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Catalysts, Volume 7, Issue 1 (January 2017)

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Cover Story (view full-size image) Mimicking a leaf’s ability to convert solar energy into chemical energy in a very sophisticated [...] Read more.
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Open AccessReview
The Use of Palladium on Magnetic Support as Catalyst for Suzuki–Miyaura Cross-Coupling Reactions
Catalysts 2017, 7(1), 35; https://doi.org/10.3390/catal7010035 - 23 Jan 2017
Cited by 21 | Viewed by 2555
Abstract
The development of new solid supports for palladium has received a lot of interest lately. These catalysts have been tested in a range of cross-coupling reactions, such as Suzuki–Miyaura, Mizoroki-Heck, and Sonogashira cross-coupling reactions, with good outcomes. Attaching the catalyst to a solid [...] Read more.
The development of new solid supports for palladium has received a lot of interest lately. These catalysts have been tested in a range of cross-coupling reactions, such as Suzuki–Miyaura, Mizoroki-Heck, and Sonogashira cross-coupling reactions, with good outcomes. Attaching the catalyst to a solid support simplifies the operations required in order to isolate and recycle the catalyst after a reaction has completed. Palladium on solid supports made of magnetic materials is particularly interesting since such catalysts can be removed very simply by utilizing an external magnet, which withholds the catalyst in the reaction vessel. This review will showcase some of the latest magnetic solid supports for palladium and highlight these catalysts’ performance in Suzuki–Miyaura cross-coupling reactions. Full article
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Open AccessEditorial
Reflections on Catalytic Selective Oxidation: Opportunities and Challenges
Catalysts 2017, 7(1), 34; https://doi.org/10.3390/catal7010034 - 20 Jan 2017
Cited by 2 | Viewed by 1290
Abstract
Currently, and looking forward, there is an ever increasing demand to perform chemical transformations with optimized atom and energy efficiency [...] Full article
(This article belongs to the Special Issue Catalysts for Selective Oxidation)
Open AccessArticle
Synergically Improving Light Harvesting and Charge Transportation of TiO2 Nanobelts by Deposition of MoS2 for Enhanced Photocatalytic Removal of Cr(VI)
Catalysts 2017, 7(1), 30; https://doi.org/10.3390/catal7010030 - 19 Jan 2017
Cited by 15 | Viewed by 2574
Abstract
Herein, MoS2/TiO2 nanobelts heterojunction have been successfully synthesized by in situ growth method for photocatalytic reduction of Cr(VI). TiO2 nanobelts (NBs) with rough surface were prepared firstly by acidic treatment process, which is beneficial for deposition and growth of [...] Read more.
Herein, MoS2/TiO2 nanobelts heterojunction have been successfully synthesized by in situ growth method for photocatalytic reduction of Cr(VI). TiO2 nanobelts (NBs) with rough surface were prepared firstly by acidic treatment process, which is beneficial for deposition and growth of MoS2 to form heterojunctions. As a result of special energy level offset and nanostructure, MoS2/TiO2 NBs composite were endowed with higher light-harvesting capacity and charge transportation efficiency, which are indispensible merits for excellent photocatalytic activity. The photocatalytic reduction of Cr(VI) reveals that the synthesized MoS2/TiO2 NBs composite have superior photocatalytic ability than other samples. Meanwhile, a photoreduction mechanism is proposed based on the systematic investigation, where the photogenerated electrons are demonstrated as the dominant reductive species to reduce Cr(VI) to Cr(III). Full article
(This article belongs to the Special Issue Heterogeneous Catalysis for Environmental Remediation)
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Open AccessArticle
Mild and Highly Efficient Copper(I) Inspired Acylation of Alcohols and Polyols
Catalysts 2017, 7(1), 33; https://doi.org/10.3390/catal7010033 - 18 Jan 2017
Cited by 6 | Viewed by 1780
Abstract
A new and highly efficient method mediated by tetrakis(acetonitrile)copper(I) triflate for activating both simple and highly hindered anhydrides in the acylation of alcohols and polyols is described. This new acylation method is mild and mostly proceeds at room temperature with low catalyst loading. [...] Read more.
A new and highly efficient method mediated by tetrakis(acetonitrile)copper(I) triflate for activating both simple and highly hindered anhydrides in the acylation of alcohols and polyols is described. This new acylation method is mild and mostly proceeds at room temperature with low catalyst loading. The method is versatile and has been extended to a wide variety of different alcohol substrates to afford the corresponding ester products in good to excellent yields. Full article
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Open AccessReview
A Short Review on the Catalytic Activity of Hydrotalcite-Derived Materials for Dry Reforming of Methane
Catalysts 2017, 7(1), 32; https://doi.org/10.3390/catal7010032 - 18 Jan 2017
Cited by 34 | Viewed by 3200
Abstract
Nickel-containing hydrotalcite-derived materials have been recently proposed as promising materials for methane dry reforming (DRM). Based on a literature review and on the experience of the authors, this review focuses on presenting past and recent achievements on increasing activity and stability of hydrotalcite-based [...] Read more.
Nickel-containing hydrotalcite-derived materials have been recently proposed as promising materials for methane dry reforming (DRM). Based on a literature review and on the experience of the authors, this review focuses on presenting past and recent achievements on increasing activity and stability of hydrotalcite-based materials for DRM. The use of different NiMgAl and NiAl hydrotalcite (HT) precursors, various methods for nickel introduction into HT structure, calcination conditions and promoters are discussed. HT-derived materials containing nickel generally exhibit high activity in DRM; however, the problem of preventing catalyst deactivation by coking, especially below 700 °C, is still an open question. The proposed solutions in the literature include: catalyst regeneration either in oxygen atmosphere or via hydrogasification; or application of various promoters, such as Zr, Ce or La, which was proven to enhance catalytic stability. Full article
(This article belongs to the Special Issue Reforming Catalysts)
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Open AccessReview
Nanostructured Inorganic Materials at Work in Electrochemical Sensing and Biofuel Cells
Catalysts 2017, 7(1), 31; https://doi.org/10.3390/catal7010031 - 18 Jan 2017
Cited by 10 | Viewed by 2806
Abstract
The future of analytical devices, namely (bio)sensors, which are currently impacting our everyday life, relies on several metrics such as low cost, high sensitivity, good selectivity, rapid response, real-time monitoring, high-throughput, easy-to-make and easy-to-handle properties. Fortunately, they can be readily fulfilled by electrochemical [...] Read more.
