for 100 g scale synthesis of glycerol oligomers using a microwave multimode source and the low priced K2CO3 as catalyst is reported. This method allows the complete conversion of glycerol to its oligomers in only 30
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Herein, an optimized method for 100 g scale synthesis of glycerol oligomers using a microwave multimode source and the low priced K2CO3 as catalyst is reported. This method allows the complete conversion of glycerol to its oligomers in only 30 min, yielding molecular weights up to 1000 g mol−1. Furthermore, a simple iterative purification process, involving the precipitation of the crude product in acetone and methanol, affords a final product composed of larger oligomers with a narrow dispersity (D < 1.5). Full article
(This article belongs to the Special Issue Catalysis of Biomass-Derived Molecules)
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Open AccessArticle Promotive Effect of Sn2+ on Cu0/Cu+ Ratio and Stability Evolution of Cu/SiO2 Catalyst in the Hydrogenation of Dimethyl Oxalate
Catalysts 2017, 7(4), 122; https://doi.org/10.3390/catal7040122
Received: 26 March 2017 / Revised: 13 April 2017 / Accepted: 14 April 2017 / Published: 19 April 2017
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Abstract
The influence of Sn2+doping on the structure and performance of silica supported copper catalyst was systematically investigated and characterised. Catalytic evaluation showed that the suitable content of Sn2+ introduced into a Cu/SiO2 catalyst evidently improved the catalytic activity and
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The influence of Sn2+doping on the structure and performance of silica supported copper catalyst was systematically investigated and characterised. Catalytic evaluation showed that the suitable content of Sn2+ introduced into a Cu/SiO2 catalyst evidently improved the catalytic activity and stability of ethylene glycol synthesis from dimethyl oxalate. X-ray diffraction and X-ray auger electron spectroscopy indicated that the Cu0/Cu+ ratio gradually increased with increasing Sn2+ content, and an appropriate proportion of Cu0/Cu+ ratio played a very significant role in this reaction. Transmission electron microscopy revealed that the active copper particles in the Cu-xSn/SiO2 catalyst were smaller than those of the Cu/SiO2 catalyst. This result may be due to the introduction of Sn2+ species transformed into SnO2. Furthermore, SnO2 effectively segregated the active copper. These effects are beneficial in inhibiting the aggregation of copper in the catalysts, thereby improving the stability of the catalyst and prolonging the life span. Full article
(This article belongs to the Special Issue Small Molecule Activation and Catalysis)
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Open AccessFeature PaperReview Merging Metallic Catalysts and Sonication: A Periodic Table Overview
Catalysts 2017, 7(4), 121; https://doi.org/10.3390/catal7040121
Received: 8 March 2017 / Revised: 7 April 2017 / Accepted: 14 April 2017 / Published: 19 April 2017
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Abstract
This account summarizes and discusses recent examples in which the combination of ultrasonic waves and metal-based reagents, including metal nanoparticles, has proven to be a useful choice in synthetic planning. Not only does sonication often enhance the activity of the metal catalyst/reagent, but
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This account summarizes and discusses recent examples in which the combination of ultrasonic waves and metal-based reagents, including metal nanoparticles, has proven to be a useful choice in synthetic planning. Not only does sonication often enhance the activity of the metal catalyst/reagent, but it also greatly enhances the synthetic transformation that can be conducted under milder conditions relative to conventional protocols. For the sake of clarity, we have adopted a structure according to the periodic-table elements or families, distinguishing between bulk metal reagents and nanoparticles, as well as the supported variations, thus illustrating the characteristics of the method under consideration in target synthesis. The coverage focuses essentially on the last decade, although the discussion also strikes a comparative balance between the more recent advancements and past literature. Full article
(This article belongs to the Special Issue Enabling Technologies toward Green Catalysis)
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Open AccessArticle Quantitative Structure-Thermostability Relationship of Late Transition Metal Catalysts in Ethylene Oligo/Polymerization
Catalysts 2017, 7(4), 120; https://doi.org/10.3390/catal7040120
