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Due to the massive discharge of antibiotics in water, it is an urgent matter to remove antibiotics from waste water. The photocatalysts with high stability and activity have attracted extensive attention from researchers. By an in-situ polymerization method, polypyrrole (PPy) was modified on the surface of TiO2 (named as TiO2/PPy). By one-step reduction method, NiCoP was grafted on the surface of TiO2/PPy (named as TiO2/PPy/NiCoP) to synthesize the photocatalyst of TiO2/PPy/NiCoP for degradation of tetracycline (TC) antibiotic. The characterization results revealed that NiCoP was deposited on the surface of TiO2/PPy successfully. The photocatalytic experiment results illustrated that 83.2% of TC could be degraded at natural pH with 20 mg of TiO2/PPy/NiCoP in 50 mL of TC solution (10 mg/L) under visible light irradiation. The high catalytic activity is attributed to the attachment of NiCoP on the surface of TiO2/PPy which can enlarge the light response range of TiO2 effectively. Scavenger studies revealed that the degradation of TC was dominated by •O2− and h+. The photodegradation efficiency of TC with TiO2/PPy/NiCoP still reached over 74% after 5 consecutive cycles, indicating the potential applications in practical wastewater.

Background: Curcumin possesses multiple bioactivities that have beneficial effects on diabetic foot ulcers. Herein, we aimed to conduct a preclinical systematic review of 9 studies, including a total of 262 animals, to assess the possible mechanisms of curcumin for wound healing in diabetic animals. Methods: Five databases were searched from inception to May 12, 2020; Rev-Man 5.3 software was applied for data analyses. Cochrane Collaboration’s tool 10-item checklist was used to evaluate the methodological quality, and data revealed scores of risk of bias ranging from 2 to 5. Results: Meta-analysis indicated that curcumin had significant effects on wound healing rate and blood vessel density when compared with control (P < 0.05). The wound regeneration properties of curcumin for diabetic wounds are thought to mainly work through the possible mechanisms of antioxidation, enhanced cell proliferation, increased collagen formation, and angiogenesis. However, the anti-inflammatory effect on wounds in diabetic animals remain controversial. Conclusions: The findings indicate that more randomized controlled trials should be pursued to obtain more reliable results regarding inflammatory response. Overall, curcumin might be a probable candidate for diabetic foot ulcers and may contribute to future clinical trials. Prospero Registration: CRD42020188981.

To efficiently remove all recurrent lymph nodes (rLNs) and minimize complications, we developed a combination approach that consisted of 68Gallium prostate-specific membrane antigen (PSMA) ligand positron emission tomography (PET)/computed tomography (CT) and integrated indocyanine green (ICG)-guided salvage lymph node dissection (sLND) for rLNs after radical prostatectomy (RP). Nineteen patients were enrolled to receive such treatment. 68Ga-PSMA ligand PET/CT was used to identify rLNs, and 5 mg of ICG was injected into the space between the rectum and bladder before surgery. Fluorescent laparoscopy was used to perform sLND. While extensive LN dissection was performed at level I, another 5 mg of ICG was injected via the intravenous route to intensify the fluorescent signal, and laparoscopy was introduced to intensively target stained LNs along levels I and II, specifically around suspicious LNs, with 68Ga-PSMA ligand PET/CT. Next, both lateral peritonea were exposed longitudinally to facilitate the removal of fluorescently stained LNs at levels III and IV. In total, pathological analysis confirmed that 42 nodes were rLNs. Among 145 positive LNs stained with ICG, 24 suspicious LNs identified with 68Ga-PSMA ligand PET/CT were included. The sensitivity and specificity of 68Ga-PSMA ligand PET/CT for detecting rLNs were 42.9% and 96.6%, respectively. For ICG, the sensitivity was 92.8% and the specificity was 39.1%. At a median follow-up of 15 (interquartile range [IQR]: 6–31) months, 15 patients experienced complete biochemical remission (BR, prostate-specific antigen [PSA] 0.2 ng ml−1. Therefore, 68Ga-PSMA ligand PET/CT integrating ICG-guided sLND provides efficient sLND with few complications for patients with rLNs after RP.

Quorum sensing (QS) plays an essential role in virulence factor production, biofilm formation, and antimicrobial resistance. As a potent QS inhibitor, hordenine can inhibit both QS and biofilm formation in Pseudomonas aeruginosa and Serratia marcescens. In this work, we tested the QS inhibitory potential of 27 hordenine analogs against QS and biofilm formation in P. aeruginosa and S. marcescens. Among the tested analogs, seven (12, 28, 27, 26, 2, 23, and 7) exhibited strong QS inhibitory activity against P. aeruginosa, five of which (12, 28, 27, 26, and 2) showed better inhibitory activity than hordenine. In addition, seven analogs (28, 12, 23, 7, 26, 2, and 27) exhibited better biofilm inhibition against P. aeruginosa than hordenine. Four analogs (7, 28, 2, and 12) showed QS inhibitory activity against S. marcescens, two of which (7 and 28) demonstrated better inhibitory activity than hordenine. Furthermore, analog 7 showed similar biofilm inhibition against S. marcescens as hordenine. Structure-activity relationship (SAR) analysis indicated that the inhibitory activities of the analogs were related to four factors, i.e., carbon chain length, presence or absence of an α,β-C Created by potrace 1.16, written by Peter Selinger 2001-2019 C bond, amino group with/without lipophilic group, such as methyl group, and hydroxyl group in benzene ring.

Ginsenoside compound K (CK) is the major intestinal bacterial metabolite of ginsenosides that exhibits anticancer potential in various cancer cells both in vitro and in vivo. The anticancer types, mechanisms, and effects of CK in the past decade have been summarized in this review. Briefly, CK exerts anticancer effects via multiple molecular mechanisms, including the inhibition of proliferation, invasion, and migration, the induction of apoptosis and autophagy, and anti-angiogenesis. Some signaling pathways play a significant role in related processes, such as PI3K/Akt/mTOR, JNK/MAPK pathway, and reactive oxygen species (ROS). Moreover, the effects of CK combined with nanocarriers for anticancer efficiency are discussed in this review. Furthermore, we aimed to review the research progress of CK against cancer in the past decade, which might provide theoretical support and effective reference for further research on the medicinal value of small molecules, such as CK.

Modified reduced graphene oxide (rtgo) was prepared by using γ - isocyanate propyl triethoxysilane (IPTS) as modifier. Graphene / polyurethane nanocomposites were prepared by in-situ polymerization. Graphene / polyurethane composites were characterized by scanning electron microscopy, TGA, DIN abrasion and electronic universal testing machine. The effects of different reaction formulations and graphene addition on the wear resistance and mechanical properties of the composites were studied. The results show that the wear resistance and tear resistance of the composite can be greatly improved after the functional graphene is compounded with polyurethane.

The Re-Os isotopic system serves as an important tracer of recycled crust in Earth's deep mantle because of the large Re/Os ratios and time-integrated enrichment of radiogenic Os in Earth's crust. However, the Re distribution in Earth's known reservoirs is mass imbalanced, and the behavior of Re during subduction remains little understood. We performed laboratory experiments to determine the partition coefficients of Re between pyrrhotite and silicate melt () at 950–1080°C, 1–3 GPa, and oxygen fugacities (in log units relative to the fayalite-magnetite-quartz [FMQ] buffer) of FMQ–1.3 to FMQ +2. The obtained values are 200–25,000, which increase with decreasing oxygen fugacity and the total iron content (FeOtot) of silicate melt but decrease with increasing temperature or decreasing pressure. Applying to constrain the behavior of Re during slab melting demonstrates that slab melts contribute minimal Re to the sub-arc mantle, with most Re dissolved in sulfides subducted into Earth's deep mantle. Deep storage of recycled oceanic basalts and sediments can explain the mass imbalance of Re in Earth's primitive mantle, depleted mantle, and crust.

