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A novel annelation strategy has been devised for stereoselective synthesis of tetrahydrocarbazoles. The pathway features a regio- and stereocontrolled condensation of indole and its substituted derivatives with electron-deficient 1,3-dienes via a Michael-Mannich reaction sequence. An extension of this method to include cross-conjugated allenes as substrates also results in a Michael-Mannich-Michael cascade, incorporating 2 equiv of indole with increasing product complexity. The formal 4π + 2π cyclization ...
The 2017 Nobel Prize in Medicine or Physiology has been awarded to Jeffrey Hall, Michael Rosbash, and Michael Young for elucidating molecular mechanisms of the circadian clock. From studies beginning in fruit flies, we now know that circadian regulation pervades most biological processes and has strong ties to human health and disease.
A novel, organobase-catalyzed and highly chemoselective Michael-Michael-acetalization cascade is presented for the efficient synthesis of spiro-indandione skeletons. Following this very simple protocol, a broad range of products could be obtained in good yields with excellent diastereocontrol. The role of steric factors in acetalization step has been evaluated.
Adult height is a function of genetic predispositions and environmental influences during childhood. Hence, any variation in height among monozygotic twins, who share genetic predispositions, is bound to reflect differences in their environmental exposure. Therefore, a height premium in earnings among monozygotic twins also reflects such exposure. In this study, we analyze the height premium over the life cycle among Swedish twins, 10,000 of whom are monozygotic. The premium is relatively constant over the ...
Using a theoretical approach grounded in implicit bias and stereotyping theories, this study examines the relationship between observable physical characteristics (skin tone, height, and gender) and earnings, as measured by income. Combining separate streams of research on the influence of these three characteristics, we draw from a sample of 31,356 individual-year observations across 4,340 individuals from the National Longitudinal Study of Youth (NLSY) 1997. We find that skin tone, height, and gender inte...
A heterogeneous enantioselective oxa-Michael-Michael reaction for the synthesis of chromans has been developed on a heterogeneous acid-base synergic catalyst with inherent silica as acidic sites and immobilized chiral amines as basic sites. Final products were afforded in selectivity of up to 98% and ee of 97% from 2-nitrovinyl phenol and 3-methyl-2-butenal. The heterogeneous synergistic catalytic mechanism has also been studied.
In recent decades, cohabitation has become an increasingly important relationship context for U.S. adults and their children, a union status characterized by high levels of instability. To understand why some cohabiting couples marry but others separate, researchers have drawn on theories emphasizing the benefits of specialization, the persistence of the male breadwinner norm, low income as a source of stress and conflict, and rising economic standards associated with marriage (the marriage bar). Because of...
Adolescent obesity not only has serious long-term health implications, but also the potential to lead to a socioeconomic trajectory of lower earnings and household income. However, the magnitude and mechanisms of such outcomes across the life course are poorly understood. Using birth cohort data from the British National Child Development Study (1958 to 2008), we examined the relationship between adolescent obesity (at age 16) and future household income, employment, wages, marriage and spousal earnings whe...
On-call medical services assumed by residents represent many hours of hard work and no studies have documented what it really is. As part of an effort to ameliorate our on-call system, we examined phone calls received by residents on call. Our objectives were to evaluate the characteristics of phone calls received by residents on call (who, when, why, need to go to the hospital) and to determine residents' perception of these calls. We also looked into implementing strategies to reduce unnecessary calls.
Graduate medical education programs typically set up call under the assumption that residents will have similar experiences. The terms black cloud and white cloud have frequently been used to describe residents with more difficult (black) or less difficult (white) call experiences. This study followed residents in the department of head and neck surgery during call to determine whether certain residents have a significantly different call experience than the norm. It is a prospective observational study con...
A widely respected veterinary surgeon and an innovator within the profession, Michael Pittaway was also a man of great charm and huge energy, who applied his skills across a wide range of interests.
Delayed return to work is common after acute respiratory distress syndrome (ARDS), but has undergone little detailed evaluation. We examined factors associated with the timing of return to work after ARDS, along with lost earnings and shifts in healthcare coverage.
