Ternary NixCo3-xS4 with Fine Hollow Nanostructure as Robust Electrocatalyst for Hydrogen Evolution

Elaborate design of efficient and stable electrocatalysts from earth-abundant elements to replace precious Pt for the hydrogen evolution reaction (HER) is an ongoing challenge. Doping metallic compounds with additional metal atoms provides the opportunity to tune their electronic and crystal structures, thus ameliorating their electrocatalytic properties. Here, we report for the first time a robust and earth-abundant Ni-doped Co3S4 catalyst grown on carbon cloth that showed high HER activity in 1 M KOH. The morphology evolution and HER activity are strongly related to the Ni substitution ratio. Electrochemical tests showed a low overpotential of 72.82 mV at 10 mA*cm-2, small Tafel slope of 49.44 mV*dec-1, and long-term durability over 46 h HER operation for the Ni0.5Co2.5S4 nanotube array self-standing on carbon cloth. These data indicate that atomic modulation of Ni plays an important role in optimizing the morphology and electrocatalytic activity by greatly expanding the active sites in the electrocatalyst. Further, the 3D self-standing nanotube array highly aids the exposure of active species and transfer of electrons and charges, substantially boosting the reaction kinetics and structure stability.

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Secondary Impact of Manganese on Catalytic Property of N-Doped Graphene in the Hydrogen Evolution Reaction

Catalysts play a key role in hydrogen production, as a green energy carrier. We have shown for the first time that manganese impurities in graphene can improve the catalytic activity of synthesized N-doped graphene (NG) for the hydrogen evolution reaction in acid media via influencing the ratio of different N-functionalities. This results in a 122 mV improvement in the over-potential following Mn impregnation of graphene. Transmission electron microscopy images confirmed the formation of manganese oxide nanoparticles on NG sheets. X-ray photoelectron spectroscopy revealed structural alteration in favour of higher quantities of quaternary and pyrrolic nitrogen functionalities, from approximately 37% in NG to 84% in Mn-inserted-doped graphene catalyst. This enhanced catalytic performance, based on density functional theory (DFT) calculations in the literature, is attributed to an increase in the number of active sites with higher activity.

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Excellent selectivity with high conversion in semi-hydrogenation of alkynes using Pd-based bimetallic catalysts

A series of active carbon supported PdPb and PdCu bimetal catalysts for selective semi-hydrogenation of alkynes with excellent selectivity and stability in liquid-phase. Pd0.33Pb0.67/C catalyst showed the best performance for various alkynes under mild reaction conditions (room temperature and ambient H2 pressure), showing 100% conversion and 98% selectivity to alkenes. Particularly, over hydrogenation was avoided under complete alkyne conversion.

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First Neutral and Cationic Tungsten Imido Alkylidene N-Heterocyclic Carbene Complexes

Abstract

The synthesis of W(NAr′)(NHC)(=CHR)(2,5-Me₂pyr)₂ (1; Ar′: 2,6-iPr₂C₆H₃; NHC: 1,3-diisopropylimidazol-2-ylidene; 2,5-Me₂pyr: 2,5-dimethylpyrrolide; R: CMe₂Ph), W(NAr′)(NHC)(=CHR)(2,5-Me₂pyr)(OC₆F₅) (2), W(NAr′)(NHC)(=CHR)(OSiPh₃)₂ (3), [W(NAr′)(NHC)(=CHR)(OSiPh₃))(MeCN)⁺][B(Ar^F)₄⁻] (4; B(Ar^F)₄⁻: B(3,5-(CF₃)₂C₆H₃)₄⁻), [W(NAr′)(NHC)(=CHR)(2,5-Me₂pyr))⁺][B(Ar^F)₄⁻] (5), [W(NAr′)(NHC)(=CHR)(OC₆F₅))(tBuCN)⁺][B(Ar^F)₄⁻] (6), W(NAr′)(NHC)(=CHR)(OtBu)₂ (7), [W(NAr′)(NHC)(=CHR)(OtBu)⁺][B(Ar^F)₄⁻] (8), and W(NAr′)(NHC)(=CHR)(OCMe(CF₃)₂)₂ (9) is described, and the reactivity of the complexes in olefin metathesis and cyclopolymerization is reported. The cationic complexes 4, 5, and 6 showed high productivity and activity in olefin metathesis reactions, with turnover numbers of up to 40 000 and turnover frequencies (TOF_5min) of up to 31 s⁻¹, and also substantial functional group tolerance toward esters, nitriles, alcohols, and sulfides, particularly in the cyclopolymerization of α,ω-diynes.