The future of analytical devices, namely (bio)sensors, which are currently impacting our everyday life, relies on several metrics such as low cost, high sensitivity, good selectivity, rapid response, real-time monitoring, high-throughput, easy-to-make and easy-to-handle properties. Fortunately, they can be readily fulfilled by electrochemical methods. For decades, electrochemical sensors and biofuel cells operating in physiological conditions have concerned biomolecular science where enzymes act as biocatalysts. However, immobilizing them on a conducting substrate is tedious and the resulting bioelectrodes suffer from stability. In this contribution, we provide a comprehensive, authoritative, critical, and readable review of general interest that surveys interdisciplinary research involving materials science and (bio)electrocatalysis. Specifically, it recounts recent developments focused on the introduction of nanostructured metallic and carbon-based materials as robust “abiotic catalysts” or scaffolds in bioelectrochemistry to boost and increase the current and readout signals as well as the lifetime. Compared to biocatalysts, abiotic catalysts are in a better position to efficiently cope with fluctuations of temperature and pH since they possess high intrinsic thermal stability, exceptional chemical resistance and long-term stability, already highlighted in classical electrocatalysis. We also diagnosed their intrinsic bottlenecks and highlighted opportunities of unifying the materials science and bioelectrochemistry fields to design hybrid platforms with improved performance. Full article
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Open AccessArticle
Visualization of Gas Distribution in a Model AP-XPS Reactor by PLIF: CO Oxidation over a Pd(100) Catalyst
Catalysts 2017, 7(1), 29; https://doi.org/10.3390/catal7010029 - 17 Jan 2017
Cited by 10 | Viewed by 1964
Abstract
In situ knowledge of the gas phase around a catalyst is essential to make an accurate correlation between the catalytic activity and surface structure in operando studies. Although ambient pressure X-ray photoelectron spectroscopy (AP-XPS) can provide information on the gas phase as well [...] Read more.
In situ knowledge of the gas phase around a catalyst is essential to make an accurate correlation between the catalytic activity and surface structure in operando studies. Although ambient pressure X-ray photoelectron spectroscopy (AP-XPS) can provide information on the gas phase as well as the surface structure of a working catalyst, the gas phase detected has not been spatially resolved to date, thus possibly making it ambiguous to interpret the AP-XPS spectra. In this work, planar laser-induced fluorescence (PLIF) is used to visualize the CO2 distribution in a model AP-XPS reactor, during CO oxidation over a Pd(100) catalyst. The results show that the gas composition in the vicinity of the sample measured by PLIF is significantly different from that measured by a conventional mass spectrometer connected to a nozzle positioned just above the sample. In addition, the gas distribution above the catalytic sample has a strong dependence on the gas flow and total chamber pressure. The technique presented has the potential to increase our knowledge of the gas phase in AP-XPS, as well as to optimize the design and operating conditions of in situ AP-XPS reactors for catalysis studies. Full article
(This article belongs to the Special Issue In Situ and Operando Characterization in Catalysis)
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Open AccessFeature PaperArticle
The Effect of Sr Addition in Cu- and Fe-Modified CeO2 and ZrO2 Soot Combustion Catalysts
Catalysts 2017, 7(1), 28; https://doi.org/10.3390/catal7010028 - 17 Jan 2017
Cited by 4 | Viewed by 2028
Abstract
This study investigates the activity of transition and alkaline-earth metal-doped catalysts supported on ceria or zirconia for the NOx-assisted oxidation of diesel particulate. A series of Cu- and Fe-impregnated catalysts over CeO2 and ZrO2 supports were prepared by incipient [...] Read more.
This study investigates the activity of transition and alkaline-earth metal-doped catalysts supported on ceria or zirconia for the NOx-assisted oxidation of diesel particulate. A series of Cu- and Fe-impregnated catalysts over CeO2 and ZrO2 supports were prepared by incipient wetness impregnation and characterized by BET, X-ray diffraction (XRD), and temperature-programmed reduction (TPR) experiments while their catalytic activity was investigated in NOx-assisted reaction by means of temperature programmed oxidation experiments (TPO). Higher activity was achieved by copper modified catalysts; the addition of Sr positively affected the performance of the materials, suggesting a synergic effect between transition metals and alkaline-earth metal. The role of copper is correlated to the oxidation of NO to NO2, while strontium seems to be mainly involved in the storage of NOx species. Full article
(This article belongs to the Special Issue Ceria-based Catalysts)
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Open AccessArticle
Chitosan–Collagen Coated Magnetic Nanoparticles for Lipase Immobilization—New Type of “Enzyme Friendly” Polymer Shell Crosslinking with Squaric Acid
Catalysts 2017, 7(1), 26; https://doi.org/10.3390/catal7010026 - 14 Jan 2017
Cited by 10 | Viewed by 3397
Abstract
This article presents a novel route for crosslinking a polysaccharide and polysaccharide/protein shell coated on magnetic nanoparticles (MNPs) surface via condensation reaction with squaric acid (SqA). The syntheses of four new types of collagen-, chitosan-, and chitosan–collagen coated magnetic nanoparticles as supports for [...] Read more.