This paper investigates the effect of varying solid alkali activators on the fresh and hardened properties and microstructural changes of one-part geopolymers (OPGs). Single and binary solid alkali activators were used to activate high calcium fly ash. The alkali activators were either solely sodium metasilicate (Na2SiO3) or a combination of sodium aluminate (NaAlO2) and sodium metasilicate (Na2SiO3). The OPG activated with anhydrous Na2SiO3 achieved an excellent 28-day compressive strength of 83.6 MPa while OPG activated with NaAlO2 and Na2SiO3 attained a compressive strength of 45.1 MPa. The Na2SiO3-activated OPG demonstrated better fluidity than the OPG activated with NaAlO2 and Na2SiO3 due to the thixotropic behaviour caused by the NaAlO2. The Na2SiO3-activated OPG consisted of sodium-calcium aluminium silicate hydrate ((N,C)-A-S-H) gel phase, while the OPG activated with NaAlO2 and Na2SiO3 comprised of the coexistence of sodium aluminium silicate hydrate (N-A-S-H) and calcium aluminium silicate hydrate (C-A-S-H) gel phases. Regardless of the distinctive properties, the OPGs are adequate for building materials applications.

Background. Colorectal cancer (CRC) is the third most common tumor worldwide. Aberrant N6-methyladenosine (m6A) modification can influence the progress of the CRC. Additionally, long noncoding RNA (lncRNA) plays a critical role in CRC and has a close relationship with m6A modification. However, the prognostic potential of m6A-related lncRNAs in CRC patients still remains to be clarified. Methods. We use “limma” R package, “glmnet” R package, and “survival” R package to screen m6A-related-lncRNAs with prognostic potential. Then, we comprehensively analysed and integrated the related lncRNAs in different TNM stages from TCGA database using the LASSO Cox regression. Meanwhile, the relationship between functional enrichment of m6A-related lncRNAs and immune microenvironment in CRC was also investigated using the TCGA database. A prognostic model was constructed and validated to determine the association between m6A-related lncRNAs in different TNM stages and the prognosis of CRC. Result. We demonstrated that three related m6A lncRNAs in different TNM stages were associated with the prognosis of CRC patients. Patients from the TCGA database were classified into the low-risk and the high-risk groups based on the expression of these lncRNAs. The patients in the low-risk group had longer overall survival than the patients in the high-risk group ( P < 0.001 ). We further constructed and validated a prognostic nomogram based on these genes with a C-index of 0.80. The receiver operating characteristic curves confirmed the predictive capacity of the model. Meanwhile, we also found that the low-risk group has the correlation with the dendritic cell (DC). Finally, we discovered the relationship between the m6A regulators and the three lncRNAs. Conclusion. The prognostic model based on three m6A-related lncRNAs exhibits superior predictive performance, providing a novel prognostic model for the clinical evaluation of CRC patients.

Atherosclerotic cardiovascular disease resulting from dysregulated lipid metabolism is the leading cause of morbidity and mortality worldwide. Apolipoprotein E (ApoE) plays a critical role in cholesterol metabolism. Knockouts in lipid-metabolizing proteins including ApoE in multiple model organisms such as mice and rats exhibiting elevated levels of cholesterol have been widely used for dissecting the pathology of atherosclerosis, but few of these animal models exhibit advanced atherosclerotic plaques leading to ischemia-induced clinical symptoms, limiting their use for translational studies. Here we report hypercholesterolemia and severe atherosclerosis characterized by stenosis and occlusion of arteries, together with clinical manifestations of stroke and gangrene, in ApoE knockout dogs generated by CRISPR/Cas9 and cloned by somatic cell nuclear transfer technologies. Importantly, the hypercholesterolemia and atherosclerotic complications in F0 mutants are recapitulated in their offspring. As the ApoE-associated atherosclerosis and clinical manifestations in mutant dogs are more similar to that in human patients compared with those in other animal models, these mutant dogs will be invaluable in developing and evaluating new therapies, including endovascular procedures, against atherosclerosis and related disorders.

Daphnenoids A-C (1-3), three unusual sesquiterpenes with distinctive ring skeletons, together with a biogenetically related daphnenoid D (4) were obtained from the herb of Daphne penicillata by molecular networking strategies. Daphnenoid A (1) possesses a unique caged tetracyclo [5.3.2.01,6.04,11] dodecane scaffold by unexpected cyclizations of C-1/C-11 and C-2/C-14. Daphnenoids B and C (2 and 3) were the first discovered natural sesquiterpenes with unique 5/5 spirocyclic systems in nature. Their structures were determined by NMR spectroscopic analysis, computer-assisted structure elucidation methods, quantum chemical calculations, and X-ray diffraction. A hypothetical biogenetic pathway begins with typical guaiane sesquiterpene (a), including a key intermediate (4) was proposed. Daphnenoids B and C (2 and 3) exhibited potential inhibitory activities on the production of NO against LPS-induced BV2 microglial cells.

A successive investigation of the endophytic fungus Stagonosporopsis oculihominis isolated from Dendrobium huoshanense led to the discovery of two undescribed secondary metabolites, (±)-stagonosporopsin A and stagonosporopsin B, and a new natural product, stagonosporopsin C. (±)-stagonosporopsin A is a pair of enantiomer. The structures of the isolated compounds, including their absolute configurations, were elucidated based on extensive spectroscopic analyses, electronic circular dichroism (ECD) calculations and X-ray diffraction. Stagonosporopsin C exhibited moderate inhibitory activity against Staphylococcus aureus subsp. aureus ATCC29213 with an MIC50 value of 41.3 μM.

To improve the cracking behavior of hydrocarbon, Ni–Mo/SiO2 bimetallic catalysts were synthesized by different preparation methods (sol-gel, co-impregnation and single-impregnation) and added the additives (citric acid, polyethylene glycol and cetyltrimethylammonium bromide) based on the most suitable method above. The cracking reaction of methylcyclohexane under supercritical conditions was performed as the probe reaction to estimate the catalytic performance, and the properties of Ni–Mo/SiO2 catalyst were characterized by N2 absorption-desorption, XRD, XPS, H2-TPR, NH3-TPD, in-situ IR of NH3 desorption, HRTEM and STEM-mapping so as to study the structure-activity relationship. The catalyst synthesized via sol-gel method showed the best conversion and heat sink, being 81.8% and 3.81 MJ/kg, which was closely related to strong mutual effect between active components and SiO2 as well as strong acid sites. Besides, the introduction of additives by sol-gel method has an affirmative influence on properties of Ni–Mo/SiO2 catalysts, being that the acidity (more L and B acid sites) was modulated and organic groups interact with metal to suppress the aggregation of metal species (Ni and Mo), thereby enhancing the catalytic activity. At 750 °C, the conversion (89.3%) as well as heat sink (3.99 MJ/kg) of MCH cracking obtained an optimum over Ni–Mo/SiO2 catalyst with addition of citric acid.

The quaternary ammonium surfactant-dodecyl benzyl ammonium chloride (DDBAC) was applied to modify Ca-montmorillonite (Ca-Mt) to obtain organo D-Mt that was used as the adsorbent for micropollutants-ampicillin (AMP) and amoxicillin (AMX). The XRD characterization indicated that DDBAC intercalated the interlayer space of Ca-Mt. When the amount of modifier was 1.4 CEC, the basal spacing enlarged from 1.53 nm to 2.97 nm, and the arrangement of modifier molecules were sloped in the interlayer of Ca-Mt along the longest axis. The saturated adsorption capacity of D-Mt-1.4 for AMP and AMX was 30.86 mg/g and 13.29 mg/g, respectively, while the saturated adsorption capacity of Ca-Mt for two contaminants was only 0.36 mg/g and 0.16 mg/g, respectively. The adsorption of the two pollutants was more consistent with Freundlich adsorption isotherm second-order kinetic model, and the thermodynamic study suggested that adsorption was more likely to occur at higher temperatures, which means that the adsorption of two pollutants was a spontaneous endothermic process. Moreover, Multiwfn wavefunction program based on Density Functional Theory (DFT) was applied to reveal the microadsorption mechanism of D-Mt to two pollutant molecules. This work confirmed that Ca-Mt functionalized by DDBAC was promising adsorbents for micro-contaminants of antibiotics and the insight of the adsorption mechanism from the atomic level, providing theoretical guidance for architecting high performance adsorbent.

