Optimizing both catalyst preparation and catalytic behaviour for the oxidative dehydrogenation of ethane of Ni-Sn-O catalysts

[EN] Bulk Ni-Sn-O catalysts have been synthesized, tested in the oxidative dehydrogenation of ethane and characterized by several physicochemical techniques. The catalysts have been prepared by evaporation of the corresponding salts using several additives in the synthesis gel, i.e. ammonium hydroxide, nitric acid, glyoxylic acid or oxalic acid, in the synthesis gel. The catalysts were finally calcined at 500 degrees C in air. Important changes in the catalytic behaviour have been observed depending on the additive. In fact, an important improvement in the catalytic performance is observed especially when some additives, such as glyoxylic or oxalic acid, are used. Thus the productivity to ethylene multiplies by 6 compared to the reference Ni-Sn-O catalyst if appropriate templates are used, and this is the result of an improvement in both the catalytic activity and the selectivity to ethylene. This improved performance has been explained in terms of the decrease of the crystallite size (and the increase in the surface area of catalyst) as well as the modification of the lattice parameter of nickel oxide.The authors would like to acknowledge the DGICYT in Spain (CTQ2015-68951-C3-1-R and CTQ2012-37925-C03-2) for financial support. We also thank the University of Valencia and SCSIE-UV for assistanceSolsona Espriu, BE.; López Nieto, JM.; Agouram, S.; Soriano Rodríguez, MD.; Dejoz, A.; Vázquez, MI.; Concepción Heydorn, P. (2016). Optimizing both catalyst preparation and catalytic behaviour for the oxidative dehydrogenation of ethane of Ni-Sn-O catalysts. Topics in Catalysis. 59(17-18):1564-1572. https://doi.org/10.1007/s11244-016-0674-zS156415725917-18Heracleous E, Lee AF, Wilson K, Lemonidou AA (2005) J Catal 231:159–171Heracleous E, Lemonidou AA (2006) J Catal 237:162–174Savova B, Loridant S, Filkova D, Millet JMM (2010) Appl Catal A 390:148–157Heracleous E, Lemonidou AA (2010) J Catal 270:67–75Solsona B, Nieto JML, Concepcion P, Dejoz A, Ivars F, Vazquez MI (2011) J Catal 280:28–39Skoufa Z, Heracleous E, Lemonidou AA (2012) Catal Today 192:169–176Zhu H, Ould-Chikh S, Anjum DH, Sun M, Biausque G, Basset JM, Caps V (2012) J Catal 285:292–303Skoufa Z, Heracleous E, Lemonidou AA (2012) Chem Eng Sci 84:48–56Zhu H, Rosenfeld DC, Anjum DH, Caps V, Basset JM (2015) ChemSusChem 8:1254–1263Heracleous E, Lemonidou AA (2015) J Catal 322:118–129Solsona B, Concepcion P, Demicol B, Hernandez S, Delgado JJ, Calvino JJ, Nieto JML (2012) J Catal 295:104–114Nieto JML, Solsona B, Grasselli RK, Concepción P (2014) Top Catal 57:1248–1255Popescu I, Skoufa Z, Heracleous E, Lemonidou AA, Marcu IC (2015) PCCP 17:8138–8147Zhang X, Gong Y, Yu G, Xie Y (2002) J Mol Catal A 180:293–298Popescu I, Skoufa Z, Heracleous E, Lemonidou A, Marcu I-C (2015) Phys Chem Chem Phys 17:8138–8147Nakamura KI, Miyake T, Konishi T, Suzuki T (2006) J Mol Catal A 260:144–151Solsona B, Dejoz AM, Vazquez MI, Ivars F, Nieto JML (2009) Top Catal 52:751–757Bortolozzi JP, Gutierrez LB, Ulla MA (2013) Appl Catal A 452:179–188Takeguchi T, Furukawa S, Inoue M (2001) J Catal 202:14–24Richardson JT, Turk B, Twigg MV (1996) Appl Catal 148:97–112Biju V, Khadar MA (2002) J Nanopart Res 4:247–253Van Veenendaal MA, Sawatzky GA (1993) Phys Rev Lett 70:2459–2462Vedrine JC, Hollinger G, Duc TM (1978) J Phys Chem 82:1515–1520Salagre P, Fierro JLG, Medina F, Sueiras JE (1996) J Mol Catal A 106:125–13

