ICN2 Publications

2017

  • A statistical analysis of nanocavities replication applied to injection moulding

    Pina-Estany J., Colominas C., Fraxedas J., Llobet J., Perez-Murano F., Puigoriol-Forcada J.M., Ruso D., Garcia-Granada A.A. International Communications in Heat and Mass Transfer; 81: 131 - 140. 2017. 10.1016/j.icheatmasstransfer.2016.11.003.

    The purpose of this paper is to investigate both theoretically and experimentally how nanocavities are replicated in the injection moulding manufacturing process. The objective is to obtain a methodology for efficiently replicate nanocavities. From the theoretical point of view, simulations are carried out using a submodeling approach combining Solidworks Plastics for a first macrosimulation and Fluent solver for a subsequent nanosimulation. The effect of the four main factors (melt temperature, mould temperature, filling time and cavity geometry) are quantified using an statistical 24 factorial experiment. It is found that the main effects are the cavity length, the mould temperature and the polymer temperature, with standardized effects of 5, 3 and 2.6, respectively. Filling time has a negative 1.3 standardized effect. From the experimental point of view, Focused Ion Beam technique is used for mechanizing nanocavities in a steel mould. The replication achieved in polycarbonate injection is quantified using an Atomic Force Microscope. It is observed how both the geometry and the position of the cavities in the mould affect its replication. © 2016 Elsevier Ltd


  • A universal strategy for metal oxide anchored and binder-free carbon matrix electrode: A supercapacitor case with superior rate performance and high mass loading

    Zhang X., Luo J., Tang P., Ye X., Peng X., Tang H., Sun S.-G., Fransaer J. Nano Energy; 31: 311 - 321. 2017. 10.1016/j.nanoen.2016.11.024.

    Despite the significant advances in preparing carbon-metal oxide composite electrodes, strategies for seamless interconnecting of these two materials without using binders are still scarce. Herein we design a novel method for in situ synthesis of porous 2D-layered carbon–metal oxide composite electrode. Firstly, 2D-layered Ni-Co mixed metal-organic frameworks (MOFs) are deposited directly on nickel foam by anodic electrodeposition. Subsequent pyrolysis and activation procedure lead to the formation of carbon–metal oxides composite electrodes. Even with an ultrahigh mass loading of 13.4 mg cm−2, the as-prepared electrodes exhibit a superior rate performance of 93% (from 1 to 20 mA cm−2), high capacitance (2098 mF cm−2 at a current density of 1 mA cm−2), low resistance and excellent cycling stability, making them promising candidates for practical supercapacitor application. As a proof of concept, several MOF derived electrodes with different metal sources have also been prepared successfully via the same route, demonstrating the versatility of the proposed method for the preparation of binder-free carbon–metal oxide composite electrodes for electrochemical devices. © 2016 Elsevier Ltd


  • Analysis of alternative splicing events for cancer diagnosis using a multiplexing nanophotonic biosensor

    Huertas C.S., Domínguez-Zotes S., Lechuga L.M. Scientific Reports; 7 ( 41368) 2017. 10.1038/srep41368.

    NanoBiosensors and Bioanalytical Applications

    Personalized medicine is a promising tool not only for prevention, screening and development of more efficient treatment strategies, but also for diminishing the side effects caused by current therapies. Deciphering gene regulation pathways provides a reliable prognostic analysis to elucidate the origin of grave diseases and facilitate the selection of the most adequate treatment for each individual. Alternative splicing of mRNA precursors is one of these gene regulation pathways and enables cells to generate different protein outputs from the same gene depending on their developmental or homeostatic status. Its deregulation is strongly linked to disease onset and progression constituting a relevant and innovative class of biomarker. Herein we report a highly selective and sensitive nanophotonic biosensor based on the direct monitoring of the aberrant alternative splicing of Fas gene. Unlike conventional methods, the nanobiosensor performs a real-time detection of the specific isoforms in the fM-pM range without any cDNA synthesis or PCR amplification requirements. The nanobiosensor has been proven isoform-specific with no crosshybridization, greatly minimizing detection biases. The demonstrated high sensitivity and specificity make our nanobiosensor ideal for examining significant tumor-associated expression shifts of alternatively spliced isoforms for the early and accurate theranostics of cancer.


  • Analysis of C9orf72 repeat expansions in a large international cohort of dementia with Lewy bodies

    Kun-Rodrigues C., Ross O.A., Orme T., Shepherd C., Parkkinen L., Darwent L., Hernandez D., Ansorge O., Clark L.N., Honig L.S., Marder K., Lemstra A., Scheltens P., van der Flier W., Louwersheimer E., Holstege H., Rogaeva E., St. George-Hyslop P., Londos E., Zetterberg H., Barber I., Braae A., Brown K., Morgan K., Maetzler W., Berg D., Troakes C., Al-Sarraj S., Lashley T., Holton J., Compta Y., Van Deerlin V., Trojanowski J.Q., Serrano G.E., Beach T.G., Clarimon J., Lleó A., Morenas-Rodríguez E., Lesage S., Galasko D., Masliah E., Santana I., Diez M., Pastor P., Tienari P.J., Myllykangas L., Oinas M., Revesz T., Lees A., Boeve B.F., Petersen R.C., Ferman T.J., Escott-Price V., Graff-Radford N., Cairns N.J., Morris J.C., Stone D.J., Pickering-Brown S., Mann D., Dickson D.W., Halliday G.M., Singleton A., Guerreiro R., Bras J. Neurobiology of Aging; 49: 214.e13 - 214.e15. 2017. 10.1016/j.neurobiolaging.2016.08.023.

