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Oxygen evolution reaction (OER) is studied on four kinds of Fe-based MOFs (Fe-MOF-235, Fe-MIL-101, Fe-MIL-88B and Fe-MIL-53) synthesized by solvothermal method using FeCl3·6H2O and terephthalic aci...

The oceans offer a virtually infinite source of uranium and could sustain nuclear power technology in terms of fuel supply. However, the current processes to extract uranium from seawater remain neither economically viable nor efficient enough to compete with uranium ore mining. Microporous polymers are emerging materials for the adsorption of uranyl ions due to their rich binding sites, but they still fall short of satisfactory performance. Here, inspired by the ubiquitous fractal structure in biology that is favourable for mass and fluid transfer, we describe a hierarchical porous membrane based on polymers of intrinsic microporosity that can capture uranium in seawater. This biomimetic membrane allows for rapid diffusion of uranium species, leading to a 20-fold higher uranium adsorption capacity in a uranium-spiked water solution (32 ppm) than the membrane with only intrinsic microporosity. Furthermore, in natural seawater, the membrane can extract as much uranium as 9.03 mg g−1 after four weeks. This work suggests a strategy to be extended to the rational design of a large family of microporous polymer adsorbents that could fulfil the vast promise of the oceans to fuel a reliable and potentially sustainable energy source. The vast amount of uranium in seawater is driving a shift from the use of mined ore to seawater extraction. Here the authors describe an adsorbent design based on polymers of intrinsic microporosity that adopts a bioinspired structure and allows efficient uranium capture.

Background: Pulmonary arterial hypertension (PAH) is a severe and fatal clinical syndrome characterized by high blood pressure and vascular remodeling in the pulmonary arterioles, which is also a rapidly progressing disease of the lung vasculature with a poor prognosis. Although PAH medication made great advances in recent years, the efficacy and safety of the medication are unsatisfactory. Therefore, we aimed to update and expand previous studies to explore the efficacy and safety of PAH-targeted medications. Methods: Relevant articles were searched and selected from published or publicly available data in PubMed, Cochrane Library, CNKI, PsycInfo, and MEDLINE (from inception until October 1st, 2020). To assess the efficacy and safety of PAH therapies, five efficacy outcomes [6-minute walking distance (6MWD), mean pulmonary arterial pressure (mPAP), WHO functional class (WHO FC) improvement, clinical worsening, death] and two safety outcomes [adverse events (AEs), serious adverse events (SAEs)] were selected. And 6MWD was regarded as the primary efficacy outcome. Results: 50 trials included with 10 996participants were selected. In terms of efficacy, all targeted drugs were more effective than placebo. For 6MWD, Bosentan + Sildenafil, Sildenafil, Bosentan + Iloprost were better than others. Bosentan + Iloprost and Bosentan + Sildenafil were better for mPAP. Bosentan + Iloprost and Ambrisentan + Tadalafil were more effective in improving WHO FC. Bosentan + Tadalafil and Bosentan + Iloprost had the Ambrisentan probability to reduce the incidence of clinical worsening. It is demonstrated that Ambrisentan had clear benefits in reducing all-cause mortality. In terms of safety, no therapies had been shown to reduce the incidence of SAEs significantly, and Ambrisentan + Tadalafil significantly increased the incidence of AEs. Conclusions: Phosphodiesterase 5 inhibitor (PDE5i) + Endothelin Receptor Antagonists (ERA) seems to be better therapy for PAH. Prostacyclin analogs (ProsA) + ERA appear promising, though additional data is warranted. Registration PROSPERO CRD42020218818.

To investigate the changes and evaluate the diagnosis value of circumpapillary vessel density (VD) in cases of acute primary angle closure (APAC).Case-control study.APAC patients with a history of unilateral acute attack were enrolled. The eyes with acute episode constituted the case group while the contralateral eyes without attack consisted of the control group. Ophthalmic examinations including slit-lamp examination, best-corrected visual acuity, intraocular pressure and visual field were carried out. Retinal nerve fiber layer (RNFL), macular ganglion cell complex (GCC) were measured by spectral-domain optical coherence tomography, while VD was assessed by optical coherence tomography angiography.The whole en face image vessel density (wiVD), circumpapillary vessel density (cpVD) and inside disk VD for both all vessels and capillary were all significantly lower in the APAC eyes compared to the fellow eyes (P 0.01 for all). In APAC eyes, the wiVD, inside disk VD and cpVD both for all vessels and capillary were all positively correlated with RNFL and GCC thicknesses but negatively correlated with the mean deviation (MD), pattern standard deviation (PSD) and the duration of acute attack (all P 0.01). From the ROC curve, the cpVDIn APAC eyes, circumpapillary VD decreased significantly compared with the fellow unaffected eyes. They were significantly correlated with thicknesses of RNFL and GCC, and visual field MD and PSD in the APAC eyes. The patients with longer duration of acute attack were more likely to have lower cpVD. For APAC, the diagnostic ability of wiVD and cpVD was similar with RNFL, GCC and MD and was higher than inside disk VD.

We report two novel roaming pathways for the H + C2H2 → H2 + C2H reaction by performing extensive quasiclassical trajectory calculations on a new, global, high-level machine learning-based potential energy surface. One corresponds to the acetylene-facilitated roaming pathway, where the H atom turns back from the acetylene + H channel and abstracts another H atom from acetylene. The other is the vinylidene-facilitated roaming, where the H atom turns back from the vinylidene + H channel and abstracts another H from vinylidene. The "double-roaming" pathways account for roughly 95% of the total cross section of the H2 + C2H products at the collision energy of 70 kcal/mol. These computational results give valuable insights into the significance of the two isomers (acetylene and vinylidene) in chemical reaction dynamics and also the experimental search for roaming dynamics in this bimolecular reaction.

