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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: 5Citation - Scopus: 8Calcium 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: 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: 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: 61Fast 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: 47Citation - Scopus: 52Biocompatible Electroactive Tetra(aniline)-Conjugated Peptide Nanofibers for Neural Differentiation(Amer Chemical Soc, 2018) Arioz, Idil; Erol, Ozlem; Bakan, Gokhan; Dikecoglu, F. Begum; Topal, Ahmet E.; Urel, Mustafa; Guler, Mustafa O.Peripheral nerve injuries cause devastating problems for the quality of patients' lives, and regeneration following damage to the peripheral nervous system is limited depending on the degree of the damage. Use of nanobiomaterials can provide therapeutic approaches for the treatment of peripheral nerve injuries. Electroactive biomaterials, in particular, can provide a promising cure for the regeneration of nerve defects. Here, a supramolecular electroactive nanosystem with tetra(aniline) (TA)-containing peptide nanofibers was developed and utilized for nerve regeneration. Self-assembled TA conjugated peptide nanofibers demonstrated electroactive behavior. The electroactive self-assembled peptide nanofibers formed a well-defined three-dimensional nanofiber network mimicking the extracellular matrix of the neuronal cells. Neurite outgrowth was improved on the electroactive TA nanofiber gels. The neural differentiation of PC-12 cells was more advanced on electroactive peptide nanofiber gels, and these biomaterials are promising for further use in therapeutic neural regeneration applications.Article Citation - WoS: 130Mnox< 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: 61Citation - Scopus: 63Fabrication of Supramolecular N/P-nanowires via Coassembly of Oppositely Charged Peptide-Chromophore Systems in Aqueous Media(Amer Chemical Soc, 2017) Khalily, Mohammad Aref; Bakan, Gokhan; Kucukoz, Betul; Topal, Ahmet Emin; Karatay, Ahmet; Yaglioglu, H. Gul; Guler, Mustafa O.Fabrication of supramolecular electroactive materials at the nanoscale with well-defined size, shape, composition, and organization in aqueous medium is a current challenge. Herein we report construction of supramolecular charge-transfer complex one-dimensional (1D) nanowires consisting of highly ordered mixed-stack pi-electron donor-acceptor (D-A) domains. We synthesized n-type and p-type beta-sheet forming short peptide-chromophore conjugates, which assemble separately into well-ordered nanofibers in aqueous media. These complementary p-type and n-type nanofibers coassemble via hydrogen bonding, charge-transfer complex, and electrostatic interactions to generate highly uniform supramolecular n/p-coassembled 1D nanowires. This molecular design ensures highly ordered arrangement of D-A stacks within n/p-coassembled supramolecular nanowires. The supramolecular n/p-coassembled nanowires were found to be formed by A D-A unit cells having an association constant (K-A) of 5.18 x 10(5) M-1. In addition, electrical measurements revealed that supramolecular n/p-coassembled nanowires are approximately 2400 and 10 times more conductive than individual n-type and p-type nanofibers, respectively. This facile strategy allows fabrication of well-defined supramolecular electroactive nanomaterials in aqueous media, which can find a variety of applications in optoelectronics, photovoltaics, organic chromophore arrays, and bioelectronics.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: 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.
