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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
Received: 6 December 2016 / Revised: 17 January 2017 / Accepted: 19 January 2017 / Published: 23 January 2017
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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
Received: 4 January 2017 / Revised: 4 January 2017 / Accepted: 17 January 2017 / Published: 20 January 2017
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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
Received: 16 December 2016 / Revised: 3 January 2017 / Accepted: 3 January 2017 / Published: 19 January 2017
Cited by 8 | PDF Full-text (6192 KB) | HTML Full-text | XML Full-text | Supplementary Files
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
Received: 23 December 2016 / Revised: 11 January 2017 / Accepted: 12 January 2017 / Published: 18 January 2017
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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.
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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
Received: 29 October 2016 / Revised: 24 December 2016 / Accepted: 12 January 2017 / Published: 18 January 2017
Cited by 10 | PDF Full-text (2017 KB) | HTML Full-text | XML Full-text
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
Received: 30 November 2016 / Revised: 9 January 2017 / Accepted: 11 January 2017 / Published: 18 January 2017
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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
Received: 24 November 2016 / Revised: 10 January 2017 / Accepted: 11 January 2017 / Published: 17 January 2017
Cited by 5 | PDF Full-text (3590 KB) | HTML Full-text | XML Full-text | Supplementary Files
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
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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
Received: 27 December 2016 / Revised: 11 January 2017 / Accepted: 11 January 2017 / Published: 17 January 2017
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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
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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
Received: 27 October 2016 / Revised: 6 January 2017 / Accepted: 10 January 2017 / Published: 14 January 2017
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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
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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
Received: 20 November 2016 / Revised: 27 December 2016 / Accepted: 27 December 2016 / Published: 14 January 2017
Cited by 5 | PDF Full-text (3947 KB) | HTML Full-text | XML Full-text
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
Received: 29 November 2016 / Revised: 4 January 2017 / Accepted: 10 January 2017 / Published: 13 January 2017
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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
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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
Received: 26 October 2016 / Revised: 18 December 2016 / Accepted: 5 January 2017 / Published: 12 January 2017
Cited by 3 | PDF Full-text (6488 KB) | HTML Full-text | XML Full-text
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
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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
Received: 11 January 2017 / Accepted: 11 January 2017 / Published: 11 January 2017
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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
Received: 22 November 2016 / Revised: 19 December 2016 / Accepted: 5 January 2017 / Published: 11 January 2017
Cited by 4 | PDF Full-text (4869 KB) | HTML Full-text | XML Full-text
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
Received: 24 November 2016 / Revised: 30 December 2016 / Accepted: 3 January 2017 / Published: 10 January 2017
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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
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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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