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Summary: MicroRNAs (miRNAs) play key regulatory roles in seed development and emerge as new key targets for engineering grain size and yield. The Zma‐miRNA169 family is highly expressed during maize seed development, but its functional roles in seed development remain elusive.Here, we generated zma‐miR169o and ZmNF‐YA13 transgenic plants. Phenotypic and genetic analyses were performed on these lines. Seed development and auxins contents were investigated.Overexpression of maize miRNA zma‐miR169o increases seed size and weight, whereas the opposite is true when its expression is suppressed. Further studies revealed that zma‐miR169 acts by negatively regulating its target gene, a transcription factor ZmNF‐YA13 that also plays a key role in determining seed size. We demonstrate that ZmNF‐YA13 regulates the expression of the auxin biosynthetic gene ZmYUC1, which modulates auxin levels in the early developing seeds and determines the number of endosperm cells, thereby governing maize seed size and ultimately yield.Overall, our present study has identified zma‐miR169o and ZmNF‐YA13 that form a functional module regulating auxin accumulation in maize seeds and playing an important role in determining maize seed size and yield, providing a set of novel molecular tools for yield improvement in molecular breeding and genetic engineering. [ABSTRACT FROM AUTHOR]

With the exponential improvement of the integration capabilities of electronic hardware devices, digital images have become an indispensable information carrier, thus promoting the development of image recognition, detection, or tracking technologies. At present, there is a blank in the field of image recognition measured by the action standard of yoga standing three-dimensional movement, which will bring huge room for researchers to play. Based on the traditional image recognition technology, there are cases where missed detection or false detection cannot be correctly identified and made a correct judgment. In this paper, the ability to capture the action is improved by optimizing the network for the positioning of the stereoscopic action target of the yoga station. The linear discriminant analysis (LDA) after adding optimization is used to reduce the dimensionality of the captured image data, which is beneficial to improving image recognition rate and reducing image loss rate. Through the analysis of the three-dimensional movement of the yoga station, the model based on the improved algorithm is compared with the traditional model, and the final image recognition accuracy is improved compared with the network model before the improvement. The image recognition error rate steadily tends to 5%, and the loss rate is also below 2%. Through the optimized convolutional neural network, this paper can accurately capture the image position, and the recognition rate has also been greatly improved, which can provide a reference for future research in other fields. [ABSTRACT FROM AUTHOR]

Objectives. To observe and analyze the long-term change of different types of arrhythmias after transcatheter closure of perimembranous ventricular septal defect (pmVSD). Methods. We retrospectively collected the data of patients who underwent pmVSD closure in our institution from March 2002 to December 2010. Results. One hundred thirty-nine patients met the inclusion criteria, of which 265 (25.5%) had early arrhythmia. They were classified into two categories: conduction abnormality (191/1039; 18.4%) and origin abnormality (94/1039; 9.0%), including 20 patients with both types of arrhythmias. The median follow-up time was 84.5 months, and 103 patients (103/191; 53.9%) with early conduction block got permanent arrhythmias, while only three patients (3/94; 3.2%) with early anomalous origin arrhythmias still had an abnormal electrocardiogram. Serious arrhythmias (28/1039; 2.7%), including II° atrioventricular block (AVB), III° AVB, and complete left bundle branch block (CLBBB), can appear immediately in the early postoperative period (21 patients) or in the late outset (seven patients) after several months or even years (6 months to 8.3 years). Twenty patients (20/21; 95.2%) with serious arrhythmia in the early postoperative period improved after early treatment, but six patients relapsed or worsened during follow-up. At the endpoint, severe arrhythmia persisted in 13 patients, of which four patients got permanent pacemaker implanted, and one patient with recurrent CLBBB died from heart failure. Conclusions. The probability of delayed CAVB or bundle branch block after VSD closure is low but often occurs several years after surgery. Therefore, long-term ECG follow-up should last for several years or even decades. Serious arrhythmias that appear early after transcatheter pmVSD closure may impose a risk of recurrence although they have been cured already. Close attention should be paid to the changes of cardiac function in patients with CLBBB after VSD closure, and the severity of such arrhythmia should be taken seriously and reexamined. [ABSTRACT FROM AUTHOR]