    C9orf72 repeat expansions are a common cause of amyotrophic lateral sclerosis and frontotemporal dementia. To date, no large-scale study of dementia with Lewy bodies (DLB) has been undertaken to assess the role of C9orf72 repeat expansions in the disease. Here, we investigated the prevalence of C9orf72 repeat expansions in a large cohort of DLB cases and identified no pathogenic repeat expansions in neuropathologically or clinically defined cases, showing that C9orf72 repeat expansions are not causally associated with DLB. © 2016 Elsevier Inc.


  • Carborane bis-pyridylalcohols as linkers for coordination polymers: Synthesis, crystal structures, and guest-framework dependent mechanical properties

    Tsang M.Y., Rodríguez-Hermida S., Stylianou K.C., Tan F., Negi D., Teixidor F., Viñas C., Choquesillo-Lazarte D., Verdugo-Escamilla C., Guerrero M., Sort J., Juanhuix J., Maspoch D., Planas J.G. Crystal Growth and Design; 17 (2): 846 - 857. 2017. 10.1021/acs.cgd.6b01682.

    Supramolecular NanoChemistry and Materials

    We report the synthesis and characterization of six novel coordination polymers (CPs) based on M(II) (M: Zn and Co), di-, tri-, and tetracarboxylate linkers and two novel bis-pyridylalcohol 1,7-bis{(pyridin-n′-yl)methanol}-1,7-dicarba-closo-dodecaboranes (n′ = 3, L1; n′ = 4, L2) ligands. The polycarboxylates are terephthalic acid (H2BDC), 1,3,5-benzenetricarboxylic acid (H3BTB), and 1,2,4,5-Tetrakis(4-carboxyphenyl)benzene (H4TCPB). Structural description of CPs reveals the flexibility of the carborane ligands and their ability to construct extended structures. The CP containing Co(II), BTB, and L2 behaves as a crystalline sponge for a variety of guests, showing a higher affinity for aromatic guest molecules. Single-crystal nanoindentation experiments indicate that a high number of specific interactions between the guests and the CP framework result in a high elastic modulus and hardness values. © 2016 American Chemical Society.


  • Direct and label-free detection of the human growth hormone in urine by an ultrasensitive bimodal waveguide biosensor

    González-Guerrero A.B., Maldonado J., Dante S., Grajales D., Lechuga L.M. Journal of Biophotonics; 10 (1): 61 - 67. 2017. 10.1002/jbio.201600154.

    NanoBiosensors and Bioanalytical Applications

    A label-free interferometric transducer showing a theoretical detection limit for homogeneous sensing of 5 × 10–8 RIU, being equivalent to a protein mass coverage resolution of 2.8 fg mm–2, is used to develop a high sensitive biosensor for protein detection. The extreme sensitivity of this transducer combined with a selective bioreceptor layer enables the direct evaluation of the human growth hormone (hGH) in undiluted urine matrix in the 10 pg mL–1 range. (Figure presented.). © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim


  • Effect of the annealing on the power factor of un-doped cold-pressed SnSe

    Morales Ferreiro J.O., Diaz-Droguett D.E., Celentano D., Reparaz J.S., Sotomayor Torres C.M., Ganguli S., Luo T. Applied Thermal Engineering; 111: 1426 - 1432. 2017. 10.1016/j.applthermaleng.2016.07.198.

    Phononic and Photonic Nanostructures

    Tin Selenide (SnSe), a thermoelectric material of the chalcogenide family, has attracted tremendous interest in the past few years due to its unprecedented thermoelectric figure-of-merit, ZT, of 2.6. In this work we have carried out an experimental study of the impact of annealing on the thermoelectric properties of polycrystalline SnSe formed by cold-pressing un-doped SnSe powders with a Hall carrier concentration of 5.37 × 1017 cm−3. The crystalline structure and morphology of the samples are characterized and properties, including electrical conductivity, Seebeck coefficient and thermal conductivity, are measured. It is found that thermal annealing has a large impact on both the microstructure and the thermoelectric properties. Notably, annealing leads to re-alignment of crystalline domains, increase in Seebeck coefficient by a factor of as much as 3, and increase in the electrical conductivity. A peak ZT of 0.11 was achieved at 772 K which is smaller than un-doped polycrystalline SnSe. © 2016 Elsevier Ltd


  • Enhanced photoelectrochemical properties of nanoflower-like hexagonal CdSe0.6Te0.4: Effect of electron beam irradiation

    Shinde S.K., Ghodake G.S., Dubal D.P., Dhaygude H.D., Kim D.-Y., Fulari V.J. Journal of Industrial and Engineering Chemistry; 45: 92 - 98. 2017. 10.1016/j.jiec.2016.09.007.