Tolerance is complex: High productivity and activity in olefin metathesis reactions, along with substantial functional group tolerance, was shown by cationic tungsten imido alkylidene N-heterocyclic carbene complexes.

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Hierarchical Ti-beta obtained by simultaneous desilication and titanation as efficient catalyst for cyclooctene epoxidation

A novel postsynthesis route to hierarchical Ti beta zeolite and its performance as efficient catalyst in heterogeneous cyclooctene epoxidation are presented. Catalytically active Ti-sites as well as meso- and macropores are simultaneously introduced into microporous beta zeolite by hydrothermal treatment using tetrabutyl orthotitanate as titanation agent and tetraethylammonium hydroxide as desilication base. Simultaneous desilication and titanation (SDT) offers the advantages of reduced experimental effort and chemical waste. The possibility to use a commercial zeolite available in high quantity as starting material is attractive for industrialization. A significant mesopore volume (Vmeso = 0.19 cm³ g 1) was introduced in the resulting hierarchical Ti beta zeolite without loss of microporosity and crystallinity compared to the purely microporous counterpart. The comparison clearly demonstrates a higher catalytic activity for the hierarchical Ti-beta in cyclooctene epoxidation and accelerated desorption kinetics associated with the highly interconnected pore system.

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Electrocatalytic Properties of Cuprous Delafossite Oxides for Alkaline Oxygen Reduction Reaction

Inspired by the oxygen-binding copper sites in biomolecules, a series of cuprous delafossite oxides (CuBO2, B = Sc, Y, La) with similar interatomic copper distances were utilized as electrocatalysts for the oxygen reduction reaction (ORR). The carbon-supported oxides showed improved onset potential, current, and electron transfer number over carbon black, with CuLaO2 having the highest prevalence of the complete four electron reduction. The oxygen electrocatalytic activity of the copper-site in delafossite oxides was demonstrated.

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On the role of acidity in bulk and nanosheet [T]MFI (T = Al3+, Ga3+, Fe3+, B3+) zeolites in the methanol-to-hydrocarbons reaction

The influence of framework substituent (Al3+, Ga3+, Fe3+ and B3+) and morphology (bulk vs. nanometer-sized sheets) of MFI zeolite on acidity and catalytic performance in the methanol-to-hydrocarbons (MTH) reaction was investigated. The Brønsted acid density and strength decreased in the order Al(OH)Si > Ga(OH)Si > Fe(OH)Si >> B(OH)Si. Pyridine-15N NMR spectra confirmed differences in the Brønsted and Lewis acid strengths but also evidenced site heterogeneity in the Brønsted acid sites. Due to the lower efficiency with which tervalent ions can be inserted into the zeolite framework, sheet-like zeolites exhibited lower acidity than bulk zeolites. The sheet-like Al-containing MFI zeolite exhibited the greatest longevity as MTH catalyst, outperforming its bulk [Al]MFI counterpart. While the lower acidity of bulk [Ga]MFI led to better catalytic performance than bulk [Al]MFI, the sheet-like [Ga]MFI sample was found to be nearly inactive due to lower and heterogeneous Brønsted acidity. All Fe- and B-substituted zeolite samples displayed very low catalytic performance due to their weak acidity. Based on product distribution, the MTH reaction was found to be dominated by the olefins-based catalytic cycle. The small contribution of the aromatics-based catalytic cycle was larger for bulk zeolite than for sheet-like zeolite, indicating that shorter residence time of aromatics can explain the lower tendency to coking and enhanced catalyst longevity.

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Improving carbon coated TiO2 films with a TiCl4 treatment for photocatalytic water purification

Using a simple thermal decomposition route, carbon-TiO2 hybrid films have been synthesized from a catechol-TiO2 surface complex. The coated films display enhanced visible region absorption, owing to the thin (~2 nm) layer of carbon encapsulating the TiO2. While photocatalytically active under visible light alone, it is demonstrated that the activity of the carbon coated films can be improved further by a hydrolytic treatment with TiCl4, leading to the introduction of small TiO2 particles (5-10nm) and doping of chlorine into the structure. The combination of the carbon layer and TiCl4 treatment gives increased photocatalytic performance for the photodegradation of dyes, phenolic pollutants and the reduction of toxic Cr(VI) to relatively benign Cr(III). In addition, the carbon coated films show improved bactericidal activity under UV irradiation, and hence have been successfully tested against the most common types of pollutant present in potential drinking waters.

