67 results on '"Rodríguez-Jiménez S"'
Search Results
2. Intravenous lipopolysaccharide challenge in early- versus mid-lactation dairy cattle. II: The production and metabolic responses
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Opgenorth, J., Mayorga, E.J., Abeyta, M.A., Rodriguez-Jimenez, S., Goetz, B.M., Freestone, A.D., and Baumgard, L.H.
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- 2024
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3. Intravenous lipopolysaccharide challenge in early- versus mid-lactation dairy cattle. I: The immune and inflammatory responses
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Opgenorth, J., Mayorga, E.J., Abeyta, M.A., Goetz, B.M., Rodriguez-Jimenez, S., Freestone, A.D., McGill, J.L., and Baumgard, L.H.
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- 2024
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4. Effects of a multistrain Bacillus-based direct-fed microbial on gastrointestinal permeability and biomarkers of inflammation during and following feed restriction in mid-lactation Holstein cows
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Goetz, B.M., Abeyta, M.A., Rodriguez-Jimenez, S., Opgenorth, J., McGill, J.L., Fensterseifer, S.R., Arias, R.P., Lange, A.M., Galbraith, E.A., and Baumgard, L.H.
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- 2024
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5. Effects of cashew nut shell extract supplementation on production, rumen fermentation, metabolism, and inflammatory biomarkers in transition dairy cows
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Goetz, B.M., Horst, E.A., Mayorga, E.J., Abeyta, M.A., Rodriguez-Jimenez, S., Carta, S., Lourenco, J.M., Callaway, T.R., Hikita, C., Watanabe, T., and Baumgard, L.H.
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- 2023
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6. Effects of Bacillus subtilis PB6 supplementation on production, metabolism, inflammatory biomarkers, and gastrointestinal tract permeability in transition dairy cows
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Goetz, B.M., Abeyta, M.A., Rodriguez-Jimenez, S., Mayorga, E.J., Opgenorth, J., Jakes, G.M., Freestone, A.D., Moore, C.E., Dickson, D.J., Hergenreder, J.E., and Baumgard, L.H.
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- 2023
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7. Effects of hindgut acidosis on production, metabolism, and inflammatory biomarkers in previously immune-activated lactating dairy cows
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Abeyta, M.A., Horst, E.A., Goetz, B.M., Mayorga, E.J., Rodriguez-Jimenez, S., Caratzu, M., and Baumgard, L.H.
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- 2023
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8. Effects of abomasally infused rumen fluid from corn-challenged donor cows on production, metabolism, and inflammatory biomarkers in healthy recipient cows
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Abeyta, M.A., Goetz, B.M., Mayorga, E.J., Rodriguez-Jimenez, S., Opgenorth, J., Freestone, A.D., Lourenco, J.M., Callaway, T.R., and Baumgard, L.H.
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- 2023
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9. Effects of hindgut acidosis on production, metabolism, and inflammatory biomarkers in feed-restricted lactating dairy cows
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Abeyta, M.A., Horst, E.A., Goetz, B.M., Mayorga, E.J., Rodriguez-Jimenez, S., Caratzu, M., and Baumgard, L.H.
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- 2023
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10. Effects of hindgut acidosis on inflammation, metabolism, and productivity in lactating dairy cows fed a high-fiber diet
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Abeyta, M.A., Horst, E.A., Goetz, B.M., Rodriguez-Jimenez, S., Mayorga, E.J., Al-Qaisi, M., and Baumgard, L.H.
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- 2023
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11. Effects of dietary antioxidant supplementation on metabolism and inflammatory biomarkers in heat-stressed dairy cows
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Abeyta, M.A., Al-Qaisi, M., Horst, E.A., Mayorga, E.J., Rodriguez-Jimenez, S., Goetz, B.M., Carta, S., Tucker, H., and Baumgard, L.H.
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- 2023
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12. Evaluating effects of zinc hydroxychloride on biomarkers of inflammation and intestinal integrity during feed restriction
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Horst, E.A., Mayorga, E.J., Al-Qaisi, M., Rodriguez-Jimenez, S., Goetz, B.M., Abeyta, M.A., Gorden, P.J., Kvidera, S.K., and Baumgard, L.H.
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- 2020
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13. Evaluating acute inflammation's effects on hepatic triglyceride content in experimentally induced hyperlipidemic dairy cows in late lactation
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Horst, E.A., van den Brink, L.M., Mayorga, E.J., Al-Qaisi, M., Rodriguez-Jimenez, S., Goetz, B.M., Abeyta, M.A., Kvidera, S.K., Caixeta, L.S., Rhoads, R.P., and Baumgard, L.H.
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- 2020
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14. Prepartal standing behavior as a parameter for early detection of postpartal subclinical ketosis associated with inflammation and liver function biomarkers in peripartal dairy cows
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Rodriguez-Jimenez, S., Haerr, K.J., Trevisi, E., Loor, J.J., Cardoso, F.C., and Osorio, J.S.
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- 2018
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15. Colostrum immunoglobulin G concentration of multiparous Jersey cows at first and second milking is associated with parity, colostrum yield, and time of first milking, and can be estimated with Brix refractometry
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Silva-del-Río, N., Rolle, D., García-Muñoz, A., Rodríguez-Jiménez, S., Valldecabres, A., Lago, A., and Pandey, P.
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- 2017
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16. Effects of a multispecies direct-fed microbial on gastrointestinal permeability during feed restriction in a growing heifer model
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Goetz, B.M., Abeyta, M.A., Rodriguez-Jimenez, S., Opgenorth, J., McGill, J.L., Bryan, K.A., and Baumgard, L.H.
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- 2024
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17. El Dasein de los cuidados desde la fenomenología hermenéutica de Martín Heidegger
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Ramírez-Pérez, M., Cárdenas-Jiménez, M., and Rodríguez-Jiménez, S.
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- 2015
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18. Una mirada fenomenológica del cuidado de enfermería
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Rodríguez-Jiménez, S., Cárdenas-Jiménez, M., Pacheco-Arce, A.L., and Ramírez-Pérez, M.
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- 2014
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19. El tutor clínico. Una mirada de los estudiantes de Licenciatura de Enfermería y Obstetricia
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Hidalgo-Rivera, J.L., Cárdenas-Jiménez, M., and Rodríguez-Jiménez, S.
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- 2013
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20. Effects of dietary microbial feed supplement on production efficacy in lactating dairy cows
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Goetz, B.M., Lefler, J., Abeyta, M.A., Horst, E.A., Mayorga, E.J., Al-Qaisi, M., Rodriguez-Jimenez, S., Martino, C., Izzo, A., La, R., Green, H.B., Moore, C.E., Embree, M., and Baumgard, L.H.
- Published
- 2021
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21. Symbiotic human–robot collaborative approach for increased productivity and enhanced safety in the aerospace manufacturing industry
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Pérez, L., Rodríguez-Jiménez, S., Rodríguez, N., Usamentiaga, R., García, D. F., Wang, Lihui, Pérez, L., Rodríguez-Jiménez, S., Rodríguez, N., Usamentiaga, R., García, D. F., and Wang, Lihui
- Abstract
Robots are perfect substitutes for skilled workforce on some repeatable, general, and strategically important tasks, but this substitution is not always feasible. Despite the evolution of robotics, some industries have been traditionally robot-reluctant because their processes involve large or specific parts and non-serialized products; thus, standard robotic solutions are not cost-effective. This work presents a novel approach for advanced manufacturing applied to the aerospace industry, combining the power and the repeatability of the robots with the flexibility of humans. The proposed approach is based on immersive and symbiotic collaboration between human workers and robots, presenting a safe, dynamic, and cost-effective solution for this traditionally manual and robot-reluctant industry. The proposed system architecture includes control, safety, and interface components for the new collaborative manufacturing process. It has been validated in a real-life case study that provides a solution for the manufacturing of aircraft ribs. The results show that humans and robots can share the working area simultaneously without physical separation safely, providing beneficial symbiotic collaboration and reducing times, risks, and costs significantly compared with manual operations., QC 20200329
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- 2020
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22. Significados sobre el arte del cuidado desde la perspectiva de los estudiantes de Licenciatura en Enfermería
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Ferro-Rivera, N., primary, Rodríguez-Jiménez, S., primary, and Cárdenas-Jiménez, M., primary
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- 2018
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23. Cambio actitudinal de estudiantes de octavo grado hacia el aprendizaje de interacciones biológicas mediante la resolución de problemas
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García Melo, A. and Rodríguez Jiménez, S.