    Present investigation deals with the effect of electron beam irradiation on the photoelectrochemical properties of cadmium selenium telluride (CdSe0.6Te0.4) thin films. Initially, CdSe0.6Te0.4 thin films were electrodeposited on fluorine doped tin oxide (FTO) coated glass and stainless steel substrates. Later, these CdSe0.6Te0.4 thin films were irradiated with high energy electron beam (10 MeV) of different doses from 10 to 30 kilograys (kGy). The effect of electron beam irradiation on different physico-chemical properties of CdSe0.6Te0.4 thin films such as morphological, structural, optical and photoelectrochemical has been investigated. It is observed that, the electron beam irradiation treatment considerably affects the properties of CdSe0.6Te0.4 thin films. The surface morphology of CdSe0.6Te0.4 thin films was changed from cauliflowers to nanoflowers, nanoroses and interconnected nanoflakes with doses of electron beams. Furthermore, the effect of electron beam irradiation on photoelectrochemical properties of CdSe0.6Te0.4 films was investigated. It is interesting to note that, the photoelectrochemical (PEC) properties of CdSe0.6Te0.4 thin films are extensively affected by electron beam irradiation. The photoconversion efficiency values of CdSe0.6Te0.4 films for different doses of electron beam are found to be 0.9%, 1.1%, 2.0% and 1.5%, respectively. © 2016


  • Evaluation of the immunological profile of antibody-functionalized metal-filled single-walled carbon nanocapsules for targeted radiotherapy

    Perez Ruiz De Garibay A., Spinato C., Klippstein R., Bourgognon M., Martincic M., Pach E., Ballesteros B., Ménard-Moyon C., Al-Jamal K.T., Tobias G., Bianco A. Scientific Reports; 7 ( 42605) 2017. 10.1038/srep42605.

    Force Probe Microscopy and Surface Nanoengineering | Electron Microscopy Division

    This study investigates the immune responses induced by metal-filled single-walled carbon nanotubes (SWCNT) under in vitro, ex vivo and in vivo settings. Either empty amino-functionalized CNTs [SWCNT-NH 2 (1)] or samarium chloride-filled amino-functionalized CNTs with [SmCl 3 @SWCNT-mAb (3)] or without [SmCl 3 @SWCNT-NH 2 (2)] Cetuximab functionalization were tested. Conjugates were added to RAW 264.7 or PBMC cells in a range of 1 μg/ml to 100 μg/ml for 24 h. Cell viability and IL-6/TNFα production were determined by flow cytometry and ELISA. Additionally, the effect of SWCNTs on the number of T lymphocytes, B lymphocytes and monocytes within the PBMC subpopulations was evaluated by immunostaining and flow cytometry. The effect on monocyte number in living mice was assessed after tail vein injection (150 μg of each conjugate per mouse) at 1, 7 and 13 days post-injection. Overall, our study showed that all the conjugates had no significant effect on cell viability of RAW 264.7 but conjugates 1 and 3 led to a slight increase in IL-6/TNFα. All the conjugates resulted in significant reduction in monocyte/macrophage cell numbers within PBMCs in a dose-dependent manner. Interestingly, monocyte depletion was not observed in vivo, suggesting their suitability for future testing in the field of targeted radiotherapy in mice. © The Author(s) 2017.


  • Frequency response of electrolyte-gated graphene electrodes and transistors

    Drieschner S., Guimerà A., Cortadella R.G., Viana D., Makrygiannis E., Blaschke B.M., Vieten J., Garrido J.A. Journal of Physics D: Applied Physics; 50 (9, 095304) 2017. 10.1088/1361-6463/aa5443.

    Advanced Electronic Materials and Devices

    The interface between graphene and aqueous electrolytes is of high importance for applications of graphene in the field of biosensors and bioelectronics. The graphene/electrolyte interface is governed by the low density of states of graphene that limits the capacitance near the Dirac point in graphene and the sheet resistance. While several reports have focused on studying the capacitance of graphene as a function of the gate voltage, the frequency response of graphene electrodes and electrolyte-gated transistors has not been discussed so far. Here, we report on the impedance characterization of single layer graphene electrodes and transistors, showing that due to the relatively high sheet resistance of graphene, the frequency response is governed by the distribution of resistive and capacitive circuit elements along the graphene/electrolyte interface. Based on an analytical solution for the impedance of the distributed circuit elements, we model the graphene/electrolyte interface both for the electrode and the transistor configurations. Using this model, we can extract the relevant material and device parameters such as the voltage-dependent intrinsic sheet and series resistances as well as the interfacial capacitance. The model also provides information about the frequency threshold of electrolyte-gated graphene transistors, above which the device exhibits a non-resistive response, offering an important insight into the suitable frequency range of operation of electrolyte-gated graphene devices. © 2017 IOP Publishing Ltd.


  • Functionalization of Polypyrrole Nanopipes with Redox-Active Polyoxometalates for High Energy Density Supercapacitors

    Dubal D.P., Ballesteros B., Mohite A.A., Gómez-Romero P. ChemSusChem; 10 (4): 731 - 737. 2017. 10.1002/cssc.201601610.