This article presents a novel route for crosslinking a polysaccharide and polysaccharide/protein shell coated on magnetic nanoparticles (MNPs) surface via condensation reaction with squaric acid (SqA). The syntheses of four new types of collagen-, chitosan-, and chitosan–collagen coated magnetic nanoparticles as supports for enzyme immobilization have been done. Structure and morphology of prepared new materials were characterized by attenuated total reflectance Fourier-transform infrared (ATR-FTIR), XRD, and TEM analysis. Next, the immobilization of lipase from Candida rugosa was performed on the nanoparticles surface via N-(3-dimethylaminopropyl)-N′-ethylcarbodiimide hydrochloride (EDC)/N-hydroxy-succinimide (NHS) mechanism. The best results of lipase activity recovery and specific activities were observed for nanoparticles with polymer shell crosslinked via a novel procedure with squaric acid. The specific activity for lipase immobilized on materials crosslinked with SqA (52 U/mg lipase) was about 2-fold higher than for enzyme immobilized on MNPs with glutaraldehyde addition (26 U/mg lipase). Moreover, a little hyperactivation of lipase immobilized on nanoparticles with SqA was observed (104% and 112%). Full article
(This article belongs to the Special Issue Immobilized Enzymes: Strategies for Enzyme Stabilization)
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Open AccessArticle
Response Surface Methodology and Aspen Plus Integration for the Simulation of the Catalytic Steam Reforming of Ethanol
Catalysts 2017, 7(1), 15; https://doi.org/10.3390/catal7010015 - 14 Jan 2017
Cited by 8 | Viewed by 3533
Abstract
The steam reforming of ethanol (SRE) on a bimetallic RhPt/CeO2 catalyst was evaluated by the integration of Response Surface Methodology (RSM) and Aspen Plus (version 9.0, Aspen Tech, Burlington, MA, USA, 2016). First, the effect of the Rh–Pt weight ratio (1:0, 3:1, [...] Read more.
The steam reforming of ethanol (SRE) on a bimetallic RhPt/CeO2 catalyst was evaluated by the integration of Response Surface Methodology (RSM) and Aspen Plus (version 9.0, Aspen Tech, Burlington, MA, USA, 2016). First, the effect of the Rh–Pt weight ratio (1:0, 3:1, 1:1, 1:3, and 0:1) on the performance of SRE on RhPt/CeO2 was assessed between 400 to 700 °C with a stoichiometric steam/ethanol molar ratio of 3. RSM enabled modeling of the system and identification of a maximum of 4.2 mol H2/mol EtOH (700 °C) with the Rh0.4Pt0.4/CeO2 catalyst. The mathematical models were integrated into Aspen Plus through Excel in order to simulate a process involving SRE, H2 purification, and electricity production in a fuel cell (FC). An energy sensitivity analysis of the process was performed in Aspen Plus, and the information obtained was used to generate new response surfaces. The response surfaces demonstrated that an increase in H2 production requires more energy consumption in the steam reforming of ethanol. However, increasing H2 production rebounds in more energy production in the fuel cell, which increases the overall efficiency of the system. The minimum H2 yield needed to make the system energetically sustainable was identified as 1.2 mol H2/mol EtOH. According to the results of the integration of RSM models into Aspen Plus, the system using Rh0.4Pt0.4/CeO2 can produce a maximum net energy of 742 kJ/mol H2, of which 40% could be converted into electricity in the FC (297 kJ/mol H2 produced). The remaining energy can be recovered as heat. Full article
(This article belongs to the Special Issue Reforming Catalysts)
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Open AccessCommunication
Aziridine- and Azetidine-Pd Catalytic Combinations. Synthesis and Evaluation of the Ligand Ring Size Impact on Suzuki-Miyaura Reaction Issues
Catalysts 2017, 7(1), 27; https://doi.org/10.3390/catal7010027 - 13 Jan 2017
Cited by 2 | Viewed by 1773
Abstract
The synthesis of new vicinal diamines based on aziridine and azetidine cores as well as the comparison of their catalytic activities as ligand in the Suzuki-Miyaura coupling reaction are described in this communication. The synthesis of three- and four-membered ring heterocycles substituted by [...] Read more.
The synthesis of new vicinal diamines based on aziridine and azetidine cores as well as the comparison of their catalytic activities as ligand in the Suzuki-Miyaura coupling reaction are described in this communication. The synthesis of three- and four-membered ring heterocycles substituted by a methylamine pendant arm is detailed from the parent nitrile derivatives. Complexation to palladium under various conditions has been examined affording vicinal diamines or amine-imidate complexes. The efficiency of four new catalytic systems is compared in the preparation of variously substituted biaryls. Aziridine- and azetidine-based catalytic systems allowed Suzuki-Miyaura reactions from aryl halides including chlorides with catalytic loadings until 0.001% at temperatures ranging from 100 °C to r.t. The evolution of the Pd-metallacycle ring strain moving from azetidine to aziridine in combination with a methylamine or an imidate pendant arm impacted the Suzuki-Miyaura reaction issue. Full article
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Open AccessArticle
Cobalt-Doped Carbon Gels as Electro-Catalysts for the Reduction of CO2 to Hydrocarbons
Catalysts 2017, 7(1), 25; https://doi.org/10.3390/catal7010025 - 12 Jan 2017
Cited by 10 | Viewed by 2130
Abstract
Two original series of carbon gels doped with different cobalt loadings and well-developed mesoporosity, aerogels and xerogels, have been prepared, exhaustively characterized, and tested as cathodes for the electro-catalytic reduction of CO2 to hydrocarbons at atmospheric pressure. Commercial cobalt and graphite sheets [...] Read more.
