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Article Citation - WoS: 128Mnox< Pdag Alloy Nanoparticles for the Additive-Free Dehydrogenation of Formic Acid at Room Temperature(Amer Chemical Soc, 2015) Bulut, Ahmet; Yurderi, Mehmet; Karatas, Yasar; Say, Zafer; Kivrak, Hilal; Kaya, Murat; Zahmakiran, MehmetFormic acid (HCOOH) has a great potential as a safe and a convenient hydrogen carrier for fuel cell applications. However, efficient and CO-free hydrogen production through the decomposition of formic acid at low temperatures (<363 K) in the absence of additives constitutes a major challenge. Herein, we present a new heterogeneous catalyst system composed of bimetallic PdAg alloy and MnOx nanoparticles supported on amine-grafted silica facilitating the liberation of hydrogen at room temperature through the dehydrogenation of formic acid in the absence of any additives with remarkable activity (330 mol H-2 center dot mol catalyst(-1)center dot h(-1)) and selectivity (>99%) at complete conversion (>99%). Moreover this new catalytic system enables facile catalyst recovery and very high stability against agglomeration, leaching, and CO poisoning. Through a comprehensive set of structural and functional characterization experiments, mechanistic origins of the unusually high catalytic activity, selectivity, and stability of this unique catalytic system are elucidated. Current heterogeneous catalytic architecture presents itself as an excellent contender for clean hydrogen production via room-temperature additive-free dehydrogenation of formic acid for on-board hydrogen fuel cell applications.Article Citation - WoS: 4Citation - Scopus: 7Calcium Carbonate/Polydopamine Composite Nanoplatform Based on Tgf-Β Blockade for Comfortable Cancer Immunotherapy(Amer Chemical Soc, 2024) Li, Yunmeng; Wang, Deqiang; Sun, Jian; Hao, Zhaokun; Tang, Letian; Sun, Wanru; Wang, RanranCancer pain seriously reduces the quality of life of cancer patients. However, most research about cancer focuses solely on inhibiting tumor growth, neglecting the issue of cancer pain. Therefore, the development of therapeutic agents with both tumor suppression and cancer pain relief is crucial to achieve human-centered treatment. Here, the work reports curcumin (CUR) and ropivacaine (Ropi) coincorporating CaCO3/PDA nanoparticles (CaPNMCUR+Ropi) that realized efficient tumor immunotherapy and cancer pain suppression. The therapeutic efficiency and mechanism are revealed in vitro and in vivo. The results indicate that CaPNMCUR+Ropi underwent tumor microenvironment-responsive degradation and realized rapid release of calcium ions, Ropi, and CUR. The excessive intracellular calcium triggered the apoptosis of tumor cells, and the transient pain caused by the tumor injection was relieved by Ropi. Simultaneously, CUR reduced the levels of immunosuppressive factor (TGF-beta) and inflammatory factor (IL-6, IL-1 beta, and TNF-alpha) in the tumor microenvironment, thereby continuously augmenting the immune response and alleviating inflammatory pain of cancer animals. Meanwhile, the decrease of TGF-beta leads to the reduction of transient receptor potential vanilloid 1 (TRPV1) expression, thereby alleviating hyperalgesia and achieving long-lasting analgesic effects. The design of the nanosystem provides a novel idea for human-centered tumor treatment in the future.Article Citation - WoS: 24Citation - Scopus: 23Revealing the Effects of Defect States on the Nonlinear Absorption Properties of the Tlinsse and Tl2in2< Crystals in Near-Infrared Optical Limiting Applications(Amer Chemical Soc, 2024) Dogan, Anil; Karatay, Ahmet; Isik, Mehmet; Yildiz, Elif Akhuseyin; Gasanly, Nizami Mamed; Elmali, AyhanThe present study represents the effect of defect states on the nonlinear absorption and optical limiting performances of TlInSSe and Tl2In2S3Se single crystals with near-infrared excitations. The band gap energies were 2.2 and 2.22 eV, and the Urbach energies were 0.049 and 0.034 eV for TlInSSe and Tl2In2S3Se, respectively. The trapping time of localized defect states was found to be 8 ns by femtosecond transient absorption measurements. The analysis of open-aperture Z-scan data depends on two different fitting models to determine the effect of defect states on the nonlinear absorption (NA) properties of the studied crystals. Model 1 only considers two-photon absorption (TPA), while model 2 includes one-photon absorption (OPA), TPA, and free carrier absorption (FCA). The NA coefficients (ss(eff)) obtained from model 2 are higher than the values (ss) obtained from model 1 at the same intensities, revealing that defect states contribute to NA through OPA. The optical limiting properties of the TlInSSe and Tl2In2S3Se crystals were examined under 1064 nm wavelength excitation. The limiting thresholds were found to be 1.16 and 0.27 mJ/cm(2) at 29.8 GW/m(2) and 99.5 GW/m(2) input intensities, respectively. The results show that TlInSSe and Tl2In2S3Se crystals have promising potential for near-infrared optical limiting applications.Article Citation - WoS: 24Citation - Scopus: 24Light-Induced Paramagnetism in Colloidal Ag+-doped Cdse Nanoplatelets(Amer Chemical Soc, 2021) Najafi, Arman; Sharma, Manoj; Delikanli, Savas; Bhattacharya, Arinjoy; Murphy, Joseph