    Electron Microscopy Division

    Hybrid materials are very attractive for the fabrication of high-performance supercapacitors. Here, we have explored organic–inorganic hybrid materials based on open-end porous 1 D polypyrrole nanopipes (PPy-NPipes) and heteropolyoxometalates (phosphotungstate ([PW12O40]3−, PW12) or phosphomolybdate ([PMo12O40]3−, PMo12)) that display excellent areal capacitances. Two different hybrid materials (PMo12@PPy and PW12@PPy) were effectively synthesized and used for symmetric supercapacitors. The anchoring of the inorganic nanoclusters onto the conducting polymer nanopipes led to electrodes that stood up to our best expectations exhibiting outstanding areal capacitances that are almost 1.5 to 2 fold higher than that of pristine PPy-NPipes. In addition, symmetric cells based on PMo12@PPy and PW12@PPy hybrid electrodes were fabricated and showed significant improvement in cell performance with very high volumetric capacitances in the range of 6.3–6.8 F cm−3 (considering the volume of whole device). Indeed, they provide extended potential windows in acidic electrolytes (up to 1.5 V) which led to ultrahigh energy densities of 1.5 and 2.2 mWh cm−3 for PMo12@PPy and PW12@PPy cells, respectively. Thus, these unique organic-inorganic hybrid symmetric cells displayed extraordinary electrochemical performances far exceeding those of more complex asymmetric systems. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim


  • Graphene-Based Biosensors: Going Simple

    Morales-Narváez E., Baptista-Pires L., Zamora-Gálvez A., Merkoçi A. Advanced Materials; 29 (7, 1604905) 2017. 10.1002/adma.201604905.

    Nanobioelectronics and Biosensors

    The main properties of graphene derivatives facilitating optical and electrical biosensing platforms are discussed, along with how the integration of graphene derivatives, plastic, and paper can lead to innovative devices in order to simplify biosensing technology and manufacture easy-to-use, yet powerful electrical or optical biosensors. Some crucial issues to be overcome in order to bring graphene-based biosensors to the market are also underscored. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim


  • Influence of texture in hybrid carbon-phosphomolybdic acid materials on their performance as electrodes in supercapacitors

    Palomino P., Suarez-Guevara J., Olivares-Marín M., Ruiz V., Dubal D.P., Gómez-Romero P., Tonti D., Enciso E. Carbon; 111: 74 - 82. 2017. 10.1016/j.carbon.2016.09.054.

    In this paper, phosphomolybdic acid H3PMo12O40 (PMo12) was anchored to four synthetic micro-mesoporous carbons and a commercial one to analyse the relationship between the porous texture of the support, the PMo12 adsorption and the performance of the resulting hybrid materials as electrodes in supercapacitors. The uptake of PMo12 on carbon supports follows a clear correlation with the micropore volume, which implies that PMo12 is mainly adsorbed in microporosity as a consequence of a greater confinement in this kind of pores instead of mesopores. Transmission electron microscopy indicates that the PMo12 adsorbed is homogeneously dispersed in the carbon texture. Finally, the addition of PMo12 to the original carbon electrodes provided capacitances up to 293 F per gram of electrode, substantially larger than the 206–240 F g−1 of the unmodified activated carbon. This result represented an increase of up to 35% in terms of gravimetric energy density and 160% in terms of volumetric energy density, after PMo12 integration into the carbon matrix. © 2016 Elsevier Ltd


  • Interfacing neurons on carbon nanotubes covered with diamond

    Seyock S., Maybeck V., Scorsone E., Rousseau L., Hébert C., Lissorgues G., Bergonzo P., Offenhäusser A. RSC Advances; 7 (1): 153 - 160. 2017. 10.1039/c6ra20207a.

    Advanced Electronic Materials and Devices

    A recently discovered material, carbon nanotubes covered with diamond (DCNTs) was tested for its suitability in bioelectronics applications. Diamond shows advantages for bioelectronics applications (wide electro chemical window and bioinertness). This study investigates the effect of electrode surface shape (flat or three dimensional) on cell growth and behavior. For comparison, flat nanocrystalline diamond substrates were used. Primary embryonic neurons were grown on top of the structures and neither incorporated the structures nor did they grow in between the single structures. The interface was closely examined using focused ion beam (FIB) and scanning electron microscopy. Of special interest was the interface between cell and substrate. 5% to 25% of the cell membrane adhered to the substrate, which fits the theoretical estimated value. While investigating the conformity of the neurons, it could be observed that the cell membrane attaches to different heights of the tips of the 3D structure. However, the aspect ratio of the structures had no effect on the cell viability. These results let us assume that not more than 25% of cell attachment is needed for the survival of a functional neuronal cell. © The Royal Society of Chemistry.


  • Kondo screening of the spin and orbital magnetic moments of Fe impurities in Cu

    Joly L., Kappler J.-P., Ohresser P., Sainctavit P., Henry Y., Gautier F., Schmerber G., Kim D.J., Goyhenex C., Bulou H., Bengone O., Kavich J., Gambardella P., Scheurer F. Physical Review B - Condensed Matter and Materials Physics; 95 (4, 041108) 2017. 10.1103/PhysRevB.95.041108.