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Actitudes ,Problemas ,Resolución ,Interacción ,Cambio ,resolución ,problemas ,cambio ,actitudes ,interacción - Abstract
Se presenta aquí una experiencia pedagógica en enseñanza de la biología, desarrollada en el espacio académico de Aula experimental de la Universidad Distrital Francisco José de Caldas, con 28 estudiantes de grado 8vo del Colegio La Candelaria, sede la Concordia, en la ciudad de Bogotá (Colombia) con un rango de edades entre los 12 y los 17 años, se escogen tres estudiantes, tomando como eje conceptual las interacciones biológicas. Este trabajo se realizó en las etapas de planificación, diseño y implementación de la unidad didáctica "Preguntando ando, con el ecosistema interactuando" la cual se centró en el enfoque de enseñanza por resolución de problemas. En la finalización de este trabajo se encontró un cambio actitudinal de los estudiantes con respecto al aprendizaje del eje conceptual, teniendo como referente los componentes actitudinales expuestos por Vilches y Furió (1997).
- Published
- 2013
24. El Daseinde los cuidados desde la fenomenología hermenéutica de Martín Heidegger
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Ramírez-Pérez, M., Cárdenas-Jiménez, M., and Rodríguez-Jiménez, S.
- Abstract
Este artículo deriva de la investigación «El arte del cuidado desde la visión de sus profesionales en su dimensión estética»; se recupera el pensamiento existencialista de Heidegger sobre la idea del ser ahí, el cuidado como «Dasein», la conciencia de la existencia de sí y comprende los significados de la persona en la vida-muerte.
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- 2015
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25. A vibratory bar for upper body: feasibility and acute effects on EMGrms activity.
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Moras G, Rodríguez-Jiménez S, Tous-Fajardo J, Ranz D, and Mujika I
- Abstract
The purpose of this study was to determine the feasibility of a purpose-designed vibratory bar (VB) as a potential vibration training device and thereafter to assess its effects on upper-body muscles' electromyographic (EMG) activity during vibration. During session 1, 16 physically active males held the VB during the bench press exercise in an isometric extended position (EP) in the following vibration conditions selected in the inverter (i): no vibration (0), 20, 30, 40, and 50 Hzi. Maximal acceleration (Accmax), frequency (Freq), and peak-to-peak amplitude (Ampp-p) obtained at the center (C) and at the end (E) of the VB were assessed using an accelerometer. During session 2, EMGrms of the triceps, deltoid, and pectoralis major were recorded in EP and isometric flexion position (FP) at 0, 25, and 45 Hzi. The Accmax, Freq, and Ampp-p values ranged from 37.4 to 96.4 mxs, 18.5 to 30.8 Hz, and 4.6 to 6.1 mm, respectively. The accelerometer's position had a significant effect on the Accmax and Ampp-p. All Freq obtained at C and E were different (p < 0.001) to the Freqi. An increase (p < 0.05) in EMGrms was observed in both vibration conditions compared with 0 Hzi, except during 25Hzi for deltoid and pectoralis muscle in FP. Although no significant differences were found in any of the muscles between 45 Hzi and 25Hzi, the highest EMGrms was elicited at 45Hzi. Although the registered VBs' parameters seem appropriate for vibration training, the frequency in the FP should be higher than 25 Hzi to induce significant increases in EMGrms in deltoid and pectoralis muscles. The use of a vibratory bar may be a suitable system to simultaneously stimulate upper-body muscles. [ABSTRACT FROM AUTHOR]
- Published
- 2010
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26. Molecularly engineered photocatalyst sheet for scalable solar formate production from carbon dioxide and water
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Wang, Q, Warnan, J, Rodríguez-Jiménez, S, Leung, JJ, Kalathil, S, Andrei, V, Domen, K, and Reisner, E
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13. Climate action ,7 Affordable and Clean Energy ,4008 Electrical Engineering ,7. Clean energy ,40 Engineering ,4017 Mechanical Engineering - Abstract
Harvesting solar energy to convert CO2 into chemical fuels is a promising technology to curtail the growing atmospheric CO2 levels and alleviate the global dependence on fossil fuels; however, the assembly of efficient and robust systems for the selective photoconversion of CO2 without sacrificial reagents and external bias remains a challenge. Here we present a photocatalyst sheet that converts CO2 and H2O into formate and O2 as a potentially scalable technology for CO2 utilization. This technology integrates lanthanum- and rhodium-doped SrTiO3 (SrTiO3:La,Rh) and molybdenum-doped BiVO4 (BiVO4:Mo) light absorbers modified by phosphonated Co(ii) bis(terpyridine) and RuO2 catalysts onto a gold layer. The monolithic device provides a solar-to-formate conversion efficiency of 0.08 ± 0.01% with a selectivity for formate of 97 ± 3%. As the device operates wirelessly and uses water as an electron donor, it offers a versatile strategy toward scalable and sustainable CO2 reduction using molecular-based hybrid photocatalysts.
27. Protocols d’higiene i cures d’infermeria en l’àmbit sociosanitari
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Morales Jovellar, Teresa, García Cuadrat, Esther, Aguiló Sánchez, Sònia, Rodríguez Jiménez, Selene, Badía Bernaus, Mireia, López Salcedo, Rosamary, Castellana-Perelló, Maria D., Montardit Bertral, Irene, Alexandre Solano, Sandra, Farran Jové, Montse, Regany Rodríguez, Marisa, Roca Llobet, Judith, Villalba Fernández, Elíbia, Gabernet-Foix, Marta, [Villalba Fernández E] Hospital Hestia Balaguer, Balaguer, Spain. [Gabernet-Foix M] Atenció integrada i cronicitat, Regió Sanitària de Lleida, Servei Català de la Salut (CatSalut), Departament de Salut, Generalitat de Catalunya, Lleida, Spain. [Morales Jovellar T] Centre Psicogeriàtric Terraferma, Alpicat, Spain. [Garcia Cuadrat E] Hospital Jaume Nadal Meroles, Lleida, Spain. [Aguiló Sánchez S] Servei de Geriatria i Sociosanitari, Hospital Universitari de Santa Maria (HUSM), Gestió de Serveis Sanitaris (GSS), Lleida, Spain. [Rodríguez Jiménez S] Unitat de Subaguts, Hospital Universitari de Santa Maria (HUSM), Gestió de Serveis Sanitaris (GSS), Lleida, Spain. [Badia Bernaus M] Programa d'Atenció Domiciliària i Equips de Suport (PADES), Hospital Universitari de Santa Maria (HUSM), Gestió de Serveis Sanitaris (GSS), Lleida, Spain. [López Salcedo R, Castellana Perelló, D, Montardit Bertral, I] Unitat Funcional d'Infeccions Nosocomials (UFIN), Hospital Universitari Arnau de Vilanova (HUAV), Institut Català de la Salut (ICS), Lleida, Spain. [Alexandre Solano S] Atenció Primària de Salut (APS), Institut Català de la Salut (ICS), Lleida, Spain. [Farran Jové M] Direcció Atenció Primària de Salut (APS), Institut Català de la Salut (ICS), Lleida, Spain. [Regany Rodríguez M] Àrea d'infermeria i continuïtat assistencial, Atenció Primària de Salut (APS), Institut Català de la Salut (ICS), Lleida, Spain. [Roca Llobet J] Facultat d'Infermeria i Fisioteràpia, Universitat de Lleida (UdL), Lleida, Spain, and Departament de Salut
- Subjects
Health Services Administration::Patient Care Management::Delivery of Health Care::Practice Patterns, Nurses' [HEALTH CARE] ,Pacient - Salut i higiene ,Publication Formats::Nurses Instruction [PUBLICATION CHARACTERISTICS] ,terapéutica::asistencia al paciente::asistencia de enfermería [TÉCNICAS Y EQUIPOS ANALÍTICOS, DIAGNÓSTICOS Y TERAPÉUTICOS] ,administración de los servicios de salud::gestión de la atención al paciente::prestación sanitaria::patrones en la práctica de enfermería [ATENCIÓN DE SALUD] ,Protocols d'infermeria ,Therapeutics::Patient Care::Nursing Care [ANALYTICAL, DIAGNOSTIC AND THERAPEUTIC TECHNIQUES, AND EQUIPMENT] ,formatos de publicación::instrucción de enfermería [CARACTERÍSTICAS DE PUBLICACIONES] - Abstract
Higiene; Cures; Infermeria; Àmbit sociosanitari Higiene; Cuidados; Enfermería; Ámbito sociosanitario Hygiene; Cures; Nursery; Socio-health field Publicació que recull el conjunt de protocols tant de cures d’infermeria com d’higiene personal, de superfícies i materials que s’ha considerat tenen més incidència en la prevenció de la transmissió de microorganismes causants de la infecció/colonització nosocomial en el col·lectiu de les persones d’especial vulnerabilitat ingressades en aquesta tipologia de centres d’atenció intermèdia i residencial. Un treball de consens d’un grup de professionals de diferents nivells assistencials de la Regió Sanitària Lleida, d’infermeres dels recursos Sociosanitaris (centres i equips de suport), Hospitalaris, d’Atenció Primària i Residencials amb integrants de la Unitat Territorial d’Infecció Nosocomial (UTIN) i de la Universitat de Lleida (UdL), amb la col·laboració del Col·legi Oficial d’Infermeres i Infermers de Lleida (COILL). Aquest treball ha estat aprovat per la Comissió Territorial d’Infeccions.