Received: 23 February 2017 / Revised: 30 March 2017 / Accepted: 14 April 2017 / Published: 18 April 2017
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Abstract
Quantitative structure–thermostability relationship was carried out for four series of bis(imino)pyridine iron (cobalt) complexes and α-diimine nickel complexes systems in ethylene oligo/polymerization. Three structural parameters were correlated with thermal stability, including bond order of metal-nitrogen (B), minimum distance (D
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Quantitative structure–thermostability relationship was carried out for four series of bis(imino)pyridine iron (cobalt) complexes and α-diimine nickel complexes systems in ethylene oligo/polymerization. Three structural parameters were correlated with thermal stability, including bond order of metal-nitrogen (B), minimum distance (D) between central metal and ortho-carbon atoms on the aryl moiety and dihedral angle (α) of a central five-membered ring. The variation degree of catalytic activities between optimum and room temperatures (AT) was calculated to describe the thermal stability of the complex. By multiple linear regression analysis (MLRA), the thermal stability presents good correlation with three structural parameters with the correlation coefficients (R2) over 0.95. Furthermore, the contributions of each parameter were evaluated. Through this work, it is expected to help the design of a late transition metal complex with thermal stability at the molecular level. Full article
(This article belongs to the Special Issue Computational Methods and Their Application in Catalysis)
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Open AccessArticle Microwave-Assisted Synthesis of Co3(PO4)2 Nanospheres for Electrocatalytic Oxidation of Methanol in Alkaline Media
Catalysts 2017, 7(4), 119; https://doi.org/10.3390/catal7040119
Received: 16 January 2017 / Revised: 11 April 2017 / Accepted: 12 April 2017 / Published: 17 April 2017
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Abstract
Low-cost and high-performance advanced electrocatalysts for direct methanol fuel cells are of key significance for the improvement of environmentally-pleasant energy technologies. Herein, we report the facile synthesis of cobalt phosphate (Co3(PO4)2) nanospheres by a microwave-assisted process and
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Low-cost and high-performance advanced electrocatalysts for direct methanol fuel cells are of key significance for the improvement of environmentally-pleasant energy technologies. Herein, we report the facile synthesis of cobalt phosphate (Co3(PO4)2) nanospheres by a microwave-assisted process and utilized as an electrocatalyst for methanol oxidation. The phase formation, morphological surface structure, elemental composition, and textural properties of the synthesized (Co3(PO4)2) nanospheres have been examined by powder X-ray diffraction (XRD), Fourier transform-infrared spectroscopy (FT-IR), field emission-scanning electron microscopy (FE-SEM), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), and nitrogen adsorption-desorption isotherm investigations. The performance of an electrocatalytic oxidation of methanol over a Co3(PO4)2 nanosphere-modified electrode was evaluated in an alkaline solution using cyclic voltammetry (CV) and chronopotentiometry (CP) techniques. Detailed studies were made for the methanol oxidation by varying the experimental parameters, such as catalyst loading, methanol concentration, and long-term stability for the electro-oxidation of methanol. The good electrocatalytic performances of Co3(PO4)2 should be related to its good surface morphological structure and high number of active surface sites. The present investigation illustrates the promising application of Co3(PO4)2 nanospheres as a low-cost and more abundant electrocatalyst for direct methanol fuel cells. Full article
(This article belongs to the Special Issue Enabling Technologies toward Green Catalysis)
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Open AccessArticle SO42−/Sn-MMT Solid Acid Catalyst for Xylose and Xylan Conversion into Furfural in the Biphasic System
Catalysts 2017, 7(4), 118; https://doi.org/10.3390/catal7040118
Received: 22 February 2017 / Revised: 1 April 2017 / Accepted: 11 April 2017 / Published: 17 April 2017
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Abstract
A sulphated tin ion-exchanged montmorillonite (SO42−/Sn-MMT) was successfully prepared by the ion exchange method of montmorillonite (MMT) with SnCl4, followed by the sulphation. This catalysis was applied as a solid acid catalyst for the heterogeneous catalytic transformations of