• Cyanobacterial nitrate bioreporters were optimized based on various combinations. • LuxABCDE responded faster than sfGFP in cyanobacterial nitrate bioreporters. • The shuttle plasmid with RSF1010 replicon improved the performance of bioreporters. • The nitrate bioavailability can be detected by bioreporter AD-AS-X at 2 h induction. • Six bioreporters effectively detecting the bioavailable nitrate in the water sample. The water eutrophication, resulting from the discharge of industrial and agricultural wastewater, leads to ecological degradation. However, to date, how to assess and manage the risks of water pollution, especially nitrogen pollution, remains a particularly noteworthy issue. Nitrate, the most important nitrogen compound, has become a bottleneck restricting total nitrogen management. The development of bioreporters monitoring nitrate pollution contributes to the estimation of water quality, especially the availability of nutrients. In this study, we obtained 9 bioreporters from 40 cyanobacterial derivatives which were constructed based on different hosts, copy numbers, and sensing elements and evaluated the performance of bioreporters. The results showed that single-celled Synechocystis was more sensitive to nitrate than filamentous Anabaena , that the reporter gene luxABCDE responded faster than sfgfp in most bioreporters, and that relatively medium-copy plasmid improved the performance of sensing elements. Nine bioreporters performed well in bioavailable nitrate detection, of which AD-AS-X and AR-NI-X, activated by nitrate repletion, had the shortest response time (2 h) and the widest response range (20–800 μM), respectively. Moreover, SR-GLN-SG, activated by nitrate deficiency, exhibited the best linear response (R2 = 0.998). After parameter optimization, exponential growth phase bioreporters, culture temperature of 30 °C, sample volume of 200 μL were determined as optimal monitoring conditions. We found that common water contaminants (copper, cadmium, and phosphorus) had no impact on the performance of bioreporters, indicating the stability of bioreporters. Six out of 9 bioreporters, especially the SR-NB-X, were highly effective in detecting the bioavailable nitrate in wastewater sample. This study provides valuable references for developing more cyanobacterial bioreporters and their practical application in nitrate detection. [Display omitted] [ABSTRACT FROM AUTHOR]

Study the effects of different packing methods, including divided into four blocks horizontally and four blocks vertically inside the box, on natural alcoholization of Yuxi K326 C03S flue-cured tobacco lamina. The results showed that : compared with the control sample, the color of those turned faster, the oiliness of those was better, the aroma appeared earlier, with a small amount of gas ; the alcoholization process had stronger chemical reaction; the peak of sensory quality was 4 months in advance. In summary, the packing method in the box could accelerate the alcoholization reaction of the tobacco leaves and greatly shorten the alcoholization cycle of the tobacco leaves. [ABSTRACT FROM AUTHOR]

Based on a Driving Forces-Pressure-State-Impact-Response (DPSIR) model, this paper takes a macroenvironmental, socioeconomic perspective to build an evaluation model to address sustainable Chinese wind power developments and to quantize the development results. From a combination of entropy weight and the Technique for Order of Preference by Similarity to Ideal Solution (TOPSIS) method, the sustainable wind power development level in China is examined, the development trends analyzed, and the trends and underlying laws identified, all of which provides new information for Chinese wind power sustainability. It was found that Chinese sustainable socioeconomic wind power development has been growing year on year. However, the wind power ecological sustainability fell and then rose slowly, indicating that these subsystems both influence the sustainable development of wind power. [ABSTRACT FROM AUTHOR]

An extensive product distribution is firstly examined in the process of 5-hydroxymethylfurfural (HMF) decarbonylation over Pd-based catalysts and some interesting results are obtained. The main side reactions are due to the high activity of the furan ring-branched hydroxymethyl, which could go through hydrogenolysis, dehydrogenation and etherification. The H 2 source was carefully explored and determined to be the hydroxymethyl dehydrogenation. The reactivity of the main intermediates was separately investigated and their evolution pathway was obtained. Noticeably, it is demonstrated that the elimination of the furanic ring-branched hydroxymethyl (in HMF or furfuryl alcohol) is completed by sequential dehydrogenation and decarbonylation via the intermediate of aldehyde (2, 5-diformylfuran or furfural). A comprehensive reaction pathway for HMF decarbonylation is proposed, which is significant for designing highly selective decarbonylation catalysts. [ABSTRACT FROM AUTHOR]

