Browsing by Author "Ertas, Ilknur Efecan"
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Article Citation Count: 48Atomic layer deposition-SiO2 layers protected PdCoNi nanoparticles supported on TiO2 nanopowders: Exceptionally stable nanocatalyst for the dehydrogenation of formic acid(Elsevier Science Bv, 2017) Kaya, Murat; Bulut, Ahmet; Yurderi, Mehmet; Ertas, Ilknur Efecan; Kivrak, Hilal; Kaya, Murat; Zahmakiran, Mehmet; Chemical EngineeringTiO2 nanopowders supported trimetallic PdCoNi alloy nanoparticles were simply and reproducibly prepared by wet-impregnation followed by simultaneous reduction method, then to enhance their stability against to sintering and leaching atomic layer deposition (ALD) technique was utilized to grow SiO2 layers amongst these surface bound PdCoNi alloy nanoparticles (PdCoNi/TiO2-ALD-SiO2). These new nanomaterials are characterized by the combination of complimentary techniques and sum of their results exhibited that the formation of ALD-SiO2 layers protected well-dispersed and highly crystalline PdCoNi alloy nanoparticles (ca. 3.52 nm) supported on TiO2 nanopowders. The catalytic performance of the resulting PdCoNi/TiO2-ALD-SiO2 in terms of activity, selectivity and stability was investigated in the dehydrogenation of aqueous formic acid (HCOOH), which has recently been suggested as a promising hydrogen storage material with a 4.4 wt% hydrogen capacity, solution under mild conditions. The results collected from our systematic studies revealed that PdCoNi/TiO2-ALD-SiO2 nanomaterial can act as highly active and selective nanocatalyst in the formic acid dehydrogenation at room temperature by providing an initial turnover frequency (TOF) value of 207 mol H-2/mol metal;: h and >99% of dehydrogenation selectivity at almost complete conversion. More importantly, the catalytic reusability experiments separately carried out with PdCoNi/TiO2-ALD-SiO2 and PdCoNi/TiO2 nanocatalysts in the dehydrogenation of formic acid under more forcing conditions pointed out that PdCoNi/TiO2-ALD-SiO2 nanocatalyst displays unprecedented catalytic stability against to leaching and sintering throughout the reusability experiments it retains almost its inherent activity, selectivity and conversion even at 20th reuse, whereas analogous PdCoNi/TiO2 completely lost its catalytic performance. (C) 2017 Elsevier B.V. All rights reserved.Article Citation Count: 130Carbon dispersed copper-cobalt alloy nanoparticles: A cost-effective heterogeneous catalyst with exceptional performance in the hydrolytic dehydrogenation of ammonia-borane(Elsevier, 2016) Kaya, Murat; Yurderi, Mehmet; Ertas, Ilknur Efecan; Celebi, Metin; Kaya, Murat; Zahmakiran, Mehmet; Chemical EngineeringHerein, we report the development of a new and cost-effective nanocatalyst for the hydrolytic dehydrogenation of ammonia-borane (NH3BH3), which is considered to be one of the most promising solid hydrogen carriers due to its high gravimetric hydrogen storage capacity (19.6 wt%) and low molecular weight. The new catalyst system consisting of bimetallic copper-cobalt alloy nanoparticles supported on activated carbon was simply and reproducibly prepared by surfactant-free deposition-reduction technique at room temperature. The characterization of this new catalytic material was done by the combination of multi-pronged techniques including ICP-MS, XRD, XPS, BFTEM, HR-TEM, STEM and HAADF-STEM-line analysis. The sum of their results revealed that the formation of copper-cobalt alloy nanoparticles (d(mean) =1.8 nm) on the surface of activated carbon (CuCo/C). These new carbon supported copper-cobalt alloy nanoparticles act as highly active catalyst in the hydrolytic dehydrogenation of ammonia-borane, providing an initial turnover frequency of TOF = 2700 h(-1) at 298 K, which is not only higher than all the non-noble metal catalysts but also higher than the majority of the noble metal based homogeneous and heterogeneous catalysts employed in