In order to well arrange active sites and avoid byproducts, the reasonable structured carrier nanocatalyst plays a crucial role in high catalytic performance, but still remains a challenge. Herein, the layered CuNi-Cu2O/NiAlOx nanosheets have been constructed through hydrothermal synthesis followed by calcination and H2 reduction treatment process. The in-situ formed CuNi nanoalloys (NAs) and nano-Cu2O were evenly distributed on the bilateral surface of layered NiAlOx nanosheets. Based on the planar structure of nanosheet, the synergy between catalytic active CuNi NAs and photocatalytic active nano-Cu2O endows CuNi-Cu2O/NiAlOx nanosheets with rapid conversion efficiency for catalyzing p-nitrophenol (p-NP, 14 mg·L−1) to p-aminophenol (p-AP) in 32 s with the reaction rate constant k up to 0.1779 s−1, and no obvious performance decay can be observed even over 27 cycles. Moreover, high concentration of p-NP at 10 and 20 g·L−1 could be reduced to p-AP within 14 and 20 min, respectively. Such designed nanoalloy/bimetal-oxide heterostructure can provide a solution for rapid conversion of aminoaromatics from nitroaromatics wastewater even at a large concentration range.

In order to solve two issues of chlorine-resistant bacteria (CRB) and disinfection byproducts (DBPs) in tap water after the chlorine-containing treatment process, an innovative core–sheath nanostru...

Metal anodes represent as a prime choice for the coming generation rechargeable batteries with high energy density. However, daunting challenges including electrode volume variation and inevitable side reactions preclude them from becoming a viable technology. Here, a facile replacement reaction was employed to fabricate a three-dimensional (3D) interdigitated metal/solid electrolyte composite electrode, which not only provides a stable host structure for buffering the volume change within the composite but also prevents side reactions by avoiding the direct contact between active metal and liquid electrolyte. As a proof-of-concept demonstration, a 3D interdigitated zinc (Zn) metal/solid electrolyte architecture was fabricated via a galvanic replacement reaction between Zn metal foil and indium (In) chloride solution followed by electrochemical activation, featuring the interdigitation between metallic Zn and amorphous indium hydroxide sulfate (IHS) with high Zn2+ conductivity (56.9 ± 1.8 mS cm-1), large Zn2+ transference number (0.55), and high electronic resistivity [(2.08 ± 0.01) × 103 Ω cm]. The as-designed Zn/IHS electrode sustained stable electrochemical Zn plating/stripping over 700 cycles with a record-low overpotential of 8 mV at 1 mA cm-2 and 0.5 mAh cm-2. More impressively, it displayed cycle-stable performance with low overpotential of 10 mV under ultrahigh current density and areal capacity (20 mA cm-2, 20 mAh cm-2), which outperformed all the reported Zn metal electrodes in mild aqueous electrolyte. The fabrication of interdigitated metal/solid electrolyte was generalized to other metal pairs, including Zn/Sn and Zn/Co, which provide inspiration for next-generation Zn metal batteries with high energy density and reversibility.

Capsaicin (trans-8-methyl-N-vanillyl-6-nonenamide), a well-known vanilloid, which is the main spicy component in chili peppers, showing several biological activities and the potential applications range from food flavorings to therapeutics. Traditional extraction of capsaicin by organic solvents was time-consuming, some new methods such as aqueous two-phase method and ionic liquid extraction method have been developed. During past few decades, an ample variety of biological effects of capsaicin have been evaluated. Capsaicin can be used in biofilms and antifouling coatings due to its antimicrobial activity, allowing it has a promising application in food packaging, food preservation, marine environment and dental therapy. Capsaicin also play a crucial role in metabolic disorders, including weight loss, pressure lowing and insulin reduction effects. In addition, capsaicin was identified effective on preventing human cancers, such as lung cancer, stomach cancer, colon cancer and breast cancer by inducing apoptosis and inhibiting cell proliferation of tumor cells. Previous research also suggest the positive effects of capsaicin on pain relief and cognitive impairment. Capsaicin, the agonist of transient receptor potential vanilloid type 1 (TRPV1), could selectively activate TRPV1, inducing Ca2+ influx and related signaling pathways. Recently, gut microbiota was also involved in some diseases therapeutics, but its influence on the effects of capsaicin still need to be deeply studied. In this review, different extraction and purification methods of capsaicin, its biological activities and pharmacological effects were systematically summarized, as well as the possible mechanisms were also deeply discussed. This article will give an updated and better understanding of capsaicin-related biological effects and provide theoretical basis for its further research and applications in human health and manufacture development.

Ischemia-reperfusion (I/R) injury causes cardiac dysfunction through several mechanisms including the irregular expression of some long noncoding RNA. However, the role of SNHG12 in myocardial I/R injury remains unclear. Here, we found the increase of the SNHG12 level in hypoxia-reoxygenation (H/R)-injured-H9c2 cells. SNHG12 silencing enhanced the apoptosis of H/R-injured H9c2 cells, while SNHG12 overexpression relieved the cardiomyocyte apoptosis induced by H/R stimulation. Additionally, the suppression of SNHG12 significantly boosted the H/R-induced expression and the production of TNF-α, IL-6, and IL-1β, as well as the activation of NF-κB, which were fully reversed after overexpression of SNHG12. Mechanistically, SNHG12 adversely regulated the production of receptor for advanced glycation end products (RAGE) in H/R-stimulated H9c2 cells. Antibody blocking of RAGE alleviated the apoptosis of H/R-injured H9c2 cells. Collectively, we have determined a valuable mechanism by which the high level of SNHG12 contributes to H9c2 cells against H/R injury through the reduction of RAGE expression.

