Amide-Directed Formation of Five-Coordinate Osmium Alkylidenes from Alkynes

The amide-directed synthesis of five-coordinate osmium alkylidene derivatives from alkynes is reported. These types of complexes, which have been elusive until now because of the tendency of osmium to give hydride alkylidyne species, are prepared by reaction of the dihydride OsH2Cl2(PiPr3)2 (1) with terminal alkynes containing a distal amide group. Complex 1 reacts with N-phenylhex-5-ynamide and N-phenylhepta-6-ynamide to give OsCl2{=C(CH3)(CH2)nNH(CO)Ph}(PiPr3)2 (n = 3 (2), 4 (3)). The relative position of carbonyl and NH groups in the organic substrates has no influence on the reaction. Thus, treatment of 1 with N-(pent-4-yn-1-yl)benzamide leads to OsCl2{=C(CH3)(CH2)3NHC(O)Ph}(PiPr3)2 (4). The new compounds are intermediate species in the cleavage of the C-C triple bond of the alkynes. Under mild conditions, they undergo the rupture of the Ca-CH3 bond of the alkylidene, which comes from the alkyne triple bond, to afford six-coordinate hydride-alkylidyne derivatives. In dichloromethane, complex 2 gives a 10:7 mixture of OsHCl2{=C(CH2)3C(O)NHPh}(PiPr3)2 (5) and OsHCl2{=CCH(CH3)(CH2)2C(O)NHPh}(PiPr3)2 (6). The first complex contains a linear separation between the alkylidyne Ca atom and the amide group, whereas the spacer is branched in the second complex. In contrast to the case for 2, complex 4 selectively affords OsHCl2{=C(CH2)3NHC(O)Ph}(PiPr3)2 (7). In spite of their instability, these compounds give the alkylidene-allene metathesis, being a useful entry to five-coordinate vinylidene complexes, including the dicarbon-disubstituted OsCl2(=C=CMe2)(PiPr3)2 (8) and the monosubstituted OsCl2(=C=CHCy)(PiPr3)2 (9)

Aortic injuries in crush trauma patients: different mechanism, different management

[Abstract] Background. The objective of this study is to report the clinical and radiological characteristics and early and long-term survival of a series of acute traumatic aortic injuries (ATAI) in crush trauma patients, and to compare such data with our last 30 years experience managing ATAI in deceleration non-crush trauma patients. Methods. From January 1980 to December 2010, 5 consecutive ATAI in crush trauma and 69 in non-crush trauma patients were admitted at our institution. ISS, RTS and TRISS scores were similar in both groups. Results. Overall in-hospital mortality was 24.3%. There was no in-hospital mortality in crush patients and 26.1% in non-crush patients (p = 0.32). All aortic-related complications occurred in non-crush patients. Median follow-up was 129 months (range 3–350 months). Non-crush group survival was 76.8% at 1 year, 73.6% at 5 years, and 71.2%% at 10 years. There was no mortality during follow-up in the crush group. Mean (SD) peak creatine phosphokinase was significantly higher in crush group than in non-crush group: 7598 (3690) IU/L vs. 3645 (2506) IU/L; p = 0.041. Incidence of acute renal injury was higher in crush trauma patients (100% vs. 36.2%; p = 0.018). Low-severity injuries were more common in crush trauma patients (100% in crush patients vs. 43.5% in non-crush patients, p = 0.04). Conclusions. Aortic injuries in crush thoracic trauma patients seem to present in a different clinical scenario from aortic injuries in high-speed thoracic trauma thus requiring distinct considerations. When planning the initial management of aortic injuries in crush trauma, the increased risk of rhabdomiolysis and subsequent acute renal failure, as well as a tendency to develop lower-risk aortic wall injuries, must be considered