    We use x-ray magnetic circular dichroism to evidence the effect of correlations on the local impurity magnetic moment in an archetypal Kondo system, namely, a dilute Cu:Fe alloy. Applying the sum rules on the Fe L2,3 absorption edges, the evolution of the spin and orbital moments across the Kondo temperature are determined separately. The spin moment presents a crossover from a nearly temperature-independent regime below the Kondo temperature to a paramagneticlike regime above. Conversely, the weak orbital moment shows a temperature-independent behavior in the whole temperature range, suggesting different Kondo screening temperature scales for the spin and orbital moments. © 2017 American Physical Society.


  • Large edge magnetism in oxidized few-layer black phosphorus nanomeshes

    Nakanishi Y., Ishi A., Ohata C., Soriano D., Iwaki R., Nomura K., Hasegawa M., Nakamura T., Katsumoto S., Roche S., Haruyama J. Nano Research; 10 (2): 718 - 728. 2017. 10.1007/s12274-016-1355-8.

    Theoretical and Computational Nanoscience

    The formation and control of a room-temperature magnetic order in two-dimensional (2D) materials is a challenging quest for the advent of innovative magnetic- and spintronic-based technologies. To date, edge magnetism in 2D materials has been experimentally observed in hydrogen (H)-terminated graphene nanoribbons (GNRs) and graphene nanomeshes (GNMs), but the measured magnetization remains far too small to allow envisioning practical applications. Herein, we report experimental evidences of large room-temperature edge ferromagnetism (FM) obtained from oxygen (O)-terminated zigzag pore edges of few-layer black phosphorus (P) nanomeshes (BPNMs). The magnetization values per unit area are ~100 times larger than those reported for H-terminated GNMs, while the magnetism is absent for H-terminated BPNMs. The magnetization measurements and the first-principles simulations suggest that the origin of such a magnetic order could stem from ferromagnetic spin coupling between edge P with O atoms, resulting in a strong spin localization at the edge valence band, and from uniform oxidation of full pore edges over a large area and interlayer spin interaction. Our findings pave the way for realizing high-efficiency 2D flexible magnetic and spintronic devices without the use of rare magnetic elements. [Figure not available: see fulltext.] © 2017, Tsinghua University Press and Springer-Verlag Berlin Heidelberg.


  • Ligand and solvent effects in the formation and self-assembly of a metallosupramolecular cage

    Adarsh N.N., Chakraborty A., Tarrés M., Dey S., Novio F., Chattopadhyay B., Ribas X., Ruiz-Molina D. New Journal of Chemistry; 41 (3): 1179 - 1185. 2017. 10.1039/C6NJ03456J.

    Two bis-pyridyl-bis-urea ligands namely N,N′-bis-(3-pyridyl)diphenylmethylene-bis-urea (L1) and N,N′-bis-(3-picolyl)diphenylmethylene-bis-urea (L2) have been reacted with a Cu(ii) salt resulting in the formation of a metallosupramolecular cage [{Cu2(μ-L1)4(DMSO)2(H2O)2}·SO4·X] (1) and a one-dimensional coordination polymer [{Cu(1)(μ-L2)2(H2O)2}{Cu(2)(μ-L2)2(H2O)2}·2SO4·9H2O·X]n (2) (where DMSO = dimethylsulfoxide, and X = disordered lattice included solvent molecules), respectively. The single crystal structures of 1 and 2 are discussed in the context of the effect of the ligands, particularly the hydrogen bonding functionality of the ligand, on the supramolecular structural diversities observed in these metal organic compounds. The supramolecular packing of 1 is clearly influenced by the nature of the solvent and ligand used; mixtures of DMSO/MeOH or DMSO/H2O lead to the formation of blue crystals or a hydrogel, respectively. © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique.


  • Metamirrors Based on Arrays of Silicon Nanowires with Height Gradients

    Otte M.A., Garcia-Martin A., Borrise X., Sepulveda B. Advanced Optical Materials; 5 (4, 1600933) 2017. 10.1002/adom.201600933.

    [No abstract available]


  • Microencapsulation with alginate/CaCO 3: A strategy for improved phage therapy

    Colom J., Cano-Sarabia M., Otero J., Aríñez-Soriano J., Cortés P., Maspoch D., Llagostera M. Scientific Reports; 7 ( 41441) 2017. 10.1038/srep41441.