the same reaction. More importantly, easy recovery and high durability of these supported CuCo nanoparticles make CuCo/C recyclable heterogeneous catalyst for the hydrolytic dehydrogenation of ammonia-borane. They retain almost their inherent activity even at 10th catalytic reuse in the hydrolytic dehydrogenation of ammonia-borane at 298K. (C) 2015 Elsevier B.V. All rights reserved.Article Citation Count: 13Keggin 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) Kaya, Murat; Saglam, Serif; Ertas, Ilknur Efecan; Keles, Muhammed Nuri; Celebi, Metin; Kaya, Murat; Zahmakiran, Mehmet; Chemical EngineeringDescribed 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 Count: 23Nanocrystalline metal organic framework (MIL-101) stabilized copper Nanoparticles: Highly efficient nanocatalyst for the hydrolytic dehydrogenation of methylamine borane(Elsevier Science Sa, 2018) Kaya, Murat; Ertas, Ilknur Efecan; Yurderi, Mehmet; Bulut, Ahmet; Zahmakiran, Mehmet; Kaya, Murat; Chemical EngineeringThe copper nanoparticles stabilized by nanocrystalline MIL-101 framework (Cu/nano-MIL-101) was reproducibly prepared by following double solvent method combined with liquid phase chemical reduction technique. The characterization of the resulting new material was done by using various analytical techniques including ICP-OES, P-XRD, N-2-adsorption-desorption, XPS, FE-SEM, SEM-EDX, BFTEM and HAADF-STEM; the summation of their results reveals that the formation of well-dispersed and very small sized (0.8 nm) copper nanoparticles within nanocrystalline MIL-101 framework. The catalytic performance of Cu/nano-MIL-101 in terms of activity and stability was tested in the hydrolytic dehydrogenation of methylamine borane (CH3NH2BH3), which has been considered as one of the attractive materials for the efficient chemical hydrogen storage. Cu/nano-MIL-101 catalyzes the hydrolytic dehydrogenation of methylamine borane with high activity (turnover frequency; TOF = 257 mot H-2/mol Cu x h) and conversion ( > 99%) under air at room temperature. Moreover, these nano-MIL-101 framework stabilized copper nanoparticles show great durability against to sintering and leaching, which make Cu/nano-MIL-101 reusable nanocatalyst in the hydrolytic dehydrogenation of methylamine-borane. Cu/nano-MIL-101 nanocatalyst retains 83% of its inherent activity at complete conversion even at 10th recycle in the hydrolytic dehydrogenation of methylamine borane.Article Citation Count: 7Nanohydrotalcite Supported Ruthenium Nanoparticles: Highly Efficient Heterogeneous Catalyst for the Oxidative Valorization of Lignin Model Compounds(Wiley-v C H verlag Gmbh, 2017) Kaya, Murat; Celebi, Metin; Karakas, Kadir; Ertas, Ilknur Efecan; Keles, Muhammed Nuri; Kaya, Murat; Zahmakiran, Mehmet; Chemical EngineeringThe 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 Count: 37Palladium Nanoparticles Decorated Graphene Oxide: Active and Reusable Nanocatalyst for the Catalytic Reduction of Hexavalent Chromium(VI)(Wiley-v C H verlag Gmbh, 2017) Kaya, Murat; Karakas, Kadir; Ertas, Ilknur Efecan; Kaya, Murat; Zahmakiran, Mehmet; Chemical EngineeringToday, 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 Citation Count: 122PdAu-MnOx nanoparticles supported on amine-functionalized SiO2 for the room temperature dehydrogenation of formic acid in the absence of additives(Elsevier Science Bv, 2016) Karatas, Yasar; Bulut, Ahmet; Yurderi, Mehmet; Ertas, Ilknur Efecan; Alal, Orhan; Gulcan, Mehmet; Zahmakiran, MehmetFormic acid (HCOOH) has recently been suggested as a promising hydrogen carrier for fuel cell applications. However efficient hydrogen production through the decomposition of formic acid in the absence of additives under mild thermodynamic conditions constitutes a major challenge because of the ease poisoning of active metals with CO formed as intermediate during formic acid decomposition. Recently, we have reported (App. Catal. B: Env. 164 (2015) 324) our discovery