- Published
- 2019
28. Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme.
- Author
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Liu Y, Bin Mohamad Annuar A, Rodríguez-Jiménez S, Yeung CWS, Wang Q, Coito AM, Manuel RR, Pereira IAC, and Reisner E
- Abstract
The integration of enzymes with semiconductor light absorbers in semiartificial photosynthetic assemblies offers an emerging strategy for solar fuel production. However, such colloidal biohybrid systems rely currently on sacrificial reagents, and semiconductor-enzyme powder systems that couple fuel production to water oxidation are therefore needed to mimic an overall photosynthetic reaction. Here, we present a Z-scheme colloidal enzyme system that produces fuel with electrons sourced from water. This "closed-cycle" semiartificial approach utilizes particulate SrTiO
3 :La,Rh and BiVO4 :Mo (light absorbers), hydrogenase or formate dehydrogenase (cocatalyst), and a molecular cobalt complex (a redox mediator). Under simulated solar irradiation, this system continuously generates molecular hydrogen or formate, while co-producing molecular oxygen for 10 h using only sunlight, water, and carbon dioxide as inputs. In-depth analysis using quartz crystal microbalance, photoelectrochemical impedance spectroscopy, transient photocurrent spectroscopy, and intensity-modulated photovoltage spectroscopy provides mechanistic understanding and characterization of the semiconductor-enzyme hybrid interface. This study provides a rational platform to assemble functional semiartificial colloidal Z-scheme systems for solar fuel synthesis.- Published
- 2024
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29. Photocatalytic CO 2 Reduction Using Homogeneous Carbon Dots with a Molecular Cobalt Catalyst.
- Author
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Kim D, Bhattacharjee S, Lam E, Casadevall C, Rodríguez-Jiménez S, and Reisner E
- Abstract
A simple and precious-metal free photosystem for the reduction of aqueous CO
2 to syngas (CO and H2 ) is reported consisting of carbon dots (CDs) as the sole light harvester together with a molecular cobalt bis(terpyridine) CO2 reduction co-catalyst. This homogeneous photocatalytic system operates in the presence of a sacrificial electron donor (triethanolamine) in DMSO/H2 O solution at ambient temperature. The photocatalytic system exhibits an activity of 7.7 ± 0.2 mmolsyngas gCDs -1 (3.6 ± 0.2 mmolCO gCDs -1 and 4.1 ± 0.1 mmolH2 gCDs -1 ) after 24 hours of full solar spectrum irradiation (AM 1.5G). Spectroscopic and electrochemical characterization supports that this photocatalytic performance is attributed to a favorable association between CDs and the molecular cobalt catalyst, which results in improved interfacial photoelectron transfer and catalytic mechanism. This work provides a scalable and inexpensive platform for the development of CO2 photoreduction systems using CDs., (© 2024 The Authors. Small published by Wiley‐VCH GmbH.)- Published
- 2024
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30. Multi-Variable Multi-Metric Optimization of Self-Assembled Photocatalytic CO 2 Reduction Performance Using Machine Learning Algorithms.
- Author
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Bonke SA, Trezza G, Bergamasco L, Song H, Rodríguez-Jiménez S, Hammarström L, Chiavazzo E, and Reisner E
- Abstract
The sunlight-driven reduction of CO
2 into fuels and platform chemicals is a promising approach to enable a circular economy. However, established optimization approaches are poorly suited to multivariable multimetric photocatalytic systems because they aim to optimize one performance metric while sacrificing the others and thereby limit overall system performance. Herein, we address this multimetric challenge by defining a metric for holistic system performance that takes multiple figures of merit into account, and employ a machine learning algorithm to efficiently guide our experiments through the large parameter matrix to make holistic optimization accessible for human experimentalists. As a test platform, we employ a five-component system that self-assembles into photocatalytic micelles for CO2 -to-CO reduction, which we experimentally optimized to simultaneously improve yield, quantum yield, turnover number, and frequency while maintaining high selectivity. Leveraging the data set with machine learning algorithms allows quantification of each parameter's effect on overall system performance. The buffer concentration is unexpectedly revealed as the dominating parameter for optimal photocatalytic activity, and is nearly four times more important than the catalyst concentration. The expanded use and standardization of this methodology to define and optimize holistic performance will accelerate progress in different areas of catalysis by providing unprecedented insights into performance bottlenecks, enhancing comparability, and taking results beyond comparison of subjective figures of merit.- Published
- 2024
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31. Electrostatic [FeFe]-hydrogenase-carbon nitride assemblies for efficient solar hydrogen production.
- Author
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Liu Y, Pulignani C, Webb S, Cobb SJ, Rodríguez-Jiménez S, Kim D, Milton RD, and Reisner E
- Abstract
The assembly of semiconductors as light absorbers and enzymes as redox catalysts offers a promising approach for sustainable chemical synthesis driven by light. However, achieving the rational design of such semi-artificial systems requires a comprehensive understanding of the abiotic-biotic interface, which poses significant challenges. In this study, we demonstrate an electrostatic interaction strategy to interface negatively charged cyanamide modified graphitic carbon nitride (
NCN CNX ) with an [FeFe]-hydrogenase possessing a positive surface charge around the distal FeS cluster responsible for electron uptake into the enzyme. The strong electrostatic attraction enables efficient solar hydrogen (H2 ) production via direct interfacial electron transfer (DET), achieving a turnover frequency (TOF) of 18 669 h-1 (4 h) and a turnover number (TON) of 198 125 (24 h). Interfacial characterizations, including quartz crystal microbalance (QCM), photoelectrochemical impedance spectroscopy (PEIS), intensity-modulated photovoltage spectroscopy (IMVS), and transient photocurrent spectroscopy (TPC) have been conducted on the semi-artificial carbon nitride-enzyme system to provide a comprehensive understanding for the future development of photocatalytic hybrid assemblies., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)- Published
- 2024
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32. Connecting Biological and Synthetic Approaches for Electrocatalytic CO 2 Reduction.
- Author
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Cobb SJ, Rodríguez-Jiménez S, and Reisner E
- Subjects
- Diffusion, Electrodes, Thermodynamics, Carbon Dioxide
- Abstract
Electrocatalytic CO
2 reduction has developed into a broad field, spanning fundamental studies of enzymatic 'model' catalysts to synthetic molecular catalysts and heterogeneous gas diffusion electrodes producing commercially relevant quantities of product. This diversification has resulted in apparent differences and a disconnect between seemingly related approaches when using different types of catalysts. Enzymes possess discrete and well understood active sites that can perform reactions with high selectivity and activities at their thermodynamic limit. Synthetic small molecule catalysts can be designed with desired active site composition but do not yet display enzyme-like performance. These properties of the biological and small molecule catalysts contrast with heterogeneous materials, which can contain multiple, often poorly understood active sites with distinct reactivity and therefore introducing significant complexity in understanding their activities. As these systems are being better understood and the continuously improving performance of their heterogeneous active sites closes the gap with enzymatic activity, this performance difference between heterogeneous and enzymatic systems begins to close. This convergence removes the barriers between using different types of catalysts and future challenges can be addressed without multiple efforts as a unified picture for the biological-synthetic catalyst spectrum emerges., (© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)- Published
- 2024
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33. Predictable electronic tuning of Fe II and Ru II complexes via choice of azine: correlation of ligand p K a with E pa (M III/II ) of complex.