Two original series of carbon gels doped with different cobalt loadings and well-developed mesoporosity, aerogels and xerogels, have been prepared, exhaustively characterized, and tested as cathodes for the electro-catalytic reduction of CO2 to hydrocarbons at atmospheric pressure. Commercial cobalt and graphite sheets have also been tested as cathodes for comparison. All of the doped carbon gels catalyzed the formation of hydrocarbons, at least from type C1 to C4. The catalytic activity depends mainly on the metal loading, nevertheless, the adsorption of a part of the products in the porous structure of the carbon gel cannot be ruled out. Apparent faradaic efficiencies calculated with these developed materials were better that those obtained with a commercial cobalt sheet as a cathode, especially considering the much lower amount of cobalt contained in the Co-doped carbon gels. The cobalt-carbon phases formed in these types of doped carbon gels improve the selectivity to C3-C4 hydrocarbons formation, obtaining even more C3 hydrocarbons than CH4 in some cases. Full article
(This article belongs to the Special Issue Sol–Gel Chemistry: A Toolbox for Catalyst Preparation)
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Open AccessEditorial
Acknowledgement to Reviewers of Catalysts in 2016
Catalysts 2017, 7(1), 24; https://doi.org/10.3390/catal7010024 - 11 Jan 2017
Viewed by 1293
Abstract
The editors of Catalysts would like to express their sincere gratitude to the following reviewers for assessing manuscripts in 2016.[...] Full article
Open AccessArticle
Catalytic Ammonia Decomposition over High-Performance Ru/Graphene Nanocomposites for Efficient COx-Free Hydrogen Production
Catalysts 2017, 7(1), 23; https://doi.org/10.3390/catal7010023 - 11 Jan 2017
Cited by 9 | Viewed by 2114
Abstract
Highly-dispersed Ru nanoparticles were grown on graphene nanosheets by simultaneously reducing graphene oxide and Ru ions using ethylene glycol (EG), and the resultant Ru/graphene nanocomposites were applied as a catalyst to ammonia decomposition for COx-free hydrogen production. Tuning the microstructures of [...] Read more.
Highly-dispersed Ru nanoparticles were grown on graphene nanosheets by simultaneously reducing graphene oxide and Ru ions using ethylene glycol (EG), and the resultant Ru/graphene nanocomposites were applied as a catalyst to ammonia decomposition for COx-free hydrogen production. Tuning the microstructures of Ru/graphene nanocomposites was easily accomplished in terms of Ru particle size, morphology, and loading by adjusting the preparation conditions. This was the key to excellent catalytic activity, because ammonia decomposition over Ru catalysts is structure-sensitive. Our results demonstrated that Ru/graphene prepared using water as a co-solvent greatly enhanced the catalytic performance for ammonia decomposition, due to the significantly improved nano architectures of the composites. The long-term stability of Ru/graphene catalysts was evaluated for COx-free hydrogen production from ammonia at high temperatures, and the structural evolution of the catalysts was investigated during the catalytic reactions. Although there were no obvious changes in the catalytic activities at 450 °C over a duration of 80 h, an aggregation of the Ru nanoparticles was still observed in the nanocomposites, which was ascribed mainly to a sintering effect. However, the performance of the Ru/graphene catalyst was decreased gradually at 500 °C within 20 h, which was ascribed mainly to both the effect of the methanation of the graphene nanosheet under a H2 atmosphere and to enhanced sintering under high temperatures. Full article
(This article belongs to the Special Issue Ruthenium Catalysts)
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Open AccessArticle
Synthesis and Application of Novel Ruthenium Catalysts for High Temperature Alkene Metathesis
Catalysts 2017, 7(1), 22; https://doi.org/10.3390/catal7010022 - 10 Jan 2017
Cited by 3 | Viewed by 1560
Abstract
Four pyridinyl alcohols and the corresponding hemilabile pyridinyl alcoholato ruthenium carbene complexes of the Grubbs second generation-type RuCl(H2IMes)(O^N)(=CHPh), where O^N = 1-(2′-pyridinyl)-1,1-diphenyl methanolato, 1-(2′-pyridinyl)-1-(2′-chlorophenyl),1-phenyl methanolato, 1-(2′-pyridinyl)-1-(4′-chlorophenyl),1-phenyl methanolato and 1-(2′-pyridinyl)-1-(2′-methoxyphenyl),1-phenyl methanolato, are synthesized in very good yields. At high temperatures, the precatalysts [...] Read more.
Four pyridinyl alcohols and the corresponding hemilabile pyridinyl alcoholato ruthenium carbene complexes of the Grubbs second generation-type RuCl(H2IMes)(O^N)(=CHPh), where O^N = 1-(2′-pyridinyl)-1,1-diphenyl methanolato, 1-(2′-pyridinyl)-1-(2′-chlorophenyl),1-phenyl methanolato, 1-(2′-pyridinyl)-1-(4′-chlorophenyl),1-phenyl methanolato and 1-(2′-pyridinyl)-1-(2′-methoxyphenyl),1-phenyl methanolato, are synthesized in very good yields. At high temperatures, the precatalysts showed high stability, selectivity and activity in 1-octene metathesis compared to the Grubbs first and second generation precatalysts. The 2-/4-chloro- and 4-methoxy-substituted pyridinyl alcoholato ligand-containing ruthenium precatalysts showed high performance in the 1-octene metathesis reaction in the range 80–110 °C. The hemilabile 4-methoxy-substituted pyridinyl alcoholato ligand improved the catalyst stability, activity and selectivity for 1-octene metathesis significantly at 110 °C. Full article
(This article belongs to the Special Issue Ruthenium Catalysts)
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Open AccessArticle
Hydrochlorination of Acetylene Catalyzed by an Activated Carbon-Supported Ammonium Hexachlororuthenate Complex
Catalysts 2017, 7(1), 17; https://doi.org/10.3390/catal7010017 - 10 Jan 2017
Cited by 7 | Viewed by 1872
Abstract
Ammonium hexachlororuthenate ((NH4)2RuCl6) complex was used as a catalyst precursor and coconut activated carbon (AC) was used as the support in the preparation process of the Ru-based catalyst. (NH4)2RuCl6/AC catalyst was [...] Read more.
