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Article Citation - WoS: 16Citation - Scopus: 17Keggin 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: 24Citation - Scopus: 24Complete Dehydrogenation of Hydrazine Borane on Manganese Oxide Nanorod-Supported Ni@ir Core-Shell Nanoparticles(Amer Chemical Soc, 2020) Yurderi, Mehmet; Top, Tuba; Bulut, Ahmet; Kanberoglu, Gulsah Saydan; Kaya, Murat; Zahmakiran, MehmetHydrazine borane (HB; N2H4BH3) has been considered to be one of the most promising solid chemical hydrogen storage materials owing to its high hydrogen capacity and stability under ambient conditions. Despite that, the high purity of hydrogen production from the complete dehydrogenation of HB stands as a major problem that needs to be solved for the convenient use of HB in on-demand hydrogen production systems. In this study, we describe the development of a new catalytic material comprised of bimetallic Ni@Ir core-shell nanoparticles (NPs) supported on OMS-2-type manganese oxide octahedral molecular sieve nanorods (Ni@Ir/OMS-2), which can reproducibly be prepared by following a synthesis protocol including (i) the oleylamine-mediated preparation of colloidal Ni@Ir NPs and (ii) wet impregnation of these ex situ synthesized Ni@Ir NPs onto the OMS-2 surface. The characterization of Ni@Ir/OMS-2 has been done by using various spectroscopic and visualization techniques, and their results have revealed the formation of well-dispersed Ni@Ir core-shell NPs on the surface of OMS-2. The catalytic employment of Ni@Ir/OMS-2 in the dehydrogenation of HB showed that Ni-0.22@Ir-0.78/OMS-2 exhibited high dehydrogenation selectivity (>99%) at complete conversion with a turnover frequency (TOF) value of 2590 h(-1) at 323 K, which is the highest activity value among all reported catalysts for the complete dehydrogenation of HB. Furthermore, the Ni-0.22@Ir-0.78/OMS-2 catalyst enables facile recovery and high stability against agglomeration and leaching, which make it a reusable catalyst in the complete dehydrogenation of HB. The studies reported herein also include the collection of wealthy kinetic data to determine the activation parameters for Ni-0.22@Ir-0.78/OMS-2-catalyzed dehydrogenation of HB.Article Citation - WoS: 25Citation - Scopus: 28The Pimpled Gold Nanosphere: a Superior Candidate for Plasmonic Photothermal Therapy(Dove Medical Press Ltd, 2020) Nasseri, Behzad; Turk, Mustafa; Kosemehmetoglu, Kemal; Kaya, Murat; Piskin, Erhan; Rabiee, Navid; Webster, Thomas J.Background: The development of highly efficient nanoparticles to convert light to heat for anti-cancer applications is quite a challenging field of research. Methods: In this study, we synthesized unique pimpled gold nanospheres (PGNSs) for plasmonic photothermal therapy (PPTT). The light-to-heat conversion capability of PGNSs and PPTT damage at the cellular level were investigated using a tissue phantom model. The ability of PGNSs to induce robust cellular damage was studied during cytotoxicity tests on colorectal adenocarcinoma (DLD-1) and fibroblast cell lines. Further, a numerical model of plasmonic (COMSOL Multiphysics) properties was used with the PPTT experimental assays. Results: A low cytotoxic effect of thiolated polyethylene glycol (SH-PEG400-SH-) was observed which improved the biocompatibility of PGNSs to maintain 89.4% cell viability during cytometry assays (in terms of fibroblast cells for 24 hrs at a concentration of 300 mu g/mL). The heat generated from the nanoparticle-mediated phantom models resulted in Delta T=30 degrees C, Delta T=23.1 degrees C and Delta T=21 degrees C for the PGNSs, AuNRs, and AuNPs, respectively (at a 300 mu g/mL concentration and for 325 sec). For the in vitro assays of PPTT on cancer cells, the PGNS group induced a 68.78% lethality (apoptosis) on DLD-1 cells. Fluorescence microscopy results showed the destruction of cell membranes and nuclei for the PPTT group. Experiments further