LaFe 11.6 Si 1.4 samples were hydrogenated at the same initial hydrogen-filling pressure of 0.6 MPa and different temperatures (from 393 K to 478 K). The hydrogen absorption kinetics performance, phase structures and Curie temperature (T C ) of these alloys were investigated. The results show that all samples have excellent hydrogen absorption kinetics performance, the NaZn 13 -type main structure of these LaFe 11.6 Si 1.4 H y alloys is stable during the fore-and-aft hydrogenation processes and their T C s vary from 326.9 K to 277.7 K by adjusting hydrogen content from 1.26 to 0.936. The high-temperature hydrogenation can markedly save the hydrogen saturation time of LaFe 11.6 Si 1.4 alloys and precisely adjust the T C of these alloys. In addition, the split of magnetocaloric transition is observed by analyzing Differential Scan Calorimetry curves of the alloys hydrogenated from 443 K to 463 K. Further investigation of two typical samples hydrogenated at 443 K and 463 K shows that the split transition peaks change into a sharp single transition peak after annealing these samples at 373 K for 24 h and the split transition peaks re-emerge after storing the annealed samples near T C for 14 days. The recovery and split of the peaks imply that the fully hydrogenated LaFe 11.6 Si 1.4 alloys at high treatment temperature are all partially hydrogenated LaFe 11.6 Si 1.4 alloys when stored or used at room temperature. [ABSTRACT FROM AUTHOR]

The first enantioselective total synthesis of (−)-salprzelactone, a seco-norabietane diterpenoid has been accomplished in only three steps. Key transformations of the synthesis include an intermolecular aldol reaction and lactonization. [ABSTRACT FROM AUTHOR]

Atherosclerosis (AS) is a principal contributor to stroke and coronary heart disease in humans characterized by chronic low‐grade inflammation. The extracellular matrix (ECM) plays critical roles in regulating the function of arteries. However, the effect of changes in ECM on AS development is rarely studied. In this context, we intend to study the effect of oxidizing agent peroxynitrite (ONOO−)‐mediated oxidization of ECM proteins on the biological behaviors of vascular smooth muscle cells (SMCs) and the development of AS. AS mouse models were established, and mouse coronary artery smooth muscle cells (MCASMCs) were cultured in vitro to derive ECM (SMC‐ECM), which was obtained by deoxycholate (DOC)‐based decellularization. Further, MCASMCs were subjected to the determination of ECM oxidative damage and ECM protein structure. Finally, roles of ONOO−‐mediated oxidization of ECM in SMC adhesion and migration and in AS development were explored through Transwell assay, transcriptome sequencing, and gene enrichment analysis. High concentration of ONOO− was found in the serum of AS mice, and ONOO− could stimulate the development of AS. SMC‐ECM with intact structure can be obtained in vitro by DOC treatment. Functionally, ONOO−‐mediated oxidization destroyed the three‐dimensional structure of SMC‐ECM proteins, affected SMC adhesion and migration and promoted the absorption efficiency of lipids while reducing the efflux of cholesterol. In addition, the expression of inflammation‐ and oxidative stress‐related genes was significantly increased in ECM subjected to ONOO−‐mediated oxidization, thereby contributing to AS progression. ONOO−‐mediated oxidative modification of ECM aggravates AS by affecting the biological behavior of SMCs. [ABSTRACT FROM AUTHOR]