- Author
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Robb MG, Bondì L, Rodríguez-Jiménez S, Garden AL, Jerabek P, and Brooker S
- Abstract
Five new mononuclear ruthenium(II) tris-ligated complexes have been synthesised, varying through the choice of azine in the family of 3-azinyl-4-(4-methylphenyl)-5-phenyl-4 H -1,2,4-triazole ligands (Lazine): [Ru(Lpyridine)](PF
6 )2 (1), [Ru(Lpyridazine)](PF6 )2 (2), [Ru(L4-pyrimidine)](PF6 )2 (3), [Ru(Lpyrazine)](PF6 )2 (4), [Ru(L2-pyrimidine)](PF6 )2 (5). Three of them, 1·2MeCN·Et2 O, 3·2MeCN·Et2 O and 4·2MeCN, have been structurally characterised, confirming the presence of the meridional isomer, as was previously reported for the FeII analogues. Cyclic voltammetry studies, in dry CH3 CN vs. Ag/0.01 M AgNO3 , show that all five RuII complexes undergo a reversible RuIII /RuII process, with the midpoint potential ( Em ) increasing from 0.87 to 1.18 V as the azine is changed: pyridine < pyridazine < 2-pyrimidine < 4-pyrimidine < pyrazine. A strong inverse linear correlation ( R2 = 0.98) is found between the RuIII /RuII redox potential and the calculated HOMO orbital energies, which is consistent with the expectation that it is easier to oxidise (lower Em ) a metal ion with a higher HOMO orbital energy. The same trend was reported earlier for the family of analogous FeII complexes, albeit at lower values of Em in all cases. In addition, the ionisation potentials of the RuII complexes, as well as those of the other group 8 analogues (FeII and OsII ), showed a linear relationship with Epa . As the MIII/II redox potentials of a family of complexes has been previously reported to correlate with ligand p Ka values, a computational protocol to calculate, in silico , the p Ka of the Lazine family of ligands was developed. A strong linear relationship was found between the readily calculated p Ka of the Lazine ligand and the Epa of the MII complex, for all three families of complexes ( R2 = 0.98).- Published
- 2024
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34. Therapeutic effects of mitoquinol during an acute heat stress challenge in growing gilts.
- Author
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Mayorga EJ, Freestone AD, Rudolph TE, Roths M, Abeyta MA, Rodríguez-Jiménez S, Goetz BM, Opgenorth J, Selsby JT, and Baumgard LH
- Subjects
- Animals, Female, Swine physiology, Organophosphorus Compounds pharmacology, Organophosphorus Compounds administration & dosage, Gastrointestinal Tract drug effects, Hot Temperature, Heat-Shock Response drug effects, Swine Diseases drug therapy, Organ Size drug effects, Random Allocation, Ubiquinone analogs & derivatives, Ubiquinone pharmacology, Ubiquinone administration & dosage
- Abstract
Study objectives were to evaluate the effects of mitoquinol (MitoQ) on production parameters, gastrointestinal tract (GIT; stomach and small and large intestines) weight, and circulating leukocytes during a 24-h acute heat stress (HS) challenge. Crossbred gilts [n = 32; 49.1 ± 2.4 kg body weight (BW)] were blocked by BW and randomly assigned to 1 of 4 environmental-therapeutic treatments: 1) thermoneutral (TN) control (n = 8; TNCON), 2) TN and MitoQ (n = 8; TNMitoQ), 3) HS control (n = 8; HSCON), or 4) HS and MitoQ (n = 8; HSMitoQ). Pigs were moved into individual pens and allowed to acclimate for 6 d. The study consisted of 2 experimental periods (P). During P1 (2 d), all pigs remained in TN conditions (20.6 ± 1.5 °C) and were fed ad libitum. During P2 (24 h), pigs were fed ad libitum and exposed to either TN or constant HS (37.3 ± 1.3 °C). Mitoquinol (40 mg/d) was orally administered twice daily (0700 and 1800 hours) during P1 and P2. As expected, pigs exposed to HS had increased rectal temperature, skin temperature, and respiration rate (+1.5 °C, +8.7 °C, and +86 bpm, respectively; P < 0.01) compared to their TN counterparts. Compared to TN, HS pigs had decreased feed intake (67%; P < 0.01) and significant BW loss (+1.5 vs. -1.9 kg, respectively; P < 0.01). Total GIT weight was decreased in HS relative to TN pigs (P < 0.01), and this was influenced by decreased luminal contents (2.43 vs. 3.26 kg, respectively; P < 0.01) and reduced empty GIT mass (3.21 vs. 3.48 kg, respectively; P = 0.03). Stomach contents remained similar between TN and HS pigs (P > 0.54) but tended to increase in MitoQ relative to CON pigs (0.90 vs. 0.63 kg, respectively; P = 0.08). Stomach content as a percentage of the previous 24 h feed intake was increased in HS compared to the TN controls (93% vs. 31%; P < 0.01). In contrast, small and large intestinal contents were decreased in HS compared to TN pigs (23% and 49%, respectively; P < 0.01). Liver weight decreased in HS relative to TN pigs (1.15 vs. 1.22 kg, respectively; P = 0.02), and was decreased in MitoQ compared to CON pigs (1.13 vs. 1.24 kg; P < 0.01). Circulating lymphocytes tended to be decreased in HS relative to TN pigs (16%; P = 0.07). In summary, acute HS increased all body temperature indices, negatively influenced animal performance, and differentially altered GIT motility as evidenced by decreased gastric emptying and increased intestinal transit. However, MitoQ supplementation did not appear to ameliorate these effects., (© The Author(s) 2024. Published by Oxford University Press on behalf of the American Society of Animal Science.)
- Published
- 2024
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35. Valorisation of lignocellulose and low concentration CO 2 using a fractionation-photocatalysis-electrolysis process.
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Rodríguez-Jiménez S, Lam E, Bhattacharjee S, and Reisner E
- Abstract
The simultaneous upcycling of all components in lignocellulosic biomass and the greenhouse gas CO
2 presents an attractive opportunity to synthesise sustainable and valuable chemicals. However, this approach is challenging to realise due to the difficulty of implementing a solution process to convert a robust and complex solid (lignocellulose) together with a barely soluble and stable gas (CO2 ). Herein, we present the complete oxidative valorisation of lignocellulose coupled to the reduction of low concentration CO2 through a three-stage fractionation-photocatalysis-electrolysis process. Lignocellulose from white birch wood was first pre-treated using an acidic solution to generate predominantly cellulosic- and lignin-based fractions. The solid cellulosic-based fraction was solubilised using cellulase (a cellulose depolymerising enzyme), followed by photocatalytic oxidation to formate with concomitant reduction of CO2 to syngas (a gas mixture of CO and H2 ) using a phosphonate-containing cobalt(ii) bis(terpyridine) catalyst immobilised onto TiO2 nanoparticles. Photocatalysis generated 27.9 ± 2.0 μmolCO gTiO 2 -1 (TONCO = 2.8 ± 0.2; 16% CO selectivity) and 147.7 ± 12.0 μmolformate gTiO 2 -1 after 24 h solar light irradiation under 20 vol% CO2 in N2 . The soluble lignin-based fraction was oxidised in an electrolyser to the value-added chemicals vanillin (0.62 g kglignin -1 ) and syringaldehyde (1.65 g kglignin -1 ) at the anode, while diluted CO2 (20 vol%) was converted to CO (20.5 ± 0.2 μmolCO cm-2 in 4 h) at a Co(ii) porphyrin catalyst modified cathode (TONCO = 707 ± 7; 78% CO selectivity) at an applied voltage of -3 V. We thus demonstrate the complete valorisation of solid and a gaseous waste stream in a liquid phase process by combining fractioning, photo- and electrocatalysis using molecular hybrid nanomaterials assembled from earth abundant elements., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)- Published
- 2023
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36. Self-Assembled Liposomes Enhance Electron Transfer for Efficient Photocatalytic CO 2 Reduction.