Salinity tolerance of ambient electric arc ionization (AEAI) was evaluated by comparing electrospray ionization for various samples at NaCl concentrations from 0 to 1000 mmol/L. AEAI-mass spectrometry (AEAI-MS) exhibited an excellent signal intensity even at NaCl concentrations of 1000 mmol/L, while the ESI-MS had no signal because high salinity has a strong inhibitory effect on analytes. The sodium adduct was verified using LiCl instead of NaCl. AEAI-MS successfully quantified saline samples with an excellent quantitative ability (R2 ≥ 0.998). We also achieved some analytical samples in the buffer solution at a very high concentration and even in a saturated salt solution. Overall, AEAI-MS has protonated ions for most target analytes. In addition, the relationship between auxiliary temperature and the distance from the sample to the arc was investigated, and the results indicated that thermal desorption plays an important role in AEAI source.

The hydroperoxy alkyl radicals are important intermediates in the low-temperature combustion for normal-alkyl cycloalkanes, and the cyclization reactions of hydroperoxy alkyl radicals to form cyclic ethers are responsible for a major fraction of the OH formation, which has the potential to promote ignition. In most of the previous modeling studies for normal-alkyl cycloalkane combustion, the kinetic data of the cyclization reactions in the detailed combustion mechanism were mainly taken from the analogous reactions in cyclohexane, methyl cyclohexane, and alkanes in published literature studies. In this work, the kinetics of the cyclization reaction class of hydroperoxy alkyl radicals in normal-alkyl cycloalkanes is studied, where the reaction class is divided into subclasses depending upon the ring size of the transition states, the types of the carbons on which the -OOH site is located and the types of the carbons on which the radical site is located, and the positions of the cyclization (on the alkyl side chain, on the cycle, or between the alkyl side chain and the cycle). Energy barriers and high-pressure-limit site rate constants and pressure-dependent rates for reactions in all subclasses are calculated, and rate rules for all subclasses are developed. The high-pressure-limit rate constants are determined from CBS-QB3 electronic structure calculations combined with canonical transition-state theory calculations, and pressure-dependent rate constants are calculated by using the Rice-Ramsberger-Kassel-Marcus/Master Equation theory at pressures varying from 0.01 to 100 atm. Comparisons of the rate constants for cyclization reactions of hydroperoxy alkyl cyclohexylperoxy radicals calculated in this work with the values of the corresponding reactions in some of the popular combustion mechanisms show that it is unreasonable to use the kinetic data of analogous reactions in alkanes, cyclohexanes, or smaller normal-alkyl cyclohexanes. Therefore, the accurate kinetic calculations and the construction of rate rules for normal-alkyl cycloalkanes are necessary and significant for the reliable modeling of the low-temperature combustion of normal-alkyl cyclohexanes.

BACKGROUND Ginger (Zingiber officinale Roscoe) is widely planted around the world. Owing to continuous planting, ginger is seriously affected by soilborne fungi, bacteria, and nematodes. Although preplant soil fumigation is an effective prevention strategy of soilborne diseases, individual fumigant and technology could not provide effective control of ginger soilborne disease. In our research, different combinations of soil fumigants and seed rhizome treatments were evaluated by monitoring the soil pathogens population, ginger growth, yield, and estimation of economic benefits. RESULTS Soil fumigation effectively reduced the population of soilborne pathogens, and chloropicrin had a better control effect on soilborne pathogens than dazomet did. Preplant soil fumigation and seed rhizome treatment not only provide good control of soilborne disease, but also reduced the incidence of plant foliar pest and disease. Average yield increase rate of seed rhizome treatment was 12.0%; the highest yield increase was 24.4%. The average cost of seed rhizome treatment only increased by about 2.86%, but the rate of net revenue increase for the seed rhizome treatment reached up to 19.1%. CONCLUSION Seed rhizome treatment is a very cost-effective soilborne disease control technology. In the management of soilborne diseases, the combined application of soil fumigation and seed rhizome treatment can reduce the risk of crops infected by soilborne diseases and ensure high and stable crop yields. © 2021 Society of Chemical Industry.

A facile and versatile method for generating radicals from Csp3-H bonds under metal-free and organic-peroxide-free conditions was developed. By combining safe persulfate and low-toxic quaternary ammonium salt, a wide variety of Csp3-H compounds including ethers, (hetero)aromatic/aliphatic ketones, alkylbenzenes, alkylheterocycles, cycloalkanes, and haloalkanes were selectively activated to generate the corresponding C-centered radicals, which could be further captured by N-arylacrylamides to deliver the valuable functionalized oxindoles. Good functional group tolerance was demonstrated. The useful polycarbonyl compound and esters were also modified with the strategy. Moreover, the combination can also be applied to the practical coupling between simple haloalkanes and N-hydroxyphthalimide (NHPI).

The reactions of the concerted HO2 elimination from alkyl peroxy radicals and the β-scission of the C-OOH bond from hydroperoxy alkyl radicals, which lead to the formation of olefins and HO2 radicals, are two important reaction classes that compete with the second O2 addition step of hydroperoxy alkyl radicals, which are responsible for the chain branching in the low-temperature oxidation of normal alkyl cycloalkanes. These two reaction classes are also believed to be responsible for the negative temperature coefficient behavior due to the formation of the relatively unreactive HO2 radical, which has the potential to inhibit ignition of normal alkyl cycloalkanes. In this work, the kinetics of the above two reaction classes in normal alkyl cycloalkanes are studied, where reactions in the concerted elimination class are divided into subclasses depending upon the types of carbons from which the H atom is eliminated and the positions of the reaction center (on the alkyl side chain or on the cycle), and the reactions in the β-scission reaction class are divided into subclasses depending upon the types of the carbons on which the radical is located and the positions of the reaction center. Energy barriers by using quantum chemical methods at the CBS-QB3 level, high-pressure-limit rate constants by using canonical transition state theory, and pressure-dependent rate constants at pressures from 0.01 to 100 atm by using Rice-Ramsberger-Kassel-Marcus/Master Equation theory are calculated for a representative set of reactions from methyl cyclohexane to n-butyl cyclohexane in each subclass, from which high-pressure-limit rate rules and pressure-dependent rate rules for each subclass are derived from the average rate constants of reactions within each subclass. A comparison of the rate constants for the reactions in the two reaction classes calculated in this work is made with the rate constants of the same reactions from available mechanisms published in the literature, where most of the rate constants are approximately estimated from analogous reactions in alkanes or small alkyl cyclohexanes, and it is found that a large difference may exist between them, indicating that the present work, which provides more accurate kinetic parameters and reasonable rate rules for these reaction classes, can be helpful to construct higher-accuracy mechanism models for normal alkyl cyclohexane combustion.

