159 research outputs found

    hcp -Co Nanowires grown on metallic foams as catalysts for Fischer-Tropsch Synthesis

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    The Fischer-Tropsch synthesis (FTS) is a structure‐sensitive exothermic reaction that enables catalytic transformation of syngas to high quality liquid fuels. Now, monolithic cobalt‐based heterogeneous catalysts were elaborated through a wet chemistry approach that allows control over nanocrystal shape and crystallographic phase, while at the same time enables heat management. Copper and nickel foams have been employed as supports for the epitaxial growth of hcp‐Co nanowires directly from a solution containing a coordination compound of cobalt and stabilizing ligands. The Co/Cufoam catalyst was tested for Fischer-Tropsch synthesis in a fixed‐bed reactor, showing stability and significantly superior activity and selectivity towards C5+ compared to a Co/SiO2‐Al2O3 reference catalyst under the same conditions

    Direct protein quantification in complex sample solutions by surface-engineered nanorod probes

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    Detecting biomarkers from complex sample solutions is the key objective of molecular diagnostics. Being able to do so in a simple approach that does not require laborious sample preparation, sophisticated equipment and trained staff is vital for point-of-care applications. Here, we report on the specific detection of the breast cancer biomarker sHER2 directly from serum and saliva samples by a nanorod-based homogeneous biosensing approach, which is easy to operate as it only requires mixing of the samples with the nanorod probes. By careful nanorod surface engineering and homogeneous assay design, we demonstrate that the formation of a protein corona around the nanoparticles does not limit the applicability of our detection method, but on the contrary enables us to conduct in-situ reference measurements, thus further strengthening the point-of-care applicability of our method. Making use of sandwich assays on top of the nanorods, we obtain a limit of detection of 110 pM and 470 pM in 10-fold diluted spiked saliva and serum samples, respectively. In conclusion, our results open up numerous applications in direct protein biomarker quantification, specifically in point-of-care settings where resources are limited and ease-of-use is of essenceThis research was supported by the European Commission FP7 NAMDIATREAM project (EU NMP4-LA-2010–246479), and the German Research Foundation (DFG grant PA 794/25-1)S

    CO2 methanation activated by magnetic heating: life cycle assessment and perspectives for successful renewable energy storage

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    Purpose Technologies with low environmental impacts and promoting renewable energy sources are required to meet the energetic demand while facing the increase of gas emissions associated to the greenhouse effect and the depletion of fossil fuels. CO2 methanation activated by magnetic heating has recently been reported as a highly efficient and innovative power-to-gas technology in a perspective of successful renewable energy storage and carbon dioxide valorisation. In this work, the life cycle assessment (LCA) of this process is performed, in order to highlight the environmental potential of the technology, and its competitivity with in respect to conventional heating technologies. Methods The IMPACT 2002+ was used for this LCA. The process studied integrates methanation, water electrolysis and CO2 capture and separation. This “cradle-to-gate” LCA study does not consider the use of methane, which is the reaction product. The functional unit used is the energy content of the produced CH4. The LCA was carried out using the energy mix data for the years 2020 and 2050 as given by the French Agency for Environment and Energy management (ADEME). Consumption data were either collected from literature or obtained from the LPCNO measurements as discussed by Marbaix (2019). The environmental impact of the CO2 methanation activated by magnetic heating was compared with the environmental impact of a power-to-gas plant using conventional heating (Helmeth) and considering the environmental impact of the natural gas extraction. Results It is shown that the total flow rate of reactants, the source of CO2 and the energy mix play a major role on the environmental impact of sustainable CH4 production, whereas the lifetime of the considered catalyst has no significant influence. As a result of the possible improvements on the above-mentioned parameters, the whole process is expected to reduce by 75% in its environmental impact toward 2050. This illustrates the high environmental potential of the methanation activated by magnetic heating when coupled with industrial exhausts and renewable electricity production. Conclusions The technology is expected to be environmentally competitive compared with existing similar processes using external heating sources with the additional interest of being extremely dynamic in response, in line with the intermittency of renewable energy production

