Dehydrogenative reagent-free annulation of alkenes with diols for the synthesis of saturated O-heterocycles

氧化反应虽然在实验室合成中有着广泛的应用，但在工业领域却由于常用氧化试剂在安全和环境友好等方面存在的诸多问题而限制其应用。开发更为高效、安全和环保的氧化方法是解决氧化反应在有机合成中应用受限的关键。近年来，徐海超教授课题组利用电化学技术实现了系列无需氧化试剂的氧化偶联新反应，为多种重要杂环化合物体系的合成提供了高效、绿色的新方法。他们通过电氧化形成高反应活性的碳、氮自由基中间体，实现了通过其它方法不易实现的化学转化。【Abstract】Dehydrogenative annulation reactions are among the most straightforward and efficient approach for the preparation of cyclic structures. However, the applications of this strategy for the synthesis of saturated heterocycles have been rare. In addition, reported dehydrogenative bond-forming reactions commonly employ stoichiometric chemical oxidants, the use of which reduces the sustainability of the synthesis and brings safety and environmental issues. Herein, we report an organocatalyzed electrochemical dehydrogenative annulation reaction of alkenes with 1,2- and 1,3-diols for the synthesis of 1,4-dioxane and 1,4-dioxepane derivatives. The combination of electrochemistry and redox catalysis using an organic catalyst allows the electrosynthesis to proceed under transition metal- and oxidizing reagent-free conditions. In addition, the electrolytic method has a broad substrate scope and is compatible with many common functional groups, providing an efficient and straightforward access to functionalized 1,4-dioxane and 1,4-dioxepane products with diverse substitution patterns.We acknowledge the financial support of this research from MOST (2016YFA0204100), NSFC (No. 21672178), the “Thousand Youth Talents Plan”, and Fundamental Research Funds for the Central Universities. 研究工作得到国家重点研发计划纳米科技重点专项（项目批准号：2016YFA0204100）、国家自然科学基金（项目批准号：21672178）、中组部青年千人计划和中央高校基本科研业务费专项资金的资助

Evidence for Superfluidity of Ultracold Fermions in an Optical Lattice

The study of superfluid fermion pairs in a periodic potential has important ramifications for understanding superconductivity in crystalline materials. Using cold atomic gases, various condensed matter models can be studied in a highly controllable environment. Weakly repulsive fermions in an optical lattice could undergo d-wave pairing at low temperatures, a possible mechanism for high temperature superconductivity in the cuprates. The lattice potential could also strongly increase the critical temperature for s-wave superfluidity. Recent experimental advances in the bulk include the observation of fermion pair condensates and high-temperature superfluidity. Experiments with fermions and bosonic bound pairs in optical lattices have been reported, but have not yet addressed superfluid behavior. Here we show that when a condensate of fermionic atom pairs was released from an optical lattice, distinct interference peaks appear, implying long range order, a property of a superfluid. Conceptually, this implies that strong s-wave pairing and superfluidity have now been established in a lattice potential, where the transport of atoms occurs by quantum mechanical tunneling and not by simple propagation. These observations were made for unitarity limited interactions on both sides of a Feshbach resonance. For larger lattice depths, the coherence was lost in a reversible manner, possibly due to a superfluid to insulator transition. Such strongly interacting fermions in an optical lattice can be used to study a new class of Hamiltonians with interband and atom-molecule couplings.Comment: accepted for publication in Natur

Correction: A novel enantioselective synthesis of 6H-dibenzopyran derivatives by combined palladium/norbornene and cinchona alkaloid catalysis

Correction for 'A novel enantioselective synthesis of 6H-dibenzopyran derivatives by combined palladium/norbornene and cinchona alkaloid catalysis' by Di Xu et al., Org. Biomol. Chem., 2015, DOI: 10.1039/c4ob02551b

Pairwise comparison matrices and the error-free property of the decision maker

Pairwise comparison is a popular assessment method either for deriving criteria-weights or for evaluating alternatives according to a given criterion. In real-world applications consistency of the comparisons rarely happens: intransitivity can occur. The aim of the paper is to discuss the relationship between the consistency of the decision maker—described with the error-free property—and the consistency of the pairwise comparison matrix (PCM). The concept of error-free matrix is used to demonstrate that consistency of the PCM is not a sufficient condition of the error-free property of the decision maker. Informed and uninformed decision makers are defined. In the first stage of an assessment method a consistent or near-consistent matrix should be achieved: detecting, measuring and improving consistency are part of any procedure with both types of decision makers. In the second stage additional information are needed to reveal the decision maker’s real preferences. Interactive questioning procedures are recommended to reach that goal

Mosaic evolution in an asymmetrically feathered troodontid dinosaur with transitional features

Asymmetrical feathers have been associated with flight capability but are also found in species that do not fly, and their appearance was a major event in feather evolution. Among non-avialan theropods, they are only known in microraptorine dromaeosaurids. Here we report a new troodontid, Jianianhualong tengi gen. et sp. nov., from the Lower Cretaceous Jehol Group of China, that has anatomical features that are transitional between long-armed basal troodontids and derived short-armed ones, shedding new light on troodontid character evolution. It indicates that troodontid feathering is similar to Archaeopteryx in having large arm and leg feathers as well as frond-like tail feathering, confirming that these feathering characteristics were widely present among basal paravians. Most significantly, the taxon has the earliest known asymmetrical troodontid feathers, suggesting that feather asymmetry was ancestral to Paraves. This taxon also displays a mosaic distribution of characters like Sinusonasus, another troodontid with transitional anatomical features.published_or_final_versio

How promising is phototherapy for cancer?