Ammonium hexachlororuthenate ((NH4)2RuCl6) complex was used as a catalyst precursor and coconut activated carbon (AC) was used as the support in the preparation process of the Ru-based catalyst. (NH4)2RuCl6/AC catalyst was prepared via an incipient wetness impregnation method and assessed in an acetylene hydrochlorination reaction. Meanwhile, the (NH4)2RuCl6/AC catalyst was analyzed with low-temperature N2 adsorption/desorption, thermogravimetry (TG), transmission electron microscopy (TEM), temperature programmed reduction (TPR), X-ray photoelectron spectra (XPS), and temperature programmed desorption (TPD) techniques. Catalytic performance test results show that the (NH4)2RuCl6/AC catalyst exhibits a superior catalytic activity with the highest acetylene conversion of 90.5% under the conditions of 170 °C and an acetylene gas hourly space velocity of 180 h−1. The characterization results illustrate that the presence of the NH4+ cation can inhibit coke deposition as well as the agglomeration of ruthenium particles, and it can also enhance the adsorption ability for reactant HCl, hence improving the catalytic activity and stability. Full article
(This article belongs to the Special Issue Ruthenium Catalysts)
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Open AccessArticle
Core-Shell Structured [email protected]2 Catalysts Exhibiting Excellent Catalytic Performance for Syngas Methanation Reactions
Catalysts 2017, 7(1), 21; https://doi.org/10.3390/catal7010021 - 09 Jan 2017
Cited by 5 | Viewed by 1611
Abstract
In this study, we prepared core-shell structured [email protected]2 catalysts using chemical precipitation and modified Stöber methods. The obtained [email protected]2 samples exhibited excellent catalysis performances, including high CO conversion of 99.0% and CH4 yield of 89.8%. Moreover, [email protected]2 exhibited excellent [...] Read more.
In this study, we prepared core-shell structured [email protected]2 catalysts using chemical precipitation and modified Stöber methods. The obtained [email protected]2 samples exhibited excellent catalysis performances, including high CO conversion of 99.0% and CH4 yield of 89.8%. Moreover, [email protected]2 exhibited excellent catalytic stability during a 100 h lifetime test, which was superior to that of the Ni/SiO2 catalyst. The prepared samples were characterized using a series of techniques, and the results indicated that the catalytic performance for syngas methanation reaction of the [email protected]2 sample was markedly improved owing to its nanoreactor structure. The strong interaction between the Ni core and the SiO2 shell effectively restrained the growth of particles, and the deposition of C species. Full article
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Open AccessArticle
Plant Extract Mediated Eco-Friendly Synthesis of [email protected] Nanocatalyst: An Efficient and Reusable Catalyst for the Suzuki-Miyaura Coupling
Catalysts 2017, 7(1), 20; https://doi.org/10.3390/catal7010020 - 09 Jan 2017
Cited by 7 | Viewed by 2868
Abstract
Suzuki-Miyaura coupling reaction catalyzed by the palladium (Pd)-based nanomaterials is one of the most versatile methods for the preparation of biaryls. However, use of organic solvents as reaction medium causes a big threat to environment due to the generation of toxic byproducts as [...] Read more.
Suzuki-Miyaura coupling reaction catalyzed by the palladium (Pd)-based nanomaterials is one of the most versatile methods for the preparation of biaryls. However, use of organic solvents as reaction medium causes a big threat to environment due to the generation of toxic byproducts as waste during the work up of these reactions. Therefore, the use of water as reaction media has attracted tremendous attention due to its environmental, economic, and safety benefits. In this study, we report on the synthesis of green [email protected] nanocatalyst based on an in situ functionalization approach which exhibited excellent catalytic activity towards the Suzuki–Miyaura cross-coupling reactions of phenyl halides with phenyl boronic acids under facile conditions in water. The green and environmentally friendly synthesis of [email protected] nanocatalyst (PG-HRG-Pd) is carried out by simultaneous reduction of graphene oxide (GRO) and PdCl2 using Pulicaria glutinosa extract (PGE) as reducing and stabilizing agent. The phytomolecules present in the plant extract (PE) not only facilitated the reduction of PdCl2, but also helped to stabilize the surface of PG-HRG-Pd nanocatalyst, which significantly enhanced the dispersibility of nanocatalyst in water. The identification of PG-HRG-Pd was established by various spectroscopic and microscopic techniques, including, high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), ultraviolet–visible spectroscopy (UV-Vis), Fourier transform infrared spectroscopy (FT-IR), and Raman spectroscopy. The as-prepared PG-HRG-Pd nanocatalyst demonstrated excellent catalytic activity towards the Suzuki-Miyaura cross coupling reactions under aqueous, ligand free, and aerobic conditions. Apart from this the reusability of the catalyst was also evaluated and the catalyst yielded excellent results upon reuse for several times with marginal loss of its catalytic performance. Therefore, the method developed for the green synthesis of PG-HRG-Pd nanocatalyst and the eco-friendly protocol used for the Suzuki coupling offers a mild and effective substitute to the existing protocols and may significantly contribute to the endeavors of green chemistry. Full article
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Open AccessArticle
Core-Shell MnO2-SiO2 Nanorods for Catalyzing the Removal of Dyes from Water
Catalysts 2017, 7(1), 19; https://doi.org/10.3390/catal7010019 - 06 Jan 2017
Cited by 7 | Viewed by 2165
Abstract
This work presented a novel core-shell MnO2@m-SiO2 for catalyzing the removal of dyes from wastewater. MnO2 nanorods were sequentially coated with polydopamine (PDA) and polyethyleneimine (PEI) forming MnO2@PDA-PEI. By taking advantage of the positively charged amine groups, [...] Read more.