• The molecular weights of components in SESs and TESs are generally below 2000 amu. • As increasing TET, more PAHs are dissolved, so H/C of TESs also declines. • MN is more conducive to the dissolution of large aromatic ring structures. The direct coal liquefaction (DCL) process is accompanied by the dissolution of the soluble fractions during the preheating stage. These soluble fractions remain in the system after dissolution and involve subsequent high-temperature hydro-liquefaction process, and their effect and role on the distributions and properties of products cannot be ignored. In this paper, soxhlet extraction (SE) with tetrahydrofuran (THF) and pyridine (PY) and in-situ thermal extraction (TE) in tetralin (THN) and 1-methyl naphthalene (MN) at 260–360 °C of Hami lignite (HM) and Bulianta sub-bituminous coal (BLT) were carried out to obtain SE soluble fractions (SESs) and TE soluble fractions (TESs), respectively. The effects of temperature and solvent on extraction behaviors of two coals were investigated and the structure and property characteristics of SESs and TESs were compared. The results indicate that the extraction yields of HM are higher than that of BLT, and TE significantly enhances the extraction yields, reaching 41.06 % and 36.40 % at 360 °C with THN and MN for HM, respectively. The TE yields (TEYs) increase with the raising of TE temperature (TET). The high TEYs received at 360 °C may be ascribed to the partial pyrolysis reactions of weak covalent bonds like side chain and bridge bond breaking in two coals. The main body of HM and BLT is a macromolecular network structure that is crosslinked by chemical bonds, and some low molecular weight compounds that are bound through non-covalent bond interactions constitute the guest. The SESs and TESs are mainly composed of aliphatics with high H/C, low condensation degree aromatics and oxygen-containing compounds containing C=O and C-O, with low heteroatom content and almost all of the mineral matters in raw coals are transformed to residues. There are significant differences in structures between SESs and TESs. As increasing the TET, the content of monocyclic aromatics in TESs decreases, and more polycyclic aromatics are dissolved, so H/C also declines. The weight-average molecular weights and molecular weight size distribution of TESs measured by the GPC method are generally larger than those estimated by MALDI-TOF-MS, which is correlated to the association structure formed between TESs and solvent or in TESs. [ABSTRACT FROM AUTHOR]

Recently, high-temperature stress induced by climate change has resulted in the degradation of Pyropia haitanensis thalli, which has adversely affected the P. haitanensis aquaculture industry. Although heat-resistant P. haitanensis strains have been developed, the mechanism underlying the stress resistance remains unclear. In this study, we investigated the effects of high-temperature stress (32 °C) on the Ca2+ flux and calmodulin (CaM) contents of P. haitanensis thalli. Gene expression and protein abundance were also analyzed. The high-temperature stress significantly increased the Ca2+ influx, as well as the expression levels of CaM s and their encoded proteins. However, when the plasma membrane Ca2+ channel was inhibited by verapamil, the Ca2+ influx, CaM expression levels, CaM abundance levels, and photosynthetic activities decreased considerably. These changes ultimately reduced the heat resistance of P. haitanensis thalli. Additionally, the expression levels of heat shock protein genes (HSP22 and HSP70) were upregulated under high-temperature conditions, whereas they were downregulated after the Ca2+ influx rate decreased. Thus, the Ca2+ signal generated by the plasma membrane's Ca2+ channels appears to be important for P. haitanensis responses to high-temperature stress. The data presented herein provide insights into the mechanisms responsible for P. haitanensis ' heat resistance. • High-temperature stress induces considerable Ca2+ influx within 15 min of treatment. • Ca2+ and calmodulin mediate responses to high-temperature stress in P. haitanensis. • Ca2+ and calmodulin may regulate HSP expression levels. [ABSTRACT FROM AUTHOR]

