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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.
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.
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.
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...
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...
The first example of a photoexcitated amine-catalyzed process for asymmetric Michael addition of o-quinodimethanes to enones is described. In the presence of simple chiral amino acid esters, a variety of Michael adducts were generally obtained in good yields and excellent stereoselectivities. This strategy can be successfully applied to 3-substituted-2-cyclohexenones and provides an asymmetric access to all-carbon quaternary centers. Furthermore, the high stereocontrol was explained by means of density-func...
The growing economic resemblance of spouses has contributed to rising inequality by increasing the number of couples in which there are two high- or two low-earning partners. The dominant explanation for this trend is increased assortative mating. Previous research has primarily relied on cross-sectional data and thus has been unable to disentangle changes in assortative mating from changes in the division of spouses' paid labor-a potentially key mechanism given the dramatic rise in wives' labor supply. We ...
A novel palladium(0)-catalyzed intermolecular arylative dearomatization of α-naphthols and subsequent aza-Michael reaction is described. Two adjacent stereocenters were constructed efficiently through consecutive arylative dearomatization and Michael addition reactions. By utilizing this method, structurally diverse benzomesembrine derivatives were synthesized with excellent yields and chemoselectivity. The benzomesembrine products were shown to undergo versatile functional-group transformations.
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 access to new oxazolo[3,2-d][1,4]oxazepin-5(3H)-ones starting from α-bromoamido alcohols and Michael acceptors under mild conditions is presented. This domino process proved to be chemo-, regio- and stereoselective and allows the formation of a large diversity of highly functional 7-membered rings in good yields up to 95%. The complete shift of the regioselectivity of the intermediate enolate from a C-C to a C-O bond formation, contrary to the already known alkylations of such ambident nucleophiles, is...
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.
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...
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.
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...
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...
Patients in a locked-in state (LIS) due to severe neurological disorders such as amyotrophic lateral sclerosis (ALS) require seamless emergency care by their caregivers or guardians. However, it is a difficult job for the guardians to continuously monitor the patients' state, especially when direct communication is not possible. In the present study, we developed an emergency call system for such patients using a steady-state visual evoked potential (SSVEP)-based brain switch. Although there have been previ...
Living in rural Maine, Jeffrey Hall's own rhythm has been thrown upside down after he received a very unexpected call one morning on the award of this year's Nobel Prize in Physiology or Medicine. Together with Michael Rosbash and Mike Young, they were recognized "for their discoveries of molecular mechanisms controlling the circadian rhythm." Cell editor Marta Koch caught up with Jeff on a calm Sunday morning, when electricity at his house had just returned after recent storms. Annotated excerpts from the...
It is sobering to publish Sell's call for every federal survey to include questions about sexual orientation and gender identity precisely when the Trump Administration excludes such questions from the proposed 2017 National Survey of Older Americans Act Participants (NSOAAP) conducted by the Administration for Community Living (ACL) in the Department of Health and Human Services. In particular, NSOAAP question DE1a, introduced in 2014, asked "Which of the following best represents how you think of yourself...
Delays in call light response are a significant patient quality and safety concern. Research on call light interventions and patient outcomes has focused exclusively on adult inpatients. This project examined the impact of increasing staff awareness and workflow redesign to improve the pediatric patient experience and outcomes based on timely response.