Background Soil fumigants-the most effective agrochemicals for managing soil-borne diseases-have been extensively used. However, high volatility, moderate toxicity, and insufficient effective duration considerably limit their application. In the present study, a combination of modified biochar and polyurea microcapsules (MCs) via interface polymerization to co-encapsulate allyl isothiocyanate (AITC) was developed as a model fumigant for controlled release (AITC@BC-MCs). Results The physical characteristics of biochar modified by sand milling were significantly improved. In addition, chemical properties and morphological features of AITC@BC-MCs characterized by integrated methods revealed successful preparation of BC-MCs. Compared with monolayer MCs, BC-MCs could significantly delay AITC release due to the composite obstruction effect. Moreover, modified biochar endowed the cargo molecules with a pH-responsive release property. Additionally, this composite showed a longer persistent duration by prolonging AITC degradation half-life, which was 3.2-3.5 times that of the AITC technical concentrate under different soil conditions. Finally, the control efficacy of AITC@BC-MC against pathogens, including nematodes and fungi, as well as against weeds was significantly enhanced at the same dose, but it did not inhibit seed germination and growth after 10 days when fumigated soil was aerated. Conclusion Construction of a composite encapsulation system enhanced pesticide efficacy, reduced dose via controlled release, and delayed fumigant degradation in soil, indicating the great potential of this strategy for developing an effective and environmentally friendly fumigant formulation. This article is protected by copyright. All rights reserved.

As a secondary Li-ion battery with high energy density, lithium-sulfur (Li-S) batteries possess high potential development prospects. One of the important ingredients to improve the safety and energy density in Li-S batteries is the solid-state electrolyte. However, the poor ionic conductivity largely limits its application for the commercial market. At present, the gel electrolyte prepared by combining the electrolyte or ionic liquid with the all-solid electrolyte is an effective method to solve the low ion conductivity of the solid electrolyte. We present a cross-linked gel polymer electrolyte with fluoroethylene carbonate (FEC) as a solid electrolyte interface (SEI) film formed for Li-S quasi-solid-state batteries, which can be simply synthesized without initiators. This gel polymer electrolyte with FEC as an additive (GPE@FEC) possesses high ionic conductivity (0.830 × 10-3 S/cm at 25 °C and 1.577 × 10-3 S/cm at 85 °C) and extremely high Li-ion transference number (tLi+ = 0.674). In addition, the strong ability toward anchoring polysulfides resulting in the high electrochemical performance of Li-S batteries was confirmed in GPE@FEC by the diffusion experiment, X-ray photoelectron spectroscopy analysis (XPS), and scanning electron microscopy (SEM) mapping of the S element. Such a high ion conductivity (IC) gel polymer electrolyte enables a competitive specific capacity of 940 mAh/g at 0.2C and supreme cycling performance for 180 cycles at 0.5C, which is far beyond that of conventional poly(ethylene oxide)-based quasi-solid-state Li-S batteries.

Daoming Zhang,1 Yuan Li,1 Haoyue Li,2 Tian Tang,1 Yongfa Zheng,1 Xufeng Guo,1 Ximing Xu1 1Cancer Center, Renmin Hospital of Wuhan University, Wuhan, People’s Republic of China; 2Department of Cardiology, Renmin Hospital of Wuhan University, Wuhan, People’s Republic of ChinaCorrespondence: Ximing XuCancer Center, Renmin Hospital of Wuhan University, 238 Jiefang Road, Wuhan, 430060, People’s Republic of ChinaTel +86-13707120651Email doctorxu120@aliyun.comObjective: To evaluate the value of serum complement component 1q (C1q) levels in predicting the efficacy of combined immunotherapy in patients with lung cancer.Methods: A total of 42 patients with lung cancer who received combined immunotherapy in the cancer center of Renmin Hospital of Wuhan University were included in this study. The clinical data of serum C1q and lactate dehydrogenase (LDH) levels before and three weeks after immunotherapy were collected.Results: Response evaluation showed that the number of patients with complete response (CR), partial response (PR), stable disease (SD), and progressive disease (PD) was 0 (0%), 26 (61.9%), 14 (33.3%), and 2 (4.8%), respectively. The CR/PR group (patients with CR or PR) showed higher pC1q (C1q level before immunotherapy) and iC1q (C1q level 3 weeks after immunotherapy) than the SD/PD group (patients with SD or PD). The LDH reduction (96.2%) and C1q increment (84.6%) in the CR/PR group 3 weeks after immunotherapy were higher than those of the SD/PD group, and the differences were statistically significant. Logistic regression analysis indicated that pC1q, iC1q, and LDH level trends 3 weeks after the treatment were significantly correlated to the efficacy of combined immunotherapy with odds ratios of 8.185, 5.500, and 0.031, respectively.Conclusion: High C1q levels before immunotherapy and increased C1q levels and decreased LDH levels 3 weeks afterward suggest good therapeutic effects of combined immunotherapy in patients with lung cancer. Serum C1q levels have certain clinical significance in predicting the efficacy of combined immunotherapy.Keywords: immunotherapy, efficacy prediction, complement component 1q

Topological morphology that dominates the surface electronic properties of nanostructures plays a key role in producing desired materials for versatile functions and applications in many fields, but its modulation for specific functions remains a big challenge. Herein, we report an acid-induced method to prepare S-doped graphitic carbon nitride/graphitic carbon nitride (S-CN/CN) homojunction by simply pyrolyzing a supramolecular precursor synthesized from melamine and H2SO4. The topological morphology and electronic structure of CN homojunction can be easily adjusted only by changing the ratio of raw materials. Moreover, the topological morphology of S-CN/CN homojunction can be further adjusted from hollow cocoon to 2D nanosheets by changing the annealing conditions. The optimized S-CN/CN homojunction shows highly efficient in charge transfer and separation and exhibits superior OER activity and high ability to degrade organic pollutants. Impressively, S-CN/CN nanosheets only demand low overpotential of 301 mV to drive a current density of 10 mAcm−2 in 1 M KOH media, and the corresponding Tafel slope is only 57.71 mV/dec, which is superior to the most advanced precious metal IrO2 catalyst. Moreover, under visible light irradiation, its photodegradation kinetic rate of RhB is 2.38, which is 47.6 times higher than that of bulk CN. This work provides useful guidance for designing and developing efficient multifunctional metal-free catalysts.

This study aimed to investigate the therapeutic potential of human umbilical cord mesenchymal stem cells derived exosomes (hUCMSC-Exo) in acute liver failure (ALF) in mice as well as its underlying mechanism. We found that a single tail vein administration of hucMSC-Exo effectively enhanced the survival rate, inhibited apoptosis in hepatocytes, and improved liver function in APAP-induced mouse model of ALF. Furthermore, the deletion of glutathione (GSH) and superoxide dismutase (SOD), generation of malondialdehyde (MDA), and the over production of cytochrome P450 E1 (CYP2E1) and 4-hydroxynonenal (4-HNE) caused by APAP were also inhibited by hucMSC-Exo, indicating that hucMSC-Exo inhibited APAP-induced apoptosis of hepatocytes by reducing oxidative stress. Moreover, hucMSC-Exo significantly down-regulated the levels of inflammatory cytokines IL-6, IL-1β, and TNF-α in APAP-treated livers. Western blot showed that hucMSC-Exo significantly promoted the activation of ERK1/2 and IGF-1R/PI3K/AKT signaling pathways in APAP-injured LO2 cells, resulting in the inhibition of apoptosis of LO2 cells. Importantly, PI3K inhibitor LY294002 and ERK1/2 inhibitor PD98059 could reverse the function of hucMSC-Exo on APAP-injured LO2 cells in some extent. Our results suggest that hucMSC-Exo offer antioxidant hepatoprotection against APAP in vitro and in vivo by inhibitiing oxidative stress-induced apoptosis via upregulation of ERK1/2 and PI3K/AKT signaling pathways.

A binucleating Schiff base ligand 2-methoxy-6-(iminomethyl)phenol (HL) and two new M(II) complexes [Zn4L4(N3)4](H2O)2 (1) and [Co4L4Cl4] (2) are synthesized. These metal complexes are characterized using various physicochemical techniques, e.g. elemental analyses and single crystal X-ray diffraction. Furthermore, both CCK-8 assay and cell colony formation results indicate that the inhibitory activity of compound 1 against Y79 retinoblastoma cancer cells is stronger than that of compound 2. In addition to this, we also reveal that compound 1 can significantly increase the ROS accumulation in Y79 retinoblastoma cancer cells, which is higher than that in the group treated with compound 2. All the results above suggest a stronger anticancer activity of compound 1 compared to compound 2 and that it has the potential of being a novel candidate for retinoblastoma cancer treatment.