Waldenstrom’s macroglobulinemia (WM) is an indolent B-cell non-Hodgkin lymphoma characterized by lymphoplasmacytic histology in the bone marrow with monoclonal IgM. Median survival can be in excess of 10 years. The 5-year cumulative incidence of death is low at about 10%. One-third of all-cause specific mortality is due to the lymphoma for which histologic transformation (HT) is rare. Here we present a case of a 60-year-old man with longstanding untreated WM, presenting with minimally symptomatic transformation to diffuse large B-cell lymphoma (DLBCL), with an accompanying review of the literature. Transformed WM, diagnosed greater than 5 years, has a reported survival period of 8 - 9 months. This case highlights that after a decade of continued stability in WM, not requiring treatment, an acute change in laboratory data with minimally progressive IgM levels, in the absence of B symptoms and clinical findings, may be the harbinger of transformation and at the time of diagnosis can have a rapidly deteriorating clinical course. In this case, the tripling of the lactate dehydrogenase (LDH) as the primary drastic change demonstrates the importance of the rapid increase in LDH as a singly reliable marker for HT. Late transformation has been borne out as a negative variable as the generally indolent course of WM is curtailed with the poor outcome in HT. Although MYD88 wildtype is a possible predictive factor for transformation, it is unclear if late transformation is clonally or non-clonally related and further molecular investigation is needed.

Tin (Sn)-based and mixed tin–lead (Sn–Pb) perovskites have attracted increased attention as promising candidates for new generation lead-free perovskite and all-perovskite tandem solar cells. Howev...

The αS2-casein (αS2-CN) is a member of the casein family associated with milk traits in ruminants, but so far the buffalo CSN1S2 gene has not been well understood. In this work, the polymorphisms of CSN1S2 in river and swamp buffalo were detected using direct sequencing of polymerase chain reaction (PCR) products. As a result, 13 single nucleotide polymorphisms (SNPs) were identified in the coding sequence (CDS) of CSN1S2 in two types of buffalo, of which eight SNPs were non-synonymous. The amino acid changes caused by c.580T>C and c.642C>G may affect the function of buffalo αS2-CN. A total of 11 CSN1S2 CDS haplotypes were defined, and accordingly 11 variants of buffalo αS2-CN were inferred and named. The CSN1S2 CDSs of both types of buffalo were 669 nucleotides, which encoded a precursor of 222 amino acids (AAs), and the first 15 AAs constitute a signal peptide. The composition and physicochemical characteristics of two types of buffalo αS2-CNs were similar but slightly different from those of cattle αS2-CN. The αS2-CN mature peptides of buffalo and the species of Bos genus contained a casein domain, and their secondary structures were highly consistent, indicating that they are functionally similar. The results here provide initial insights into the variation, characteristics and biological function of buffalo CSN1S2.

Objective The objective of this study was to verify the lipid-lowering effect of Juhe Fang extract (JHFE) and to determine its characteristic chemical profile in vitro and in vivo. Methods A hyperlipidemia model was established by feeding mice a high-fat diet (HFD). After treatment for 30 days, serum total cholesterol (TC), triglyceride (TG), high-density lipoprotein cholesterol (HDL-C) and low-density lipoprotein cholesterol (LDL-C) levels were measured with an automatic biochemistry analyzer. The components from JHFE obtained from in vivo and in vitro experiments were investigated using an UPLC-Q Exactive-Orbitrap MS/MS. Results The TC, TG, and LDL-C in the serum significantly decreased and the HDL-C significantly increased after JHFE treatment. A total of 95 compounds from JHEF including 15 phenolic acids (PA), 4 phenylethanoid glycosides (PG), 24 flavonoids (F), 14 triterpenoids (T), 10 diterpenoid glycosides (D), 18 alkaloids (A) and 10 others (O) were identified. Trigonelline was discovered for the first time in a herbal medicine of Juhe Fang. Furthermore, 68 compounds were identified in vivo including 28 prototype compounds and 40 metabolites. The metabolic characteristics of these components were revealed including identification of new metabolites of 4-hydroxyphenyl ethyl-8-O-[α-L- arabinopyranosyl-(1 → 6)]-β-D-glucopyranoside (PEG) and lirinidine. A total of 43 components from JHFE were absorbed and/or metabolized. The contribution rate of each type of chemical component from JHFE to its lipid-lowering effect from high to low were A, F, PG, PA, D and T. Conclusion The results of this study showed that JHFE demonstrated a significant lipid-lowering effect in a high-fat diet (HFD)-induced hyperlipidemia mouse model. Specific types of PA, PG, F, D, T and A formed the pharmaceutical architecture of the lipid-lowering effect of JHFE. This study should prove useful for clarifying the components responsible for the lipid-lowering effect of JHFE and provide a basis for precision quality control research.

Chemical reduction of a benzo-fused double [7]helicene (1) with two alkali metals, K and Rb, provided access to three different reduced states of 1. The doubly-reduced helicene 12- has been characterized by single-crystal X-ray diffraction as a solvent-separated ion triplet with two potassium counterions. The triply- and tetra-reduced helicenes, 13- and 14- , have been crystallized together in an equimolar ratio and both form the contact-ion complexes with two Rb+ ions each, leaving three remaining Rb+ ions wrapped by crown ether and THF molecules. As structural consequence of the stepwise reduction of 1, the central axis of helicene becomes more compressed upon electron addition (1.42 A in 14- vs. 2.09 A in 1). This is accompanied by an extra core twist, as the peripheral dihedral angle increases from 16.5° in 1 to 20.7° in 14- . Theoretical calculations provided the pattern of negative charge build-up and distribution over the contorted helicene framework upon each electron addition, and the results are consistent with the X-ray crystallographic and NMR spectroscopic data.