    Supramolecular NanoChemistry and Materials

    Bacteriophages are promising therapeutic agents that can be applied to different stages of the commercial food chain. In this sense, bacteriophages can be orally administered to farm animals to protect them against intestinal pathogens. However, the low pH of the stomach, the activities of bile and intestinal tract enzymes limit the efficacy of the phages. This study demonstrates the utility of an alginate/CaCO3 encapsulation method suitable for bacteriophages with different morphologies and to yield encapsulation efficacies of ∼100%. For the first time, a cocktail of three alginate/CaCO3-encapsulated bacteriophages was administered as oral therapy to commercial broilers infected with Salmonella under farm-like conditions. Encapsulation protects the bacteriophages against their destruction by the gastric juice. Phage release from capsules incubated in simulated intestinal fluid was also demonstrated, whereas encapsulation ensured sufficient intestinal retention of the phages. Moreover, the small size of the capsules (125-150 μm) enables their use in oral therapy and other applications in phage therapy. This study evidenced that a cocktail of the three alginate/CaCO3-encapsulated bacteriophages had a greater and more durable efficacy than a cocktail of the corresponding non-encapsulated phages in as therapy in broilers against Salmonella, one of the most common foodborne pathogen. © 2017 The Author(s).


  • Mimics of microstructures of Ni substituted Mn1−xNixCo2O4 for high energy density asymmetric capacitors

    Tamboli M.S., Dubal D.P., Patil S.S., Shaikh A.F., Deonikar V.G., Kulkarni M.V., Maldar N.N., Inamuddin, Asiri A.M., Gomez-Romero P., Kale B.B., Patil D.R. Chemical Engineering Journal; 307: 300 - 310. 2017. 10.1016/j.cej.2016.08.086.

    The preparation of nanostructured hierarchical Mn1−xNixCo2O4 metal oxides as efficient supercapacitors of different structures and configurations especially for the miniaturized electronics is still a challenge. In this context, we report template free facile hydrothermal synthesis of hierarchical nanostructured Mn1−xNixCo2O4 with excellent supercapacitive performance. Significantly, the morphology of pure MnCo2O4 transformed from 3D microcubes to 1D nanowires with incorporation of Ni. The electrochemical study shows highest specific capacitance i.e. 1762 F/g for Mn0.4Ni0.6Co2O4 with high cycling stability of 89.2% which is much higher than pristine MnCo2O4 and NiCo2O4. Later, asymmetric capacitor has been fabricated successfully using Mn0.4Ni0.6Co2O4 nanowires as positive electrode and activated carbon (AC) as negative electrode in a KOH aqueous electrolyte. An asymmetric cell could be cycled reversibly in the high-voltage range of 0–1.5 V and displays intriguing performances with a specific capacitance of 112.8 F/g (6.87 F/cm3) and high energy density of 35.2 Wh/kg (2.1 mWh/cm3). Importantly, this asymmetric capacitor device exhibits an excellent long cycle life along with 83.2% specific capacitance retained after 2000 cycles. © 2016 Elsevier B.V.


  • Modeling the Optical Responses of Noble Metal Nanoparticles Subjected to Physicochemical Transformations in Physiological Environments: Aggregation, Dissolution and Oxidation

    Piella J., Bastús N.G., Puntes V. Zeitschrift fur Physikalische Chemie; 231 (1): 33 - 50. 2017. 10.1515/zpch-2016-0874.

    Inorganic Nanoparticles

    Herein, we study how optical properties of colloidal dispersions of noble metal nanoparticles (Au and Ag) are affected by processes such as aggregation and oxidative dissolution. The optical contributions of these processes to the extinction spectra in the UV-vis region are often overlapped, making difficult its interpretation. In this regard, modeling the UV-vis spectra (in particular absorbance curve, peaks position, intensity and full width at half maximum-FWHM) of each process separately offers a powerful tool to identify the transformation of NPs under relevant and complex scenarios, such as in biological media. The proper identification of these transformations is crucial to understand the biological effects of the NPs. © 2017 Walter de Gruyter GmbH, Berlin/Boston.


  • Morphological modification of CdSe0.6Te0.4 nanostructures by electron irradiation and the effect on photoelectrochemical cells

    Shinde S.K., Ghodake G.S., Dubal D.P., Dhaygude H.D., Kim D.-Y., Rath M.C., Fulari V.J. Journal of Materials Science: Materials in Electronics; 28 (2): 1976 - 1984. 2017. 10.1007/s10854-016-5754-0.

    Novel Energy-Oriented Materials

    Morphologically well-ordered synthesis of nanomaterials by modification simple and cost effective. Electron irradiation is a promising pathway to develop various nanostructured materials. We report on the successful fabrication of hierarchical CdSe0.6Te0.4 nanostructures (nanonests, nanobrick-like small spheres with hybrid nanostructure, marigold, and nanoflowers) by electron beam irradiation in electrodeposition. These CdSe0.6Te0.4 nanostructures were employed as electrode material in solar cells, and the relationship between photoelectrochemical properties and CdSe0.6Te0.4 nanostructures was investigated, and showed that the photoelectrochemical properties strongly depend on CdSe0.6Te0.4 nanostructure morphology. The power conversion efficiency for nanonests, nanobrick-like small spheres with hybrid nanostructure, marigold, and nanoflowers of CdSe0.6Te0.4 were 0.88, 0.71, 1.03, and 0.94 %, respectively. © 2016, Springer Science+Business Media New York.


  • One-Pot Synthesis of Cationic Gold Nanoparticles by Differential Reduction

    Sperling R.A., Garciá-Fernández L., Ojea-Jiménez I., Piella J., Bastús N.G., Puntes V. Zeitschrift fur Physikalische Chemie; 231 (1): 7 - 18. 2017. 10.1515/zpch-2016-0864.