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Rodríguez-Jiménez S, Song H, Lam E, Wright D, Pannwitz A, Bonke SA, Baumberg JJ, Bonnet S, Hammarström L, and Reisner E
- Subjects
- Carbon Dioxide chemistry, Catalysis, Electrons, Liposomes, Porphyrins
- Abstract
Light-driven conversion of CO
2 to chemicals provides a sustainable alternative to fossil fuels, but homogeneous systems are typically limited by cross reactivity between different redox half reactions and inefficient charge separation. Herein, we present the bioinspired development of amphiphilic photosensitizer and catalyst pairs that self-assemble in lipid membranes to overcome some of these limitations and enable photocatalytic CO2 reduction in liposomes using precious metal-free catalysts. Using sodium ascorbate as a sacrificial electron source, a membrane-anchored alkylated cobalt porphyrin demonstrates higher catalytic CO production (1456 vs 312 turnovers) and selectivity (77 vs 11%) compared to its water-soluble nonalkylated counterpart. Time-resolved and steady-state spectroscopy revealed that self-assembly facilitates this performance enhancement by enabling a charge-separation state lifetime increase of up to two orders of magnitude in the dye while allowing for a ninefold faster electron transfer to the catalyst. Spectroelectrochemistry and density functional theory calculations of the alkylated Co porphyrin catalyst support a four-electron-charging mechanism that activates the catalyst prior to catalysis, together with key catalytic intermediates. Our molecular liposome system therefore benefits from membrane immobilization and provides a versatile and efficient platform for photocatalysis.- Published
- 2022
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37. Shorter Alkyl Chains Enhance Molecular Diffusion and Electron Transfer Kinetics between Photosensitisers and Catalysts in CO 2 -Reducing Photocatalytic Liposomes.
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Klein DM, Rodríguez-Jiménez S, Hoefnagel ME, Pannwitz A, Prabhakaran A, Siegler MA, Keyes TE, Reisner E, Brouwer AM, and Bonnet S
- Subjects
- Carbon Dioxide, Electrons, Kinetics, Liposomes, Organometallic Compounds
- Abstract
Covalent functionalisation with alkyl tails is a common method for supporting molecular catalysts and photosensitisers onto lipid bilayers, but the influence of the alkyl chain length on the photocatalytic performances of the resulting liposomes is not well understood. In this work, we first prepared a series of rhenium-based CO
2 -reduction catalysts [Re(4,4'-(Cn H2n+1 )2 -bpy)(CO)3 Cl] (ReCn ; 4,4'-(Cn H2n+1 )2 -bpy=4,4'-dialkyl-2,2'-bipyridine) and ruthenium-based photosensitisers [Ru(bpy)2 (4,4'-(Cn H2n+1 )2 -bpy)](PF6 )2 (RuCn ) with different alkyl chain lengths (n=0, 9, 12, 15, 17, and 19). We then prepared a series of PEGylated DPPC liposomes containing RuCn and ReCn , hereafter noted Cn , to perform photocatalytic CO2 reduction in the presence of sodium ascorbate. The photocatalytic performance of the Cn liposomes was found to depend on the alkyl tail length, as the turnover number for CO (TON) was inversely correlated to the alkyl chain length, with a more than fivefold higher CO production (TON=14.5) for the C9 liposomes, compared to C19 (TON=2.8). Based on immobilisation efficiency quantification, diffusion kinetics, and time-resolved spectroscopy, we identified the main reason for this trend: two types of membrane-bound RuCn species can be found in the membrane, either deeply buried in the bilayer and diffusing slowly, or less buried with much faster diffusion kinetics. Our data suggest that the higher photocatalytic performance of the C9 system is due to the higher fraction of the more mobile and less buried molecular species, which leads to enhanced electron transfer kinetics between RuC9 and ReC9 ., (© 2021 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH.)- Published
- 2021
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38. Effects of continuously infusing glucose or casein into the terminal ileum on biomarkers of metabolism, inflammation, and intestinal morphology in growing pigs.
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Mayorga EJ, Horst EA, Al-Qaisi M, Goetz BM, Abeyta MA, Rodríguez-Jiménez S, Lei S, Acosta JA, Patience JF, Serao MCR, and Baumgard LH
- Subjects
- Animal Feed analysis, Animals, Biomarkers, Caseins, Diet, Female, Ileum, Inflammation veterinary, Swine, Glucose, Swine Diseases
- Abstract
Study objectives were to determine the effects of continuously infusing glucose (GLC) or casein (CAS) into the terminal ileum on biomarkers of metabolism, inflammation, and intestinal morphology in growing pigs. Crossbred gilts (n = 19; 81 ± 3 kg body weight [BW]) previously fitted with T-cannulas at terminal ileum were used in the current experiment. Following 4 d of acclimation, pigs were enrolled in 2 experimental 4-d periods (P). During P1, pigs were housed in individual pens and fed ad libitum for collection of baseline parameters. At the beginning of P2, pigs were assigned to 1 of 3 infusion treatments: 1) control (CON; water; 3 liters/d; n = 7), 2) GLC (dextrose 50%; 500 g/d; n = 6;), or 3) CAS (casein sodium salt; 300 g/d; n = 6). Water, GLC, and CAS solutions were continuously infused at a rate of 125 mL/h for the entirety of P2. Animals were euthanized at the end of P2, and intestinal tissue was collected. During P2, average daily feed intake differed across treatments and was reduced in GLC compared with CON pigs (14%), while CAS pigs consumed an intermediate amount (P = 0.05). Average daily gain and final BW were similar across treatments. A treatment by time interaction was observed for blood urea nitrogen (BUN; P < 0.01), as it decreased in GLC (21%) while it gradually increased in CAS (76%) pigs relative to CON pigs. Mild hyperthermia occurred with both GLC and CAS infusions relative to CON (+0.3 and 0.2 °C, respectively; P < 0.01). Blood neutrophils increased in CAS relative to CON pigs (26%) but remained similar between CON and GLC treatments (P < 0.01). Blood monocytes decreased in GLC relative to CON pigs (24%) while CAS pigs had an intermediate value (P = 0.03). Circulating lipopolysaccharide binding protein tended to decrease in GLC (29%) relative to CON pigs but remained similar between CON and CAS pigs (P = 0.10). Plasma tumor necrosis factor-alpha was similar across treatments. Ileum villus height:crypt depth was increased in CAS compared with CON pigs (33%; P = 0.05) while GLC pigs had an intermediate value. Colon myeloperoxidase-stained area increased in CAS compared with CON pigs (45%; P = 0.03) but remained similar between GLC and CON pigs. In summary, continuously infusing GLC or CAS into the terminal ileum appeared to stimulate a mild immune response and differently altered BUN patterns but had little or no effects on blood inflammatory markers, intestinal morphology, or key production parameters., (© The Author(s) 2021. Published by Oxford University Press on behalf of the American Society of Animal Science. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.)
- Published
- 2021
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39. Rapamycin administration during an acute heat stress challenge in growing pigs.
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Mayorga EJ, Horst EA, Goetz BM, Rodríguez-Jiménez S, Abeyta MA, Al-Qaisi M, Lei S, Rhoads RP, Selsby JT, and Baumgard LH
- Subjects
- Animals, Body Temperature, Heat-Shock Response, Hot Temperature, Respiratory Rate, Sirolimus pharmacology, Stress, Physiological, Swine, Heat Stress Disorders drug therapy, Heat Stress Disorders veterinary, Swine Diseases
- Abstract
Study objectives were to determine the effects of rapamycin (Rapa) on biomarkers of metabolism and inflammation during acute heat stress (HS) in growing pigs. Crossbred barrows (n = 32; 63.5 ± 7.2 kg body weight [BW]) were blocked by initial BW and randomly assigned to 1 of 4 environmental-therapeutic treatments: 1) thermoneutral (TN) control (n = 8; TNCon), 2) TN and Rapa (n = 8; TNRapa), 3) HS control (n = 8; HSCon), or 4) HS and Rapa (n = 8; HSRapa). Following 6 d of acclimation to individual pens, pigs were enrolled in two experimental periods (P). During P1 (10 d), pigs were fed ad libitum and housed in TN conditions (21.3 ± 0.2°C). During P2 (24 h), HSCon and HSRapa pigs were exposed to constant HS (35.5 ± 0.4°C), while TNCon and TNRapa pigs remained in TN conditions. Rapamycin (0.15 mg/kg BW) was orally administered twice daily (0700 and 1800 hours) during both P1 and P2. HS increased rectal temperature and respiration rate compared to TN treatments (1.3°C and 87 breaths/min, respectively; P < 0.01). Feed intake (FI) markedly decreased in HS relative to TN treatments (64%; P < 0.01). Additionally, pigs exposed to HS lost BW (4 kg; P < 0.01), while TN pigs gained BW (0.7 kg; P < 0.01). Despite marked changes in phenotypic parameters caused by HS, circulating glucose and blood urea nitrogen did not differ among treatments (P > 0.10). However, the insulin:FI increased in HS relative to TN treatments (P = 0.04). Plasma nonesterified fatty acids (NEFA) increased in HS relative to TN treatments; although this difference was driven by increased NEFA in HSCon compared to TN and HSRapa pigs (P < 0.01). Overall, circulating white blood cells, lymphocytes, and monocytes decreased in HS compared to TN pigs (19%, 23%, and 33%, respectively; P ≤ 0.05). However, circulating neutrophils were similar across treatments (P > 0.31). The neutrophil-to-lymphocyte ratio (NLR) was increased in HS relative to TN pigs (P = 0.02); however, a tendency for reduced NLR was observed in HSRapa compared to HSCon pigs (21%; P = 0.06). Plasma C-reactive protein tended to differ across treatments (P = 0.06) and was increased in HSRapa relative to HSCon pigs (46%; P = 0.03). Circulating haptoglobin was similar between groups. In summary, pigs exposed to HS had altered phenotypic, metabolic, and leukocyte responses; however, Rapa administration had limited impact on outcomes measured herein., (© The Author(s) 2021. Published by Oxford University Press on behalf of the American Society of Animal Science. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.)