Rechargeable aqueous Zn metal batteries are promising candidates for renewable energy storage. However, Zn metal is chemically active and suffers from chemical corrosion in aqueous electrolyte due to its low redox potential. It is of vital importance to reveal the corrosion mechanism, and improve the chemical stability and electrochemical reversibility of Zn metal anode for its practical application. In this work, it is revealed that a Zn metal electrode readily gets oxidized during its resting in aqueous ZnSO4 electrolyte, forming zinc hydroxide sulfate and hydrogen gas, leading to the increased internal resistance and swollen problems of batteries, and eventually battery failure. To inhibit such chemical corrosion, an anti-corrosive metallic Cu is introduced to Zn metal anode to construct a uniform Cu/Zn composite with dense structure, which is electrochemically converted to Cu–Zn alloy/Zn composite during battery cycling. The as-achieved Cu–Zn/Zn electrode exhibits stable cycling for over 1500 cycles at 1 ​mA/cm2 and 0.5 mAh/cm2 with little change in overpotential (46 ​mV) after resting for 1 month, while the bare Zn electrode shows large voltage fluctuation and high overpotential (>400 ​mV) under the same condition, suggesting the importance of inhibiting the chemical corrosion of Zn metal anode for rechargeable aqueous batteries.

Low vitamin D status is associated with progression in patients with renal cell carcinoma (RCC). The present study found that vimentin, a mesenchymal marker, was accordingly upregulated, and E‐cadherin, an epithelial marker, was downregulated in RCC patients with low vitamin D status. Thus, we investigated the effects of calcitriol or vitamin D3, an active form of vitamin D, on epithelial‐mesenchymal transition (EMT) in RCC cells. RCC cells were treated by two models. In model 1, three RCC cell lines, ACHN, 786‐O and CAKI‐2, were incubated with either LPS (2.0 μg/mL) or transforming growth factor (TGF)‐β1 (10 ng/mL) in the presence or absence of calcitriol (200 nmol/L). In model 2, two RCC cell lines, ACHN and CAKI‐2, were incubated with calcitriol (200 nmol/L) only. Calcitriol inhibited migration and invasion not only in TGF‐β1‐stimulated but also in TGF‐β1‐unstimulated RCC cells. Moreover, calcitriol suppressed E‐cadherin downregulation and vimentin upregulation not only in TGF‐β1‐stimulated but also in TGF‐β1‐unstimulated ACHN and CAKI‐2 cells. Calcitriol attenuated LPS‐induced upregulation of MMP‐2, MMP‐7, MMP‐9, MMP‐26 and urokinase‐type plasminogen activator (u‐PA) in ACHN cells. In addition, calcitriol blocked TGF‐β1‐induced nuclear translocation of ZEB1, Snail and Twist1 in ACHN and CAKI‐2 cells. Mechanistically, calcitriol suppressed EMT through different signaling pathways: (i) calcitriol suppressed Smad2/3 phosphorylation by reinforcing physical interaction between vitamin D receptor (VDR) and Smad3 in TGF‐β1‐stimulated RCC cells; (ii) calcitriol inhibited signal transducer and activator of transcription (STAT)3 activation in LPS‐stimulated RCC cells; (iii) calcitriol inhibited β‐catenin/TCF‐4 activation by promoting integration of VDR with β‐catenin in TGF‐β1‐unstimulated RCC cells. Taken together, calcitriol inhibits migration and invasion of RCC cells partially by suppressing Smad2/3‐, STAT3‐ and β‐catenin‐mediated EMT., Calcitriol suppressed EMT through two different signaling pathways: (i) calcitriol suppressed Smad2/3 phosphorylation by reinforcing physical interaction between vitamin D receptor (VDR) and Smad3 in TGF‐β1‐stimulated RCC cells; (ii) calcitriol inhibited β‐catenin/TCF‐4 activation by promoting integration of VDR with β‐catenin in TGF‐β1‐unstimulated RCC cells. Taken together, calcitriol inhibits migration and invasion of RCC cells by suppressing Smad2/3‐ and β‐catenin‐mediated EMT.

Crops show considerable capacity to adjust their photosynthetic characteristics to seasonal changes in temperature. However, how photosynthesis acclimates to changes in seasonal temperature under future climate conditions has not been revealed. We measured leaf photosynthesis (An ) of wheat (Triticum aestivum L.) and rice (Oryza sativa L.) grown under four combinations of two levels of CO2 (ambient and enriched up to 500 µmol/mol) and two levels of canopy temperature (ambient and increased by 1.5-2.0°C) in temperature by free-air CO2 enrichment (T-FACE) systems. Parameters of a biochemical C3 -photosynthesis model and of a stomatal conductance (gs ) model were estimated for the four conditions and for several crop stages. Some biochemical parameters related to electron transport and most gs parameters showed acclimation to seasonal growth temperature in both crops. The acclimation response did not differ much between wheat and rice, nor among the four treatments of the T-FACE systems, when the difference in the seasonal growth temperature was accounted for. The relationships between biochemical parameters and leaf nitrogen content were consistent across leaf ranks, developmental stages, and treatment conditions. The acclimation had a strong impact on gs model parameters: when parameter values of a particular stage were used, the model failed to correctly estimate gs values of other stages. Further analysis using the coupled gs -biochemical photosynthesis model showed that ignoring the acclimation effect did not result in critical errors in estimating leaf photosynthesis under future climate, as long as parameter values were measured or derived from data obtained before flowering.