revealed a penetration depth of sufficient PPTT damage in a physical tumor model after hematoxylin and eosin (H&E) staining through pathological studies (at depths of 2, 3 and 4 cm). Severe structural damages were observed in the tissue model through an 808-nm laser exposed to the PGNSs. Conclusion: Collectively, such results show much promise for the use of the present PGNSs and photothermal therapy for numerous anti-cancer applications.Master Thesis Poli (n- Metilanilin) Eklenmiş Gümüş Nanopartiküllerin Antibakteriyel Aktivitesinin Araştırılması(2022) Aldarajı, Mostafa Kamıl Maala; İşgör, Sultan Belgin; Kaya, Muratİnsanlar, hayvanlar ve mahsuller, belirli bakteri türlerinin neden olduğu birçok hastalıktan muzdarip olabilir. Bu bakterilerin, karşılaşabilecekleri en uygun araçları belirlemek için derinlemesine araştırılması gerekir. Bu bakteri türleri arasında (Escherichia coli) ve (Staphylococcus aureus) bulunur. Gümüş, bakterileri yok edebilecek bazı kimyasal ve fiziksel özelliklere sahip olduğu için bu bakterilerin yayılmasının tedavisinde kullanılan en önemli mineral elementlerden biridir. Etkinliği incelenen bu özelliklerden biri Nanoteknolojidir. Bunlar 1 ila 100 nanometre arasında değişen parçacıklardır. Bu parçacıkların dış zarlara nüfuz edebildiği ve hücreye girebileceği bulunmuştur. Bunu kullanarak, protein üretimini durdurmak için çalışır ve gümüş nanopartiküller ile bulunan yüksek toksisite nedeniyle canlı hücreyi öldürmeye başlar. Ek olarak, gümüş nanopartiküllere poli (n-metil anilin) ilave edildi. PNMA 0.025 M monomer çözeltisi ile hazırlandı. Elde edilen PNMA kürelerinin boyutu 200-550 nm arasındadır. Poli (N-metil anilin) gümüş nanopartikülleri (PNMA-AGNP'LER) başarıyla hazırlamak için oksidatif kimyasal polimerizasyon ve sıvı emprenye yöntemleri kullanıldı. Elde edilen partikülleri karakterize etmek için SEM, TEM, EDX ve ICP-Oe'ler kullanıldı. Bu bileşiklerin; PNMA ve Ag-Pnma'nın Escherichia coli ve Staphylococcus aureus'a karşı antibakteriyel etkileri incelenmiş ve bu bileşiklerin penisilin/streptomisin ortak antibiyotiği ile etkileri karşılaştırılmıştır.Master Thesis Amin Borandan Hidrojen Üretilmesi için Üzerine Bimetalik Gümüş-bakır Nanoparçacıkları Eklenmiş Silika Kaplı Kobalt Ferrit Manyetik Nanoparçacıkların Hazırlanması(2016) Mohammed, Salma S. Abdalla; Kaya, MuratHidrojen en önemli temiz enerji kaynaklarından biri olarak bilinmektedir ve mobil uygulamalar için hidrojen taşıyıcı sistemler ve bu sistemlerden hidrojen eldesini sağlayacak metodların geliştirilmesi çok önemlidir. Literatürde olarak metal hidrürler, kimyasal hidrürler, organic moleküller, metal organic kafes yapıları ve karbon nanotüpler gibi hidrojen depolama malzemeleri ile ilgili bir çok yayın bulunmaktadır.Bunlar arasında kimyasal hidrürler yüksek hidrojen depolama kapasiteleri sebebi ile büyük ilgi görmektedir. Kararlılığı ve toksik olmaması yanında kütlece 19.6 % oranında hidrojene sahip olması sebebi ile amin boran önemli bir bidrojen depolama malzemesi olarak bilinmektedir. Uygun katalizör kullanımı ile normal şartlarda 1 mol amin borandan 3 mol hidrojen eldesi mümkündür. Amin borandan hidrojen eldesinde kinetic parametrelerin iyileştirilmesi için yüksek etkiye sahip katalizörlerin heliştirilmesi, hidrojen enerjisinin mobil uygulamaları için çok önemlidir. Bunun yanında katalizörün reaksiyon ortamından ayrılması ve tekrar kullanımı, üstesinden gelinmesi gereken diğer önemli konulardır. Bu çalışmada, amin borandan hidrolitik olarak hidrojen eldesin için katalizör olarak manyetik olarak ayrılabilen CoFe2O4@SiO2 destek malzemesine ıslak emdirme yöntemi ile ekelenmiş gümüş-bakır nanoparçacıklarının hazırlanması için kolay bir yöntem rapor edilmiştir. Hazırlanan katalizör oda sıcaklığında amin borandan hidrojen eldesi reaksiyonunda mükemmel katalitik aktivite göstermiştir. İlk çevrim frekansı 146 dk-1 olarak hesaplanmıştır. Buna ek olarak, CoFe2O4@SiO2 destek malzemesi üzerine eklenmiş AgCu