    Homogeneous Biosensing Based on Magnetic Particle Labels

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    The growing availability of biomarker panels for molecular diagnostics is leading to an increasing need for fast and sensitive biosensing technologies that are applicable to point-of-care testing. In that regard, homogeneous measurement principles are especially relevant as they usually do not require extensive sample preparation procedures, thus reducing the total analysis time and maximizing ease-of-use. In this review, we focus on homogeneous biosensors for the in vitro detection of biomarkers. Within this broad range of biosensors, we concentrate on methods that apply magnetic particle labels. The advantage of such methods lies in the added possibility to manipulate the particle labels by applied magnetic fields, which can be exploited, for example, to decrease incubation times or to enhance the signal-to-noise-ratio of the measurement signal by applying frequency-selective detection. In our review, we discriminate the corresponding methods based on the nature of the acquired measurement signal, which can either be based on magnetic or optical detection. The underlying measurement principles of the different techniques are discussed, and biosensing examples for all techniques are reported, thereby demonstrating the broad applicability of homogeneous in vitro biosensing based on magnetic particle label actuation

    Ultrastable Magnetic Nanoparticles Encapsulated in Carbon for Magnetically Induced Catalysis

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    [EN] Magnetically induced catalysis using magnetic nanoparticles (MagNPs) as heating agents is a new efficient method to perform reactions at high temperatures. However, the main limitation is the lack of stability of the catalysts operating in such harsh conditions. Normally, above 500 degrees C, significant sintering of MagNPs takes place. Here we present encapsulated magnetic FeCo and Co NPs in carbon (Co@C and FeCo@C) as an ultrastable heating material suitable for high-temperature magnetic catalysis. Indeed, FeCo@C or a mixture of FeCo@C:Co@C (2:1) decorated with Ni or Pt-Sn showed good stability in terms of temperature and catalytic performances. In addition, consistent conversions and selectivities regarding conventional heating were observed for CO2 methanation (Sabatier reaction), propane dehydrogenation (PDH), and propane dry reforming (PDR). Thus, the encapsulation of MagNPs in carbon constitutes a major advance in the development of stable catalysts for high-temperature magnetically induced catalysis.The authors thank the Instituto de Tecnologia Quimica (ITQ), Consejo Superior de Investigaciones Cientificas (CSIC), Universitat Politecnica de ValĂšncia (UPV) for the facilities and Severo Ochoa programe (SEV-2016-0683), "Juan de la Cierva" by MINECO (IJCI-2016-27966), and Primero Proyectos de InvestigaciĂłn PAID-06-18 (SP20180088) for financial support. The authors acknowledge ERC Advanced Grants (MONACAT-2015-694159 and SynCatMatch-2014671093). We also thank the Electron Microscopy Service of the UPV for TEM facilities.MartĂ­nez-Prieto, LM.; Marbaix, J.; Asensio, JM.; Cerezo-Navarrete, C.; Fazzini, P.; Soulantica, K.; Chaudret, B.... (2020). Ultrastable Magnetic Nanoparticles Encapsulated in Carbon for Magnetically Induced Catalysis. ACS Applied Nano Materials. 