Incorporating pressure–volume traits into the leaf economics spectrum

In recent years, attempts have been made in linking pressure–volume parameters and the leaf economics spectrum to expand our knowledge of the interrelationships among leaf traits. We provide theoretical and empirical evidence for the coordination of the turgor loss point and associated traits with net CO2 assimilation (An) and leaf mass per area (LMA). We measured gas exchange, pressure–volume curves and leaf structure in 45 ferns and angiosperms, and explored the anatomical and chemical basis of the key traits. We propose that the coordination observed between mass-based An, capacitance and the turgor loss point (πtlp) emerges from their shared link with leaf density (one of the components of LMA) and, specially, leaf saturated water content (LSWC), which in turn relates to cell size and nitrogen and carbon content. Thus, considering the components of LMA and LSWC in ecophysiological studies can provide a broader perspective on leaf structure and function.Publishe

Influence of phenological barriers and habitat differentiation on the population genetic structure of the balearic endemic Rhamnus ludovici-salvatoris Chodat and R. alaternus L

[EN] Rhamnus ludovici-salvatoris, endemic to the Gymnesian Islands, coexists with the related and widespread R. alaternus in Mallorca and Menorca. In both species, the population genetic structure using RAPD, and flowering during a 3-year period to check for possible phenological barriers, were analyzed. Rhamnus ludovici-salvatoris showed lower genetic diversity and stronger population structure than R. alaternus, the Cabrera population being less diverse and the most differentiated. Rhamnus ludovici-salvatoris flowered one month later, although flowering of both species coincided sporadically. These congeners seem to have diverged through isolation by time and differentiation in habitat. The population genetic structure of R. ludovici-salvatoris could mainly be due to the existence of small populations on the one hand, and a gene flow caused by rare hybridization events on the other, which may also explain the presence of morphologically intermediate individuals in Menorca. The conservation of R. ludovici-salvatoris populations may include population reinforcements and other in situ interventions.Ferriol Molina, M.; Llorens García, L.; Gil, L.; Boira Tortajada, H. (2009). Influence of phenological barriers and habitat differentiation on the population genetic structure of the balearic endemic Rhamnus ludovici-salvatoris Chodat and R. alaternus L. Plant Systematics and Evolution. 277(1-2):105-116. doi:10.1007/s00606-008-0110-3S1051162771-2Affre L, Thompson JD, Debussche M (1997) Genetic structure of continental and island populations of the Mediterranean endemic Cyclamen balearicum (Primulaceae). Amer J Bot 84(4): 437–451BOIB (2005) Decreto 75/2005. BOIB 106: 29–32Bolmgren K, Oxelman B (2004) Generic limits in Rhamnus L. s.l. (Rhamnaceae) inferred from nuclear and chloroplast DNA sequence phylogenies. Taxon 53(2):383–390Bolòs O, Molinier R (1958) Recherches phytosociologiques dans l’île de Majorque. 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Hydrogen recovery from waste gas streams to feed (High-temperature PEM) fuel cells: environmental performance under a life-cycle thinking approach

Fossil fuels are being progressively substituted by a cleaner and more environmentally friendly form of energy, where hydrogen fuel cells stand out. However, the implementation of a competitive hydrogen economy still presents several challenges related to economic costs, required infrastructures, and environmental performance. In this context, the objective of this work is to determine the environmental performance of the recovery of hydrogen from industrial waste gas streams to feed high-temperature proton exchange membrane fuel cells for stationary applications. The life-cycle assessment (LCA) analyzed alternative scenarios with different process configurations, considering as functional unit 1 kg of hydrogen produced, 1 kWh of energy obtained, and 1 kg of inlet flow. The results make the recovery of hydrogen from waste streams environmentally preferable over alternative processes like methane reforming or coal gasification. The production of the fuel cell device resulted in high contributions in the abiotic depletion potential and acidification potential, mainly due to the presence of platinum metal in the anode and cathode. The design and operation conditions that defined a more favorable scenario are the availability of a pressurized waste gas stream, the use of photovoltaic electricity, and the implementation of an energy recovery system for the residual methane stream.The authors are grateful for the funding of the Spanish Ministry of Economy and Competitiveness through the Ceres-Procom Project CTM2016-76176 (AEI/FEDER, UE) and the funding of European Union through the Project SOE1/P1/E0293 (INTERREG SUDOE/FEDER, UE), “Energy Sustainability at the Sudoe Region: Red PEMFC-Sudoe”