The concise synthesis of dysifragilones A and B and dysidavarones has been accomplished for the first time in a divergent way from a common intermediate. The synthetic route features an intramolecular reductive Heck reaction to construct the 6/5/6/6/-tetracycle of dysifragilones A and B and an intramolecular palladium-catalyzed α-arylation of a sterically hindered ketone to forge the tetracyclo[7.7.1.02,7.010,15]heptadecane core structure of dysidavarone C. The late-stage introduction of amino and ethoxy groups is effective.

A released exopolysaccharide (rEPS)-producing strain (LM187) with good acid resistance, bile salt resistance, and cholesterol-lowering properties was isolated from Sichuan paocai and identified as Leuconostoc mesenteroides subsp. mesenteroides. The purified rEPS, designated as rEPS414, had a uniform molecular weight of 7.757 × 105 Da. Analysis of the monosaccharide composition revealed that the molecule was mainly composed of glucose. The Fourier transform-infrared spectrum showed that rEPS414 contained both α-type and β-type glycosidic bonds. 1H and 13C nuclear magnetic resonance spectra analysis showed that the purified rEPS contained arabinose, galactose, and rhamnose, but less uronic acid. Scanning electron microscopy demonstrated that the exopolysaccharide displayed a large number of scattered, fluffy, porous cellular network flake structures. In addition, rEPS414 exhibited strong in vitro antioxidant activity. These results showed that strain LM187 and its rEPS are promising probiotics with broad prospects in industry.

In this work, CO2 effervescence–assisted emulsification microextraction method using an efficient switchable solvent was proposed for the enrichment of azaperone and azaperol in swine adipose samples. The azaperone and azaperol in swine adipose were extracted by 1% (v/v) ammoniated acetonitrile at 55 °C. A medium-chain fatty acid as switchable-hydrophilicity solvent is used for further enrichment and purification, and it is able to be easily switched into hydrophobic/hydrophilic forms in pH changeable media. The main parameters were optimized as follows: 100 mg octanoic acid, 0.3 mL acetic acid–water solution (1:1, v/v), and 0.5 mL 3.0 mol L−1 Na2CO3 solution. Under the optimal conditions, azaperone and azaperol showed good linearity within the studied range, and the values of the correlation coefficient were higher than 0.999. The limits of detection for the method ranged from 5 to 10.0 ng kg−1. The recoveries of azaperone and azaperol in swine adipose were 95–104%, with relative standard deviations ranging from 3 to 5%. The proposed method was successfully applied for the analysis of azaperone and azaperol in swine adipose samples.

NOx- reduction acts a pivotal part in sustaining globally balanced nitrogen cycle and restoring ecological environment, ammonia (NH3) is an excellent energy carrier and the most valuable product among all the products of NOx- reduction reaction, the selectivity of which is far from satisfaction due to the intrinsic complexity of multiple-electron NOx--to-NH3 process. Here, we utilize the Schottky barrier-induced surface electric field, by the construction of high density of electron-deficient Ni nanoparticles inside nitrogen-rich carbons, to facilitate the enrichment and fixation of all NO x - anions on the electrode surface, including NO 3 - and NO 2 - , and thus ensure the final selectivity to NH 3 . Both theoretical and experimental results demonstrate that NO x - anions were continuously captured by the electrode with largely enhanced surface electric field, providing excellent Faradaic efficiency of 99 % from both electrocatalytic NO 3 - and NO 2 - reduction. Remarkably, the NH 3 yield rate could reach the maximum of 25.1 mg h -1 cm -2 in electrocatalytic NO 2 - reduction reaction, outperforming the maximum in the literature by a factor of 6.3 in neutral solution. With the universality of our electrocatalyst, all sorts of available electrolytes containing NO x - pollutants, including seawater or waste water, could be directly used for ammonia production in potential through sustainable electrochemical technology.

Although some regulatory agencies have claimed that consumer exposures to tetrabromobisphenol A (TBBPA) are not likely to cause adverse health effects in humans or the environment, the safety of tetrabromobisphenol A (TBBPA) has been questioned. Here, we summarize the literature concerning in vivo and in vitro neurotoxicity of TBBPA over the past decades. Most laboratory rodent studies reported that gavage administration of TBBPA at doses below 1000 mg/kg/day generally exerted no or limited effects on neuropathology and locomotor behaviors, but increased anxiety and auditory impairments were observed in several studies. In fish and amphibians, waterborne exposure to TBBPA was generally reported to disrupt neurodevelopment and lead to neurobehavioral alterations. Moreover, in vitro studies support the observations that TBBPA could exert neurotoxic effects in vertebrates. Thus, we suggest that TBBPA could have adverse effects on the nervous system in vertebrates. Given rapid excretion and low availability of TBBPA in laboratory rodents following single gavage administration, we speculate that single-daily gavage could result in an underestimation of the neurotoxic effects of TBBPA in rodents. Thus, we propose to employ multiple-daily administration routes (such as dermal, inhalation, and drinking water), to further assess the neurotoxic effects of TBBPA in mammals.

The overuse of synthetic colorants may result in hepatocellular damage, renal failure, and potential immunotoxicity. Therefore, the content of synthetic colorants in foods must be strictly controlled. A simple sensor based on 1-butylpyridinium hexafluorophosphate@glassy carbon microspheres composites electrode (GCILE) was constructed for the rapid and sensitive detection of sunset yellow (SY) and tartrazine (TZ). Composite materials were investigated using scanning electron microscopy and Fourier transform infrared spectroscopy. Then the electrochemical properties of the sensors were characterized using cyclic voltammetry. Furthermore, the electrochemical behaviors of SY and TZ were studied at the GCILE using differential pulse voltammetry. The effects of pH value, the different ratios of glassy carbon microspheres and ionic liquid, accumulation time, and accumulation potential on current responses of SY and TZ were discussed in detail. The GCILE displayed favorable electrocatalytic activity to SY and TZ. Under the optimum experimental conditions, the linear ranges of SY and TZ were 0.02–5 μM and 0.5–15 μM, respectively. When the noise–signal ratio (S/N) was 3, the detection limits of SY and TZ were 0.01 and 0.1 μM, respectively. Interference studies showed that common interfering substances did not affect the detection of SY and TZ. The proposed method was applied for analyzing azo dyes in beverages.