nanoparçacıklar, kaydadeğer kararlılık ve tekrar kullanılabilme kabiliyeti göstermiştir ve amin borandan hidrojen eldesinde 10. kullanımda bile tam çevrimde hemen hemen ilk aktivitesini korumuştur.Article Citation - WoS: 35Citation - Scopus: 37Hydroxyapatite-Nanosphere Supported Ruthenium(0) Nanoparticle Catalyst for Hydrogen Generation From Ammonia-Borane Solution: Kinetic Studies for Nanoparticle Formation and Hydrogen Evolution(Royal Soc Chemistry, 2014) Durak, Halil; Gulcan, Mehmet; Zahmakiran, Mehmet; Ozkar, Saim; Kaya, MuratThe development of readily prepared effective heterogeneous catalysts for hydrogen generation from ammonia-borane (AB; NH3BH3) solution under mild conditions still remains a challenge in the field of "hydrogen economy". In this study, we report our finding of an in situ generated, highly active ruthenium nanocatalyst for the dehydrogenation of ammonia-borane in water at room temperature. The new catalyst system consists of ruthenium(0) nanoparticles supported on nanohydroxyapatite (RuNPs@nano-HAp), and can be reproducibly prepared under in situ conditions from the ammonia-borane reduction of Ru3+ ions exchanged into nanohydroxyapatite (Ru3+@nano-HAp) during the hydrolytic dehydrogenation of ammonia-borane at 25 +/- 0.1 degrees C. Nanohydroxyapatite-supported ruthenium(0) nanoparticles were characterized by a combination of advanced analytical techniques. The sum of their results shows the formation of well-dispersed ruthenium(0) nanoparticles with a mean diameter of 2.6 +/- 0.6 nm on the surface of the nanospheres of hydroxyapatite by keeping the host matrix intact. The resulting RuNPs@nano-HAp are highly active catalyst in the hydrolytic dehydrogenation of ammonia-borane with an initial TOF value of 205 min(-1) by generating 3.0 equiv. of H-2 per mole of ammonia-borane at 25 +/- 0.1 degrees C. Moreover, they are sufficiently stable to be isolated and bottled as solid materials, which can be reused as active catalyst under the identical conditions of first run. The work reported here also includes the following results: (i) monitoring the formation kinetics of the in situ generated RuNPs@nano-HAp by hydrogen generation from the hydrolytic dehydrogenation of ammonia-borane as the reporter reaction. The sigmoidal kinetics of catalyst formation and concomitant dehydrogenation fits well to the two-step, slow nucleation, followed by autocatalytic surface growth mechanism, P -> Q (rate constant k(1)) and P + Q -> 2Q (rate constant k(2)), in which P is Ru3+@nano-HAp and Q is the growing, catalytically active RuNPs@nano-HAp; (ii) the compilation of kinetic data for the RuNPs@nano-HAp catalyzed hydrolytic dehydrogenation of ammonia-borane depending on the temperature and catalyst concentration to determine the dependency of reaction rate on catalyst concentration and activation parameters (E-a, Delta H-#, and Delta S-#) of the reaction.Article Citation - WoS: 142Citation - Scopus: 148Carbon Dispersed Copper-Cobalt Alloy Nanoparticles: a Cost-Effective Heterogeneous Catalyst With Exceptional Performance in the Hydrolytic Dehydrogenation of Ammonia-Borane(Elsevier, 2016) Bulut, Ahmet; Yurderi, Mehmet; Ertas, Ilknur Efecan; Celebi, Metin; Kaya, Murat; Zahmakiran, MehmetHerein, 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 - WoS: 23Citation - Scopus: 27Nanocrystalline Metal Organic Framework (mil-101) Stabilized Copper Nanoparticles: Highly Efficient Nanocatalyst for the Hydrolytic Dehydrogenation of Methylamine Borane(Elsevier Science Sa, 2018) Baguc, Ismail Burak; Ertas, Ilknur Efecan; Yurderi, Mehmet; Bulut, Ahmet; Zahmakiran, Mehmet; Kaya, MuratThe 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 - WoS: 153Citation - Scopus: 156Pd-mnox< Nanoparticles Dispersed on Amine-Grafted Silica: Highly Efficient Nanocatalyst for Hydrogen Production From Additive-Free Dehydrogenation of Formic Acid Under Mild Conditions(Elsevier Science Bv, 