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PEGylation greatly enhances laccase polymerase activity

Laccase catalyzes the oxidation and polymerization of phenolic compounds in the presence of oxygen. Herein, we report for the first time that a previous pegylation of laccase enhances the polymerase activity by 3-fold comparing with the native enzyme, as confirmed by UV-Vis spectroscopy. The polymerization of catechol increased only 1.5-fold when polyethyleneglycol (PEG) was added to the medium reaction. Molecular dynamic simulations suggest the formation of a miscible complex of polycatechol and PEG, which is responsible to push the reaction forward. In a negative control experiment set, all catalysts were entrapped inside acrylamide gels and here the native laccase showed a relatively higher activity. These results suggest that the mobility of PEG is a key feature for the enhancement of the reaction.

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Access to (Hetero)arylated Selenophenes via Palladium-catalysed Stille, Negishi or Suzuki Couplings or C−H Bond Functionalization Reaction

Abstract

(Hetero)aryl-substituted selenophenes exhibit important physical properties especially for optoelectronics. Palladium-catalysed coupling reactions currently represent the most efficient methods to prepare such (hetero)arylated selenophene derivatives. Initially, Stille coupling was the most efficient reaction for the synthesis of these compounds; however, over the last decade, Suzuki coupling has become the most commonly employed. Recently, Pd-catalysed arylation via the C−H bond activation of selenophenes has proved to be a very convenient alternative method for the preparation of several arylated selenophenes as there is no need to prepare organometallic derivatives. In this Review, the progress and substrate scope in the synthesis of both C2- and C3-arylated selenophenes via Pd-catalysis are summarized.

Selenophenes stereotypes: The progress and substrate scope of the palladium catalyzed synthesis of both C2- and C3-arylated selenophenes are summarized in this Review—from Stille, Suzuki, and Negishi coupling through to C−H bond activation

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Hydrodeoxygenation of Phenol over Zirconia-Supported Catalysts: The Effect of Metal Type on Reaction Mechanism and Catalyst Deactivation

Abstract

This work aims at investigating the effect of the type of metal (Pt, Pd, Rh, Ru, Cu, Ni, Co) on the performance of ZrO₂-supported catalysts for the hydrodeoxygenation of phenol in the gas phase at 573 K and 1 atm. Two different reaction pathways take place depending on the type of the metal. For Pt/ZrO₂ and Pd/ZrO₂ catalysts, phenol is mainly tautomerized, followed by hydrogenation of the C=C bond of the tautomer intermediate formed, producing cyclohexanone and cyclohexanol. By contrast, the direct dehydroxylation of phenol followed by hydrogenolysis might also occur over more oxophilic metals such as Rh, Ru, Co, and Ni. In addition to the metals, the oxophilic sites of this support represented by Zr⁴⁺ and Zr³⁺ cations near the perimeter of the metal particles also increased the selectivity to deoxygenated products. All catalysts were significantly deactivated mainly owing to the growth of metal particle size and the decrease in the density of oxophilic sites.

Metal effects: The product distribution in the hydrodeoxygenation of phenol is investigated as a function of the type of the metal. Two different reaction pathways take place depending on the type of the metal in the ZrO₂-supported catalysts; phenol tautomerization, followed by hydrogenation of the C=C bond (Pt,Pd) and direct dehydroxylation of phenol followed by hydrogenolysis (Rh,Ru,Co,Ni).

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Auto-reduction Behaviour of Cobalt on Graphitic Carbon Nitride Coated Alumina Supports for Fischer-Tropsch Synthesis

The graphitic carbon nitride (g-C3N4)-coated alumina (CN-Al) is investigated as a support material for a cobalt-based Fischer-Tropsch synthesis (FTS) catalyst. The g-C3N4 blocks the interaction between cobalt and alumina to hinder the formation of irreducible cobalt oxide species, and improves the dispersion of metallic cobalt species on the CN-Al support. Furthermore, the coated g-C3N4 is decomposed during the pre-annealing process under inert condition to evolve reductive carbon monoxide gas that directly reduces the cobalt oxide species to metallic cobalt. Hence, the catalyst can be activated without typical hydrogen pretreatment. Moreover, the reduction promotion by expensive noble metals like Pt is not needed either. Because of the improved dispersion and reducibility of the cobalt species on CN-Al support, the catalytic FTS activity is higher compared to the conventional Co/Al2O3 catalyst.

