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Article Citation - WoS: 16Citation - Scopus: 16Keggin Type-Polyoxometalate Decorated Ruthenium Nanoparticles: Highly Active and Selective Nanocatalyst for the Oxidation of Veratryl Alcohol as a Lignin Model Compound(Wiley-v C H verlag Gmbh, 2017) Baguc, Ismail Burak; Saglam, Serif; Ertas, Ilknur Efecan; Keles, Muhammed Nuri; Celebi, Metin; Kaya, Murat; Zahmakiran, MehmetDescribed herein is a new nanocatalyst system that efficiently works in the aerobic oxidation of veratryl alcohol (VA), which is formed by cleavage of beta-O-4 linkages in lignin, to veratraldehyde (VAL) under mild reaction conditions. The new nanocatalyst system comprised of ruthenium(0) nanoparticles supported on the Keggin type polyoxometalate (POM; K-3[PMo12O40]) network (Ru/POM) can simply and reproducibly be prepared by the dimethylamine-borane ((CH3)(2)NHBH3) reduction of ruthenium(III) chloride trihydrate (RuCl3.3H(2)O) in isopropanol solution of K-3[P Mo12O40] at room temperature. The characterization of Ru/POM by the combination of various analytical techniques reveals that the formation of well-dispersed ruthenium(0) nanoparticles with a mean diameter of 4.7 +/- 1.2nm on the surface of POM network structure. This new Ru/POM nanocatalyst displays remarkable activity (TOF=7.5mol VAld/mol Ru x h) at high selectivity (> 98%) and almost complete conversion (98%) in the aerobic oxidation of VA to VAld under mild conditions.Article Citation - WoS: 9Citation - Scopus: 10Chromium Based Metal-Organic Framework Mil-101 Decorated Palladium Nanoparticles for the Methanolysis of Ammonia-Borane(Royal Soc Chemistry, 2020) Caner, Nurdan; Yurderi, Mehmet; Bulut, Ahmet; Kanberoglu, Gulsah Saydan; Kaya, Murat; Zahmakiran, MehmetPalladium nanoparticles stabilized by an MIL-101 metal-organic framework (Pd@MIL-101) are synthesized by a novel synthesis approach. A Pd@MIL-101 catalyst facilitates H(2)generation from the methanolysis of ammonia-borane with record catalytic activity (TOF = 1080 min(-1)) at room temperature. Moreover, the exceptional stability of Pd@MIL-101 makes it a reusable heterogeneous catalyst in this catalytic transformation.Article Citation - WoS: 2Synthesis of n-polyethereal Polypyrroles and Their Application for the Preconcentration of Rare Earth Ions(John Wiley & Sons inc, 2008) Koksel, Bahar; Cihaner, Atilla; Kaya, Murat; Volkan, Muervet; Onal, Ahmet M.Conducting polymers containing polyether pseudocages (PI, PII, PIII) have been synthesized via chemical oxidation of 1,5-bis(1,1-pyrrole)-3-oxabutane (MI), 1,8-bis(I,I-pyrrole)-3,6-dioxahexane (MII), and 1,11-bis(1,1-pyrrole)-3,6,9-trioxaundecane (MIII) using anhydrous FeCl3 in CHCl3. Because as obtained polymer resins did not give any response toward any cations, they were reduced (undoped) using chemical reducing agents. Tetrabutylammonium hydroxide was found to be more effective in undoping to obtain more reproducible and reusable polymer resins. The undoped polymer resins were tried in the extraction of rare earth metal ions from the aqueous medium. Among them, only PIII resin removes La(III), Eu(III) and Yb(III) and can be employed for the preconcentration of these metal ions. For batch extraction of La(III), Eu(III) and Yb(III) at neutral pH values, percent recoveries of 98.0 +/- 1.0, 90.7 +/- 1.4, 87.3 +/- 4.0, respectively, has been obtained. The sorption capacity is found as 1.3 mg of La(III) per gram of PIII resin. The PIII resin could be reused at least five times without significant change in its sorption capacity. (c) 2008 Wiley Periodicals, Inc.Article Citation - WoS: 8Citation - Scopus: 8Nanohydrotalcite Supported Ruthenium Nanoparticles: Highly Efficient Heterogeneous Catalyst for the Oxidative Valorization of Lignin Model Compounds(Wiley-v C H verlag Gmbh, 2017) Baguc, Ismail Burak; Celebi, Metin; Karakas, Kadir; Ertas, Ilknur Efecan; Keles, Muhammed Nuri; Kaya, Murat; Zahmakiran, MehmetThe catalytic transformation of lignocellulosic biomass derived chemicals into value-added chemicals under mild conditions remains a challenge in the fields of synthetic chemistry and catalysis. Herein, we describe a new heterogeneous catalyst system that efficiently works in the oxidative valorization of lignin model compounds. This new heterogeneous catalyst system comprised of nano-sized hydrotalcite (n-HT; Mg6Al2 (CO3)(OH)(16)) supported ruthenium(0) nanoparticles (Ru/ n-HT) was prepared by ion-exchange of [Ru(OH2)Cl-5](2-) anions with the extraframework CO32- anions of n-HT followed by their borohydride reduction (NaBH4) in water at room temperature. The characterization of Ru/n-HT was done by the combination of various spectroscopic and the sum of their results revealed that the formation of well-dispersed ruthenium(0) nanoparticles with a mean diameter of 3.2 +/- 0.9 nm on the surface of n-HT structure. The catalytic performance of Ru/n-HT in terms of activity, selectivity and stability was tested in the aerobic oxidation of cinnamyl, veratryl and vanillyl alcohols, which are important lignin model compounds used to mimic the propyl side chain, the phenolic and non-phenolic, respectively functional groups of lignin. We found that Ru/ n-HT nanocatalyst displays remarkable activity at high selectivity and almost complete conversion in these catalytic transformations under mild reaction conditions (at 373 K under 3 bar initial O-2 pressure).Article Citation - WoS: 13Citation - Scopus: 13Ruthenium Nanoparticles Supported on Reduced Graphene Oxide: Efficient Catalyst for the Catalytic Reduction of Cr(vi) in the Presence of Amine-Boranes(Wiley-v C H verlag Gmbh, 2020) Yurderi, Mehmet; Bulut, Ahmet; Kanberoglu, Gulsah Saydan; Kaya, Murat; Kanbur, Yasin; Zahmakiran, MehmetHexavalent chromium (Cr(VI)) is a toxic, mutagen and carcinogen contaminant exist in surface and groundwater, while its reduced form trivalent chromium (Cr(III)) is known as an essential element to normal carbohydrate, lipid and protein metabolism in nature. Addressed herein, for the first time, ruthenium nanoparticles supported on reduced graphene oxide (Ru@rGO) catalyze the reduction of aqueous Cr(VI) to Cr(III) in the presence of amine-boranes; ammonia-borane (AB; NH3BH3), methylamine-borane (MeAB; CH3NH2BH3), dimethylamine-borane (DMAB; (CH3)(2)NHBH3) as reducing agents under mild conditions (at room temperature and under air). Ru@rGO catalyst was reproducibly fabricated through a double-solvent method followed by wet-chemical reduction and characterized by using various spectroscopic and visualization techniques, which showed that the formation of well-dispersed and highly crystalline ruthenium(0) nanoparticles with a mean particle size of 2.7 +/- 0.9 nm on the surface of rGO. The catalytic performance of Ru@rGO was investigated in terms of activity and stability in the ammonia-borane assisted reduction of Cr(VI) to Cr(III), and the sum of the results gained from these catalytic tests revealed that Ru@rGO acts as both active (TOF=7.6 mol Cr2O72-/mol Ru.min) and stable (80% of its initial activity at 90% conversion at 5(th)reuse) heterogeneous catalyst in this significant catalytic transformation. This study also reports kinetic studies for Ru@rGO catalyzed Cr(VI) reduction in the presence of ammonia-borane depending on ruthenium ([Ru]), ammonia-borane ([AB]) concentrations and temperature to shed some light on the nature of the catalytic reaction and activation parameters.Article Citation - WoS: 41Citation - Scopus: 45Palladium Nanoparticles Decorated Graphene Oxide: Active and Reusable Nanocatalyst for the Catalytic Reduction of Hexavalent Chromium(vi)(Wiley-v C H verlag Gmbh, 2017) Celebi, Metin; Karakas, Kadir; Ertas, Ilknur Efecan; Kaya, Murat; Zahmakiran, MehmetToday, the catalytic reduction of Cr(VI) to Cr(III) stands one of the most important challenges in the environmental chemistry and catalysis due to highly stable, contaminant and toxic nature of Cr(VI). In this study, we show that a new nanocatalyst system comprised of 3-aminopropyltriethoxysilane (APTS) stabilized palladium(0) nanoparticles grafted onto the surface of graphene oxide (Pd/GO) efficiently works in the catalytic reduction of Cr(VI) to Cr(III) under mild reaction conditions. Pd/GO nanocatalyst was reproducibly prepared through two-steps procedure: (i) H-2 reduction of Pd(dba)2(dba= dibenzylideneacetone) in the presence of APTS in THF to synthesize colloidal APTS stabilized palladium(0) nanoparticles and then (ii) the deposition of 3-aminopropyltriethoxysilane stabilized palladium 0) nanoparticles onto the surface of graphene oxide (GO) by impregnation. The characterization of Pd/GO was carried out by advanced analytical