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A sulphated tin ion-exchanged montmorillonite (SO42−/Sn-MMT) was successfully prepared by the ion exchange method of montmorillonite (MMT) with SnCl4, followed by the sulphation. This catalysis was applied as a solid acid catalyst for the heterogeneous catalytic transformations of xylose and xylan into furfural in the bio-based 2-methyltetrahydrofuran/H2O biphasic system. These prepared catalysts were characterized by X-ray powder diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), temperature programmed desorption of ammonia (NH3-TPD), pyridine adsorbed Fourier transform infrared spectroscopy (Py-FTIR), element analysis (EA) and Brunauer-Emmett-Teller (BET) method. Their catalytic performance for xylose and xylan into furfural was also investigated. The reaction parameters such as the initial xylose and xylan concentration, the amounts of catalyst, the organic-to-aqueous phase volume ratio, the reaction temperature and time were studied to optimize the reaction conditions. Results displayed that SO42−/Sn-MMT contained both Brønsted acid and Lewis acid sites, and SO42− ions were contributive to the formation of stronger Brønsted acid sites, which could improve the reaction efficiency. Reaction parameters had significant influence on the furfural production. The substitution of water by the saturated NaCl solution in the aqueous phase also had an important effect on the xylose and xylan conversion. The highest furfural yields were achieved up to 79.64% from xylose and 77.35% from xylan under the optimized reaction conditions (160 °C, 120 min; 160 °C, 90 min). Moreover, the prepared catalyst was stable and was reused five times with a slight decrease (10.0%) of the furfural yield. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis for Environmental Remediation)
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Open AccessArticle Novel Synthesis of Plasmonic Ag/AgCl@TiO2 Continues Fibers with Enhanced Broadband Photocatalytic Performance
Catalysts 2017, 7(4), 117; https://doi.org/10.3390/catal7040117
Received: 28 February 2017 / Revised: 2 April 2017 / Accepted: 13 April 2017 / Published: 17 April 2017
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Abstract
The plasmonic Ag/AgCl@TiO2 fiber (S-CTF) photocatalyst was synthesized by a two-step approach, including the sol-gel and force spinning method for the preparation of TiO2 fibers (TF), and the impregnation-precipitation-photoreduction strategy for the deposition of Ag/AgCl onto the fibers. NaOH aqueous solution
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The plasmonic Ag/AgCl@TiO2 fiber (S-CTF) photocatalyst was synthesized by a two-step approach, including the sol-gel and force spinning method for the preparation of TiO2 fibers (TF), and the impregnation-precipitation-photoreduction strategy for the deposition of Ag/AgCl onto the fibers. NaOH aqueous solution was utilized to hydrolyze TiCl4, to synthesize TF and remove the byproduct HCl, and the produced NaCl was recycled for the formation and deposition of Ag/AgCl. The surface morphology, specific surface area, textural properties, crystal structure, elemental compositions and optical absorption of S-CTF were characterized by a series of instruments. These results revealed that the AgCl and Ag0 species were deposited onto TF successfully, and the obtained S-CTF showed improved visible light absorption due to the surface plasmon resonance of Ag0. In the photocatalytic degradation of X-3B, S-CTF exhibited significantly enhanced activities under separate visible or UV light irradiation, in comparison to TF. Full article
(This article belongs to the Special Issue Titanium Dioxide Photocatalysis)
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Open AccessArticle Hydrothermal Fabrication of High Specific Surface Area Mesoporous MgO with Excellent CO2 Adsorption Potential at Intermediate Temperatures
Catalysts 2017, 7(4), 116; https://doi.org/10.3390/catal7040116
Received: 5 March 2017 / Revised: 10 April 2017 / Accepted: 11 April 2017 / Published: 15 April 2017
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Abstract
In this work, we report on a novel sodium dodecyl sulfate (SDS)-assisted magnesium oxide (MgO)-based porous adsorbent synthesized by hydrothermal method for intermediate CO2 capture. For industrial MgO, its CO2 adsorption capacity is normally less than 0.06 mmol g−1,