[Display omitted] • In-situ Py-TOF-MS reveals interactions between coal and mixed plastic. • H-rich radicals from PP react with phenoxy radicals from coal to form diphenols. • The further addition of LDPE enhances the inhibitory effect on HM pyrolysis. • The co-pyrolysis of HM with PP/LDPE/PS generates more aromatic products. Online detection of pyrolysis volatiles is essential for exploring the mechanism of coal and plastics co-pyrolysis. In-situ pyrolysis time-of-flight mass spectrometry (Py-TOF-MS) equipped with double ionization sources, vacuum ultraviolet photoionization (VUVPI) and electron ionization (EI), was used to analyze the release of primary volatiles during the pyrolysis and co-pyrolysis of Hami coal (HM) with mixed plastic (PP/LDPE and PP/LDPE/PS, with ratios of 3:2 and 12:8:1, respectively). Meanwhile, the interaction mechanism was discussed at the molecular level. According to the thermogravimetric (TG) results and the total ion currents (TIC) of primary volatiles with temperature, the inclusion of plastic shortens the overall reaction time. In-situ Py-TOF-MS results indicate that the volatiles produced from HM pyrolysis at lower temperatures induce the decomposition of PP and promote further dehydrogenation of long-chain C–C. Besides, the addition of PP visibly facilitates the transportation of hydrogen, which reacts with phenoxy from HM pyrolysis to produce diphenol. The further addition of LDPE after PP enhances the inhibitory effect of molten plastic on HM pyrolysis, resulting in a decrease in the content of diphenol, such as benzenediol (from 1.34% to 0.71%), methyl-benzenediol (from 1.12% to 0.68%) and dimethyl benzenediol/ethyl benzenediol (from 0.68% to 0.50%). The co-pyrolysis of HM with PP/LDPE/PS generates more aromatic products compared to that of theoretical value, such as styrene (from 0.29% to 3.16%), 1-ethenyl-3-methyl benzene (from 0.07% to 0.31%) and 1-butene-2,4-diphenyl (from 0.19% to 0.65%). This indicates that co-pyrolysis strengthens the breakage of C ar -C β bond in the PS backbone. The addition of PS to the mixture plastic also promotes intramolecular and intermolecular hydrogen transfer in the system. For the evolution of inorganic gases, the addition of mixed plastics promotes the decomposition of aliphatic and aromatic carboxylic acids in coal at lower temperatures, resulting in a decrease in CO 2. [ABSTRACT FROM AUTHOR]

• The carbon skeleton structure of MLS mainly consists of aliphatic (47.90%) and aromatic (40.10%) carbons. • Evaporation of hexane soluble fraction (HS) and cleavage of C al C al and C ar C al bonds are dominant during MLS pyrolysis. • Fine quantitative linear relationships between gasification reactivity and physico-chemical structures of MLS char are established. Efficient utilization of mild liquefaction solid product (MLS) of Hami coal is critical to improve energy efficiency of the whole process, which accounts for >30 wt% of raw coal. In this work, the structure features of MLS were characterized by the solid-stage 13C NMR (SS-NMR) and its pyrolysis behavior was measured by a thermogravimetric analyzer (TGA) coupled with a mass spectrometer (MS). Additionally, the chars of MLS were prepared in a quartz tube fixed-bed reactor at different temperatures. Then the physico-chemical structure and CO 2 gasification reactivity of the MLS chars were measured by multiple methods, including Fourier Transform Infrared Spectrometer (FTIR), scanning electron microscope (SEM), X-ray diffraction (XRD) and TGA. According to the SS-NMR analysis, the aromaticity of MLS is relatively high even though it contains ca. 47.90% aliphatic carbon. The evaporation of hexane soluble fraction (HS) and cleavage of C al C al and C ar C al bonds are dominant in the process of MLS pyrolysis according to the TGA-MS analysis. With the increase of final pyrolysis temperature, the yield of char and H/C atomic ratio gradually decrease from 69.4% to 54.9% and from 0.664 to 0.110, respectively. In addition, the side chains and functional groups of char gradually reduce, the char becomes dense and dim, and the degree of ordering of char increases. Well quantitative linear relationships (R2 > 0.95) between gasification reactivity, carbon crystalline stacking layer number (n) and H/C atomic ratio are established, which could be used to finely evaluate the CO 2 gasification reactivity of MLS and pyrolysis chars. [ABSTRACT FROM AUTHOR]

Pyropia haitanensis is a high-yield commercial seaweed in China. Pyropia haitanensis farms often suffer from problems such as severe germplasm degeneration, while the mechanisms underlying resistance to abiotic stresses remain unknown because of lacking genomic information. Although many previous studies focused on using next-generation sequencing (NGS) technologies, the short-read sequences generated by NGS generally prevent the assembly of full-length transcripts, and then limit screening functional genes. In the present study, which was based on hybrid sequencing (NGS and single-molecular real-time sequencing) of the P. haitanensis thallus transcriptome, we obtained high-quality full-length transcripts with a mean length of 2998 bp and an N50 value of 3366 bp. A total of 14,773 unigenes (93.52%) were annotated in at least one database, while approximately 60% of all unigenes were assembled by short Illumina reads. Moreover, we herein suggested that the genes involved in the biosynthesis of polyunsaturated fatty acids and heat shock proteins play an important role in the process of development and resistance to abiotic stresses in P. haitanensis. The present study, together with previously published ones, may facilitate seaweed transcriptome research. [ABSTRACT FROM AUTHOR]