Rechargeable lithium-sulfur batteries have attracted tremendous scientific attention owing to their high energy density. However, their practical application is greatly hindered by the notorious shuttling of soluble lithium polysulfide (LPS) intermediates with sluggish redox reactions and uncontrolled precipitation behavior. Herein, we report a semiliquid cathode composed of an active LPS solution/carbon nanofiber (CNF) composite layer, capped with a carbon nanotube (CNT) thin film decorated with metallic Mo nanoclusters that regulate the electrochemical redox reactions of LPS. The trace amount (0.05 mg cm

Lithium-sulfur (Li-S) battery has been regarded as a promising energy-storage system due to its high theoretical specific capacity of 1675 mAh g−1 and low cost of raw materials. However, several challenges remain to make Li-S batteries viable, including the shuttling of soluble lithium polysulfide intermediates and pulverization of Li metal anode. Engineering stable electrode-separator interfaces without causing large mass/volume increase of inactive materials and electrolyte uptake is an effective approach to improve the cycling stability of Li-S batteries while maintaining high available energy density. Herein, we report the engineering of a stable electrode-separator interface with an ultrathin conductive polymer nanolayer on the pore walls of both surfaces of the separator via a simple and scalable approach using in-situ vapor-phase polymerization of polypyrrole (PPy) on commercial Celgard separator with only a small increase in overall mass and volume. The inherent hydrophilicity of PPy enables the separator to have enhanced electrolyte uptake, which facilitates homogenous Li+ flux and thus uniform plating and stripping of metallic lithium at the anode side during the charge/discharge processes. Meanwhile, the chemical immobilization effect of PPy suppresses the migration of the soluble polysulfides and improves the stability of the sulfur cathode. We showed that a Li||Li symmetrical cell with the PPy modified separator gave a low and stable overpotential of less than 30 mV for over 250 h' stripping and plating test at 1 mA cm−2 with a fixed areal capacity of 3 mAh cm−2, which was significantly better than that using a regular Celgard separator. Using the PPy modified separator, Li-S cell with sulfur/carbon black composite cathode and lithium anode delivered stable cycling for 250 cycles at 0.5 C with a low capacity decay rate of 0.083% per cycle. Even for a Li-S cell with a high-areal-capacity sulfur cathode (4.8 mAh cm−2), good cycling stability was achieved. It gave a reversible areal capacity of 3.6 mAh cm−2 after 150 charge/discharge cycles at 0.2 C with 75.6% capacity retention. Besides, the as-achieved separator showed better thermal stability than the bare counterpart. This work offers an alternative approach for achieving a practical Li-S battery toward high energy density and long cycle life through simple and scalable separator-electrode interface engineering without significant increase in volume and mass.

Two-dimensional (2D) hybrid perovskites have shown many attractive properties associated with their soft lattices and multiple quantum well structure. Herein, we report the synthesis and characterization of two new multifunctional 2D hybrid perovskites, (PED)CuCl 4 and (BED) 2 CuCl 6 , which show reversible thermochromic behavior, dramatic temperature-dependent conductivity change, and strong ferromagnetism. Upon temperature change, the (PED)CuCl 4 and (BED) 2 CuCl 6 crystals exhibit a reversible color change between yellow and red-brown. The associated structural changes were monitored by in situ temperature-dependent powder X-ray diffraction (PXRD). The (BED) 2 CuCl 6 exhibits superior thermal stability, with a thermochromic working temperature up to 443 K. The conductivity of (BED) 2 CuCl 6 changes over six orders of magnitude upon temperature change. The 2D perovskites exhibit ferromagnetic properties with Curie temperatures around 13 K. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

A variety of biobased polymers have been derived from diverse natural resources. However, the mechanical properties of some of these polymers are inferior due to low chain entanglement. We report a...

Background: Cysteine-rich 61 (CYR61) and inflammation was upregulated in the lungs of patients with chronic obstructive pulmonary disease (COPD). However, the association between CYR61 and inflammation was unclear in COPD patients. This study aimed to analyze the association of serum CYR61 with pulmonary inflammation and lung function indexes in COPD patients.Methods: One hundred and fifty COPD patients and 150 control subjects were enrolled. Serum and pulmonary CYR61 was detected. Lung function indexes were evaluated in COPD patients.Results: Serum CYR61 level was elevated and pulmonary CYR61 expression was upregulated in COPD patients. An increased CYR61 was associated with decreased pulmonary function indexes in COPD patients. Further analyses showed that nuclear factor-kappa B (NF-κB) p65-positive nuclei was elevated in the lungs of COPD patients with high level of CYR61. Accordingly, serum monocyte chemotactic protein (MCP)-1 and tumor necrosis factor α (TNF-α), two downstream inflammatory cytokines of NF-κB pathway, were increased in parallel with CYR61, among which serum MCP-1 and TNF-α were the highest in COPD patients with high level of CYR61. Moreover, a positive correlation, determined by multivariate regression that excluded the influence of age, gender and smoking, was observed between serum CYR61 and inflammatory cytokines in COPD patients.Conclusion: These results provide evidence that an increased CYR61 is associated with pulmonary inflammation and COPD progression. Inflammatory cytokines may be the mediators between CYR61 elevation and COPD progression.