Using radium isotopes to characterize water ages and coastal mixing rates: A sensitivity analysis

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Using Monte Carlo models, this study investigated how uncertainties in Ra isotope activities and the derived activity ratios (AR) arising from analytical uncertainty and natural variability affect the uncertainty associated with Ra-derived water ages and eddy diffusion coefficients, both of which can be used to calculate SGD. Analytical uncertainties associated with Ra-224, Ra-226, and Ra-228 activities were reported in most published studies to be less than 10% of sample activity; those reported for Ra-223 ranged from 7% to 40%. Relative uncertainty related to natural variability-estimated from the variability in Ra-223 and Ra-224 activities of replicate field samples-ranged from 15% to 50% and was similar for Ra-223 activity, Ra-224 activity, and the Ra-224/Ra-223 AR. Our analysis revealed that AR-based water ages shorter than 3-5 d often have relative uncertainties greater than 100%, potentially limiting their utility. Uncertainties in eddy diffusion coefficients estimated based on cross-shore gradients in short-lived Ra isotope activity were greater when fewer points were used to determine the linear trend, when the coefficient of determination (R-2) was low, and when Ra-224, rather than Ra-223, was used. By exploring the uncertainties associated with Ra-derived water ages and eddy diffusion coefficients, this study will enable researchers to apply these methods more effectively and to reduce uncertainty

Groundwater and nutrient discharge through karstic coastal springs (Castelló, Spain)

Altres ajuts: Support from the Fulbright Commission for a post-doctoral fellowship to J.G-O. (ref 2007-0516) is gratefully acknowledged. Support for the research of PM was received through the prize ICREA Academia, funded by the Generalitat de Catalunya.Discharge of groundwater and associated chemical compounds into coastal karstic regions, which are abundant in the Mediterranean basin, is envisaged to be significant. In this study, we evaluate the groundwater discharge and its nutrient load to the open karstic site of Badum (Castelló, East Spain). Salinity profiles evidenced that groundwater discharge from coastal brackish springs causes a buoyant fresher layer, as identified with thermal infrared images. Chemical tracers (radium isotopes, dissolved inorganic silicate and seawater major elements) have been used to determine a brackish groundwater proportion in coastal waters of 36% in October 2006 and 44% in June 2007. Based on a radium-derived residence time of 2.7 days in October 2006 and 2.0 days in June 2007, total SGD fluxes have been estimated in 71 500 and 187 000m³ d⁻¹, respectively, with fresh-SGD contributions representing 71% and 85%. The calculated SGD-associated nutrient fluxes, most likely of natural origin, were 1500 and 8300 μmolm⁻² d⁻¹ of DIN and 19 and 40 μmolm⁻² d⁻¹ of DIP in October 2006 and June 2007, respectively. These inputs may actually lead to or enhance P limitation, thereby altering the structure of biological communities in the area

Support effects on NiO-based catalysts for the oxidative dehydrogenation (ODH) of ethane

