A new 3D Ag(I)-based coordination network, [Ag2(pz)(bdc)·H2O]n (1; pz = pyrazine and H2bdc = benzene-1,3-dicarboxylic acid), was constructed by one-pot assembly and structurally established by single-crystal X-ray diffraction at different temperatures. Upon cooling from 298 to 93 K, 1 undergo an interesting single-crystal to single-crystal phase transition from orthorhombic Ibca (Z = 16) to Pccn (Z = 32) at around 148 K. Both phases show a rare 2-fold-interpenetrated 4-connected lvt network but incorporate different [Ag2(COO)2] dimeric secondary building units. It is worth mentioning that complex 1 shows red- and blue-shifted luminescences in the 290-170 and 140-80 K temperature ranges, respectively. The variable-temperature single-crystal X-ray crystallographic studies suggest that the argentophilic interactions and rigidity of the structure dominated the luminescence chromism trends at the respective temperature ranges. Upon being mechanically ground, 1 exhibits a slight mechanoluminescence red shift from 589 to 604 nm at 298 K.
Assembly of small clusters into rigid bodies with precise shape and symmetry has been witnessed by the significant advances in cluster-based metal-organic frameworks (MOFs), however, nanosized silver cluster based MOFs remain largely unexplored. Herein, two anion-templated silver clusters, CO3 @Ag20 and SO4 @Ag22 , were ingeniously incorporated into a 2D sql lattice (1, [CO3 @Ag20 (iPrS)10 (NO3 )8 (DMF)2 ]n ) and an unprecedented 3D two-fold interpenetrated dia network (2, [SO4 @Ag22 (iPrS)12 (NO3 )6 ⋅2 NO3 ]n ), respectively, under mild solvothermal conditions. Their atomically precise structures were confirmed by single-crystal X-ray diffraction analysis and further consolidated by IR spectroscopy, thermogravimetric analysis (TGA), and elemental analysis. Each drum-like CO3 @Ag20 cluster is extended by twelve NO3 (-) ions to form the 2D sql lattice of 1, whereas each ball-shaped SO4 @Ag22 cluster with a twisted truncated tetrahedral geometry is pillared by four [Ag6 (NO3 )3 ] triangular prisms to form the 3D interpenetrated dia network of 2. Notably, 2 is the first interpenetrated 3D MOF constructed from silver clusters. These results demonstrate the dual role of the anions, which not only internally act as anion templates to induce the formation of silver thiolate clusters but also externally extend the cluster units into the rigid networks. The photoluminescent and electrochemical properties of 2 are discussed in detail.
This work presents a mixed-ligand metal−organic framework (m-MOF) integrated with two ligands, one as a luminophore and the other as a coreactant, on one metal node for self-enhanced electrochemiluminescence (ECL). Both 9,10-di(pcarboxyphenyl)anthracene (DPA) and 1,4-diazabicyclo[2.2.2]octane (D-H 2 ) ligands can be oxidized, generating the cation radicals DPA +• and D-H 2 +• , respectively. The latter can be deprotonated to form the neutral radical (D-H • ) and then react with DPA +• to produce excited DPA* for ECL emission without exogenous coreactants. As a result of the incorporation into the MOF framework and the intrareticular charge transfer between the two ligands, the ECL intensity of the m-MOF was increased 26.5-fold compared with that of the mixture of DPA and D-H 2 in aqueous solution. Moreover, with the process of second oxidation of D-H 2 , stepwise ECL emission was observed as a result of local excitation in the DPA unit, which was identified through density functional theory calculations. Overall, the implementation of the mixed-ligand approach, which combines the luminophore and coreactant as linkers in reticular materials, enriches the fundamentals and applications of ECL systems.
Chronic psychological stress is associated with an increased risk for relapse of inflammatory bowel diseases (IBD) and impedes the treatment of this condition. However, the impact of stress on the risk of IBD onset remains unclear. The goal of the present study was to examine whether chronic unpredictable mild stress (CUMS) could initiate or aggravate the onset of colon inflammation in rats which, in turn, would be capable of triggering bowel disease. We found that CUMS exposure increased infiltration of CD-45 positive cells and MPO activity, as well as augmented the expression of the inflammatory cytokines, IFN-γ and IL-6 within the colon of these rats. In addition, CUMS treatment changed the composition and diversity of gut microbiota and enhanced intestinal epithelial permeability, indicating the presence of a defect in the intestinal barrier. This CUMS-induced disruption of mucosal barrier integrity was associated with a reduction in expression of the tight junction protein, occludin 1, and an inhibition in mucosal layer functioning via reductions in goblet cells. Results from bacterial cultures revealed an increased presence of bacterial invasion after CUMS treatment as compared with that observed in controls. Thus, our data indicate that CUMS treatment induces alterations of the fecal microbiome and intestinal barrier defects, which facilitates bacterial invasion into colonic mucosa and further exacerbates inflammatory reactions within the colon. Accordingly, chronic stress may predispose patients to gastrointestinal infection and increase the risk of inflammation-related gut diseases.