3(7):7076-7087. https://doi.org/10.1021/acsanm.0c01392S7076708737Ceylan, S., Friese, C., Lammel, C., Mazac, K., & Kirschning, A. (2008). Inductive Heating for Organic Synthesis by Using Functionalized Magnetic Nanoparticles Inside Microreactors. Angewandte Chemie International Edition, 47(46), 8950-8953. doi:10.1002/anie.200801474Ceylan, S., Coutable, L., Wegner, J., & Kirschning, A. (2011). Inductive Heating with Magnetic Materials inside Flow Reactors. Chemistry - A European Journal, 17(6), 1884-1893. doi:10.1002/chem.201002291Houlding, T. K., Gao, P., Degirmenci, V., Tchabanenko, K., & Rebrov, E. V. (2015). Mechanochemical synthesis of TiO2/NiFe2O4 magnetic catalysts for operation under RF field. Materials Science and Engineering: B, 193, 175-180. doi:10.1016/j.mseb.2014.12.011Asensio, J. M., Miguel, A. B., Fazzini, P., van Leeuwen, P. W. N. M., & Chaudret, B. (2019). Hydrodeoxygenation Using Magnetic Induction: High‐Temperature Heterogeneous Catalysis in Solution. Angewandte Chemie International Edition, 58(33), 11306-11310. doi:10.1002/anie.201904366Liu, Y., Gao, P., Cherkasov, N., & Rebrov, E. V. (2016). Direct amide synthesis over core–shell TiO2@NiFe2O4 catalysts in a continuous flow radiofrequency-heated reactor. RSC Advances, 6(103), 100997-101007. doi:10.1039/c6ra22659kLiu, Y., Cherkasov, N., Gao, P., FernĂĄndez, J., Lees, M. R., & Rebrov, E. V. (2017). The enhancement of direct amide synthesis reaction rate over TiO 2 @SiO 2 @NiFe 2 O 4 magnetic catalysts in the continuous flow under radiofrequency heating. Journal of Catalysis, 355, 120-130. doi:10.1016/j.jcat.2017.09.010Meffre, A., Mehdaoui, B., Connord, V., Carrey, J., Fazzini, P. F., Lachaize, S., 
 Chaudret, B. (2015). Complex Nano-objects Displaying Both Magnetic and Catalytic Properties: A Proof of Concept for Magnetically Induced Heterogeneous Catalysis. Nano Letters, 15(5), 3241-3248. doi:10.1021/acs.nanolett.5b00446Bordet, A., Lacroix, L.-M., Fazzini, P.-F., Carrey, J., Soulantica, K., & Chaudret, B. (2016). Magnetically Induced Continuous CO2Hydrogenation Using Composite Iron Carbide Nanoparticles of Exceptionally High Heating Power. Angewandte Chemie International Edition, 55(51), 15894-15898. doi:10.1002/anie.201609477Mortensen, P. M., EngbĂŠk, J. S., Vendelbo, S. B., Hansen, M. F., & Østberg, M. (2017). Direct Hysteresis Heating of Catalytically Active Ni–Co Nanoparticles as Steam Reforming Catalyst. Industrial & Engineering Chemistry Research, 56(47), 14006-14013. doi:10.1021/acs.iecr.7b02331Marbaix, J., Mille, N., Lacroix, L.-M., Asensio, J. M., Fazzini, P.-F., Soulantica, K., 
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    A setup to measure the temperature-dependent heating power of magnetically heated nanoparticles up to high temperature.

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    Magnetic heating, namely, the use of heat released by magnetic nanoparticles (MNPs) excited with a high-frequency magnetic field, has so far been mainly used for biological applications. More recently, it has been shown that this heat can be used to catalyze chemical reactions, some of them occurring at temperatures up to 700 °C. The full exploitation of MNP heating properties requires the knowledge of the temperature dependence of their heating power up to high temperatures. Here, a setup to perform such measurements is described based on the use of a pyrometer for high-temperature measurements and on a protocol based on the acquisition of cooling curves, which allows us to take into account calorimeter losses. We demonstrate that the setup permits to perform measurements under a controlled atmosphere on solid state samples up to 550 °C. It should in principle be able to perform measurements up to 900 °C. The method, uncertainties, and possible artifacts are described and analyzed in detail. The influence on losses of putting under vacuum different parts of the calorimeter is measured. To illustrate the setup possibilities, the temperature dependence of heating power is measured on four samples displaying very different behaviors. Their heating power increases or decreases with temperature, displaying temperature sensibilities ranging from -2.5 to +4.4% K-1. This setup is useful to characterize the MNPs for magnetically heated catalysis applications and to produce data that will be used to test models permitting to predict the temperature dependence of MNP heating power