    Inorganic Nanoparticles

    The size-controlled synthesis of cationic particles by differential reduction of HAuCl4 precursor in the presence of NaBH4 and 1-aminoundecane-12-thiol (AUT) is reported. The number of seed particles is determined by the fraction of the initially Au precursor reduced by NaBH4 present in the reaction mixture, which are then grown larger by the AUT, acting as both weak reducing agent and stabilizing surfactant. By this methodology, size controlled synthesis is achieved in a two-step one-pot synthesis at room temperature. © 2017 Walter de Gruyter GmbH, Berlin/Boston.


  • Potassium disorder in the defect pyrochlore KSbTeO6: A neutron diffraction study

    Alonso J.A., Mayer S., Falcón H., Turrillas X., Fernández-Díaz M.T. Crystals; 7 (1, 24) 2017. 10.3390/cryst7010024.

    KSbTeO6 defect pyrochlore has been prepared from K2C2O4, Sb2O3, and 15% excess TeO2 by solid-state reaction at 850 °C. Direct methods implemented in the software EXPO2013 allowed establishing the basic structural framework. This was followed by a combined Rietveld refinement from X-ray powder diffraction (XRD) and neutron powder diffraction (NPD) data, which unveiled additional structural features. KSbTeO6 is cubic, a = 10.1226(7) Å, space group Fd3m, Z = 8 and it is made of a mainly covalent framework of corner-sharing (Sb,Te)O6 octahedra, with weakly bonded K+ ions located within large cages. The large K-O distances, 3.05(3)–3.07(3) Å, and quite large anisotropic atomic displacement parameters account for the easiness of K+ exchange for other cations of technological importance. © 2016 by the authors; licensee MDPI, Basel, Switzerland.


  • Solution-based synthesis and processing of Sn- and Bi-doped Cu3SbSe4 nanocrystals, nanomaterials and ring-shaped thermoelectric generators

    Liu Y., García G., Ortega S., Cadavid D., Palacios P., Lu J., Ibáñez M., Xi L., De Roo J., López A.M., Martí-Sánchez S., Cabezas I., Mata M.D.L., Luo Z., Dun C., Dobrozhan O., Carroll D.L., Zhang W., Martins J., Kovalenko M.V., Arbiol J., Noriega G., Song J., Wahnón P., Cabot A. Journal of Materials Chemistry A; 5 (6): 2592 - 2602. 2017. 10.1039/c6ta08467b.

    Advanced Electron Nanoscopy

    Copper-based chalcogenides that comprise abundant, low-cost, and environmental friendly elements are excellent materials for a number of energy conversion applications, including photovoltaics, photocatalysis, and thermoelectrics (TE). In such applications, the use of solution-processed nanocrystals (NCs) to produce thin films or bulk nanomaterials has associated several potential advantages, such as high material yield and throughput, and composition control with unmatched spatial resolution and cost. Here we report on the production of Cu3SbSe4 (CASe) NCs with tuned amounts of Sn and Bi dopants. After proper ligand removal, as monitored by nuclear magnetic resonance and infrared spectroscopy, these NCs were used to produce dense CASe bulk nanomaterials for solid state TE energy conversion. By adjusting the amount of extrinsic dopants, dimensionless TE figures of merit (ZT) up to 1.26 at 673 K were reached. Such high ZT values are related to an optimized carrier concentration by Sn doping, a minimized lattice thermal conductivity due to efficient phonon scattering at point defects and grain boundaries, and to an increase of the Seebeck coefficient obtained by a modification of the electronic band structure with Bi doping. Nanomaterials were further employed to fabricate ring-shaped TE generators to be coupled to hot pipes, which provided 20 mV and 1 mW per TE element when exposed to a 160 °C temperature gradient. The simple design and good thermal contact associated with the ring geometry and the potential low cost of the material solution processing may allow the fabrication of TE generators with short payback times. © The Royal Society of Chemistry.


  • Spin precession in anisotropic media

    Raes B., Cummings A.W., Bonell F., Costache M.V., Sierra J.F., Roche S., Valenzuela S.O. Physical Review B - Condensed Matter and Materials Physics; 95 (8, 085403) 2017. 10.1103/PhysRevB.95.085403.

    Theoretical and Computational Nanoscience | Physics and Engineering of Nanodevices

    We generalize the diffusive model for spin injection and detection in nonlocal spin structures to account for spin precession under an applied magnetic field in an anisotropic medium, for which the spin lifetime is not unique and depends on the spin orientation. We demonstrate that the spin precession (Hanle) line shape is strongly dependent on the degree of anisotropy and on the orientation of the magnetic field. In particular, we show that the anisotropy of the spin lifetime can be extracted from the measured spin signal, after dephasing in an oblique magnetic field, by using an analytical formula with a single fitting parameter. Alternatively, after identifying the fingerprints associated with the anisotropy, we propose a simple scaling of the Hanle line shapes at specific magnetic field orientations that results in a universal curve only in the isotropic case. The deviation from the universal curve can be used as a complementary means of quantifying the anisotropy by direct comparison with the solution of our generalized model. Finally, we applied our model to graphene devices and find that the spin relaxation for graphene on silicon oxide is isotropic within our experimental resolution. © 2017 American Physical Society.