Oncological phototherapy, including current photodynamic therapy (PDT), developmental photoactivated chemotherapy (PACT) and photothermal therapy (PTT), shows promising photo-efficacy for superficial and internal tumours. The dual application of light and photochemotherapeutic agents allows accurate cancer targeting, low invasiveness and novel mechanisms of action. Current advances in new light sources and photoactive agents are encouraging for future development

Exogenous WNT5A and WNT11 proteins rescue CITED2 dysfunction in mouse embryonic stem cells and zebrafish morphants

Mutations and inadequate methylation profiles of CITED2 are associated with human congenital heart disease (CHD). In mouse, Cited2 is necessary for embryogenesis, particularly for heart development, and its depletion in embryonic stem cells (ESC) impairs cardiac differentiation. We have now determined that Cited2 depletion in ESC affects the expression of transcription factors and cardiopoietic genes involved in early mesoderm and cardiac specification. Interestingly, the supplementation of the secretome prepared from ESC overexpressing CITED2, during the onset of differentiation, rescued the cardiogenic defects of Cited2-depleted ESC. In addition, we demonstrate that the proteins WNT5A and WNT11 held the potential for rescue. We also validated the zebrafish as a model to investigate cited2 function during development. Indeed, the microinjection of morpholinos targeting cited2 transcripts caused developmental defects recapitulating those of mice knockout models, including the increased propensity for cardiac defects and severe death rate. Importantly, the co-injection of anti-cited2 morpholinos with either CITED2 or WNT5A and WNT11 recombinant proteins corrected the developmental defects of Cited2-morphants. This study argues that defects caused by the dysfunction of Cited2 at early stages of development, including heart anomalies, may be remediable by supplementation of exogenous molecules, offering the opportunity to develop novel therapeutic strategies aiming to prevent CHD.Agência financiadora: Fundação para a Ciência e a Tecnologia (FCT) Comissão de Coordenação e Desenvolvimento Regional do Algarve (CCDR Algarve) ALG-01-0145-FEDER-28044; DFG 568/17-2 Algarve Biomedical Center (ABC) Municipio de Louléinfo:eu-repo/semantics/publishedVersio

Network model of immune responses reveals key effectors to single and co-infection dynamics by a respiratory bacterium and a gastrointestinal helminth

Co-infections alter the host immune response but how the systemic and local processes at the site of infection interact is still unclear. The majority of studies on co-infections concentrate on one of the infecting species, an immune function or group of cells and often focus on the initial phase of the infection. Here, we used a combination of experiments and mathematical modelling to investigate the network of immune responses against single and co-infections with the respiratory bacterium Bordetella bronchiseptica and the gastrointestinal helminth Trichostrongylus retortaeformis. Our goal was to identify representative mediators and functions that could capture the essence of the host immune response as a whole, and to assess how their relative contribution dynamically changed over time and between single and co-infected individuals. Network-based discrete dynamic models of single infections were built using current knowledge of bacterial and helminth immunology; the two single infection models were combined into a co-infection model that was then verified by our empirical findings. Simulations showed that a T helper cell mediated antibody and neutrophil response led to phagocytosis and clearance of B. bronchiseptica from the lungs. This was consistent in single and co-infection with no significant delay induced by the helminth. In contrast, T. retortaeformis intensity decreased faster when co-infected with the bacterium. Simulations suggested that the robust recruitment of neutrophils in the co-infection, added to the activation of IgG and eosinophil driven reduction of larvae, which also played an important role in single infection, contributed to this fast clearance. Perturbation analysis of the models, through the knockout of individual nodes (immune cells), identified the cells critical to parasite persistence and clearance both in single and co-infections. Our integrated approach captured the within-host immuno-dynamics of bacteria-helminth infection and identified key components that can be crucial for explaining individual variability between single and co-infections in natural populations

A wideband linear tunable CDTA and its application in field programmable analogue array

This document is the Accepted Manuscript version of the following article: Hu, Z., Wang, C., Sun, J. et al. ‘A wideband linear tunable CDTA and its application in field programmable analogue array’, Analog Integrated Circuits and Signal Processing, Vol. 88 (3): 465-483, September 2016. Under embargo. Embargo end date: 6 June 2017. The final publication is available at Springer via https://link.springer.com/article/10.1007%2Fs10470-016-0772-7 © Springer Science+Business Media New York 2016In this paper, a NMOS-based wideband low power and linear tunable transconductance current differencing transconductance amplifier (CDTA) is presented. Based on the NMOS CDTA, a novel simple and easily reconfigurable configurable analogue block (CAB) is designed. Moreover, using the novel CAB, a simple and versatile butterfly-shaped FPAA structure is introduced. The FPAA consists of six identical CABs, and it could realize six order current-mode low pass filter, second order current-mode universal filter, current-mode quadrature oscillator, current-mode multi-phase oscillator and current-mode multiplier for analog signal processing. The Cadence IC Design Tools 5.1.41 post-layout simulation and measurement results are included to confirm the theory.Peer reviewedFinal Accepted Versio