Background The association between visceral adiposity index (VAI) and diabetic complications has been reported in cross-sectional studies, while the effect of VAI on complication development remains unclear. This study aims to evaluate the longitudinal association of VAI and Chinese VAI (CVAI) with the incidence of diabetic nephropathy and retinopathy using a Chinese cohort. Methods A total of 8 948 participants with type 2 diabetes from Beijing Health Management Cohort were enrolled during 2013–2014, and followed until December 31, 2019. Nephropathy was confirmed by urine albumin/creatinine ratio and estimated glomerular filtration rate; retinopathy was diagnosed using fundus photograph. Results The mean (SD) age was 53.35 (14.66) years, and 6 154 (68.8%) were men. During a median follow-up of 4.82 years, 467 participants developed nephropathy and 90 participants developed retinopathy. One-SD increase in VAI and CVAI levels were significantly associated with an increased risk of nephropathy, and the adjusted hazard ratios (HR) were 1.127 (95% CI 1.050–1.210) and 1.165 (95% CI 1.003–1.353), respectively. On contrary, VAI and CVAI level were not associated with retinopathy after adjusting confounding factors. Conclusion VAI and CVAI are independently associated with the development of nephropathy, but not retinopathy in Chinese adults with diabetes.
The various benefits of urban green space are gaining increasing attention nowadays. Hence, the distribution of green space has become a scrutinized concern for spatial equity among local governments and the planning scholars. This study is the first quantitative evaluation of urban park accessibility using house-level data in urban China, from the perspective of social equity. We chose Nanjing as the empirical case and examined 2709 real estate units and 79 parks within the city. Accessibility is measured by the 10-min walking distance from homes to the adjacent urban parks. Using the Street Network Analysis model in ArcGIS and the statistical methods in SPSS, the result shows that 60.5% of the real estates in Nanjing are located within a 10-min walk to access urban parks. However, this accessibility is positively correlated with housing prices, and negatively correlated with the age of the buildings, holding all other factors constant. While affluent homeowners capture a high-quality green amenity, newly-built low-income communities, where most residents are classified as a vulnerable population, have the lowest percentage of accessible green space. This study reveals the existing spatial disparities of urban park accessibility among different socio-economic groups in Nanjing, China. Additionally, we found that urban redevelopment projects with greening and the large-scale affordable housing construction are pricing out the urban poor and rural immigrants from the inner city to the urban peripheral areas. This will reduce the accessibility to urban parks and other public service facilities among the lower income families, and exacerbate the inequality among the rich and the poor in terms of their quality of life. Main findings of this study can inform policy decisions regarding equitable park provision in the construction of the green city and the sustainable development in urban China and other developing countries.
The controllable growth of metal nanoparticles on nanomaterials is becoming a useful strategy for developing nanocomposites with designated performance. Here, a DNAcontrolled strategy for growth of Pt nanoparticles on graphene oxide (GO−PtNPs) to regulate the nanozyme activity and a triplex-hybridization chain reaction (tHCR) for triggering the assembly of DNA probes to amplify the target-induced nanozyme catalytic signal were designed. The tHCR with one linear and two hairpin probes could be specially triggered by a tHCR trigger to form a long double-stranded DNA structure in the presence of target nucleic acid, which hindered the adsorption of these probes on a GO surface, and thus accelerated the growth of PtNPs. The formed GO−PtNPs showed strong catalytic activity toward the oxidation of 3,3,5,5-tetramethylbenzidine, thereby producing an amplified "turn-on" detection signal. The proposed method showed very high sensitivity with the detection limits down to 14.6 pM for mutant KRAS DNA and 21.7 pM for let-7a microRNA. This method was validated with better analytical performance than a general HCR system and could be effectively used for the identification of single-nucleotide polymorphisms, thus providing a novel approach for simple and sensitive detection of nucleic acids.
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