  • Structural, optical, and photoelectrochemical properties of nanosphere-like CdXZn1-XS synthesized by electrochemical route

    Dhaygude H.D., Shinde S.K., Dubal D.P., Velhal N.B., Kim D.-Y., Fulari V.J. Ionics; 23 (1): 223 - 231. 2017. 10.1007/s11581-016-1797-8.

    Novel Energy-Oriented Materials

    Here, we present the effect of different Zn contents on the structural, morphological, and optical properties of CdXZn1-XS thin films deposited by electrodeposition method on stainless steel and indium-doped tin oxide (ITO) glass substrates. Electrosynthesized CdXZn1-XS thin films are characterized by using X-ray diffraction (XRD), UV-Vis spectrophotometer, field emission scanning electron microscope (FE-SEM), and surface wettability analysis. XRD pattern reveals that the CdXZn1-XS thin films are polycrystalline in nature with hexagonal crystal structure. FE-SEM micrograph displays that these CdXZn1-XS thin films exhibit the different sizes of sphere-like nanostructures by varying the X value. The optical absorption study indicates that drastic variation in band gap energy of CdXZn1-XS thin films. In advance photovoltaic measurements, CdXZn1-XS thin films are to be studied by forming the photoelectrochemical (PEC) cell having CdXZn1-XS/0.5 M (Na2SO3)/C configuration. The efficiency values of CdXZn1-XS are found to be 0.2, 0.35, 0.32, 0.25, and 0.23 % respectively at X content. © 2016, Springer-Verlag Berlin Heidelberg.


  • Synthesis and optical characterization of Er-doped bismuth titanate nanoparticles grown by sol–gel hydrothermal method

    Fuentes S., Muñoz P., Llanos J., Vega M., Martin I.R., Chavez-Angel E. Ceramics International; 43 (4): 3623 - 3630. 2017. 10.1016/j.ceramint.2016.11.200.

    The Er3+-doped bismuth titanate (Bi4Ti3O12, BIT) nanoparticles were synthesized by a combined sol–gel and hydrothermal method under a partial oxygen pressure of 30 bar. The composition and morphology were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and Raman scattering. They showed pure and homogeneous spherical BIT nanoparticles with a size below the 30 nm. The incorporation of Er ions showed a strong decrease in the lattice parameters, as well as averaged particle size. The photoluminescence up-conversion (excitation wavelength =1480 nm) showed an enhancement of the infrared emission (980 nm) as Er concentration increased, achieving a maximum for 6% mol, while photoluminescence spectra (excitation wavelength =473 nm) showed a strong green emission (529 and 553 nm) with a maximum at 4% mol. © 2016 Elsevier Ltd and Techna Group S.r.l.


  • Unveiling the nucleation & coarsening mechanisms of solution-derived self-Assembled epitaxial Ce0.9Gd0.1O2-yNanostructures

    Queralto A., De La Mata M., Arbiol J., Hühne R., Obradors X., Puig T. Crystal Growth and Design; 17 (2): 504 - 516. 2017. 10.1021/acs.cgd.6b01358.

    Advanced Electron Nanoscopy

    Self-Assembling approaches based on chemical solution deposition (CSD) are ideal methods for the cost-effective production of epitaxial nanostructures with high throughput. Therefore, an in-depth investigation of the nucleation and coarsening processes involved in the self-Assembly of nanostructures is mandatory to achieve a good control over nanostructure shape, dimensions, and orientation. Heteroepitaxial Ce0.9Gd0.1O2-y (CGO) is an ideal model system to unveil the underlying nanostructure development mechanisms in addition to their promising properties for catalysis, gas sensors, and ionic conductivity. Rapid thermal annealing furnaces have been used to study separately the thermodynamic and kinetic nucleation and coarsening mechanisms of self-Assembled CGO isotropic and anisotropic nanostructures based on strain-engineering and surface energies control. Different CGO nanoislands are obtained: isotropic (001)CGO nanodots are grown on (001)-oriented Y2O3:ZrO2(YSZ) and LaAlO3 (Lao) substrates, whereas (011)Lao substrates promote the growth of elongated (011)CGO nanowires. HRTEM and RHEED analyses are used to study the early stages of nucleation, as well as the shape and interfacial structure of CGO nanostructures. A systematic study with the heating ramp, annealing temperature and time, and strain in combination with thermally activated theoretical models provides information on the nucleation behavior, nucleation barriers, and atomic diffusion coefficients along in-plane and out-of-plane island orientations. Highly anisotropic atomic diffusion constants have been shown to be at the origin of the high aspect ratios of some of the nanostructures. Overall, our study provides a general method for the evaluation of nucleation and coarsening of multiple CSD-derived oxide nanostructures and understanding the shape development by combining thermodynamic and kinetic approaches. ©2016 American Chemical Society.