BACKGROUND Cadmium is a ubiquitous toxic heavy metal and environmental toxicant. Inflammation exerts central roles in the process of chronic obstructive pulmonary disease (COPD). However, few epidemiological studies on the correlation between cadmium exposure and COPD are available. The aim of this study was to evaluate the correlations among serum cadmium, inflammatory cytokines and pulmonary function in COPD patients. METHODS All 940 COPD patients were finally recruited in this study. Demographic characteristics and clinical information were extracted. Fasting serum was collected. Serum cadmium was detected through graphite furnace atomic absorption spectrophotometry. Serum inflammatory cytokines were measured using enzyme-linked immunosorbent assay. RESULTS All patients were classified into three groups according to the tertile division of serum cadmium concentration: low (

Lithium-sulfur (Li-S) batteries suffer from sluggish sulfur redox reactions under high-sulfur-loading and lean-electrolyte conditions. Herein, a typical Co@NC heterostructure composed of Co nanoparticles and a semiconductive N-doped carbon matrix is designed as a model Mott-Schottky catalyst to exert the electrocatalytic effect on sulfur electrochemistry. Theoretical and experimental results reveal the redistribution of charge and a built-in electric field at the Co@NC heterointerface, which are critical to lowering the energy barrier of polysulfide reduction and Li2S oxidation in the discharge and charge process, respectively. With Co@NC Mott-Schottky catalysts, the Li-S batteries display an ultrahigh capacity retention of 92.1% and a system-level gravimetric energy density of 307.8 Wh kg-1 under high S loading (10.73 mg cm-2) and lean electrolyte (E/S = 5.9 μL mgsulfur-1) conditions. The proposed Mott-Schottky heterostructure not only deepens the understanding of the electrocatalytic effect in Li-S chemistry but also inspires a rational catalyst design for advanced high-energy-density batteries.

The presence of the intrinsic band gap of 3.06 eV makes atomically thin carbon nitride sheets (CNs) a promising spin-based semiconductor material. However, the absence of localized spins makes the pristine CNs intrinsically nonmagnetic. Here we report the realization of strong room-temperature (RT) ferromagnetism with a high Curie temperature of ca. 524.2 K in atomically thin 2D CNs by annealing pristine CNs at 700 °C. In particular, the RT saturated magnetization reaches as high as 0.71 emu/g, which is the highest value reported so far in carbon-based materials. The structural characterization combined with density functional theory calculations reveals that (i) the seven C-C bonds per unit cell were formed after annealing and (ii) the C-C bonds can introduce high-density localized spins and realize the long-range ferromagnetic couplings among these spins.

Tensile tests were carried on the electroplated Cu films with various densities of twin grain boundary. With TEM images and a selected area diffraction pattern, nano-twinned structure can be observed and defined in the electroplated Cu films. The density of the nano-twin grain structure can be manipulated with the concentration of gelatin in the Cu-sulfate electrolyte solution. We found that the strength of the Cu films is highly related to the twin-boundary density. The Cu film with a greater twin-boundary density has a larger fracture strength than the Cu film with a lesser twin-boundary density. After tensile tests, necking phenomenon (about 20 μm) occurred in the fractured Cu films. Moreover, by focused ion beam (FIB) cross-sectional analysis, the de-twinning can be observed in the region where necking begins. Thus, we believe that the de-twinning of the nano-twinned structure initiates the plastic deformation of the nano-twinned Cu films. Furthermore, with the analysis of the TEM images on the nano-twinned structure in the necking region of the fractured Cu films, the de-twinning mechanism attributes to two processes: (1) the ledge formation by the engagement of the dislocations with the twin boundaries and (2) the collapse of the ledges with the opposite twin-boundaries. In conclusion, the plastic deformation of nano-twinned Cu films is governed by the de-twinning of the nano-twinned structure. Moreover, the fracture strength of the nano-twinned Cu films is proportional to the twin-boundaries density.

Roaming is a novel mechanism in reaction dynamics. It describes an unusual pathway, which can be quite different from the conventional minimum-energy path, leading to products. While roaming has been reported or suggested in a number of unimolecular reactions, it has been rarely reported for bimolecular reactions. Here, we report a high-level computational study of roaming dynamics in the important bimolecular combustion reaction H + C2H4 → H2 + C2H3, using a new, high-level machine learning-based potential energy surface. In addition to the complex-mediated roaming mechanism, a non-complex forming roaming mechanism is found. It can be described as a direct inelastic collision where the departing H atom roams and then abstracts an H atom. We denoted this as “collision-induced” roaming. These two roaming mechanisms have different angular distributions; however, both produce highly internally excited C2H3. The roaming pathway leads to remarkably different dynamics as compared with the direct abstraction pathway. A clear signature of the roaming mechanism is highly internally excited C2H3, which could be observed experimentally., Collision-induced and complex-mediated roaming mechanisms are revealed for an important bimolecular reaction in combustion.

BackgroundResistin is an endogenous ligand of Toll-like receptor 4 that activates several inflammatory signals. But the physiological function of resistin in community-acquired pneumonia (CAP) remains unknown. The goal of this research was to explore the associations between serum resistin and the severity and prognosis in CAP patients through a retrospective cohort study.MethodsAll 212 CAP patients and 106 healthy cases were enrolled. Demographic characteristics were extracted. Serum resistin was determined via enzyme-linked immunosorbent assay. The prognosis was tracked in CAP patients.ResultsSerum resistin on admission was raised in CAP patients compared with control cases. The level of resistin was gradually increased in parallel with CAP severity scores in CAP patients. Pearson and Spearman analyses revealed that serum resistin was positively correlated with CAP severity scores, white blood cells, urea nitrogen, creatinine, and inflammatory cytokines among CAP patients. There were negative relationships between resistin and hematocrit and albumin in CAP patients. Besides, linear and logistic regression analyses further indicated that serum resistin on admission was positively associated with CAP severity scores among CAP patients. Follow-up research revealed that serum resistin elevation on admission prolonged hospital stay in CAP patients.ConclusionSerum resistin on admission is positively correlated with the severity and hospital stay in CAP patients, indicating that resistin may be involved in the physiological process of CAP. Serum resistin may be a potential biomarker in the diagnosis and prognosis for CAP.