The cyclic fructose was converted to furfural via open-ring tautomer over beta zeolite, and the selective splitting of C C bond was proved to be located between C5 and C6 atom. [Display omitted] • Insights the mechanism of furfural formation with respect to fructose isomers. • Investigating the furfural formation in view of shape selectivity of zeolites to fructose tautomer. • In situ NMR monitored the cleavage of C C bond of fructose using isotope 13C labeling. The mechanism for the formation of furfural by dehydration of d -fructose via selective carbon-carbon (C C) bond cleavage was investigated over beta zeolite (Hβ). Several different pore size zeolites were employed to determine the shape selectivity of fructose isomers. Zeolitic pore sizes that smaller than the kinetic diameter of cyclic fructose also produced yield furfural (∼22.5%), while the high yield (66.0%) of hydroxymethylfurfural (HMF) can be achieved over large pore zeolite (USY zeolite), which could accommodate the cyclic fructose. These results indicated that the furfural formation likely began with acyclic fructose. In situ 13C NMR and GC MS studies, using labeled 13C-1-fructose as substrate, suggested that the conversion of fructose to furfural involved with splitting of the C5-C6 bond. Furthermore, the C1 compound from the cleavage of C C bond was identified as formaldehyde, inferring that the selective scission of C C bond was ascribe to the retro-aldol reaction. Interestingly, in situ NMR studies implied that the acyclic fructose mainly derived from pyranose forms. In addition, compared with glucose, fructose directly converted to furfural at the higher yield and reaction rate. [ABSTRACT FROM AUTHOR]

[Display omitted] • Cu-ZnO/ZrO 2 was fabricated by combination of Cu-Zn rosasite and monoclinic ZrO 2. • TOFs based on surface Cu, ZnO and ZrO 2 sites are calculated respectively. • Structural promotion and direct bifunctional effects of the oxides were demonstrated. • A high yield of ethylene glycol (92%) and stable performance were finally achieved. Supported Cu, commonly containing active Cu and oxide supports, is widely used in hydrogenation of carbon-oxygen bonds. The central premise before rational improvement of Cu catalysts is to gain the fundamental insights into the relationship between catalytic performance and oxide components. Herein, ternary Cu-ZnO/ZrO 2 catalysts were fabricated by a one-pot precipitation-deposition method. The Zn and Cu cations formed the rosatite mineral in solution by precipitation method and then deposited in-situ on the monoclinic ZrO 2 (m-ZrO 2) nanoparticles. The catalyst was thus featured with well-dispersed Cu-ZnO species from mineral precursor and bifunctional sites from m-ZrO 2. The trends of reaction rates normalized by the surface sites demonstrated the synergy effects of the oxide components. The catalyst gave greatly promoted reactivity (up to 92% ethylene glycol yield) and stability (over 300 h) for synthesis of ethylene glycol from dimethyl oxalate hydrogenation. The structure-performance relationship revealed that oxide components contribute to both the structural promotion and direct bifunctional effects, giving great potential for improving supported metal catalysts. [ABSTRACT FROM AUTHOR]

Polygonati Rhizoma, a typical homology of medicine and food, possesses remarkable anti-fatigue, anti-aging, metabolic regulatory, immunomodulatory, anti-inflammatory, neuroprotective, anti-diabetes, and anti-cancer effects. Among bioactive phytochemicals in Polygonati Rhizoma, polysaccharides play important roles in the health-promoting activities through the mechanisms mentioned above and potential synergistic effects with other bioactives. In this review, we briefly introduce the updated biosynthesis of polysaccharides, the purification method, the structure characterization, and food applications, and discuss in detail the biological activities of Polygonati Rhizoma polysaccharides and associated mechanisms, aiming at broadening the usage of Polygonati Rhizoma as functional food and medicine. [ABSTRACT FROM AUTHOR]