[EN] We report on the effect of NiO-support interactions on the chemical nature of Ni species in a series of supported NiO catalysts for the ODH of ethane. SiO2, TiO2-anatase, a high surface area TiO2 and a porous clay hetero-structure (PCH) with TiO2 and SiO2 pillars were used as supports, which led to a selectivity to ethylene in the range 30-90% over supported NiO catalysts. The catalysts were characterized by means of XRD, N-2-Adsorption, H-2-TPR, XPS and in situ (under H-2 reductive atmosphere) and ex situ XAS spectroscopy. The catalytic performance of supported materials is discussed in terms of their reducibility and specific reduction kinetics, but also taking into account the specific chemical nature of Ni species on each catalyst. The influence of the particle size and the presence of Ni and O vacancies on the catalytic performance in the ODH of ethane is inferred.Authors would like to thank the DGICYT in Spain CTQ2015-68951-C3-1-R, CTQ2015-68951-C3-3-R, CTQ2012-37925-C03-2 and ENE2017-88818-C2-1-R. Also authors want to acknowledge the ALBA Synchrotron Light Source (Project ID: 2015021258 at CLAESS beamline). Authors from ITQ thank Project SEV-2016-0683 for financial support. D. D. also thanks MINECO and Severo Ochoa Excellence Program for his fellowship (SVP-2014-068669). Authors from UV thank the University of Valencia (UV-INV-AE16-484416 project) and MINECO (MAT2017-84118-C2-1-R project) for funding.Delgado-Muñoz, D.; Sanchís, R.; Cecilia, JA.; Rodríguez-Castellón, E.; Caballero, A.; Solsona, B.; López Nieto, JM. (2019). Support effects on NiO-based catalysts for the oxidative dehydrogenation (ODH) of ethane. Catalysis Today. 333:10-16. https://doi.org/10.1016/j.cattod.2018.07.010S101633

Fast-growing growth hormone transgenic coho salmon (Oncorhynchus kisutch) show a lower incidence of vaterite deposition and malformations in sagittal otoliths

DGS is a Serra Húnter Tenure-Track lecturer, and this work has been partially funded by the Ministerio de Ciencia y Tecnología grant number RTI2018-100757-B-100. RHD acknowledges support from the Canadian Regulatory System for Biotechnology (grant number 61740).In fish otoliths, CaCO3 normally precipitates as aragonite, and more rarely as vaterite or calcite. A higher incidence of vaterite deposition in otoliths from aquaculture-reared fish has been reported and it is thought that high growth rates under farming conditions might promote its deposition. To test this hypothesis, otoliths from growth hormone (GH) transgenic coho salmon (TF) and non-transgenic (NT) fish of matching size were compared. Once morphometric parameters were normalized by animal length, we found that TF fish otoliths were smaller (-24%, -19%, -20% and -30%; P<0.001 for length, width, perimeter and area, respectively) and rounder (-12%, +13.5%, +15% and -15.5% in circularity, form factor, roundness and ellipticity; P<0.001) than otoliths from non-transgenic fish of matching size. Interestingly, transgenic fish had smaller eyes (-30% eye diameter) and showed a strong correlation between eye and otolith size. We also found that the percentage of otoliths showing vaterite deposition was significantly smaller in transgenic fish (21-28%) compared to non-transgenic (69%; P&lt;0.001). Likewise, the area affected with vaterite deposition within individual otoliths was reduced in transgenic fish (21-26%) compared to non-transgenic (42.5%; P<0.001). Our results suggest that high growth rates per se are not sufficient to cause vaterite deposition in all cases, and that GH overexpression might have a protective role against vaterite deposition, an hypothesis that needs further investigation.Publisher PDFPeer reviewe

Altered thiol chemistry in human amyotrophic lateral sclerosis-linked mutants of superoxide dismutase 1

Neurodegenerative diseases share a common characteristic, the presence of intracellular or extracellular deposits of protein aggregates in nervous tissues. Amyotrophic Lateral Sclerosis (ALS) is a severe and fatal neurodegenerative disorder, which affects preferentially motoneurons. Changes in the redox state of superoxide dismutase 1 (SOD1) are associated with the onset and development of familial forms of ALS. In human SOD1 (hSOD1), a conserved disulfide bond and two free cysteine residues can engage in anomalous thiol/disulfide exchange resulting in non-native disulfides, a hallmark of ALS that is related to protein misfolding and aggregation. Because of the many competing reaction pathways, traditional bulk techniques fall short at quantifying individual thiol/disulfide exchange reactions. Here, we adapt recently developed single-bond chemistry techniques to study individual disulfide isomerization reactions in hSOD1. Mechanical unfolding of hSOD1 leads to the formation of a polypeptide loop held by the disulfide. This loop behaves as a molecular jump rope that brings reactive Cys-111 close to the disulfide. Using force-clamp spectroscopy, we monitor nucleophilic attack of Cys-111 at either sulfur of the disulfide and determine the selectivity of the reaction. Disease-causing mutations G93A and A4V show greatly altered reactivity patterns, which may contribute to the progression of familial ALS