BackgroundSeveral studies demonstrate that endoplasmic reticulum (ER) stress-mediated epithelial-mesenchymal transition (EMT) is involved in the process of bleomycin (BLM)-induced pulmonary fibrosis. Tauroursodeoxycholic acid (TUDCA), a bile acid with chaperone properties, is an inhibitor of ER stress. This study aimed to investigate the preventive effects of TUDCA on BLM-induced EMT and lung fibrosis.MethodsThe model of lung fibrosis was established by intratracheal injection with a single dose of BLM (3.0 mg/kg). In TUDCA + BLM group, mice were intraperitoneally injected with TUDCA (250 mg/kg) daily.ResultsBLM-induced alveolar septal destruction and inflammatory cell infiltration were alleviated by TUDCA. BLM-induced interstitial collagen deposition, as determined by Sirius Red staining, was attenuated by TUDCA. BLM-induced elevation of pulmonary α-smooth muscle actin (α-SMA) and reduction of pulmonary E-cadherin were attenuated by TUDCA. BLM-induced pulmonary Smad2/3 phosphorylation was suppressed by TUDCA. BLM-induced elevation of Ki67 and PCNA was inhibited by TUDCA in mice lungs. In addition, BLM-induced elevation of HO-1 (heme oxygenase-1) and 3-NT (3-nitrotyrosine) was alleviated by TUDCA. Finally, BLM-induced upregulation of pulmonary GRP78 and CHOP was attenuated by TUDCA.ConclusionsThese results provide evidence that TUDCA pretreatment inhibits Smad2/3-medited EMT and subsequent lung fibrosis partially through suppressing BLM-induced ER stress and oxidative stress.

Ternary copper tin sulfides (CTS) have been attracted great attention as anode materials for lithium ion batteries (LIBs) owning to their high theoretical capacities and unique lithium storage mechanisms. However, the practical applications of CTS are plagued from the serious volumetric variation during the charge/discharge process. Herein, a high Cu/(Sn + S) element ratio copper tin sulfides, Cu4SnS4/Sn (CTS-4), with unique walnut-like microspheres was successfully prepared and firstly investigated as LIB anode materials. Compared with low Cu/(Sn + S) ratio Cu2SnS3 (CTS-3), CTS-4 delivers efficient lithium storage performance, cycling stability and rate capability. The considerable electrochemical performance is attributed to the higher conductivity and favorable Li+ diffusion coefficient of CTS-4 resulting from unique element ratio. This work will provide insight towards designing and building new anode materials for high-performance LIBs.

A new rapid modified one-step QuEChERS (quick, easy, cheap, effective, rugged, and safe) approach was developed for the simultaneous determination of 20 perfluoroalkyl substances (PFASs) from samples of cucumber, lettuce, eggplant, tomato, and leek. Several parameters were optimized. Similar pretreatment approaches were employed for comparison; the results verified the satisfactory performance of this new method. The detection limits of this method for the selected matrices ranged from 0.003 to 0.034 μg kg−1, and the method was verified to be satisfactory in terms of precision, accuracy, and matrix effects. 35 greenhouse vegetable samples were determined. PFASs were detected in 26 samples, with perfluorooctanoic acid (PFOA) being detected most frequently and much higher levels of PFBA and PFPeA being found in some samples. The total PFAS concentrations ranged from not detectable to 0.683 μg kg−1. This method could be applied for large scale determination of vegetables to research the migration and accumulation trends of PFASs from the environment to crops in the future.

A detailed chemical research of soft coral Sarcophyton ehrenbergi from the South China Sea yielded five new cembranoids 1-5 featuring an α,β-unsaturated-γ-lactone moiety rarely at C-6 to C-19, along with one known related diterpene 6. The structures and absolute configurations of 1-5 were established in the light of extensive spectroscopic data analysis, chemical reaction, X-ray diffraction analysis, TDDFT/ECD (time-dependent density functional theory/electronic circular dichroism) calculations, and biosynthesis path. This study led to the stereostructural revision of 6, which was misassigned by erroneously applying the empirical ECD helicity rule, indicating a challenging and risky work to determine the structure of this type of marine cembranoids. In the TNF-α inhibitory biotest, compound 2 exhibited a potent inhibitory activity (IC50 = 8.5 μM), which was analogous to the positive control dexamethasone (IC50 = 8.7 μM).

Several epidemiological reports demonstrated that vitamin D deficiency elevated risk of preterm delivery. We investigate the effects of oral cholecalciferol (VD3) supplementation on lipopolysaccharide (LPS)-induced preterm delivery. Pregnant mice were randomly assigned to either oral VD3 (25 μg/kg) or corn oil once daily from gestational day (GD)13 to GD15, and were intraperitoneally injected with either LPS (200 μg/kg) or normal saline on GD15. As expected, LPS was effective in inducing preterm delivery and fetal death. LPS-induced preterm delivery and fetal death were alleviated in VD3-pretreated mice. LPS-induced down-regulation of genes for placental progesterone biosynthetic enzymes was blocked in VD3-pretreated mice. LPS-induced reduction of serum progesterone was correspondingly attenuated by VD3. Although oral VD3 had no effect on estradiol production, it attenuated LPS-induced up-regulation of placental ERβ in mice. LPS-induced placental COX-2 up-regulation and serum PGF2α elevation were alleviated in VD3-pretreated mice. Additionally, LPS-evoked elevations of the placental Tnfα, Il1β, Mcp1 and Mip2 mRNAs were attenuated by VD3. VD3 promoted placental vitamin D receptor nuclear translocation and simultaneously alleviated LPS-induced nuclear translocation of NF-κB p65 and p50 subunits. These results provide evidence that oral VD3 supplementation alleviates LPS-induced preterm delivery and fetal demise partially through regulating placental steroid hormones and prostaglandins.