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New Carbon Nanodots-Silica Hybrid Photocatalyst for Highly Selective Solar Fuel Production from CO2

Photocatalytic CO2 reduction for solar fuel production has attracted considerable attention as it can simultaneously reduce the effects of worldwide fossil-fuel shortage and global warming. As a means to achieve this we herein report the facile and eco-friendly synthesis of highly active carbon nanodots-silica hybrid photocatalyst (CNDSH) by a reverse microemulsion method with a nonionic surfactant. The photocatalyst-biocatalyst coupled system developed using CNDSH as photocatalyst functions efficiently to carry out high NADH regeneration (74.10 ± 0.17 %) followed by its consumption in exclusive formic acid production (203.33 ± 1.9 µmol) from CO2. This research work is a benchmark example of carbon nanodots-silica hybrid photocatalyst system for solar fuel production and expected to trigger further interest in the development of efficient and eco-friendly CO2 reduction systems.

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The French Conference on Catalysis—FCCat 1

Vive la catalyse française! From state-of-the-art model approaches to advanced characterization and kinetic studies, by materials and complexes synthesis or post-treatment, the systems showcased by this special issue in honor of French Catalysis are involved in natural gas and biomass conversion, pollutant mitigation, oxygen and hydrogen evolution reactions, to name a few.

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Cover Picture: The Pivotal Role of Catalysis in France: Selected Examples of Recent Advances and Future Prospects. (ChemCatChem 12/2017)

The Front Cover shows the potential of catalysis in France.In their Review, H. Olivier-Bourbigou et al. summarize the most significant breakthroughs reported in France over the last ten years in the field of heterogeneous catalysis. The Review focuses on the development of catalytic systems for specific applications, such as petrochemistry, biomass transformation, environmental applications and CO₂ for energy. The significant cross-disciplinary approaches, essential to understand and optimize catalytic processes, are also described. More information can be found in the Review by H. Olivier-Bourbigou et al. on page 2029 in Issue 12, 2017 (DOI: 10.1002/cctc.201700426).

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Cover Feature: Chemical Weathering of Alumina in Aqueous Suspension at Ambient Pressure: A Mechanistic Study (ChemCatChem 12/2017)

The Cover depicts the formation of surface mixed phases and Si grafting on the lateral facets of γ-alumina. In their Full Paper, J. Abi Aad et al. demonstrate that formation of surface mixed phases and Si grafting on the lateral facets of γ-alumina respectively inhibits and suppresses the alumina transformation to boehmite through a dissolution-precipitation process under hydrothermal conditions. More information can be found in the Full Paper by J. Abi Aad et al. on page 2186 in Issue 12, 2017 (DOI: 10.1002/cctc.201700140).

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Inside Cover: Facile Synthesis of Cu@CeO2 and Its Catalytic Behavior for the Hydrogenation of Methyl Acetate to Ethanol (ChemCatChem 12/2017)

The Cover shows a facile method to fabricate a Cu@CeO₂ catalyst that exhibits excellent activity and stability in the hydrogenation of methyl acetate.In their Communication, Y. Wang et al. demonstrate that the core–shell structure of Cu@CeO₂ not only prevents the aggregation of Cu particles but also enlarges the contact area between Cu and CeO₂, which greatly increases the Cu⁺ surface area. Moreover, the Cu⁰ and Cu⁺ active sites are well distributed on the core–shell interface, which results in a close relative position and an enhanced synergetic catalysis effect for the hydrogenation of methyl acetate. More information can be found in the Communication by Y. Wang et al. on page 2085 in Issue 12, 2017 (DOI: 10.1002/cctc.201700111).