techniques. The summation of the results acquired from these analyses reveals that the formation of well-dispersed and highly crystalline palladium(0) nanoparticles on the surface of GO. The catalytic performance of the resulting Pd/GO in terms of activity and stability was assessed in the catalytic reduction of Cr(VI) to Cr(III) in aqueous solution in the presence of formic acid (HCOOH) as a reducing agent. We found that Pd/GO nanocatalyst exhibits high activity (TOF= 3.6 mol Cr2O72-/mol Pdxmin) and reusability (> 90% at 5th reuse) in this catalytic transformation at room temperature.Article Gold-Assembled Silica-Coated Cobalt Nanoparticles as Efficient Magnetic Separation Units and Surface-Enhanced Raman Scattering Substrate Lütfiye Sezen Yildirim1,, Murat Kaya2,∗,, Mürvet Volkan(Tubitak Scientific & Technological Research Council Turkey, 2019) Yıldırım, Lütfiye Sezen; Kaya, Murat; Volkan, MürvetMagnetic and optical bifunctional nanoparticles that combine easy separation, preconcentration, and efficientSERS capabilities have been fabricated with high sensitivity and reproducibility through a low-cost method. Thesegold nanoparticles attached on magnetic silica-coated cobalt nanospheres (Co@SiO2 /AuNPs) display the advantageof strong resonance absorption due to gaps at nanoscale between neighboring metal nanoparticles bringing large fieldenhancements, known as “hot spots”. The prepared particles can be controlled by using an external magnetic field,which makes them very promising candidates in biological applications and Raman spectroscopic analysis of dissolvedorganic species. The magnetic property of the prepared particles lowers the detection limits through preconcentrationwith solid-phase extraction in SERS analysis. The performance of the prepared nanostructures was evaluated as a SERSsubstrate using brilliant cresyl blue (BCB) and rhodamine 6G (R6G) as model compounds. The solid-phase affinityextraction of 4-mercapto benzoic acid (4-MBA) using bifunctional Co@SiO2 /AuNPs nanoparticles followed by magneticseparation and the measurement of the SERS signal on the same magnetic particles without elution were investigated.Approximately 50-fold increase in SERS intensity was achieved through solid-phase extraction of 8.3 × 10 −6 M 4-MBAin 10 min.Article Citation - WoS: 29Amine-Functionalized Graphene Nanosheet-Supported Pdauni Alloy Nanoparticles: Efficient Nanocatalyst for Formic Acid Dehydrogenation(Royal Soc Chemistry, 2018) Bulut, Ahmet; Yurderi, Mehmet; Kaya, Murat; Aydemir, Murat; Baysal, Akin; Durap, Feyyaz; Zahmakiran, MehmetFormic acid (HCOOH), a major by-product of biomass processing with high energy density, stability and non-toxicity, has a great potential as a safe and a convenient liquid hydrogen (H-2) storage material for combustion engines and fuel cell applications. However, high-purity hydrogen release from the catalytic decomposition of aqueous formic acid solution at desirable rates under mild conditions stands as a major challenge that needs to be solved for the practical use of formic acid in on-demand hydrogen generation systems. Described herein is a new nanocatalyst system comprised of 3-aminopropyltriethoxysilane-functionalized graphene nanosheet-supported PdAuNi alloy nanoparticles (PdAuNi/f-GNS), which can reproducibly be prepared by following double solvent method combined with liquid-phase chemical reduction, all at room temperature. PdAuNi/f-GNS selectively catalyzes the decomposition of aqueous formic acid through the dehydrogenation pathway (similar to 100% H-2 selectivity), in the absence of any promoting additives (alkali formates, Bronsted bases, Lewis bases, etc.). PdAuNi/f-GNS nanocatalyst provides CO-free H-2 generation with a turnover frequency of 1090 mol H-2 mol metal(-1) h(-1) in the additive-free dehydrogenation of formic acid at almost complete conversion (>= 92%) even at room temperature. The catalytic activity provided by PdAuNi/f-GNS nanocatalyst is higher than those obtained with the heterogeneous catalysts reported to date for the additive-free dehydrogenation of formic acid. Moreover, PdAuNi/f-GNS nanoparticles show high durability against sintering, clumping and leaching throughout the catalytic runs, so that the PdAuNi/f-GNS nanocatalyst retains almost its inherent catalytic activity and selectivity at the end of the 10th recycle.