The application of six novel α,β-dipeptides as chiral organocatalysts in the asymmetric Michael addition reaction between enolizable aldehydes and N-arylmaleimides or nitroolefins is described. With N-arylmaleimides as substrates, the best results were achieved with dipeptide 2 as a catalyst in the presence of aq. NaOH. Whereas dipeptides 4 and 6 in conjunction with 4-dimethylaminopyridine (DMAP) and thiourea as a hydrogen bond donor proved to be highly efficient organocatalytic systems in the enantiosele...
A diastereodivergent approach to highly substituted bicyclo[3.1.0]hexanes has been developed through a transannular alkylation reaction that builds up the bicyclic core employing asymmetric organocatalysis as the tool for the installation of all stereocenters. On one hand, a Michael/Michael cascade process between enals and 4-alkenyl sulfamidate imines under the iminium/enamine activation manifold provides a oxathiazole-2,2-dioxide-fused cyclohexane adduct that, after isolation, is subsequently engaged in a...
On the 22(nd) May 2017, suicide bomber Salman Abedi detonated an improvised explosive device (IED) in the Manchester Arena killing 22 people and injuring 116 others. Following the 'massacre in Manchester', the leader of the Labour Party, Jeremy Corbyn, linked UK foreign policy with terrorism on British soil. Controversial and contentious though Corbyn's claims may be, the terrorists themselves have also reported that what motivates them to carry out their abominable atrocities are British military operation...
The first chiral Brønsted acid-catalyzed asymmetric cascade allylboration/oxo-Michael reaction between o-formyl chalcones and allylboronate has been successfully realized, which afforded chiral 1,3-disubstituted 1,3-dihydroisobenzofurans with yield, diastereoselective ratio (dr) and enantioselective excess (ee) up to 94%, 2.5:1 and 98%, respectively. In addition, 2,3-dienylboronic pinacol ester was also applied into this cascade reaction with good catalytic results.
This Cell Systems Call features invited summaries of 32 of the 38 papers accepted for presentation in the "regular track" at the 2017 Research in Computational Molecular Biology conference. The editors have categorized the summaries into cancer genomics, genetics, mass spectrometry, metagenomics, network analysis, phylogenetics, sequence annotation, sequence informatics, single-cell data analysis, and structural biology.
The major function of the enzyme human tissue transglutaminase (TG2) is the crosslinking of proteins via a transamidation between the γ-carboxamide of a glutamine and the ε-amino group of a lysine. Overexpression of TG2 can lead to undesirable outcomes and has been linked to conditions such as fibrosis, celiac disease and neurodegenerative diseases. Accordingly, TG2 is a tempting drug target. The most effective TG2 inhibitors to date are small-molecule peptidomimetics featuring electrophilic warheads that...
In order to quantify the electrophilic reactivities of common Michael acceptors, we measured the kinetics of the reactions of monoacceptor-substituted ethylenes (H2C═CH-Acc, 1) and styrenes (PhCH═CH-Acc, 2) with pyridinium ylides 3, sulfonium ylide 4, and sulfonyl-substituted chloromethyl anion 5. Substitution of the 57 measured second-order rate constants (log k) and the previously reported nucleophile-specific parameters N and sN for 3-5 into the correlation log k = sN(E + N) allowed us to calculate 1...
In this article we report on the mechanistic studies of the Michael addition of amines and hydrazines to nitrostyrenes. Under the present conditions the corresponding N-alkyl/aryl substituted benzyl imines and N-methyl/phenyl substituted benzyl hydrazones were observed via a retro-aza-Henry type process. By combining organic synthesis and characterization experiments with computational chemistry calculations, we reveal that this reaction proceeds via a protic solvent mediated mechanism. Experiments in deute...
Bifunctional secondary amine-thiourea organocatalysts were successfully applied in the stereocontrolled synthesis of barbiturate fused tetrahydropyrano scaffold. As compared with the generally used tertiary amine-thiourea organocatalysts, they exhibited Bifunctional secondary amine-thiourea organocatalysts were successfully applied in the stereocontrolled synthesis of barbiturate-fused tetrahydropyrano scaffolds. Compared with typically used tertiary amine-thiourea organocatalysts, the developed catalysts e...