Gaoqi Zhang,1 Jilei Zhang,2 Xinrui Yang,1 Xinpei Zhang,1 Siyuan Yang,1 Jing Wang,1 Kai Hu,1 Jinlong Shi,3,4 Xiaoyan Ke,1 Lin Fu11Department of Hematology and Lymphoma Research Center, Peking University, Third Hospital, Beijing, People’s Republic of China; 2Department of Otolaryngology, Peking University People’s Hospital, Beijing 100044, People’s Republic of China; 3Department of Biomedical Engineering, Chinese PLA General Hospital, Beijing 100853, People’s Republic of China; 4Department of Medical Big Data, Chinese PLA General Hospital, Beijing 100853, People’s Republic of ChinaBackground: Overexpression of dedicator of cytokinesis 1 (DOCK1) has been confirmed as an unfavorable prognostic marker in acute myeloid leukemia (AML). Purpose: This study is to explore the clinical implications of DOCK1 on AML patients underwent allogeneic hematopoietic stem cell transplantation (allo-HSCT). Patients and methods: We analyzed 71 de novo AML patients treated with allo-HSCT and divided them into two groups (DOCK1high, vs DOCK1low,) by the median expression level of DOCK1. Results: High DOCK1 expression was associated with older age (P=0.019), wild-type CEBPA (P=0.002), IDH1/2 mutations (P=0.010) and RUNX1 mutation (P=0.005). Univariate analyses showed that DOCK1high, and RUNX1 mutation were associated with shorter OS (P

To overcome obstacle of unbalanced hole and electron diffusion behavior in perovskites, a novel type of rationally designed bulk-heterojunction with C60-fullerene electron extraction material coupled with perovskite is for the first time reported. A facile strategy is developed for pyrrole to modify C60 to realize co-soluble of C60 and perovskites, achieving co-deposition of perovskite/pyrrole-fullerene bulk-heterojunction film via a one-step-spin-coating process. The unique perovskite/pyrrole-fullerene bulk-heterojunction exhibits increased mobility, quenched fluorescence intensity, decreased electron lifetime, large recombination resistance and reduced trap density of states, greatly enhancing charge extraction and transfer ability, thus boosting photoelectric conversion efficiency of solar cells. Introducing pyrrole-fullerene can effectively reduce grain boundaries and electron trap density to suppress electron-hole recombination. The enlarged interfacial area between pyrrole-fullerene and perovskite is essential for facilitating extraction of more free electrons from perovskite to fullerene electron acceptor, resulting in a balance of charge extraction and transport. A maximum power conversion efficiency of 18.9% with virtually no hysteresis for the bulk-heterojunction based perovskite solar cells with an optimized concentration of bulk-heterojunction can be obtained. The present strategy for high-performance bulk-heterojunction perovskite solar cells can be potential for industrial photovoltaic applications for its facile and low-cost process route.

The aim of the present study was designed to investigate that Platycodon grandiflorum saponins (PGS) exerted protective effects against testicular injury induced by scrotal hyperthermia. PGS (15, 30 mg/kg) were administered intragastrically to mice for 14 days, then exposed to a single scrotal heat treatment at 43 °C for 18 min on the 7th day. Heat stress (HS) induced spermatogenic damage was associated with a significant loss of leydig cells and the changes of serum testosterone, oxidative stress and apoptosis markers, and activated MAPK signaling pathway. In contrast, PGS treatment normalized HS-induced histopathological changes and prevented the activation of MAPK signaling pathway, which was contributed to oxidative stress and apoptosis in the testis of treated mice. In conclusion, our findings clearly demonstrated that PGS exhibited a significant protective effect against HS-induced testicular dysfunction, largely dependent upon the inhibition of oxidative stress associated apoptosis via partly regulation of MAPK signaling pathway.

A detailed chemical investigation of the Chinese soft coral Lemnalia flava yielded four new nardosinane-type sesquiterpenoids (1–4), one new neolemnane-type sesquiterpenoid (5), and one new sesquiterpenoid with an uncommon 6/9 fused bicyclic skeleton (6), together with two known related compounds (7 and 8). The structures and absolute configurations of 1–8 were determined on the basis of extensive spectroscopic data analyses, X-ray diffraction analysis, chemical reactions, and computer-assisted structural elucidation including 13C NMR data calculation, residual dipolar coupling based NMR analysis, and time-dependent density functional theoryelectronic circular dichroism calculation. Plausible biogenetic pathways of two uncommon sesquiterpenoids (4 and 6) were proposed.

A new 5α,8α-epidioxysterol, namely yalongsterol A (1), along with two known related steroids 5α,8α-epidioxy-24-methyl-cholesta-6,24(28)-dien-3β-ol (2) and (22E,24S)-5α,8α-epidioxy-24-methyl-cholesta-6,22-dien-3β-ol (3), were isolated from the South China Sea soft coral Sinularia sp. Their structures were established by extensive spectroscopic analyses and comparisons of the spectral data with those reported in the literature. In bioassay, compounds 1-3 showed moderate immunosuppressive activities against T and/or B lymphocyte cells with IC50 values ranging from 19.30 to 59.49 μM, and low cytotoxicity on murine splenocytes with CC50 values ranging from 40.88 to 62.29 μM.[Formula: see text].