This work presented a novel core-shell MnO2@m-SiO2 for catalyzing the removal of dyes from wastewater. MnO2 nanorods were sequentially coated with polydopamine (PDA) and polyethyleneimine (PEI) forming MnO2@PDA-PEI. By taking advantage of the positively charged amine groups, MnO2@PDA-PEI was further silicificated, forming MnO2@PDA-PEI-SiO2. After calcination, the composite MnO2@m-SiO2 was finally obtained. MnO2 nanorod is the core and mesoporous SiO2 (m-SiO2) is the shell. MnO2@m-SiO2 has been used to degrade a model dye Rhodamine B (RhB). The shell m-SiO2 functioned to adsorb/enrich and transfer RhB, and the core MnO2 nanorods oxidized RhB. Thus, MnO2@m-SiO2 combines multiple functions together. Experimental results demonstrated that MnO2@m-SiO2 exhibited a much higher efficiency for degradation of RhB than MnO2. The RhB decoloration and degradation efficiencies were 98.7% and 84.9%, respectively. Consecutive use of MnO2@m-SiO2 has demonstrated that MnO2@m-SiO2 can be used to catalyze multiple cycles of RhB degradation. After six cycles of reuse of MnO2@m-SiO2, the RhB decoloration and degradation efficiencies were 98.2% and 71.1%, respectively. Full article
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Open AccessArticle
Facile Sonication Synthesis of WS2 Quantum Dots for Photoelectrochemical Performance
Catalysts 2017, 7(1), 18; https://doi.org/10.3390/catal7010018 - 06 Jan 2017
Cited by 11 | Viewed by 3518
Abstract
Two-dimensional transition metal dichalcogenides, such as tungsten disulfide (WS2), have been actively studied as suitable candidates for photocatalysts due to their unique structural and electronic properties. The presence of active sites at the edges and the higher specific surface area of [...] Read more.
Two-dimensional transition metal dichalcogenides, such as tungsten disulfide (WS2), have been actively studied as suitable candidates for photocatalysts due to their unique structural and electronic properties. The presence of active sites at the edges and the higher specific surface area of these materials are crucial to the photocatalytic activity of the hydrogen evolution reaction. Here, WS2 quantum dots (QDs) have been successfully synthesized by using a combination of grinding and sonication techniques. The morphology of the QDs was observed, using transmission electron microscopy and an atomic force microscope, to have uniform sizes of less than 5 nm. Photoelectrochemical (PEC) measurements show that the current density of WS2 QDs under illumination is almost two times higher than that of pristine WS2. Furthermore, these high-quality WS2 QDs may have various applications in optoelectronics, solar cells, and biomedicine. Full article
(This article belongs to the Special Issue Soluble Nanoparticles in Catalytic Applications)
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Open AccessFeature PaperReview
Catalyst, Membrane, Free Electrolyte Challenges, and Pathways to Resolutions in High Temperature Polymer Electrolyte Membrane Fuel Cells
Catalysts 2017, 7(1), 16; https://doi.org/10.3390/catal7010016 - 06 Jan 2017
Cited by 8 | Viewed by 2042
Abstract
High temperature polymer electrolyte membrane fuel cells (HT-PEMFCs) are being studied due to a number of benefits offered versus their low temperature counterparts, including co-generation of heat and power, high tolerance to fuel impurities, and simpler system design. Approximately 90% of the literature [...] Read more.
High temperature polymer electrolyte membrane fuel cells (HT-PEMFCs) are being studied due to a number of benefits offered versus their low temperature counterparts, including co-generation of heat and power, high tolerance to fuel impurities, and simpler system design. Approximately 90% of the literature on HT-PEM is related to the electrolyte and, for the most part, these electrolytes all use free phosphoric acid, or similar free acid, as the ion conductor. A major issue with using phosphoric acid based electrolytes is the free acid in the electrodes. The presence of the acid on the catalyst sites leads to poor oxygen activity, low solubility/diffusion, and can block electrochemical sites through phosphate adsorption. This review will focus on these issues and the steps that have been taken to alleviate these obstacles. The intention is this review may then serve as a tool for finding a solution path in the community. Full article
(This article belongs to the Special Issue Catalysis in Membrane Reactors)
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Open AccessReview
The Protagonism of Biocatalysis in Green Chemistry and Its Environmental Benefits
Catalysts 2017, 7(1), 9; https://doi.org/10.3390/catal7010009 - 01 Jan 2017
Cited by 22 | Viewed by 2660
Abstract
The establishment of a bioeconomy era requires not only a change of production pattern, but also a deep modernization of the production processes through the implementation of novel methodologies in current industrial units, where waste materials and byproducts can be utilized as starting [...] Read more.
The establishment of a bioeconomy era requires not only a change of production pattern, but also a deep modernization of the production processes through the implementation of novel methodologies in current industrial units, where waste materials and byproducts can be utilized as starting materials in the production of commodities such as biofuels and other high added value chemicals. The utilization of renewable raw resources and residues from the agro-industries, and their exploitation through various uses and applications through technologies, particularly solid-state fermentation (SSF), are the main focus of this review. The advocacy for biocatalysis in green chemistry and the environmental benefits of bioproduction are very clear, although this kind of industrial process is still an exception and not the rule. Potential and industrial products, such as biocatalysts, animal feed, fermentation medium, biofuels (biodiesel, lignocelulose ethanol, CH4, and H2), pharmaceuticals and chemicals are dealt with in this paper. The focus is the utilization of renewable resources and the important role of enzymatic process to support a sustainable green chemical industry. Full article
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Open AccessFeature PaperReview
Recent Advances in the BiVO4 Photocatalyst for Sun-Driven Water Oxidation: Top-Performing Photoanodes and Scale-Up Challenges
Catalysts 2017, 7(1), 13; https://doi.org/10.3390/catal7010013 - 01 Jan 2017
Cited by 77 | Viewed by 5686
Abstract
Photoelectrochemical (PEC) water splitting, which is a type of artificial photosynthesis, is a sustainable way of converting solar energy into chemical energy. The water oxidation half-reaction has always represented the bottleneck of this process because of the thermodynamic and kinetic challenges that are [...] Read more.