Magmatic sulfur plays an important role in affecting mantle oxidation state, volcanic eruption, formation of ore deposits, and global climate change. To better understand the sulfur cycle in subduction zones and to constrain the sulfur concentration at anhydrite saturation (SCAS) in subducting slab-derived silicate melts, forty-three experiments were conducted at 0.5–5 GPa and 900–1200 °C using a piston cylinder and a multi-anvil apparatus. The experimentally produced silicate melts are rhyodacitic to rhyolitic in composition, and the measured SCAS values range from 170 to 3500 ppm. The SCAS values increase with increasing temperature and the water and CaO content of the silicate melts, but the effect of pressure varying from 0.5 to 5 GPa is negligible. Using our new and all available literature SCAS data (n = 252), we tested the accuracy of all previous SCAS models that were calibrated for predicting SCAS in silicate melts at various conditions. We find that the Z–T model ( Zajacz and Tsay, 2019 ) works as the greatest SCAS model in capturing all SCAS data with a mean and median absolute error of 5% and 4%, respectively. The success of the Z–T model in capturing all SCAS data demonstrates its robustness in predicting SCAS in silicate melts relevant for magmatism in subduction zones. Applying the Z–T model to slab melting reveals that slab-derived silicate melts of global subduction zones can dissolve 130–1200 ppm S6+, but they cannot contribute enough sulfur to explain the estimated sulfur abundance (200–500 ppm) in the metasomatized sub-arc mantle, which thus requires the addition of sulfur by slab-derived aqueous fluids. The addition of slab S6+ can cause oxidation of the sub-arc mantle in an fO2 range of FMQ+0.5 to FMQ+2, consistent with the fO2 values observed for the metasomatized sub-arc mantle peridotites. However, during partial melting of the metasomatized sub-arc mantle, S2− would play as a reducer and the fO2 of primitive arc basalts cannot be higher than FMQ+0.5 to FMQ+1, which is consistent with the sub-arc mantle fO2 inferred from the V–Sc, Fe–Zn, V–Ga, and Cu–Re systematics of primitive arc basalts. The fO2 above FMQ+1 of arc basalts may thus be obtained during magmatic differentiation in the lithosphere. We finally modeled the fate of S6+ during the differentiation of parental arc basalts with fO2 varying from FMQ+0.5 to FMQ+1.5 in a thickened continental arc setting. We find that significant fractions of S6+ in the parental arc basalts are converted into S2− and lost in sulfides during arc magmatic differentiation, and the estimated 400 ppm sulfur in Earth’s continental crust implies that Earth’s continental crust cannot have formed from arc basalts with fO2 significantly higher than FMQ+0.5 to FMQ+1.

This article presents the experimental characterization of SiC MOSFETs exposed to heavy-ion irradiation. Different leakage paths related to the drain bias used during the tests are observed, suggesting different damage sites in the devices, which can be further verified through the post-irradiation measurements. TCAD simulations are utilized to explore the underlying failure mechanisms. Based on the evolution of the gate oxide field, it is shown that the damage first occurs in the middle of the JFET region, while gradually spreads to the channel region with the increase of drain bias, but terminates at the source region. A preliminary model to roughly emulate the drain bias dependence of such degradation behaviors is developed, and the simulation results match the experiments well. Additionally, the emission microscope (EMMI) is carried out so as to detect the latent damage at the die level. The findings in this article demonstrate that more attention should be paid to the damaged gate oxide induced by the heavy-ion strike before SiC MOSFETs could act as a drop-in replacement of Si-based counterparts in avionic applications.

The colonization of bacterial communities and biofilm formation on microplastics (MPs) have aroused great concern recently. However, the influence of time and polymer types on the structural and functional characteristics of biofilms remains unclear. In this study, three types of MPs (polyethylene, polypropylene, and polystyrene) were exposed for different time periods (10, 20 and 30 days) in seawater using a microcosm experiment. Microscopic spectroscopy and high-throughput gene sequencing techniques were used to reveal the temporal changes of structural and functional characteristics of MPs associated biofilms. The results indicate that the biofilm formation is affected by both the incubation time and the polymer type. In addition, bacterial diversity and community structure in the biofilms show selectivity towards seawater, and tend to shift over time and among different polymer types. Moreover, biofilms are shown to harbor plastic degrading bacteria, leading to the changes of functional groups and surface hydrophobicity, and thereby enhancing the biodegradation of MPs.

Global warming is increasing the frequency and duration of heat waves, which is defined as when air temperature exceeds a threshold for more than specific consecutive days. Ecosystem around the globe will be impaired by heat waves just like the exposures to dangerously high temperatures as a public health threat to human. However, the knowledge of the response of lake and reservoir ecosystem to heat waves is largely unknown although it has been argued that climate warming may increase the incidence of harmful algal blooms. We examined the long-term trend of heat waves and how the variability of phytoplankton biomass responds to lake heat waves on a deep reservoir (Lake Qiandaohu). Long-term (1980-2020) meteorological observation in the lake watershed showed a significant warming trend of 0.36 °C per decade for the yearly average of daily average air temperature and the yearly average of daily maximum air temperature of 18.32 °C was observed in 2016. Meanwhile, a significant increasing number of heat wave events lasting longer was observed, and Lake Qiandaohu suffered an unusually severe lake heat wave in summer 2016. Significant correlations were found between the yearly average of daily maximum air temperature and heat days, heat wave events, and heat wave days. Nuisance phytoplankton bloom was found in Lake Qiandaohu by high frequency observation and remote sensing monitoring in summer 2016. Remote sensing estimation from two Landsat 8 Operational Land Imager (OLI) images showed that the average chlorophyll a (Chla) was 7.45 ± 4.89 μg/L on July 18 before heat wave and 18.96 ± 0.98 μg/L on August 19 during the heat wave. Two heat wave events lasting from July 20 to August 2 and August 11 to 26 with average surface water temperature of 29.93 and 31.99 °C promoted two marked phytoplankton blooms with average Chla concentrations of 11.75 ± 4.08 and 10.53 ± 1.65 μg/L in the central lake region, respectively, as evidenced by high-frequency buoy data. These findings suggest that heat waves are likely to yield an increased threat of harmful algal bloom in freshwater ecosystems. With lake heat waves projected to increase in frequency, duration, and spatial extent with global climate change, more studies are needed to improve our understanding of lake heat waves and their potential effects on the species, communities, frequency of phytoplankton bloom, and also help providing advanced schemes of water quality management.

Herein, we report facile synthesis and multiple inherent properties of low-bandgap mesoporous C 4 N particles and showcase its previously-unexplored use as universal responsive bifunctional oxygen catalysts for constructing visible-light-sensitive (VLS) rechargeable Zn-air battery (RZAB) and polymer-air battery (RPAB) towards solar energy conversion/storage. Compared to widely-studied g-C 3 N 4 , as-obtained C 4 N shows a smaller bandgap of 1.99 eV with larger photocurrent response and can function simultaneously as visible-light-harvesting antenna and bifunctional oxygen reduction/evolution (ORR/OER) catalyst, enabling effective photo-coupling to tune oxygen catalysis. In addition to good energy storage performance, the C 4 N-enabled VLS-RZAB displays a low charge voltage of 1.35 V under visible light - below the theoretical RZAB voltage of 1.65 V, corresponding to a high energy efficiency of 97.78 %. Pairing C 4 N cathode with polymer anode also endows an entirely-new all-polymer VLS-RPAB with light-boosted charge performance, implying the generality of our strategy. Combined theoretical and experimental studies unveil that the ORR and OER active sites in C 4 N are separate carbon sites near pyrazine-nitrogen atoms and photo-generated energetic holes can activate OER for improved reaction kinetics. This study not only highlights a rarely-explored carbon nitride polymer and its new property and application but also opens new opportunities to develop organic semiconductors for photo-coupled rechargeable batteries towards solar energy utilization.

α-Site alcohol radicals are the most important products of H-abstract reactions from alcohols since the hydroxyl moiety weakens the α-site C-H bond. Reactions between α-site alcohol radicals and O2 play an important role in combustion of alcohols, especially at relatively low temperatures. However, reliable reaction pathways and rate constants for these reactions are still lacking. Theoretical studies on reactions in α-hydroxyethyl radical (CH3C•HOH) + O2 and α-hydroxypropyl radical (C2H5C•HOH and CH3C•OHCH3) + O2 reaction systems are performed in this work. Pressure-dependent rate constants for the involved reactions in a wide range of temperatures are determined using the Rice-Ramsperger-Kassel-Marcus/master equation (RRKM/ME) method. Our results show that rate constants for reactions in the α-hydroxypropyl radical + O2 system are quite different from those in the CH3C•HOH + O2 system. Detailed reaction pathways for these reaction systems are clarified, although combustion characteristics of ethanol and propanol do not change much with the obtained rate constants for these reactions. Important reaction channels in producing enols, especially in the combustion of propanol, are also provided. The obtained rate constants for these reactions over a wide range of temperatures and pressures are helpful in developing combustion mechanisms for ethanol and propanol.