Rhodium(III)-Catalyzed Dearomatizing (3+2) Annulation of 2-Alkenylphenols and Alkynes

Appropriately substituted 2-alkenylphenols undergo a mild formal [3C+2C] cycloaddition with alkynes when treated with a Rh(III) catalyst and an oxidant. The reaction, which involves the cleavage of the terminal C–H bond of the alkenyl moiety and the dearomatization of the phenol ring, provides a versatile and efficient approach to highly appealing spirocyclic skeletons and occurs with high selectivityWe thank the financial support provided by the Spanish Grants SAF2010-20822-C02 and CSD2007-00006 Consolider Ingenio 2010, the Xunta de Galicia Grants GR2013-041 and EM2013/036, the ERDF, and the European Research Council (Advanced Grant No. 340055). M.G. thanks Xunta de Galicia for a Parga Pondal contractS

Rowing against the wind: how do times of austerity shape academic entrepreneurship in unfriendly environments?

[EN] Academic spin-offs (ASOs) help universities transfer knowledge or technology through business projects developed by academic staff. This investigation aims at analyzing the critical factors for spin-off creation at universities operating in crisis-raven, entrepreneurship-unfriendly environments. Such factors revolve around four types of resources: environmental, institutional, organizational, and personal. Focusing on a Southern European context, as an example of an unfriendly environment affected by economic crisis, an entrepreneurial university (the Technical University of Valencia in Spain, UPV) is our research setting. Through a case study approach, we examine the potential of UPV as a springboard for ASOs. Our results show an adverse local environment, a rather favorable influence of institutional and organizational drivers, and a mixed role of personal factors. Our findings illustrate that UPV consistently supports spin-off creation due to a greater (rather positive) reflexivity from its institutional, organizational and personal resources than the (negative) imprinting of the unfriendly environment. This helps counter-balance the structural unfriendliness for academic entrepreneurship, and trigger a crisis-led risk-taking attitude by academic staff. Hence, UPV should continue with its current strategy of supporting academic entrepreneurship, and might transfer best practices to other universities also affected by unfavorable environmental conditions. Generally speaking, we would advise universities facing adverse circumstances to develop rules and mechanisms for academic entrepreneurship, carefully revise and improve malfunctions, and become involved throughout the whole process of spin-off development. All in all, our study advances understanding of how the different drivers for ASO creation can be revamped by universities located in unfriendly environments, having in mind the key role that universities play in fostering social and economic development through academic entrepreneurship in such environments.The authors would like to thank the Universitat Politecnica de Valencia (grant PAID-06-12-0916), and the Spanish Ministry of Economy and Competitiveness (grant ECO2011-29863), for their financial support for this research.Seguí-Mas, E.; Oltra, V.; Tormo-Carbó, G.; Sarrión Viñes, F. (2017). Rowing against the wind: how do times of austerity shape academic entrepreneurship in unfriendly environments?. International Entrepreneurship and Management Journal. 1-42. doi:10.1007/s11365-017-0478-zS142Acs, Z. J., Audretsch, D. B., & Lehmann, E. E. (2013). The knowledge spillover theory of entrepreneurship. Small Business Economics, 41, 757–774.Alemany, L. (2011). 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The Tertiary Level in a Functional Cluster-based Hierarchical VoD Server

A Video-On-Demand (VoD) server provides video services to the end user, that can request a piece of video at any time, without any previously established timetable. The growing demand of such services suggests the design of exible and scalable VoD servers, both in storage capacity and bandwidth. The tertiary level of a VoD server that is being implemented in top of a cheap Linux cluster, based on a hierarchical distributed architecture, using the functional programming language Erlang, is proposed in this paper