Photoelectrochemical (PEC) water splitting, which is a type of artificial photosynthesis, is a sustainable way of converting solar energy into chemical energy. The water oxidation half-reaction has always represented the bottleneck of this process because of the thermodynamic and kinetic challenges that are involved. Several materials have been explored and studied to address the issues pertaining to solar water oxidation. Significant advances have recently been made in the use of stable and relatively cheap metal oxides, i.e., semiconducting photocatalysts. The use of BiVO4 for this purpose can be considered advantageous because this catalyst is able to absorb a substantial portion of the solar spectrum and has favourable conduction and valence band edge positions. However, BiVO4 is also associated with poor electron mobility and slow water oxidation kinetics and these are the problems that are currently being investigated in the ongoing research in this field. This review focuses on the most recent advances in the best-performing BiVO4-based photoanodes to date. It summarizes the critical parameters that contribute to the performance of these photoanodes, and highlights so far unresolved critical features related to the scale-up of a BiVO4-based PEC water-splitting device. Full article
(This article belongs to the Special Issue Water Oxidation Catalysis)
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Open AccessFeature PaperReview
C-Homoscorpionate Oxidation Catalysts—Electrochemical and Catalytic Activity
Catalysts 2017, 7(1), 12; https://doi.org/10.3390/catal7010012 - 01 Jan 2017
Cited by 17 | Viewed by 1909
Abstract
A survey of the electrochemical properties of homoscorpionate tris(pyrazol-1-yl)methane complexes is presented. The relationship between structural features and catalytic efficiency toward the oxidative functionalization of inexpensive and abundant raw-materials to added-value products is also addressed. Full article
(This article belongs to the Special Issue New Trends in Scorpionate Catalysts)
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Open AccessArticle
The Distribution and Strength of Brönsted Acid Sites on the Multi-Aluminum Model of FER Zeolite: A Theoretical Study
Catalysts 2017, 7(1), 11; https://doi.org/10.3390/catal7010011 - 01 Jan 2017
Cited by 3 | Viewed by 2459
Abstract
One of the fundamental issues in catalysis is to identify the catalytic active site. Due to its prominent pore topology and acidity, ferrierite (FER) zeolite has attracted extensive interest in various catalytic reactions such as isomerization of butenes. However knowledge on the active [...] Read more.
One of the fundamental issues in catalysis is to identify the catalytic active site. Due to its prominent pore topology and acidity, ferrierite (FER) zeolite has attracted extensive interest in various catalytic reactions such as isomerization of butenes. However knowledge on the active Brönsted acid site is still absent. In the present study, we perform extensive density functional theory calculations to explore the distribution and strength of the Brönsted acid sites and their potential catalytic activity for the double-bond isomerization of 1-butene to 2-butene. We employ a two-layered ONIOM scheme (our Own N-layered Integrated molecular Orbital + molecular Mechanics) to describe the structure and energetic properties of FER zeolite. We find that the hydrogen bond could improve the stability of Brönsted acid sites effectively, and, as a result, Al4-O6-Si2 and Al4-O-(SiO)2-Al4 are the most stable sites for 1-Al substitution and 2-Al substitution, respectively. We further find that the Brönsted acid strength tends to decrease with the increase of Al contents and increase when the distance between the Al atoms is increased in 2-Al substitution. Finally it is demonstrated that the strength of acid sites determines the catalytic activity for the double bond isomerization of 1-butene to 2-butene. Full article
(This article belongs to the Special Issue Computational Methods and Their Application in Catalysis)
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Open AccessArticle
N2O Direct Dissociation over MgxCeyCo1−xyCo2O4 Composite Spinel Metal Oxide
Catalysts 2017, 7(1), 10; https://doi.org/10.3390/catal7010010 - 01 Jan 2017
Cited by 7 | Viewed by 2200
Abstract
A series of Mg- and/or Ce-doped Co3O4 (MgxCo1−xCo2O4 CexCo1−xCo2O4, MgxCeyCo1−xyCo2O4) [...] Read more.
A series of Mg- and/or Ce-doped Co3O4 (MgxCo1−xCo2O4 CexCo1−xCo2O4, MgxCeyCo1−xyCo2O4) composite spinel metal-oxide catalyst was prepared by a coprecipitation method and evaluated for N2O direct decomposition. The activity measurement results suggest that Mg0.025Ce0.05Co0.925Co2O4 with a Mg/Ce mole ratio of 0.5 exhibited the highest N2O conversion activity, achieving 100% N2O conversion at T = 250 °C (35 vol % N2O balanced by He, gas hourly space velocity (GHSV) = 30,000 h−1). Characterizations using X-ray diffraction (XRD), Brunauer–Emmett–Teller method (BET), hydrogen temperature-programmed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS) reveal that there were three main reasons for the excellent catalytic behavior of Mg0.025Ce0.05Co0.925Co2O4: (a) Mg and Ce co-doping could reduce the grain size of composite spinel metal oxide, which thereby significantly increased the BET specific surface area of Mg0.025Ce0.05Co0.925Co2O4 (111.2 g·m2 with respect to that of 32.5 g·m−2 for Co3O4); (b) Mg and Ce co-doping could improve the redox ability of Mg0.025Ce0.05Co0.925Co2O4, including reductions of Co3+ → Co2+ and Co2+ → Co0; and (c) Mg and Ce co-doping not only could improve the migration ability of surface atomic O, but also could increase the concentrations of surface atomic O. Full article
(This article belongs to the Special Issue Ceria-based Catalysts)
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Open AccessArticle
Lipase B from Candida antarctica Immobilized on a Silica-Lignin Matrix as a Stable and Reusable Biocatalytic System
Catalysts 2017, 7(1), 14; https://doi.org/10.3390/catal7010014 - 31 Dec 2016
Cited by 21 | Viewed by 2510
Abstract
A study was conducted of the possible use of a silica-lignin hybrid as a novel support for the immobilization of lipase B from Candida antarctica. Results obtained by elemental analysis, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and atomic force [...] Read more.