- Published
- 2021
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40. Roadmap towards solar fuel synthesis at the water interface of liposome membranes.
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Pannwitz A, Klein DM, Rodríguez-Jiménez S, Casadevall C, Song H, Reisner E, Hammarström L, and Bonnet S
- Subjects
- Lipid Bilayers chemistry, Liposomes chemistry, Water chemistry, Lipid Bilayers metabolism, Liposomes metabolism, Solar Energy, Water metabolism
- Abstract
Artificial photosynthesis has experienced rapid developments aimed at producing photocatalytic systems for the synthesis of chemical energy carriers. Conceptual advances of solar fuel systems have been inspired by improved understanding of natural photosynthesis and its key operational principles: (a) light harvesting, (b) charge separation, (c) directional proton and electron transport between reaction centres and across membranes, (d) water oxidation and (e) proton or CO2 reduction catalysis. Recently, there has been a surge of bio-inspired photosynthetic assemblies that use liposomes as nanocompartments to confine reaction spaces and enable vectorial charge transport across membranes. This approach, already investigated in the 1980s, offers in principle a promising platform for solar fuel synthesis. However, the fundamental principles governing the supramolecular assemblies of lipids and photoactive surfactant-like molecules in membranes, are intricate, and mastering membrane-supported photochemistry requires thorough understanding of the science behind liposomes. In this review, we provide an overview of approaches and considerations to construct a (semi)artificial liposome for solar fuel production. Key features to consider for the use of liposomes in solar fuel synthesis are highlighted, including the understanding of the orientation and binding of different components along the membrane, the controlled electron transport between the reaction centres, and the generation of proton gradients as driving force. Together with a list of experimental techniques for the characterisation of photoactive liposomes, this article provides the reader with a roadmap towards photocatalytic fuel production at the interface of lipid membranes and aqueous media.
- Published
- 2021
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41. Electroactive Metal Complexes Covalently Attached to Conductive PEDOT Films: A Spectroelectrochemical Study.
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Rodríguez-Jiménez S, Bennington MS, Akbarinejad A, Tay EJ, Chan EWC, Wan Z, Abudayyeh AM, Baek P, Feltham HLC, Barker D, Gordon KC, Travas-Sejdic J, and Brooker S
- Abstract
The successful covalent attachment, via copper(I)-catalyzed azide alkyne cycloaddition (CuAAC), of alkyne-functionalized nickel(II) and copper(II) macrocyclic complexes onto azide (N
3 )-functionalized poly(3,4-ethylenedioxythiophene) ( PEDOT ) films on ITO-coated glass electrodes is reported. To investigate the surface attachment of the selected metal complexes, which are analogues of the cobalt-based complex previously reported to be a molecular catalyst for hydrogen evolution, first, three different PEDOT films were formed by electropolymerization of pure PEDOT or pure N3 -PEDOT , and last, 1:2N3 -PEDOT:PEDOT were formed by co-polymerizing a 1:4 mixture of N3 -EDOT:EDOT monomers. The successful surface immobilization of the complexes on the latter two azide-functionalized films, by CuAAC, was confirmed by X-ray photoelectron spectroscopy (XPS) and electrochemistry as well as by UV-vis-NIR and resonance Raman spectroelectrochemistry. The ratio between the N3 groups, and hence, the number of surface-attached metal complexes after CuAAC functionalization, in pristine N3 -PEDOT versus 1:2N3 -PEDOT:PEDOT is expected to be 3:1 and seen to be 2.86:1 with a calculated surface coverage of 3.28 ± 1.04 and 1.15 ± 0.09 nmol/cm2 , respectively. The conversion, to the metal complex attached films, was lower for the N3 -PEDOT films (Ni 74%, Cu 76%) than for the copolymer 1:2N3 -PEDOT:PEDOT films (Ni 83%, Cu 91%) due to the former being more sterically congested. The Raman and UV-vis-NIR results were simulated using density functional theory (DFT) and time-dependent DFT (TD-DFT), respectively, and showed good agreement with the experimental data. Importantly, the spectroelectrochemical behavior of both anchored metal complexes is analogous to that of the free metal complexes in solution. This proves that PEDOT films are promising conducting scaffolds for the covalent immobilization of metal complexes, as the existing electrochromic features of the complexes are preserved on immobilization, which is important for applications in electrocatalytic proton and carbon dioxide reduction, optoelectronics, and sensing.- Published
- 2021
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42. Treating mental health crises at home: Patient satisfaction with home nursing care.
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Giménez-Díez D, Maldonado Alía R, Rodríguez Jiménez S, Granel N, Torrent Solà L, and Bernabeu-Tamayo MD
- Subjects
- Adult, Cross-Sectional Studies, Female, Humans, Male, Middle Aged, Qualitative Research, Home Care Services standards, Mental Disorders therapy, Mental Health Services standards, Nurse-Patient Relations, Patient Satisfaction, Psychiatric Nursing standards
- Abstract
WHAT IS KNOWN ON THE SUBJECT?: Most studies have focused on whether hospital admissions have been reduced by the introduction of crisis services, rather than focusing on how these services are employed. Research has also shown that home assistance decreases costs and increases the level of patient satisfaction, thereby being more efficient in terms of the cost/effectiveness ratio than is traditional hospital care. Patient satisfaction with nursing care has long been identified as a key element of quality of care; however, satisfaction with nursing care among patients and families receiving crisis resolution at home has not been studied yet. WHAT THE PAPER ADDS TO EXISTING KNOWLEDGE?: There is limited research on patient satisfaction with CRHTTs. This study provides new insights and data including that on relationships between patient satisfaction and the teams' attention to person-centred mental health care. The difference between this study and other studies on patient satisfaction with crisis resolution home treatment teams is that this study focused on patients' and families' satisfaction with the nursing care provided by crisis resolution home treatment teams rather than with the general service provided. This study is the first of its kind with such a focus. WHAT ARE THE IMPLICATIONS FOR PRACTICE?: This research has both academic and clinical implications. Patients' and their families' satisfaction with nursing care is an integral aspect for evaluating mental health services, and this is especially important regarding services provided by crisis resolution home treatment teams because such teams are currently being introduced in countries such as Spain. Closely examining patients and families' satisfaction with nursing care can also foster improvements in current practices. Nurses in crisis teams might need to focus on equalizing power relations, which the data gathered in this study suggests is most important to patient satisfaction. ABSTRACT: Introduction Crisis resolution home treatment teams (CRHTT) provide short-term, intensive home treatment to people experiencing mental health crises. Patient satisfaction has long been identified as a key element of quality of care; however, satisfaction with nursing care as part of this service has not been studied yet. Aim To assess patients' and their families' satisfaction with the nursing care provided through a home care program offered by a hospital in Catalonia which administers person-centred care. Method A mixed methods research design was conducted. A cross-sectional study including quantitative survey data and qualitative interview data with a phenomenological focus was conducted. Results Twenty interviews were conducted. Patients and relatives reported high satisfaction that seems to be related to the person-centred nature of the care. Discussion The findings provide new insights, including how home treatment tends to equalize power relations between nurses and patients/the patient's family members, and how nurses increase sensitivity when focusing on service users' needs and priorities, leading to high patient and family satisfaction. Implications for practice This research has both academic and clinical implications. It highlights what mental health patients and their families value most about home care and interactions with nurses, and also drives improvements in current practices., (© 2019 John Wiley & Sons Ltd.)