that the separately nucleated MnOx nanoparticles act as CO-sponge around catalytically active Pd nanoparticles exist on the same support and enhances both the activity and CO-resistivity of Pd nanoparticles. Using this important finding, herein, we present a new catalyst system consists of the physical mixture of PdAu alloy and MnOx nanoparticles supported on amine-grafted silica (PdAu-MnOx/N-SiO2) for the room temperature dehydrogenation of formic acid in the absence of any additives. PdAu-MnOx/N-SiO2 catalyst was simply prepared by deposition-reduction technique in water at room temperature with high reproducibility and characterized by the combination of various spectroscopic tools including ICP-OES, P-XRD, DR/UV-vis, XPS, BFTEM, STEM-EDX, STEM-line analysis and CO-stripping voltammetry techniques. The sum of their results shows that the formation of physical mixture of PdAu alloy and MnOx (dmean=2.2 nm) nanoparticles on the surface of support material. This new catalytic material facilitates the hydrogen liberation through the additive-free formic acid dehydrogenation at room temperature with previously unprecedented activity (TOF=785 mol H-2 mol catalyst(-1) h(-1)), converging to that of the existing state of the art homogenous catalysts. This new superior catalytic system enables facile catalyst recovery and very high stability against agglomeration, leaching and CO poisoning, which make it highly reusable catalyst (retains >92% activity and 85% conversion at the 5th catalytic reuse) in the additive-free formic acid dehydrogenation at room temperature. (C) 2015 Elsevier B.V. All rights reserved.Article Citation Count: 114Supported copper-copper oxide nanoparticles as active, stable and low-cost catalyst in the methanolysis of ammonia-borane for chemical hydrogen storage(Elsevier Science Bv, 2015) Kaya, Murat; Bulut, Ahmet; Ertas, Ilknur Efecan; Zahmakiran, Mehmet; Kaya, Murat; Chemical EngineeringThe physical mixture of copper (Cu) copper(I) oxide (Cu2O) and copper(II) oxide (CuO) nanoparticles supported on activated carbon (Cu-Cu2O-CuO/C) were reproducibly prepared by a simple deposition-reduction technique without using any stabilizer in water at room temperature. The characterization of the resulting material by ICP-OES, P-XRD, XPS, DR-UV/vis, BFTEM and HRTEM techniques reveals that the formation of well-dispersed highly crystalline 3.8 +/- 1.7 nm nanoparticles on the surface of activated carbon. These carbon supported Cu-Cu2O-CuO nanoparticles were employed as heterogeneous catalyst in the methanolysis of ammonia-borane (NH3BH3), which has been considered as one of the attractive materials for the efficient storage of hydrogen, under mild conditions. We found that only 3.0 mol % Cu-Cu2O-CuO/C catalyst is enough to catalyze the methanolysis of ammonia-borane with high activity (TOF = 24 min(-1)) and conversion (>99%) at room temperature. More importantly, the exceptional stability of supported Cu-Cu2O-CuO nanoparticles against to sintering and leaching make Cu-Cu2O-CuO/C recyclable catalyst for the methanolysis of ammonia-borane. Cu-Cu2O-CuO/C catalyst retains >76% of its initial activity with 94% of conversion even at 8th recycle in the methanolysis of ammonia-borane at complete conversion. The study reported here also includes the collection of kinetic data for Cu-Cu2O-CuO/C catalyzed methanolysis of ammonia-borane depending on catalyst [Cu], substrate [NH3BH3] concentrations and temperature to determine the rate expression and the activation parameters (E-a, Delta H-#, and Delta S-#) of the catalytic reaction. (C) 2014 Published by Elsevier B.V.Correction Citation Count: 2Supported copper-copper oxide nanoparticles as active, stable and low-cost catalyst in the methanolysis of ammonia-borane for chemical hydrogen storage (vol 165, pg 169, 2015)(Elsevier, 2016) Kaya, Murat; Bulut, Ahmet; Ertas, Ilknur Efecan; Zahmakiran, Mehmet; Kaya, Murat; Chemical Engineering[No Abstract Available]