A study was conducted of the possible use of a silica-lignin hybrid as a novel support for the immobilization of lipase B from Candida antarctica. Results obtained by elemental analysis, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and atomic force microscopy (AFM), as well as the determination of changes in porous structure parameters, confirmed the effective immobilization of the enzyme on the surface of the composite matrix. Based on a hydrolysis reaction, a determination was made of the retention of activity of the immobilized lipase, found to be 92% of that of the native enzyme. Immobilization on a silica-lignin matrix produces systems with maximum activity at pH = 8 and at a temperature of 40 °C. The immobilized enzyme exhibited increased thermal and chemical stability and retained more than 80% of its activity after 20 reaction cycles. Moreover immobilized lipase exhibited over 80% of its activity at pH range 7–9 and temperature from 30 °C to 60 °C, while native Candida antarctica lipase B (CALB) exhibited the same only at pH = 7 and temperature of 30 °C. Full article
(This article belongs to the Special Issue Immobilized Enzymes: Strategies for Enzyme Stabilization)
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Open AccessArticle
In Situ FTIR Analysis of CO-Tolerance of a Pt-Fe Alloy with Stabilized Pt Skin Layers as a Hydrogen Anode Catalyst for Polymer Electrolyte Fuel Cells
Catalysts 2017, 7(1), 8; https://doi.org/10.3390/catal7010008 - 29 Dec 2016
Cited by 6 | Viewed by 3666
Abstract
The CO-tolerance mechanism of a carbon-supported Pt-Fe alloy catalyst with two atomic layers of stabilized Pt-skin (Pt2AL–PtFe/C) was investigated, in comparison with commercial Pt2Ru3/C (c-Pt2Ru3/C), by in situ attenuated total reflection Fourier transform [...] Read more.
The CO-tolerance mechanism of a carbon-supported Pt-Fe alloy catalyst with two atomic layers of stabilized Pt-skin (Pt2AL–PtFe/C) was investigated, in comparison with commercial Pt2Ru3/C (c-Pt2Ru3/C), by in situ attenuated total reflection Fourier transform infrared (ATR-FTIR) spectroscopy in 0.1 M HClO4 solution at 60 °C. When 1% CO (H2-balance) was bubbled continuously in the solution, the hydrogen oxidation reaction (HOR) activities of both catalysts decreased severely because the active sites were blocked by COad, reaching the coverage θCO ≈ 0.99. The bands in the IR spectra observed on both catalysts were successfully assigned to linearly adsorbed CO (COL) and bridged CO (COB), both of which consisted of multiple components (COL or COB at terraces and step/edge sites). The Pt2AL–PtFe/C catalyst lost 99% of its initial mass activity (MA) for the HOR after 30 min, whereas about 10% of the initial MA was maintained on c-Pt2Ru3/C after 2 h, which can be ascribed to a suppression of linearly adsorbed CO at terrace sites (COL, terrace). In contrast, the HOR activities of both catalysts with pre-adsorbed CO recovered appreciably after bubbling with CO-free pure H2. We clarify, for the first time, that such a recovery of activity can be ascribed to an increased number of active sites by a transfer of COL, terrace to COL, step/edge, without removal of COad from the surface. The Pt2AL–PtFe/C catalyst showed a larger decrease in the band intensity of COL, terrace. A possible mechanism for the CO-tolerant HOR is also discussed. Full article
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Open AccessArticle
Dehydrogenative Oxidation of Alcohols Catalyzed by Highly Dispersed Ruthenium Incorporated Titanium Oxide
Catalysts 2017, 7(1), 7; https://doi.org/10.3390/catal7010007 - 28 Dec 2016
Cited by 2 | Viewed by 2004
Abstract
Ruthenium incorporated titanium oxides (RuxTiO2) were prepared by a one-step hydrothermal method using Ti(SO4)2 and RuCl3 as the precursor of Ti and Ru, respectively. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscope (TEM), [...] Read more.
Ruthenium incorporated titanium oxides (RuxTiO2) were prepared by a one-step hydrothermal method using Ti(SO4)2 and RuCl3 as the precursor of Ti and Ru, respectively. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscope (TEM), Energy-dispersive X-ray spectroscopy (EDS) mapping, and BET were applied for the analyses of catalysts. Ruthenium atoms are well dispersed in the anatase phase of TiO2 and the crystallite size of RuxTiO2 (≈17 nm) is smaller than that of pure TiO2 (≈45 nm). In particular, we found that our homemade pure TiO2 exhibits a strong Lewis acid property. Therefore, the cooperation of ruthenium atoms playing a role in the hydride elimination and the Lewis acid site of TiO2 can efficiently transfer primary alcohols into corresponding aldehydes in an oxidant-free condition. Full article
(This article belongs to the Special Issue Ruthenium Catalysts)
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Open AccessArticle
Hydrothermal Stability of Ru/SiO2–C: A Promising Catalyst for Biomass Processing through Liquid-Phase Reactions
Catalysts 2017, 7(1), 6; https://doi.org/10.3390/catal7010006 - 27 Dec 2016
Cited by 3 | Viewed by 1946
Abstract
In this work, structural and morphological properties of SiO2–C composite material to be used as support for catalysts in the conversion of biomass-derived oxygenated hydrocarbons, such as glycerol, were investigated in liquid water under various temperatures conditions. The results show that [...] Read more.
In this work, structural and morphological properties of SiO2–C composite material to be used as support for catalysts in the conversion of biomass-derived oxygenated hydrocarbons, such as glycerol, were investigated in liquid water under various temperatures conditions. The results show that this material does not lose surface area, and the hot liquid water does not generate changes in the structure. Neither change in relative concentrations of oxygen functional groups nor in Si/C ratio due to hydrothermal treatment was revealed by X-ray photoelectron spectroscopy (XPS) analysis. Raman analysis showed that the material is made of a disordered graphitic structure in an amorphous silica matrix, which remains stable after hydrothermal treatment. Results of the hydrogenolysis of glycerol using a Ru/SiO2–C catalyst indicate that the support gives more stability to the active phase than a Ru/SiO2 consisting of commercial silica. Full article
(This article belongs to the Special Issue Ruthenium Catalysts)
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