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In this work, we report on a novel sodium dodecyl sulfate (SDS)-assisted magnesium oxide (MgO)-based porous adsorbent synthesized by hydrothermal method for intermediate CO2 capture. For industrial MgO, its CO2 adsorption capacity is normally less than 0.06 mmol g−1, with a specific surface area as low as 25.1 m2 g−1. Herein, leaf-like MgO nanosheets which exhibited a disordered layer structure were fabricated by the introduction of SDS surfactants and the control of other synthesis parameters. This leaf-like MgO adsorbent showed an excellent CO2 capacity of 0.96 mmol g−1 at moderate temperatures (~300 °C), which is more than ten times higher than that of the commercial light MgO. This novel mesoporous MgO adsorbent also exhibited high stability during multiple CO2 adsorption/desorption cycles. The excellent CO2 capturing performance was believed to be related to its high specific surface area of 321.3 m2 g−1 and abundant surface active adsorption sites. This work suggested a new synthesis scheme for MgO based CO2 adsorbents at intermediate temperatures, providing a competitive candidate for capturing CO2 from certain sorption enhanced hydrogen production processes. Full article
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Open AccessCommunication Lipase-Mediated Amidation of Anilines with 1,3-Diketones via C–C Bond Cleavage
Catalysts 2017, 7(4), 115; https://doi.org/10.3390/catal7040115
Received: 9 March 2017 / Revised: 10 April 2017 / Accepted: 12 April 2017 / Published: 14 April 2017
Cited by 3 | PDF Full-text (6938 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
In this work, an efficient and green lipase-mediated technique has been mined for the amidation of anilines with 1,3-diketones via C–C bond cleavage. Under the optimal conditions, high yields (64.3%–96.2%) could be obtained when Novozym 435 was used as the catalyst. Furthermore, Novozym
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In this work, an efficient and green lipase-mediated technique has been mined for the amidation of anilines with 1,3-diketones via C–C bond cleavage. Under the optimal conditions, high yields (64.3%–96.2%) could be obtained when Novozym 435 was used as the catalyst. Furthermore, Novozym 435 exhibited a satisfying reusability and more than 80% of yield can be obtained after seven cycles. This work provides a more rapid and mild strategy for amide synthesis with high yield and expands the application of enzyme in organic synthesis. Full article
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Open AccessArticle Steam Reforming of Bio-Compounds with Auto-Reduced Nickel Catalyst
Catalysts 2017, 7(4), 114; https://doi.org/10.3390/catal7040114
Received: 15 February 2017 / Revised: 31 March 2017 / Accepted: 31 March 2017 / Published: 13 April 2017
Cited by 1 | PDF Full-text (5611 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
As an extension of chemical looping combustion, chemical looping steam reforming (CLSR) has been developed for H2 production. During CLSR, a steam reforming (SR) process occurs following the reduction of catalysts by the reforming feedstock itself (termed “auto-reduction”), as opposed to a separate,
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As an extension of chemical looping combustion, chemical looping steam reforming (CLSR) has been developed for H2 production. During CLSR, a steam reforming (SR) process occurs following the reduction of catalysts by the reforming feedstock itself (termed “auto-reduction”), as opposed to a separate, dedicated reducing agent like H2. This paper studied SR performances of four common bio-compounds (ethanol, acetone, furfural, and glucose) with a nickel catalyst that had undergone auto-reduction. A packed bed reactor was used to carry out the experiment of auto-reduction and subsequent SR. The effects of temperature and steam to carbon ratio (S/C) on the carbon conversions of the bio-compounds to gases and yields of gaseous products were investigated. The carbon deposition on spent catalysts was characterized by CHN elemental analysis and Scanning Electron Microscopy-Energy Dispersive X-ray Spectroscopy (SEM-EDX). The SR performance with the auto-reduced catalyst was close to that with the H2-reduced catalyst. In general, an increase in temperature or S/C would lead to an increase in H2 yields. The dependence of SR performance on temperature or S/C was specific to the type of bio-compounds. Accordingly, the main bottlenecks for SR of each bio-compound were summarized. A large amount of CH4 existed in the reforming product of ethanol. Severe carbon deposition was observed for SR of acetone at temperatures below 650 °C. A high thermal stability of furfural molecules or its derivatives restricted the SR of furfural. For SR of glucose, the main problem was the severe agglomeration of catalyst particles due to glucose coking. Full article
(This article belongs to the Special Issue Reforming Catalysts)
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Open AccessFeature PaperReview Abatement of VOCs Using Packed Bed Non-Thermal Plasma Reactors: A Review
Catalysts 2017, 7(4), 113; https://doi.org/10.3390/catal7040113
Received: 20 December 2016 / Revised: 6 April 2017 / Accepted: 7 April 2017 / Published: 12 April 2017