    High temperature structural and magnetic properties of cobalt nanowires

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    We present in this paper the structural and magnetic properties of high aspect ratio Co nanoparticles (~10) at high temperatures (up to 623 K) using in situ X ray diffraction (XRD) and SQUID characterizations. We show that the anisotropic shapes, the structural and texture properties are preserved up to 500 K. The coercivity can be modelled by u0Hc=2(Kmc+Kshape)/Ms with Kmc the magnetocrystalline anisotropy constant, Kshape the shape anisotropy constant and Ms the saturation magnetization. Hc decreases linearly when the temperature is increased due to the loss of the Co magnetocrystalline anisotropy contribution. At 500K, 50% of the room temperature coercivity is preserved corresponding to the shape anisotropy contribution only. We show that the coercivity drop is reversible in the range 300 - 500 K in good agreement with the absence of particle alteration. Above 525 K, the magnetic properties are irreversibly altered either by sintering or by oxidation.Comment: 8 pages, 7 figures, submitted to Journal of Solid State Chemistr

    Chemical Ordering in Bimetallic FeCo Nanoparticles: From a Direct Chemical Synthesis to Application As Efficient High-Frequency Magnetic Material

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    Single-crystalline FeCo nanoparticles with tunable size and shape were prepared by co-decomposing two metal-amide precursors under mild conditions. The nature of the ligands introduced in this organometallic synthesis drastically affects the reactivity of the precursors and, thus, the chemical distribution within the nanoparticles. The presence of the B2 short-range order was evidenced in FeCo nanoparticles prepared in the presence of HDAHCl ligands, combining 57 Fe Mössbauer, zero-field 59 Co ferromagnetic nuclear resonance (FNR), and X-ray diffraction studies. This is the first time that the B2 structure is directly formed during synthesis without the need of any annealing step. The as-prepared nanoparticles exhibit magnetic properties comparable with the ones for the bulk (M s = 226 Am 2 ·kg -1 ). Composite magnetic materials prepared from these FeCo nanoparticles led to a successful proof-of-concept of the integration on inductor-based filters (27% enhancement of the inductance value at 100 MHz)

    Chemical ordering in bimetallic FeCo nanoparticles: From a direct chemical synthesis to application as efficient high-frequency magnetic material

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    Single-crystalline FeCo nanoparticles with tunable size and shape were prepared by co-decomposing two metal-amide precursors under mild conditions. The nature of the ligands introduced in this organometallic synthesis drastically affects the reactivity of the precursors and, thus, the chemical distribution within the nanoparticles. The presence of the B2 short-range order was evidenced in FeCo nanoparticles prepared in the presence of HDAHCl ligands, combining 57Fe Mössbauer, zero-field 59Co ferromagnetic nuclear resonance (FNR), and X-ray diffraction studies. This is the first time that the B2 structure is directly formed during synthesis without the need of any annealing step. The as-prepared nanoparticles exhibit magnetic properties comparable with the ones for the bulk (Ms = 226 Am2·kgÂż1). Composite magnetic materials prepared from these FeCo nanoparticles led to a successful proof-of-concept of the integration on inductor-based filters (27% enhancement of the inductance value at 100 MHz).This work was performed in the frame of TOURS 2015, and the project was supported by the French “Programme de l’économie numĂ©rique des Investissements d’Avenir”. We gratefully acknowledge the International Associated Laboratory (LIA)-M2OZART for financial support. Some of the HR-STEM and EELS studies were conducted at the Laboratorio de Microscopias Avanzadas, Instituto de Nanociencia de Aragon, Universidad de Zaragoza, Spain. R.A. gratefully acknowledges the support from the Spanish Ministry of Economy and Competitiveness (MINECO) through project MAT2016-79776-P (AEF/FEDER. UE). In IPCMS Strasbourg, the work was supported by the CNRS LIA “NANOFUNC” and the LABEX NIE (no. ANR-11-LABX-0058_NIE)
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