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Back Cover: Biomass-assisted Zeolite Syntheses as a Tool for Designing New Acid Catalysts (ChemCatChem 12/2017)

The Cover shows an alternative route involving sugar cane-derived biomass to produce zeolites with tailored properties.In their Concept, B. Louis et al. highlight the impact of the presence of sugars, lignin, biomass hydrolysates and biomass residues on the crystallization of various zeolite structures. The presence of those biosourced secondary templates (BSST) induces morphological/textural changes and, sometimes, modifications of the chemical composition and acidic properties. The BSST strategy may serve as a basis for the rational synthesis of heterogeneous catalysts. More information can be found in the Concept by B. Louis et al. on page 2065 in Issue 12, 2017 (DOI: 10.1002/cctc.201700062).

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Inside Back Cover: Selective Oxidation of n-Butane and Isobutane Catalyzed by Boron Nitride (ChemCatChem 12/2017)

The Cover shows n-butane accompanied by an oxygen molecule traversing a boron nitride bridge. Upon crossing the bridge, n-butane is selectively transformed to 1-butene while another, less fortunate molecule falls over the cliff to become CO₂.In their Full Paper, J. M. Venegas et al. report that hexagonal boron nitride selectively catalyzes the oxidative dehydrogenation of n-butane and isobutane to their respective olefins. Boron nitride is unique in that overoxidation of the desired olefins to carbon oxides is kept to a minimum and instead the minor side-products are lighter olefins. The observed reaction kinetics point to a fundamentally different mechanism to that observed with conventional metal oxide catalysts. More information can be found in the Full Paper by J. M. Venegas et al. on page 2118 in Issue 12, 2017 (DOI: 10.1002/cctc.201601686).

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Oxidation of cyclohexene in the presence of transition metal substituted phosphotungstates and hydrogen peroxide: catalysis and reaction pathways

Homogeneous catalytic oxidations of cyclohexene by transition metal substituted phosphotungstates [PW₁₁M(L)O₃₉]m- (PW₁₁M, M = Co(II), Cu(II), Fe(III), Ni(II), Mn(II), L = H₂O or absence) with hydrogen peroxide in acetonitrile were experimentally studied. The catalytic activities of allylic oxidation were found to strongly depend on the transition metals, and PW₁₁Co showed the highest activity. The product distribution and the catalyst stability were dominated by mole ratio of hydrogen peroxide to PW₁₁M, whose low or high led to stable structure of PW₁₁M and predominant formation of allylic oxidation products or decomposition of PW₁₁M. Different from the activation of allylic C-H bond by radicals, the oxidation of C=C double bond was based on tungsten-peroxo species. A reaction mechanism composed of radical and non-radical processes was proposed from nuclear magnetic resonance (NMR), electron paramagnetic resonance (EPR) and kinetic data, to describe the reaction pathways of cyclohexene oxidation.

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Delays in breast cancer diagnosis after a state policy limiting Medicaid enrollment

In this issue of Cancer, Tarazi et al investigate the effects of a state policy that substantially limited Medicaid enrollment on the timeliness of breast cancer diagnosis. They observe a statistically significant increase of 3.3 percentage points in the percentage of women diagnosed with late-stage disease after the policy change among women living in low-income versus high-income areas. See also pages 000-000.

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HPV testing with abnormal cervical cytology speeds up diagnosis of cervical disease

Testing for human papillomavirus (HPV) in women with abnormal cervical cytology leads to faster diagnosis of cervical disease and fewer missed cases, a large observational study has found.1Cervical...

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Proton pump inhibitor use does not raise dementia and Alzheimer’s risk, study suggests

A US study1 has not confirmed earlier reports that proton pump inhibitor (PPI) use is linked to an increased risk of dementia and Alzheimer's disease.2 In contrast, the latest study, published in the...

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HPV testing with abnormal cervical cytology speeds up diagnosis of cervical disease

Testing for human papillomavirus (HPV) in women with abnormal cervical cytology leads to faster diagnosis of cervical disease and fewer missed cases, a large observational study has found.1Cervical...

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Proton pump inhibitor use does not raise dementia and Alzheimer’s risk, study suggests

A US study1 has not confirmed earlier reports that proton pump inhibitor (PPI) use is linked to an increased risk of dementia and Alzheimer's disease.2 In contrast, the latest study, published in the...

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Professional Ethics: Making the Right Decision

Professionals today are faced with many ethical dilemmas and it has become crucial for clinicians to understand how ethical decisions are made, what are the necessary considerations and how to apply each to the many ethical dilemmas they may face. This course will give an overview of the why's and how's to making an ethical decision and will provide the practitioner with a framework for exploring ethical dilemmas.

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