We have investigated computationally the effect of π-conjugated extension on the charge transfer properties of triphenylene and coronene; where we have added fused benzene or triazole rings in the ...

Iron and oxalic acids are widely distributed in the atmosphere and easily form ferric oxalate complex (Fe(III)-Ox). The tropospheric aqueous-phase could provide a medium to enable the photo-Fenton reaction with Fe(III)-Ox under solar irradiation. Although the photolysis mechanisms of Fe(III)-Ox have been investigated extensively, information about the oxidation of volatile organic compounds (VOC), specifically the potential for Secondary Organic Aerosol (SOA) formation in the Fe(III)-Ox system, is lacking. In this study, a ubiquitous VOC methacrolein (MACR) is chosen as a model VOC, and the oxidation of MACR with Fe(III)-Ox is investigated under typical atmospheric water conditions. The effects of oxalate concentration, Fe(III) concentration, MACR concentration, and pH on the oxidation of MACR are studied in detail. Results show that the oxidation rate of MACR greatly accelerates in the presence of oxalate when compared with only Fe(III). The oxidation rate of MACR also accelerates with increasing concentration of oxalate. The effect of Fe(III) is found to be more complicated. The oxidation rate of MACR first increases and then decreases with increasing Fe(III) concentration. The oxidation rate of MACR increases monotonically with decreasing pH in the common atmospheric water pH range or with decreasing MACR concentration. The production of ferrous and hydrogen peroxide, pH, and aqueous absorbance are monitored throughout the reaction process. The quenching experiments verify that ·OH and \begin{document}$\rm{O}_{\small 2}^{\overline {\,\cdot\,}} $\end{document} are both responsible for the oxidation of MACR. MACR is found to rapidly oxidize into small organic acids with higher boiling points and oligomers with higher molecular weight, which contributes to the yield of SOA. These results suggest that Fe(III)-Ox plays an important role in atmospheric oxidation.

Despite significant medical advances, congestive heart failure remains associated with high mortality rate. Therefore, there is a continuing need for better therapeutics. In this study, we have examined the effect of daidzein against congestive heart failure induced by administration of doxorubicin. Blood pressure, electrocardiogram, B-type natriuretic peptide, and markers of oxidative stress were assessed as measures of cardioprotective effect of daidzein. To further assess the mechanism, terminal deoxynucleotidyl transferase-mediated dUTP nick-end labeling assay, Western blot assay, and histopathology were performed. Daidzein reduced blood pressure, reversed the altered pattern of electrocardiogram, levels of B-type natriuretic peptide, and oxidative stress markers in doxorubicin-induced cardiotoxicity in rats. Furthermore, treatment with daidzein ameliorated apoptosis and expression of proinflammatory proteins and oxidative pathway.

Perovskite solar cells exhibit great potential to become commercial photovoltaic technology due to their high power conversion efficiency, low cost, solution processability, and facile large-area device manufacture. Interface engineering plays a significant role to optimize device performance. For the anode in the inverted devices, this review introduces the progress on the modification of poly(3,4-ethylenedioxythiophene): poly(styrene sulfonate) including chemical structure alteration, physical doping, and solution treatment. We present the recent advances of dopant-free hole transport materials widely applied in mesoporous and conventional devices, outlining their innovation with novel molecular design concepts toward promising material properties, and device performance. For the cathode, various metal oxide and organic electron transport materials are covered and the different modification strategies and related mechanisms are highlighted. Most importantly, simple synthesis process, inexpensive raw materials and highly reproducible photovoltaic performance are the main consideration for the design of all the interface materials. Finally, an outlook and some suggestions regarding the future interface engineering are proposed based on the summary of the current development status and working mechanism of interface materials.

A novel catalyst with a yolk-shell structure was designed to overcome the leaching of noble metals in heterogeneous catalysis. Through a template method, palladium (Pd) nanoparticles were encapsulated by hollow spherical covalent organic frameworks (COFs) consisting of 2,4,6-trihydroxybenzene-1,3,5-tricarbaldehyde (Tp) and p-phenylenediamine (Pa). The final catalyst with a yolk-shell structure was denoted as (Pd/C)@TpPa COFs. The unique morphology and chemical structure of this novel composite (Pd/C)@TpPa COFs were confirmed by a transmission electron microscope (TEM), a laser particle analyzer, X-ray diffraction (XRD), and N2 adsorption and desorption. Subsequently, to demonstrate its catalytic performance brought by structural design, this novel catalyst was applied to catalyze the Suzuki reaction. Interestingly, this catalyst exhibited a brilliant size cutoff efficiency for aryl benzene amounting to 100% and achieved a high conversion with only 0.05 mol% Pd loading. Besides, this catalyst could be readily recovered via filtration and reused for at least five consecutive cycles without any significant loss in its activity.

To constrain the behavior of chalcophile (sulfide-loving) elements during arc magmatic differentiation and to understand the formation conditions of Earth’s continental crust, the partition coefficients (D) of Mn, Co, Cu, Zn, As, Se, Mo, Ag, Cd, Sn, Sb, Te, Re, Au, Pb, and Bi between monosulfide-solid-solution (MSS), Cu-rich sulfide liquid (SL; containing 11–45 wt.% Cu), and hydrous silicate melt (SM) of basaltic to dacitic compositions were determined at 1000–1200 °C, 0.5–1.0 GPa, and fO2 1–1.5 log units above the fayalite–magnetite–quartz (FMQ) buffer. The D SL / S M values are 16–160 for Co, 1100–8400 for Cu, 50–220 for Se, 1200–5900 for Ag, 50–1800 for Cd, 700–3300 for Te, 15–510 for Re, 5700–90,000 for Au, 20–440 for Pb, and 140–3300 for Bi. The D SL / S M values for Mn, Zn, As, Mo, Sn, and Sb are below 1–40. The D MSS / S M values are 55–260 for Co, 530–1700 for Cu, 74–110 for Se, 30–110 for Ag, 4–40 for Cd, 15–70 for Te, 200–5900 for Re, and 140–270 for Au. The D MSS / S M values for Mn, Zn, As, Mo, Sn, Sb, Pb, and Bi are below 1–3. The D SL / S M of Au increase with increasing Cu content of the sulfide liquid, but the D SL / S M of the other elements little affected by the Cu concentration in the sulfide liquid. Because of their distinct dissolution mechanisms in the silicate melt, the D SL / S M and D MSS / S M of Mn, Co, Zn, Cd, Sn, and Pb are mainly controlled by the silicate melt FeOtot content ([FeOtot]); the D SL / S M and D MSS / S M for Re, Mo, As, Sb, and Bi are mainly controlled by [FeOtot] and fO2; the D SL / S M and D MSS / S M for Cu, Ag, and Au are mainly controlled by [FeOtot] and the content of reduced sulfur in the silicate melt; and the D SL / S M and D MSS / S M for Se and Te are mainly controlled by fO2. Using all available D SL / S M and D MSS / S M data, a partitioning model was developed for predicting D SL / S M and D MSS / S M of chalcophile elements as a multi-function of temperature, pressure, fO2, and silicate melt and sulfide compositions. Sulfide phase relations suggest that the sulfides precipitating from arc magmas containing >100 µg/g Cu in the silicate melt occur as Cu-rich sulfide liquid, whereas the sulfides precipitating from arc magmas containing 30–70 µg/g Cu in the silicate melt occur as mixed MSS and Cu-rich sulfide liquid. Modeling the Cu evolution trends of global arc magmas illustrates that the precipitating sulfides are dominantly MSS in continental arcs with a crustal thickness of >30 km, with the proportion of sulfide liquid being less than 20%; whereas, in island arcs with a crustal thickness of

Accumulated evidence shows that OGT-mediated O-GlcNAcylation plays an important role in response to DNA damage repair. However, it is unclear if the “eraser” O-GlcNAcase (OGA) participates in this cellular process. Here, we examined the molecular mechanisms and biological functions of OGA in DNA damage repair, and found that OGA was recruited to the sites of DNA damage and mediated deglycosylation following DNA damage. The recruitment of OGA to DNA lesions is mediated by O-GlcNAcylation events. Moreover, we have dissected OGA using deletion mutants and found that C-terminal truncated OGA including the pseudo HAT domain was required for the recruitment of OGA to DNA lesions. Using unbiased protein affinity purification, we found that the pseudo HAT domain was associated with DNA repair factors including NONO and the Ku70/80 complex. Following DNA damage, both NONO and the Ku70/80 complex were O-GlcNAcylated by OGT. The pseudo HAT domain was required to recognize NONO and the Ku70/80 complex for their deglycosylation. Suppression of the deglycosylation prolonged the retention of NONO at DNA lesions and delayed NONO degradation on the chromatin, which impaired non-homologus end joining (NHEJ). Collectively, our study reveals that OGA-mediated deglycosylation plays a key role in DNA damage repair.