R.; Pientka, James; Petrou, AthosWe describe a study of the magneto-optical properties of Ag+-doped CdSe colloidal nanoplatelets (NPLs) that were grown using a novel doping technique. In this work, we used magnetic circularly polarized luminescence and magnetic circular dichroism spectroscopy to study light-induced magnetism for the first time in 2D solution-processed structures doped with nominally nonmagnetic Ag+ impurities. The excitonic circular polarization (P-X) and the exciton Zeeman splitting (Delta E-Z) were recorded as a function of the magnetic field (B) and temperature (T). Both Delta E-Z and P-X have a Brillouin-function-like dependence on B and T, verifying the presence of paramagnetism in Ag+-doped CdSe NPLs. The observed light-induced magnetism is attributed to the transformation of nonmagnetic Ag+ ions into Ag2+, which have a nonzero magnetic moment. This work points to the possibility of incorporating these nanoplatelets into spintronic devices, in which light can be used to control the spin injection.Article Citation - WoS: 143Citation - Scopus: 157Donor-Acceptor Polymer Electrochromes With Tunable Colors and Performance(Amer Chemical Soc, 2010) Icli, Merve; Pamuk, Melek; Algi, Fatih; Onal, Ahmet M.; Cihaner, AtillaTo demonstrate the effect of donor (D) and acceptor (A) units on the structure property relationships of electrochromic polymers, design, synthesis, characterization and polymerization of a series of D A type systems, 1-5, based on thiophene, 3,4-ethylenedioxythiophene, and 3,3-didecyl-3,4-dihydro-2H-thieno[3,4-b][1,4]dioxepine as D units and 2,1,3-benzoselenadiazole, 2,1,3-benzothiadiazole and 2-decyl-2H-benzo[d][1,2,3]triazole as A units are highlighted. It is found that these units play key roles on the redox behavior, band gap, neutral state color, and the electrochromic performance (stability, optical contrast, coloration efficiency, and switching time) of the system. It is noted that electropolymerization of these D-A systems provides processable low band gap electrochromes, P1-P5, exhibiting high redox stability, coloration efficiency, transmittance and/or contrast ratio and low response time. Furthermore, P1-P5 reflect various hues of blue and green pallets of the RGB color-space in the neutral state. In particular, it is noteworthy that P5 is an excellent blue-to-colorless polymeric electrochrome, which, to our best knowledge, exhibits the highest optical contrast and coloration efficiency among the D A type systems. The panoramic breadth of the neutral state colors and intriguing features of these polymeric materials further confirm that D A approach allows engineering tunable electrochromes, which hold promise for commercialization of polymeric ROB electrochromics.Article Citation - WoS: 22Citation - Scopus: 23Complete 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: 3Citation - Scopus: 3Synthesis of Silver Nanoparticle-Immobilized Antibacterial Anion-Exchange Membranes for Salinity Gradient Energy Production by Reverse Electrodialysis(Amer Chemical Soc, 2024) Eti, Mine; Cihanoglu, Aydin; Hamaloglu, Kadriye Ozlem; Altiok, Esra; Guler, Enver; Tuncel, Ali; Kabay, NalanBiofouling, stemming from the attachment of living microorganisms, such as bacteria, which form resilient biofilms on membrane surfaces, presents a significant challenge that hampers the efficiency of anion-exchange membranes (AEMs) in reverse electrodialysis (RED) applications. This limitation curtails the generation of electrical power from salinity gradients, which notably is a sustainable form of energy known as osmotic energy. RED stands as a clean and promising process to harness this renewable energy source. This study aimed to impart antibacterial activity to synthesized AEMs by using silver nanoparticles (AgNPs). For that purpose, AgNPs were synthesized at 30 degree celsius using two different pH values (6.0 and 9.0) and immobilized into synthesized AEMs using the dip-coating technique. In nanoparticle synthesis, ascorbic acid and trisodium citrate were used as a reductant and a stabilizer, respectively, to take control of the particle size and agglomeration behavior. The results indicated that AgNPs synthesized at pH 6.0 were dispersed on the AEM surface without agglomeration. The stability of AgNPs immobilized on the membrane surface was tested under low- and high-saline solutions. The antibacterial activities of AEMs were determined with the colony-counting method using Gram-negative (Escherichia coli) bacterial suspension. The viability of bacteria dramatically decreased after the immobilization of AgNPs in the AEMs. In the short- and long-term RED tests, it has been observed that the AEMs having AgNPs have high energy-generating potentials, and power density up to 0.372 W/m(2) can be obtained.Article Citation - WoS: 58Fast Neutron Imaging With Semiconductor Nanocrystal Scintillators(Amer Chemical Soc, 2020) McCall, Kyle M.; Sakhatskyi, Kostiantyn; Lehmann, Eberhard; Walfort, Bernhard; Losko, Adrian S.; Montanarella, Federico; Kovalenko, Maksym, VFast neutrons offer high penetration capabilities for both light and dense materials due to their comparatively low interaction cross sections, making them ideal for the