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Abstract
Non thermal plasma (NTP) reactors packed with non-catalytic or catalytic packing material have been widely used for the abatement of volatile organic compounds such as toluene, benzene, etc. Packed bed reactors are single stage reactors where the packing material is placed directly in
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Non thermal plasma (NTP) reactors packed with non-catalytic or catalytic packing material have been widely used for the abatement of volatile organic compounds such as toluene, benzene, etc. Packed bed reactors are single stage reactors where the packing material is placed directly in the plasma discharge region. The presence of packing material can alter the physical (such as discharge characteristics, power consumption, etc.) and chemical characteristics (oxidation and destruction pathway, formation of by-products, etc.) of the reactor. Thus, packed bed reactors can overcome the disadvantages of NTP reactors for abatement of volatile organic compounds (VOCs) such as lower energy efficiency and formation of unwanted toxic by-products. This paper aims at reviewing the effect of different packing materials on the abatement of different aliphatic, aromatic and chlorinated volatile organic compounds. Full article
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Open AccessReview Improving the Stability of Cold-Adapted Enzymes by Immobilization
Catalysts 2017, 7(4), 112; https://doi.org/10.3390/catal7040112
Received: 13 January 2017 / Revised: 30 March 2017 / Accepted: 4 April 2017 / Published: 12 April 2017
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Abstract
Cold-adapted enzymes have gained considerable attention as biocatalysts that show high catalytic activity at low temperatures. However, the use of cold-adapted enzymes at ambient temperatures has been hindered by their low thermal stabilities caused by their inherent structural flexibilities. Accordingly, protein engineering and
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Cold-adapted enzymes have gained considerable attention as biocatalysts that show high catalytic activity at low temperatures. However, the use of cold-adapted enzymes at ambient temperatures has been hindered by their low thermal stabilities caused by their inherent structural flexibilities. Accordingly, protein engineering and immobilization have been employed to improve the thermal stability of cold-adapted enzymes. Immobilization has been shown to increase the thermal stability of cold-adapted enzymes at the critical temperatures at which denaturation begins. This review summarizes progress in immobilization of cold-adapted enzymes as a strategy to improve their thermal and organic solvent stabilities. Full article
(This article belongs to the Special Issue Immobilized Enzymes: Strategies for Enzyme Stabilization)
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Open AccessFeature PaperArticle Unprecedented Multifunctionality of Grubbs and Hoveyda–Grubbs Catalysts: Competitive Isomerization, Hydrogenation, Silylation and Metathesis Occurring in Solution and on Solid Phase
Catalysts 2017, 7(4), 111; https://doi.org/10.3390/catal7040111
Received: 28 February 2017 / Revised: 30 March 2017 / Accepted: 6 April 2017 / Published: 9 April 2017
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Abstract
This contribution showcases the interplay of several non-metathetic reactions (isomerization, silylation and “hydrogen-free” reduction) with metathesis in systems comprising a functionalized olefin and a soluble or resin-immobilized silane. These competing, one-pot reactions occur under activation by second-generation Ru-alkylidene catalysts. Different olefinic substrates were
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This contribution showcases the interplay of several non-metathetic reactions (isomerization, silylation and “hydrogen-free” reduction) with metathesis in systems comprising a functionalized olefin and a soluble or resin-immobilized silane. These competing, one-pot reactions occur under activation by second-generation Ru-alkylidene catalysts. Different olefinic substrates were used to study the influence of the substitution pattern on the reaction outcome. Emphasis is placed upon the rarely reported yet important transformations implying a solid phase-supported silane reagent. Catalytic species involved in and reaction pathways accounting for these concurrent processes are evidenced. An unexpected result of this research was the clearly proved partial binding of the olefin to the resin, thereby removing it from the reacting ensemble. Full article
(This article belongs to the Special Issue Ruthenium Catalysts)
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