2015) Bulut, Ahmet; Yurderi, Mehmet; Karatas, Yasar; Zahmakiran, Mehmet; Kivrak, Hilal; Gulcan, Mehmet; Kaya, MuratHerein we report the development of a new highly active, selective and reusable nanocatalyst for additive-free dehydrogenation of formic acid (HCOOH), which has great potential as a safe and convenient hydrogen carrier for fuel cells, under mild conditions. The new catalyst system consisting of bimetallic Pd-MnOx nanoparticles supported on aminopropyl functionalized silica (Pd-MnOx/SiO2-NH2) was simply and reproducibly prepared by deposition-reduction technique in water at room temperature. The characterization of Pd-mnO(x)/SiO2-NH2 catalyst was done by the combination of multipronged techniques, which reveals that the existence of highly crystalline individually nucleated Pd(0) and MnOx nanoparticles (d(mean) = 4.6 +/- 1.2 nm) on the surface of aminopropyl functionalized silica. These supported Pd-MnOx nanoparticles can catalyze the additive-free dehydrogenation of formic acid with record activity (TOF = 1300 h(-1)) at high selectivity (>99%) and conversion (>99%) under mild conditions (at 50 degrees C and under air). Moreover, easy recovery plus high durability of these supported Pd-MnOx nanoparticles make them a reusable heterogeneous catalyst in the additive-free dehydrogenation of formic acid. (C) 2014 Elsevier B.V. All rights reserved.Master Thesis Manyetik-pedot-tio2 Nanokompozit Malzemenin Hazırlanması ve Fotokatalitik Uygulaması(2016) Erabe, Naden Mohammed Alı; Kaya, MuratGeleneksel atık su arıtma yöntemlerinin kirletici maddeleri etkili bir şekilde uzaklaştırılmasında yetersiz kalması nedeniyle yeni, etkili ve düşük maliyetli tekniklerin araştırılmasına neden olmuştur. Sıkı çevresel düzenlemelere katkı sağlamak için, bu organik maddelerin oksidasyonu önemlidir. Radikaller, sık sık kullanılan diğer yükseltgenlerle kıyaslandığında mükemmel bir oksitleme gücüne sahiptirler ve tam olarak bozulmayı sağlarlar. Geliştirilmiş oksidasyon prosesleri (AOPs) adı verilen yöntemler, homojen ve heterojen fotokatalitik yöntemleri kapsar. Bu yöntemlerde, yarıiletkenin aktivasyonu elektron ve deliklerin oluşmasına neden olur. Bu deliğin su ile tepkimesi hidroksil radikalini oluştururken, kirleticileri ortadan kaldırmak için bir seri indirgenme-yükseltgenme tepkimelerinin meydana gelmesini sağlar. Bu günlerde, özellikle TiO2'in yarı iletken fotokatalizör olarak kullanımı, havada ve su atık endüstrisinde elverişli olarak kullanılabilmesi nedeniyle önemlidir. Düşük maliyetli, çevre dostu, sürdürülebilir işleme metotlarının elde edilebilmesini sağlar. Ancak, küçük boyutta fotokatalizör parçacıklarının, büyük hacimlerdeki sudan uzaklaştırılması için daha fazla çaba gereklidir. Bu da, kullanımında büyük bir dezavantaja neden olmaktadır. Bu tezde, yüksek fotokatalitik aktivitesi ve iyi-ayırma özelliği olan malzeme elde edebilmek için, manyetik, geri dönüştürülebilir, yeni bir SiO2-CoFe2O4/PEDOT/TiO2 nanokompozit malzemenin fotokatalizör olarak kullanılabilmesi için hazırlanışı ile ilgili basit bir prosedür önermekteyiz. Nanokompozit katalizörün karakterizasyonu taramalı elektron mikroskopu (SEM), geçirimli elektron mikroskobu (TEM), yüksek çözünürlüklü geçirimli elektron mikroskobu (HR-TEM), SEM ile birleştirilen enerji dağılım X-Ray ve Raman spektroskopisi teknikleri ile yapılmıştır. SiO2-CoFe2O4/PEDOT/TiO2 nanokompozit malzemenin fotokatalitik aktivitesi metilen mavisinin UV ışığı altında boya giderimi ile araştırılmıştır. Ayrıca, TiO2 ve PEDOT'un fotokatalitik aktivitesi, son yapı ile karşılaştırılmıştır. Sonuç olarak, PEDOT polimerin varlığı ve TiO2 ile PEDOT arasındaki sinerjik ilişki, fotokatalitik tepkimede önemli bir rol oynar. Yüksek fotokatalitik aktivitesinin yanında, SiO2-CoFe2O4/PEDOT/TiO2 nanokompozit malzemenin, manyetik olarak ayrılma avantajı vardır. PEDOT içermesi, fotokatalitik aktivitesini arttırmasının yanı sıra, manyetik nanoparçacıklarının eklenmesi, son yapının manyetik özelliğinin de olmasına olanak sağlar.
