A nickel‐catalyzed asymmetric diarylation reaction of vinylarenes enables the preparation of chiral α,α,β‐triarylated ethane scaffolds, which exist in a number of biologically active molecules. The use of reducing conditions with aryl bromides as coupling partners obviates the need for stoichiometric organometallic reagents and tolerates a broad range of functional groups. The application of an N‐oxyl radical as a ligand to a nickel catalyst represents a novel approach to facilitate nickel‐catalyzed cross‐coupling reactions.
A Ni-catalyzed reductive cyclization of 1,6-dienes affords 3,4-disubstituted cyclopentane and pyrrolidine derivatives with high trans diastereoselectivity. This cyclization reaction enables the efficient synthesis of trans-3,4-dimethyl gababutin, a pharmaceutical lead for treating neuropathic pain, and trans-3,4dimethylpyrrolidine, a precursor to drug candidates and pesticides. The trans selectivity distinguishes this reaction from relevant precedents that proceed via hydrogen-atom transfer and lead to cis products. Mechanistic investigation, including kinetic, spectroscopic, and radical clock studies, attributes the trans diastereoselectivity to a classic, organometallic catalytic cycle mediated by Ni(I) and Ni(III) intermediates. The electron-rich Ni(I) intermediate, stabilized by a redox-active a-diimine ligand, is responsible for the chemoselectivity toward reductive cyclization as opposed to the redox-neutral cycloisomerization observed with previous Ni(II) catalysts.
A reductive dicarbofunctionalization reaction of alkenes has been developed and applied to the preparation of substituted carbo- and heterocycles. The reaction conditions avoid the use of air-sensitive organometallic reagents, and are compatible with a broad range of bromo-electrophiles and a wide variety of substituents to give cyclic products in excellent yields.
Mental Toughness (MT) is considered a necessary ingredient for high level performance.Unsurprisingly, scholarly interest in the development of mental toughness has increased over the past decade, with much of this work informed by qualitative designs. No study to date has systematically reviewed and integrated this body of qualitative research on MT development. The primary purpose of this study was to create an integrated theoretical framework that incorporates extant MT development research in sport and performance settings. Three subsequent aims were to (i) systematically review and evaluate the qualitative literature regarding key developmental factors and processes for MT; (ii) synthesise knowledge of key developmental factors and processes for MT; and (iii) generate an integrated framework that can inform future research and advancement in theory with regard to MT development. Following a systematic search of online journals, search engines, and databases, 10 papers met the criteria for inclusion and were retained. These studies served as the primary data for meta-data, meta-method, and meta-theory analyses, which were integrated using a meta-synthesis approach. Four key themes were identified from the existing qualitative evidence: personal characteristics, interactions with environment, progressive development, and breadth of experience. These unique themes were integrated with existing theory to propose a Bioecological Model of MT Development that encompasses interdependent interactions among the person, proximal processes, context, and time. We describe how this model can be used as a heuristic for research and practice, and underscore the importance of methodological diversity for future work on the development of MT.
Despite the global health community's historical focus on providing basic, costeffective primary health care delivered at the community level, recent trends in the developing world show increasing demand for the implementation of emergency care infrastructures, such as prehospital care systems and emergency departments, as well as specialised training programmes. However, the question remains whether, in a setting of limited global health care resources, it is logical to divert these already-sparse resources into the development of emergency care frameworks.The existing literature overwhelmingly supports the idea that emergency care systems, both community-based and within medical institutions, improve important outcomes, including significant morbidity and mortality. Crucial to the success of any public health or policy intervention, emergency care systems also seem to be strongly desired at the community and governmental levels. Integrating emergency care into existing health care systems will ideally rely on modest, low-cost steps to augment current models of primary health care delivery, focusing on adapting the lessons learned in the developed world to the unique needs and local variability of the rest of the globe.
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