- Published
- 2020
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43. Qualitative Guest Sensing via Iron(II) Triazole Complexes.
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Rodríguez-Jiménez S and Brooker S
- Abstract
The pyridazine-pyridine triazole-based Rat ligand, L
pydzpy [4-(4-methylphenyl)-3-(3-pyridazinyl)-5-(2-pyridinyl)-1,2,4-triazole], is potentially ditopic. Nevertheless, Lpydzpy is shown herein to exclusively form mononuclear iron(II) complexes, [FeII (Lpydzpy )2 (NCE)2 ]·solvent, in the presence of coordinating NCE anions (E = S or Se). Specifically, a new family of 10 mononuclear complexes, in which Lpydzpy binds in a monotopic bidentate manner, has been made: two solvent-free complexes, [FeII (Lpydzpy )2 (NCS)2 ] (1) and [FeII (Lpydzpy )2 (NCSe)2 ] (2); six solvatomorphs, 1·4CH3 CN, 2·4CH3 CN, 1·2.25CH3 CN, 2·3CH3 CN, 2·tetrahydrofuran, and 2·CHCl3 ; and a pair of desolvated polymorphs, 1' and 2'. Seven of them are spin crossover-active, the exceptions being 1, 2, and 2'. This is confirmed by single-crystal X-ray diffraction (XRD) for 1, 2, 1·4CH3 CN, and 2·4CH3 CN and is consistent with variable-temperature optical microscopy observations on single crystals of 1·4CH3 CN and 2·4CH3 CN and on samples of 1' and 2'. Powder XRD, thermogravimetric analysis, and solid-state magnetometry reveal that desolvated 1' and 2' are capable of absorbing and desorbing a range of volatile guests: CH3 CN in both cases and also tetrahydrofuran and CHCl3 in the case of 2'.- Published
- 2019
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44. Predictable Electronic Tuning By Choice of Azine Substituent in Five Iron(II) Triazoles: Redox Properties and DFT Calculations.
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Rodríguez-Jiménez S, Bondì L, Yang M, Garden AL, and Brooker S
- Abstract
Five new mononuclear iron(II) tris-ligand complexes, and four solvatomorphs, have been made from the azine-substituted 1,2,4-triazole ligands (L
azine ): [FeII (Lpyridazine )3 ](BF4 )2 (1), [FeII (Lpyrazine )3 ](BF4 )2 (2), [FeII (Lpyridine )3 ](BF4 )2 (3), [FeII (L2pyrimidine )3 ](BF4 )2 (4), and [FeII (L4pyrimidine )3 ](BF4 )2 (5). Single-crystal XRD and solid-state magnetometry reveal that all of them are low-spin (LS) iron(II), except for solvatomorph 5⋅4 H2 O. Evans method NMR studies in CD2 Cl2 , (CD3 )2 CO and CD3 CN show that all are LS in these solvents, except 5 in CD2 Cl2 (consistent with L4pyrimidine imposing the weakest field). Cyclic voltammetry in CH3 CN vs. Ag/0.01 m AgNO3 reveals an, at best quasi-reversible, FeIII/II redox process, with Epa increasing from 0.69 to 0.99 V as the azine changes: pyridine< pyridazine<2-pyrimidine<4-pyrimidine< pyrazine. The observed Epa values correlate linearly with the DFT calculated HOMO energies for the LS complexes., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)- Published
- 2019
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45. Solvent Polarity Predictably Tunes Spin Crossover T 1/2 in Isomeric Iron(II) Pyrimidine Triazoles.
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Rodríguez-Jiménez S, Barltrop AS, White NG, Feltham HLC, and Brooker S
- Abstract
Two isomeric pyrimidine-based Rdpt-type triazole ligands were made: 4-(4-methylphenyl)-3-(2-pyrimidyl)-5-phenyl-4 H-1,2,4-triazole (L
2pyrimidine ) and 4-(4-methylphenyl)-3-(4-pyrimidyl)-5-phenyl-4 H-1,2,4-triazole (L4pyrimidine ). When reacted with [FeII (pyridine)4 (NCE)2 ], where E = S, Se, or BH3 , two families of mononuclear iron(II) complexes are obtained, including six solvatomorphs, giving a total of 12 compounds: [FeII (L2pyrimidine )2 (NCS)2 ] (1), [FeII (L2pyrimidine )2 (NCSe)2 ] (2), 2·1.5H2 O, [FeII (L2pyrimidine )2 (NCBH3 )2 ]·2CHCl3 (3·2CHCl3 ), 3 and 3·2H2 O, [FeII (L4pyrimidine )2 (NCS)2 ] (4), 4·H2 O, [FeII (L4pyrimidine )2 (NCSe)2 ] (5), 5·2CH3 OH, 5·1.5H2 O, and [FeII (L4pyrimidine )2 (NCBH3 )2 ]·2.5H2 O (6·2.5H2 O). Single-crystal X-ray diffraction reveals that the N6 -coordinated iron(II) centers in 1, 2, 3·2CHCl3 , 4, 5, and 5·2CH3 OH have two bidentate triazole ligands equatorially bound and two axial NCE co-ligands trans-coordinated. All structures are high spin (HS) at 100 K, except 3·2CHCl3 , which is low spin (LS). Solid-state magnetic measurements show that only 3·2CHCl3 ( T1/2 above 400 K) and 5·1.5H2 O ( T1/2 = 110 K) undergo spin crossover (SCO); the others remain HS at 300-50 K. When 3·2CHCl3 is heated at 400 K it desorbs CHCl3 becoming 3, which remains HS at 400-50 K. UV-Vis studies in CH2 Cl2 , CHCl3 , (CH3 )2 CO, CH3 CN, and CH3 NO2 solutions for the BH3 analogues 3 and 6 led to a 6:1 ratio of Lnpyrimidine /Fe(II) being employed for the solution studies. These revealed SCO activity in all five solvents, with T1/2 values for the 2-pyrimidine complex (247-396 K) that were consistently higher than for the 4-pyrimidine complex (216-367 K), regardless of solvent choice, consistent with the 2-pyrimidine ring providing a stronger ligand field than the 4-pyrimidine ring. Strong correlations of solvent polarity index with the T1/2 values in those solvents are observed for each complex, enabling predictable T1/2 tuning by up to 150 K. While this correlation is tantalizing, here it may also be reflecting solvent-dependent speciation-so future tests of this concept should employ more stable complexes. Differences between solid-state (ligand field; crystal packing; solvent content) and solution (ligand field; solvation; speciation) effects on SCO are highlighted.- Published
- 2018
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46. A Simple Method of Predicting Spin State in Solution.
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Rodríguez-Jiménez S, Yang M, Stewart I, Garden AL, and Brooker S
- Abstract
A simple method, using density functional theory (DFT), of predicting spin-state in advance of synthesis is reported. Specifically, an excellent correlation is observed between the switching temperatures (T
1/2 ) in CDCl3 solution of five spin-crossover (SCO)-active [FeII (Lazine )2 (NCBH3 )2 ] complexes and the DFT-calculated (and observed)15 N NMR chemical shift (δNA ) of the five different azine-substituted 1,2,4-triazole ligands employed, Lazine = 4-(4-methylphenyl)-3-phenyl-5-(azine)-1,2,4-triazole, where azine = pyridine, pyridazine, 4-pyrimidine, pyrazine, and 2-pyrimidine. To test the generality of this finding, DFT was also employed to readily predict the δNA values for a family of 16 literature ligands, known as bppX,Y [X,Y-substituted 2,6-(pyrazol-1-yl)pyridines], which have produced 16 SCO-active [FeII (bppX,Y )2 ](Z)2 complexes (Z = BF4 or in one case PF6 ) in (CD3 )2 CO solution: again an excellent correlation was found between the computed δNA and the observed T1/2 . These correlations represent a key advance in the field, as they allow a simple DFT calculation on a modified ligand to be used to reliably predict, before synthesis of the ligand or complex, the T1/2 that would result from that modification. Achieving such easily predictable tuning of T1/2 , and hence of spin-state, is a significant step forward in the field of SCO and also has big implications in many other fields in which spin-state is key, including catalysis, metallo-enzyme modeling studies, and host-guest chemistry.- Published
- 2017
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47. Solid Versus Solution Spin Crossover and the Importance of the Fe-N≡C(X) Angle.