[Display omitted] • Highly dispersed Pd/Al 2 O 3 was prepared based on electrostatic attraction strategy. • Action mechanism of pH of impregnation solution was explored. • Catalysts with small Pd nanoparticles showed superior catalytic performance. • Structure sensitive behavior of catalysts was discussed. • Surface properties of catalysts were characterized by in situ FTIR. Decarbonylation of 5-hydroxymethylfurfural (HMF) provides a potential way to utilize the abundant natural hexoses derived from cellulose or hemicellulose. Herein, we propose for the first time that a Pd/Al 2 O 3 prepared based on an electrostatic attraction strategy can efficiently convert HMF into furfuryl alcohol (FOL). Ammonia solution with high pH value could realize the electrostatic attraction assumption in the interface of support and palladium complex, while diluted hydrochloric acid with low pH value could cause the instability of H+ ions on Al 2 O 3 surface, leading to larger Pd nanoparticles (NPs) of the catalyst and lowering the decarbonylation activity. A structure-sensitive behavior was discussed that the intrinsic activity of catalyst rised with the decreased size of Pd NPs, which could be illustrated by that the smaller particles exposed more defective Pd sites, on which the decarbonylation adsorption mode of η2(C, O) was preferred. FOL yield of 95% was obtained through modulation of reaction conditions. [ABSTRACT FROM AUTHOR]

Background: Circulating fibrinogen-to-albumin ratio (FAR) has been proposed as a novel inflammatory biomarker and a cardiovascular disease risk predictor. However, its prognostic value in patients with acute decompensated heart failure (ADHF) and different glycemic metabolic states remains ambiguous. Methods: A total of 1031 hospitalized patients with ADHF from January 2018 to May 2021 were included in the study. The primary endpoints were the major adverse cardiac and cerebral events (MACCEs). Patients were categorized into high-level FAR (FAR-H) and low-level FAR (FAR-L) groups based on the optimal cut-off value of FAR obtained from restricted cubic spline function analysis. The Kaplan–Meier plots and three multivariate-adjusted Cox proportional hazard models were used to determine the association between FAR and the risk of developing MACCEs in patients with ADHF at different glycemic metabolic states. Results: MACCEs occurred in 483 (46.8%) patients during a median follow-up time of 520 days. The optimal FAR cut-off value was 0.079. Upon analyzing the Kaplan–Meier plots, the incidence of MACCEs was significantly different between the FAR groups in all patients and patients with diabetes mellitus (p < 0.05). After adjusting for the confounding factors, the hazard ratio (HR) for MACCEs in the FAR-H group was 1.29 compared with the FAR-L group in all patients (Model 3: 95% CI 1.07–1.56, p = 0.007). Additionally, high FAR was associated with MACCEs in three multivariate Cox models (Model 1, HR = 1.52, 95% CI 1.17–1.96, p = 0.002; Model 2, HR = 1.46, 95% CI 1.13–1.89, p = 0.004; Model 3, HR = 1.48, 95% CI 1.14–1.92, p = 0.003) in DM patients. But no significant differences were found between the FAR groups for prediabetes mellitus (Pre-DM) and normal glucose regulation (NGR) using the three Cox models (all p-values were > 0.05). Conclusions: Elevated FAR was independently associated with poor prognosis in patients with ADHF and DM and thus could be used as a risk stratification tool and a potential therapeutic target in the future. [ABSTRACT FROM AUTHOR]