Structural characterization of Niobium Phosphate Catalysts used for the Oxidative Dehydrogenation of Ethane to Ethylene

Extended abstract of a paper presented at Microscopy and Microanalysis 2011 in Nashville, Tennessee, USA, August 7–August 11, 2011.</jats:p

NiO diluted in high surface area TiO2 as efficient catalysts for the oxidative dehydrogenation of ethane

[EN] Catalysts consisting of NiO diluted in high surface area TiO2 can be as efficient in the oxidative dehydrogenation of ethane as the most selective NiO-promoted catalysts reported previously in the literature. By selecting the titania matrix and the NiO loading, yields to ethylene over 40% have been obtained. In the present article, three different titanium oxides (TiO2) have been employed as supports or diluters of nickel oxide and have been tested in the oxidative dehydrogenation of ethane to ethylene. All TiO2 used present anatase as the main crystalline phase and different surface areas of 11,55 and 85 m(2) g(-1). It has been observed that by selecting an appropriate nickel loading and the titanium oxide extremely high selectivity towards ethylene can be obtained. Thus, nickel oxide supported on TiO2 with high surface areas (i.e. 55 and 85 m(2) g(-1)) have resulted to give the best catalytic performance although the optimal nickel loading is different for each case. The optimal catalyst has been obtained for NiO-loadings up to 5-10 theoretical monolayers regardless of the TiO2 employed. Free TiO2 is inactive whereas unsupported NiO is active and unselective (forming mainly carbon dioxide) and, therefore, unmodified NiO particles have to be avoided in order to obtain the optimal catalytic performance. The use of low surface area titania (11 m(2) g(-1)) have led to the lowest selectivity to olefin due to the presence of an excess of free NiO particles. (C) 2017 Elsevier B.V. All rights reserved.The authors would like to acknowledge the DGICYT in Spain CTQ2012-37925-C03-2, CTQ2015-68951-C3-1-R, CTQ2015-68951-C3-3-R and SEV-2012-0267 Projects for financial support. D.D. also thanks Severo Ochoa Excellence fellowship (SVP-2014-068669). We also thank the University of Valencia (UV-INV-AE-16-484416 project) and SCSIE-UV for assistanceSanchis, R.; Delgado-Muñoz, D.; Agouram, S.; Soriano Rodríguez, MD.; Vázquez, MI.; Rodriguez-Castellon, E.; Solsona, B.... (2017). NiO diluted in high surface area TiO2 as efficient catalysts for the oxidative dehydrogenation of ethane. Applied Catalysis A General. 536:18-26. https://doi.org/10.1016/j.apcata.2017.02.012S182653

Characterization of vaginal microbiota in women with preterm labor with intra-amniotic inflammation

This study aims to investigate the relation between vaginal microbiota and exposition to intra-amniotic inflammation (IAI). We conducted a prospective cohort study in women with preterm labor <34 weeks who had undergone amniocentesis to rule out IAI. Vaginal samples were collected after amniocentesis. Women with IAI included those with positive amniotic fluid (AF) for a microorganism identified by specific culture media and Sanger sequencing 16S ribosomal RNA gene and/or high AF interleukin (IL)-6 levels. Vaginal microbiota was characterized by 16S ribosomal RNA gene amplicon sequencing. Specific quantitative PCR targeted to Lactobacillus spp. was also performed. Regression models were used to evaluate associations between vaginal microbiota and exposition to IAI. Concerning our results, 64 women were included. We observed an inverse association between AF IL-6 levels and load of Lactobacillus spp. Depletion in Lactobacillus spp. load was significantly associated with an early gestational age at delivery and a short latency to delivery. Microbial-diversity was found to be a risk factor for the subsequent occurrence of clinical chorioamnionitis. To the contrary, higher Lactobacillus spp. load had a protective role. In conclusion, the study identifies reduced bacterial load of Lactobacillus spp. in women exposed to IAI and found microbial-diversity and Lactobacillus spp. depletion to be associated with a worse perinatal outcome