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Rodríguez-Jiménez S and Brooker S
- Abstract
A new family of mononuclear [Fe
II (Rdpt)2 (NCE)2 ] complexes (E = S, Se, or BH3 ) is formed by 1:2 reaction of [FeII (pyridine)4 (NCE)2 ] with the monotopic pyridyl triazole ligand 4-(4-methylphenyl)-3-(2-pyridinyl)-5-phenyl-4H-1,2,4-triazole (tolpyph). The three complexes are obtained as six different solvatomorphs: [FeII (tolpyph)2 (NCS)2 ]·H2 O (1·H2 O), 1·1.5CH3 OH·0.5H2 O, [FeII (tolpyph)2 (NCSe)2 ] (2), 2·1.5H2 O, [FeII (tolpyph)2 (NCBH3 )2 ] (3), and 3·H2 O. Single-crystal X-ray diffraction reveals that 1·1.5CH3 OH·0.5H2 O and 2 are high-spin (HS) at 100 K, while 3 is low-spin (LS) at 100 K and HS at 373 K. Compound 3 is the first structurally characterized example of an [FeII (Rdpt)2 (NCE)2 ]-type complex with NCBH3 co-ligand: the crystal packing is dominated by aromatic stacking interactions. Solid-state magnetic measurements show that 1·H2 O and 2·1.5H2 O remain HS down to 50 K, whereas 3·H2 O undergoes spin crossover (SCO) with a T1/2 of 309 K, slightly above room temperature. A literature survey of analogous trans-[FeII (Rdpt)2 (NCX)2 ]-type complexes (53 distinct crystal structures) shows that for the complexes that are SCO active in the solid state the Fe-N≡C(X) angle is usually close to straight, 162-178°, whereas it is usually lower, 142-159°, for the complexes that remain HS. UV-vis studies in CHCl3 solution show that in each case the use of a 6:1 ratio of tolpyph/Fe(II) is required to ensure the iron(II) is present in solution as [FeII (tolpyph)2 (NCE)2 ]. Interestingly, using this ratio, all three compounds are SCO-active in CDCl3 solution-in dramatic contrast to the solid-state findings. Specifically, while compounds 1 and 2 are not SCO-active in the solid state (they remain HS), they undergo gradual SCO in CDCl3 solution, with T1/2 values of 290 and 310 K, respectively. In CDCl3 solution, compound 3 has a T1/2 value of 288 K, which is 21 K lower than in the solid state. These results highlight the differences between solid state (ligand field; crystal packing) and solution (ligand field; solvation) effects on SCO, with the latter studies revealing room-temperature SCO for all three of these complexes.- Published
- 2017
- Full Text
- View/download PDF
48. Non-Porous Iron(II)-Based Sensor: Crystallographic Insights into a Cycle of Colorful Guest-Induced Topotactic Transformations.
- Author
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Rodríguez-Jiménez S, Feltham HL, and Brooker S
- Abstract
Materials capable of sensing volatile guests at room temperature by an easily monitored set of outputs are of great appeal for development as chemical sensors of small volatile organics and toxic gases. Herein the dinuclear iron(II) complex, [Fe
II 2 (L)2 (CH3 CN)4 ](BF4 )4 ⋅2 CH3 CN (1) [L=4-(4-methylphenyl)-3-(3-pyridazinyl)-5-pyridyl-4H-1,2,4-triazole], is shown to undergo reversible single-crystal-to-single-crystal (SCSC) transformations upon exposure to vapors of different guests: 1 (MeCN)⇌2 (EtOH)→3 (H2 O)⇌1 (MeCN). Whilst 1 and 2 remain dimetallic, SCSC to 3 involves conversion to a 1D polymeric chain (due to a change in L bridging mode), which, remarkably, can undergo SCSC de-polymerization, reforming dimetallic 1. Additionally, SC-XRD studies of two ordered transient forms, 1TF3 and 2TF3, confirm that guest exchange occurs by diffusion of the new guests into the non-porous lattices as the old guests leave. These reversible SCSC events also induce color and magnetic responses. Indeed dark red 1 is spin crossover active (T1/2 ↓ 356 K; T1/2 ↑ 369 K), whilst orange 2 and yellow 3 remain high spin., (© 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)- Published
- 2016
- Full Text
- View/download PDF
49. W5″ Test: A simple method for measuring mean power output in the bench press exercise.
- Author
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Tous-Fajardo J, Moras G, Rodríguez-Jiménez S, Gonzalo-Skok O, Busquets A, and Mujika I
- Subjects
- Adolescent, Adult, Humans, Male, Reproducibility of Results, Young Adult, Muscle Strength physiology, Muscle, Skeletal physiology, Resistance Training
- Abstract
The aims of the present study were to assess the validity and reliability of a novel simple test [Five Seconds Power Test (W5″ Test)] for estimating the mean power output during the bench press exercise at different loads, and its sensitivity to detect training-induced changes. Thirty trained young men completed as many repetitions as possible in a time of ≈5 s at 25%, 45%, 65% and 85% of one-repetition maximum (1RM) in two test sessions separated by four days. The number of repetitions, linear displacement of the bar and time needed to complete the test were recorded by two independent testers, and a linear encoder was used as the criterion measure. For each load, the mean power output was calculated in the W5″ Test as mechanical work per time unit and compared with that obtained from the linear encoder. Subsequently, 20 additional subjects (10 training group vs. 10 control group) were assessed before and after completing a seven-week training programme designed to improve maximal power. Results showed that both assessment methods correlated highly in estimating mean power output at different loads (r range: 0.86-0.94; p < .01) and detecting training-induced changes (R(2): 0.78). Good to excellent intra-tester (intraclass correlation coefficient (ICC) range: 0.81-0.97) and excellent inter-tester (ICC range: 0.96-0.99; coefficient of variation range: 2.4-4.1%) reliability was found for all loads. The W5″ Test was shown to be a valid, reliable and sensitive method for measuring mean power output during the bench press exercise in subjects who have previous resistance training experience.
- Published
- 2016
- Full Text
- View/download PDF
50. Force Outputs during Squats Performed Using a Rotational Inertia Device under Stable versus Unstable Conditions with Different Loads.
- Author
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Vázquez-Guerrero J, Moras G, Baeza J, and Rodríguez-Jiménez S
- Subjects
- Adult, Athletes, Biomechanical Phenomena, Humans, Knee Joint physiology, Male, Muscle Contraction physiology, Muscle, Skeletal physiology, Reproducibility of Results, Resistance Training, Stress, Mechanical, Young Adult, Muscle Strength physiology, Weight Lifting
- Abstract
The purpose of the study was to compare the force outputs achieved during a squat exercise using a rotational inertia device in stable versus unstable conditions with different loads and in concentric and eccentric phases. Thirteen male athletes (mean ± SD: age 23.7 ± 3.0 years, height 1.80 ± 0.08 m, body mass 77.4 ± 7.9 kg) were assessed while squatting, performing one set of three repetitions with four different loads under stable and unstable conditions at maximum concentric effort. Overall, there were no significant differences between the stable and unstable conditions at each of the loads for any of the dependent variables. Mean force showed significant differences between some of the loads in stable and unstable conditions (P < 0.010) and peak force output differed between all loads for each condition (P < 0.045). Mean force outputs were greater in the concentric than in the eccentric phase under both conditions and with all loads (P < 0.001). There were no significant differences in peak force between concentric and eccentric phases at any load in either stable or unstable conditions. In conclusion, squatting with a rotational inertia device allowed the generation of similar force outputs under stable and unstable conditions at each of the four loads. The study also provides empirical evidence of the different force outputs achieved by adjusting load conditions on the rotational inertia device when performing squats, especially in the case of peak force. Concentric force outputs were significantly higher than eccentric outputs, except for peak force under both conditions. These findings support the use of the rotational inertia device to train the squatting exercise under unstable conditions for strength and conditioning trainers. The device could also be included in injury prevention programs for muscle lesions and ankle and knee joint injuries.
- Published
- 2016
- Full Text
- View/download PDF
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