imaging of large-scale objects such as large fossils or as-built plane turbines, for which X-rays or thermal neutrons do not provide sufficient penetration. However, inefficient fast neutron detection limits widespread application of this technique. Traditional phosphors such as ZnS:Cu embedded in plastics are utilized as scintillators in recoil proton detectors for fast neutron imaging. However, these scintillation plates exhibit significant light scattering due to the plastic-phosphor interface along with long-lived afterglow (on the order of minutes), and therefore alternative solutions are needed to increase the availability of this technique. Here, we utilize colloidal nanocrystals (NCs) in hydrogen-dense solvents for fast neutron imaging through the detection of recoil protons generated by neutron scattering, demonstrating the efficacy of nanomaterials as scintillators in this detection scheme. The light yield, spatial resolution, and neutron-vs-gamma sensitivity of several chalcogenide (CdSe and CuInS2)-based and perovskite halide-based NCs are determined, with only a short-lived afterglow (below the order of seconds) observed for all of these NCs. FAPbBr(3) NCs exhibit the brightest total light output at 19.3% of the commercial ZnS:Cu(PP) standard, while CsPbBrCl2:Mn NCs offer the best spatial resolution at similar to 2.6 mm. Colloidal NCs showed significantly lower gamma sensitivity than ZnS:Cu; for example, 79% of the FAPbBr(3) light yield results from neutron-induced radioluminescence and hence the neutron-specific light yield of FAPbBr(3) is 30.4% of that of ZnS:Cu(PP). Concentration and thickness-dependent measurements highlight the importance of increasing concentrations and reducing self-absorption, yielding design principles to optimize and foster an era of NC-based scintillators for fast neutron imaging.Article Citation - WoS: 5Citation - Scopus: 5Designing a Solution Processable Poly(3,4-Ethylenedioxyselenophene) Analogue(Amer Chemical Soc, 2018) Ertan, Salih; Cihaner, AtillaA new derivative (EDOS-POSS) of 3,4-ethylenedioxyselenophene integrated with alkyl-substituted polyhedral oligomeric silsesquioxane (POSS) cage was synthesized and characterized. The electroactive monomer was successfully polymerized via both chemical and electrochemical methods. The obtained polymer called PEDOS-POSS was solution-processable and soluble in common organic solvents like tetrahydrofuran, toluene, dichloromethane, and chloroform. PEDOS-POSS polymer exhibited electrochromic behavior: pure blue when neutralized and highly transparent when oxidized. When compared to the parent PEDOS (1.40 eV with lambda(max) = 673 nm), PEDOS-POSS polymer film has a somewhat higher band gap (1.50 eV with lambda(max) = 668 and 724 nm). Also, PEDOS POSS exhibited high optical contrast ratio (59%) and coloration efficiency (593 cm(2)/C for 95% switching) with a low switching time (0.7 s) due to the presence of POSS cage in the polymer backbone. In addition, PEDOS-POSS polymer film was highly robust and stable under ambient conditions (without purging the electrolyte solution with inert gas). Polymer films demonstrated high electrochemical stability; for example, it retained 76% of its electroactivity after 5000 cycles. Furthermore, the polymers exhibited fluorescent properties and exhibited a reddish orange emission centered about at 640 nm. Based on the findings, to the best of our knowledge, it can be concluded that the polymers are the first examples of soluble and fluorescent PEDOS derivatives. These promising properties make PEDOS-POSS polymer a potential material for bioapplications like imaging the cancer cells as well as optoelectronic applications.Article Citation - WoS: 102Citation - Scopus: 107Copper(0) Nanoparticles Supported on Silica-Coated Cobalt Ferrite Magnetic Particles: Cost Effective Catalyst in the Hydrolysis of Ammonia-Borane With an Exceptional Reusability Performance(Amer Chemical Soc, 2012) Kaya, Murat; Zahmakiran, Mehmet; Ozkar, Saim; Volkan, MurvetHerein we report the development of a new and cost-effective nanocomposite catalyst for the hydrolysis of ammonia-borane (NH3BH3), which is considered to be one of the most promising solid hydrogen carriers because of its high gravimetric hydrogen storage capacity (19.6% wt) and low molecular weight. The new catalyst system consisting of copper nanoparticles supported on magnetic SiO2/CoFe2O4 particles was reproducibly prepared by wet-impregnation of Cu(II) ions on SiO2/CoFe2O4 followed by in situ reduction of the Cu(II) ions on the surface of magnetic support during the hydrolysis of NH3BH3 and characterized by ICP-MS, XRD, XPS, TEM, HR-TEM and N-2 adsorption-desorption technique. Copper nanoparticles supported on silica coated cobalt(II) ferrite SiO2/CoFe2O4 (CuNPs@SCF) act as highly active catalyst in the hydrolysis of ammonia-borane, providing an initial turnover frequency of TOF = 2400 h(-1) at room temperature, 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, they were easily recovered by using a permanent magnet in the reactor wall and reused for up, to 10 recycles without losing their inherent catalytic activity significantly, which demonstrates the exceptional reusability of the CuNPs@SCF catalyst.
