Even though 2,2'-diiodo- and 2,2'-dibromobiaryls represent accomplished precursors for heterofluorenes and other extended π-conjugated systems, their preparation still remains nontrivial when structural diversity of the biaryl backbone is required. Herein, we report a convenient method for the preparation of various 2,2'-diiodobiaryls from 2-iodobiaryls via cyclic diaryliodonium intermediates. An iodinative ring-opening of the diaryliodonium salts, mediated by a copper/diamine catalyst system, is able to afford the corresponding 2,2'-diiodobiaryls under mild conditions. The versatility of this two-step approach is demonstrated by the preparation of hitherto unexplored tetraiodoteraryls and their conversion into ladder-type π-conjugated systems.
In this work, we describe the SuFEx-based polycondensation between bisalkylsulfonyl fluorides (AA monomers) and bisphenol bis(t-butyldimethylsilyl) ethers (BB monomers) using [Ph3P=N-PPh3]+[HF2]− as the catalyst. The AA monomers were prepared via the highly reliable Michael addition of ethenesulfonyl fluoride and amines/anilines while the BB monomers were obtained from silylation of bisphenols by t-butyldimethylsilyl chloride. With these reactions, we were able to achieve a remarkable diversity of monomeric building blocks by exploiting readily available amines, anilines, and bisphenols as starting materials. The SuFEx-based polysulfonate formation reaction exhibited excellent efficiency and functional group tolerance, producing polysulfonates with a variety of side chain functionalities in >99% conversion within 10 min to 1 h. When bearing an orthogonal group on the side chain, the polysulfonates can be further functionalized via click-chemistry based post-polymerization modification.
This paper is concerned with regression models for correlated mixed discrete and continuous outcomes constructed using copulas. Our approach entails specifying marginal regression models for the outcomes, and combining them via a copula to form a joint model. Specifically, we propose marginal regression models (e.g. generalized linear models) to link the outcomes' marginal means to covariates. To account for associations between outcomes, we adopt the Gaussian copula to indirectly specify their joint distributions. Our approach has two advantages over current methods: one, regression parameters in models for both outcomes are marginally meaningful, and two, the association is 'margin-free', in the sense that it is characterized by the copula alone. By assuming a latent variable framework to describe discrete outcomes, the copula used still uniquely determines the joint distribution. In addition, association measures between outcomes can be interpreted in the usual way. We report results of simulations concerning the bias and efficiency of two likelihood-based estimation methods for the model. Finally, we illustrate the model using data on burn injuries.
ObjectiveTo the best of our knowledge, the association of insulin resistance (IR) with chronic kidney disease (CKD) has not been well studied in normal-weight individuals. The aim of this study is to examine whether IR is associated with CKD in non-diabetic subjects with normal weight. We also examine whether the presence of obesity modifies the association of IR with CKD.MethodsData were drawn from a cross-sectional survey in China. Both estimated glomerular filtration rate and urinary albumin to creatinine ratio were used as markers of CKD. Logistic regression models and the quartiles of homeostatic model assessment of insulin resistance were used to explore the associations of IR with CKD in entire cohort, normal-weight and overweight/obese subpopulations.ResultsIn normal-weight subpopulation, the prevalence of IR and metabolic syndrome were 11.11% and 8.99%, respectively. In the entire cohort, the highest quartile HOMA-insulin resistance had a 70% increased risk for CKD (RR 1.70, 95% CI 1.07, 2.71, P=0.03, comparing the highest to the lowest quartile). However, when adding obesity to the model, the association was abolished. IR was associated with CKD in overweight/obese subpopulation but not in normal-weight subpopulation.ConclusionIR and MetS in normal-weight individuals is common in the Chinese population. IR is associated with CKD in overweight/obese subpopulation but not in normal-weight subpopulation and the presence of obesity modifies the association of IR with CKD.
We performed this study to investigate the prevalences of insulin resistance and metabolic syndrome (MetS) in a Chinese population with normal weight. We also examined whether fat mass is associated with insulin resistance and MetS in normal-weight individuals. Data were drawn from a cross-sectional study in China. Subjects with diabetes were excluded. The prevalences of insulin resistance and MetS were calculated. Multivariate logistic regression analysis was performed repeated separately for body mass index (BMI) and waist circumference (WC) in both men and women. We also used the combination of BMI and WC to predict insulin resistance and MetS. 8.55 % of normal-weight men and 12.62 % of normal-weight women had insulin resistance. 7.41 % of normal-weight men and 10.24 % of normal-weight women had MetS. WC was associated with incident insulin resistance and MetS independent of BMI in both men and women. BMI was independently associated with incident MetS in women. Normal-weight individuals with insulin resistance and/or MetS are not rare in the Chinese population. Fat mass is associated with insulin resistance and MetS in normal-weight subjects. The current findings support using both BMI and WC in clinical practice.
Benzo[b]heteroles containing heteroatoms other than nitrogen and oxygen have received considerable attention for their potential applications in materials science. This poses an increasing demand for efficient, selective, and broad-scope methods for their synthesis. This review article summarizes the recent developments in synthetic methods and approaches to access representative members of the benzoheterole family.
Rapidly aSSembled: The combination of cobalt-catalyzed migratory arylzincation and copper-mediated/catalyzed chalcogenative cyclization allows the construction of benzothiophenes and benzoselenophenes from arylzinc reagents, alkynes, and elemental chalcogens. Benzothiophenes and benzoselenophenes diversely functionalized at the benzene ring moiety can be prepared, which are not readily accessible by conventional methods.
Benzo[b]phosphole derivatives have attracted significant attention for their unique optoelectronic properties with potential for application in materials science. Herein we report a modular approach to a benzo[b]phosphole derivative based on a one-pot sequential coupling of an arylzinc reagent, an alkyne, dichlorophenylphosphine (or phosphorus trichloride and a Grignard reagent), and an oxidant (for example H2O2, S, or Se). The approach allows for the construction of a library of previously inaccessible, structurally diverse benzo[b]phosphole derivatives with unprecedented ease.
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