The development of new tools that could meet the demand of sustainable energy production has attracted worldwide scientific attention. Over the past few decades, significant research efforts have been carried out to efficiently reduce water to H2 (green fuel) over semiconductor photocatalysts. Numerous semiconductor photocatalysts have been employed in photocatalysis for optimum H2 production. All the techniques were chosen based on their flexibility, cost-effectiveness, and ease of availability. Recently, polymeric carbon nitride (g-C3N4) received worldwide attention in visible light photocatalysis for energy and environmental applications due to its low price, robust nature, and superior thermal stability. Nevertheless, g-C3N4 (CN) exhibits shortfalls such as high charge carrier's recombination rate and weak reduction ability. To overcome these drawbacks, herein, for the first time we have fabricated B-TiO2/MIL-53(Fe)/CN ternary composite via hydrothermal and wet-chemical methods. The resultant B-TiO2/MIL53(Fe)/CN ternary composite shows drastically improved photocatalytic activity for hydrogen evolution compared to the bare CN, B-TiO2, and MIL53(Fe) components. The B-TiO2/MIL53(Fe)/CN ternary composite produced approximately 166.3 and 581.2 μmol h−1 g−1 of hydrogen under visible light and UV–visible light irradiations, respectively, with the assistance of co-catalyst Pt. Photo-luminescence (PL) and the fluorescence (FL) spectroscopy measurements reveal that the enhanced photoactivity is due to the greatly promoted charge carrier's separation and transfer at the interfacial contact of the well-aligned three-component systems. This work will promote the design and development of efficient photocatalyst based on CN for clean energy production and environmental purification.

Context Maternal lipids during pregnancy and placental growth factors are associated with excess fetal growth. However, how these factors interact to increase the risk of delivering large-for-gestational-age (LGA) neonates remains unclear. In this study, we investigated the relationship between maternal plasma triglycerides (TGs) and free fatty acids (FFAs) during pregnancy, cord blood insulin-like growth factors (IGF), and LGA. Objective In a cell model, we studied the effect of different FAs on placental IGF-1 secretion. Methods This cohort study included pregnant women with term pregnancy and without diabetes or hypertensive disorders in pregnancy. Maternal fasting plasma TGs and FFAs were measured in the second trimester. Cord blood IGF-1, IGF-2, and IGF binding protein-1 and protein-3 were measured at the time of delivery. A human trophoblast cell line, 3A-sub-E, was used to evaluate the effect of different FFAs on placental IGF-1 secretion. Results We recruited 598 pregnant women–neonate pairs. Maternal plasma TG (180 mg/dL [152.5-185.5 mg/dL] vs 166 mg/dL [133-206 mg/dL], P = .04) and cord blood IGF-1 concentrations (72.7 ± 23.0 vs 54.1 ± 22.8 ng/mL, P < .001) were higher in the LGA group and were significantly associated with birth weight z score. Maternal plasma free palmitic acid (PA) and stearic acid (SA), but not oleic acid (OA) or linoleic acid (LA), were significantly associated with cord blood IGF-1 concentrations. In 3A-sub-E cells, treatment with PA, SA, and LA, but not OA, induced IGF-1 expression and secretion. Conclusion Certain FFAs can induce placental IGF-1 secretion, which suggests a potential pathophysiology linking maternal plasma lipids and LGA.

Pyroptosis is a form of regulated cell death mediated by gasdermin family members, among which the function of GSDMC has not been clearly described. Herein, we demonstrate that the metabolite α-ketoglutarate (α-KG) induces pyroptosis through caspase-8-mediated cleavage of GSDMC. Treatment with DM-αKG, a cell-permeable derivative of α-KG, elevates ROS levels, which leads to oxidation of the plasma membrane-localized death receptor DR6. Oxidation of DR6 triggers its endocytosis, and then recruits both pro-caspase-8 and GSDMC to a DR6 receptosome through protein-protein interactions. The DR6 receptosome herein provides a platform for the cleavage of GSDMC by active caspase-8, thereby leading to pyroptosis. Moreover, this α-KG-induced pyroptosis could inhibit tumor growth and metastasis in mouse models. Interestingly, the efficiency of α-KG in inducing pyroptosis relies on an acidic environment in which α-KG is reduced by MDH1 and converted to L-2HG that further boosts ROS levels. Treatment with lactic acid, the end product of glycolysis, builds an improved acidic environment to facilitate more production of L-2HG, which makes the originally pyroptosis-resistant cancer cells more susceptible to α-KG-induced pyroptosis. This study not only illustrates a pyroptotic pathway linked with metabolites but also identifies an unreported principal axis extending from ROS-initiated DR6 endocytosis to caspase-8-mediated cleavage of GSDMC for potential clinical application in tumor therapy.

Carbon (C) substrates are critical for regulating denitrification, a process that results in nitrous oxide (N2O) and dinitrogen (N2) emissions from soil. However, the impacts of C substrates on concomitant soil emissions of carbon dioxide (CO2) and N2O under varying soil types and soil water contents are not well studied. Three repacked Pallic grassland soils, varying in texture and phosphorus (P) status, containing NO3−-15N were held at three levels of matric potential (ψ, −3, −5 and −7 kPa), while receiving daily substrate additions (acetate, glucose and water control) for 14 days. The CO2 and N2O emissions were measured daily. Additionally, the N2O:(N2 + N2O) ratios were determined using 15N on days 3 and 14. Results showed that N2O emissions increased exponentially as soil gas diffusivity declined, and N2O peak emissions were higher with glucose than with acetate addition, with a range (± standard deviation) of 0.1 ± 0.0 to 42.7 ± 2.1 mg N m−2 h−1. The highest cumulative N2O emission (2.5 ± 0.2 g N m−2) was measured following glucose addition with a soil ψ of −3 kPa. In comparison with added glucose, acetate resulted in a twofold increase in N2 emissions in soils with relatively low gas diffusivities. The N2O:(N2O + N2) emissions ratios varied with substrate (glucose, 0.91; acetate, 0.81) on day 3, and had declined by day 14 under substrate addition (≤0.10). Cumulative CO2 emissions were enhanced with increasing soil gas diffusivity and were higher for soils amended with glucose (ranging from 22.5 ± 1.3 to 36.6 ± 1.8, g C m−2) than for those amended with acetate. Collectively, the results demonstrate that the increase of N2O, N2 and CO2 emissions and changes in the N2O:(N2 + N2O) ratio vary over time in response to C substrate type and soil gas diffusivity. Highlights: Co-regulation of CO2 and N2O emissions was assessed for varying soil types and C substrates. Soil diffusivity explained concurrently cumulative N2O and CO2 emissions. Acetate enhanced N2O reduction to N2 in three grassland soils more than glucose. C substrate effects on soil N2O, N2 and CO2 emissions were soil type specific.