The properties of the binary mixtures of a new cationic amino acid surfactant arginine dihydrochloride dodecyl ester (ADDE) and alkyl polyglycosides (APGs) were studied systematically by evaluating surface tension, conductivity, dynamic light scattering (DLS), transmission electron microscopy (TEM), biological and cytotoxic activity measurements. Higher surface activity and more diverse self-assembly behaviors for the mixed system (ADDE/APG) compared to single systems (ADDE or APG alone) were seen due to the synergistic effects between ADDE and APG. The interaction and micelle thermodynamic parameters of ADDE/APG mixtures show strong intermolecular interaction, both in the mixed micelles and at the gas/liquid interface, and indicate that the micellization is an enthalpy-driven process. At the total solution concentration of 50 mmol L−1 and higher mole fraction of ADDE (αADDE ≥ 0.5), primarily large aggregates are formed according to DLS results with typically spherical vesicles of about 200 nm in diameter as shown by TEM. The experimental results also show that the antimicrobial activities of ADDE/APG mixtures are outstanding at a low concentration of 0.5 mmol L−1 and are attributed to ADDE containing amino and guanidinium cationic groups within the same molecule. And the hemolytic activity results of ADDE/APG mixtures clearly indicate that the maximum blood compatible concentration was under 0.5 mmol L−1. This research will be beneficial for broadening the application field of amino acid surfactant ADDE. [ABSTRACT FROM AUTHOR]

Our work focuses on exploring Cr-free Cu-catalysts for the highly efficient conversion of biomass-derived furfural to value-added bio-fuel 2-methylfuran. Three supported Cu-catalysts (Cu/SiO 2 , Cu/Al 2 O 3 , and Cu/ZnO) were prepared by the typical precipitation method, and Cu/SiO 2 catalyst exhibited the best catalytic performance with an 89.5% yield to 2-MF. A series of characteristic results indicated that the high yield of 2-methylfuran on Cu/SiO 2 catalyst was assigned to synergistic effect of metal and the weak acid sites. Among them, Cu/ZnO catalyst exhibited maximum furfuryl alcohol selectivity because of the large Cu particles, while Cu/Al 2 O 3 catalyst had low 2-methylfuran selectivity due to the insufficient weak acid sites. For Cu/SiO 2 catalyst, the highly dispersed Cu particles and the strong metal-support interaction are propitious to its superior catalytic activity. Therefore, copper species are composed on different supports as a result of the different interaction of metal-support to affect their catalytic activity, while products selectivity is related to the acidic property of catalyst. In addition, temperature programmed desorption of furfural indicated that the adsorption–desorption properties of catalyst surface species would influence the rate of furfural hydrogenation. [ABSTRACT FROM AUTHOR]

A novelsilver(I)-catalyzed ring-contractive rearrangement of 5-substituted6-diazo-2-cyclohexenones has been developed, providing a new and efficientaccess to 5-alkylidene-2-cyclopentenones. The AgOTf-catalyzed reactionproceeds through metal–carbenoid formation followed by endocyclicallyl [1,2] migration with excellent stereoselectivity and broad substratescope. [ABSTRACT FROM AUTHOR]

China suffers from frequent large-scale earthquakes, posing a significant challenge to the development and integrity of its rural water supply system (RWSS). The earthquake resilience of water supply systems is understood to be a function of multifaceted factors, which are time- and space-dependent. Measuring the seismic-resilience of RWSS in China remains a challenge. This paper proposes a multi-stage comprehensive evaluation framework, focusing on the relationship between multi-dimensional factors and the seismic- resilience of RWSS in rural areas, across three stages: before, during and after earthquake events. This study comprises four steps: (1) Development of a multi-stage evaluation conceptual framework; (2) identification of seismic-resilience factors; (3) verification of the relationships between factors and stages; and (4) formation of the final evaluation framework. The relationship between multi-dimensional factors is confirmed by a method of triangulation through the quantitative analysis of PLS-SEM combined with the qualitative literature analysis, highlighting the causal approach of the resilience of RWSSs, so as to better understand the resilience state of each stage of disaster. Understanding these factors and their influence on the seismic capacity of RWSS will enable local authorities to recognize the existing advantages and disadvantages of these factors, so as to carry out better resilience practice in all stages of disasters. [ABSTRACT FROM AUTHOR]

Background: Dilated cardiomyopathy (DCM) is one of the common causes of heart failure. Myocardial injury triggers an inflammatory response and recruits immune cells into the heart. High expression of Krüppel-like factor 2 (KLF2) in endothelial cells (ECs) potentially exerts an anti-inflammatory effect. However, the role of extracellular vesicles (EVs) from KLF2-overexpressing ECs (KLF2-EVs) in DCM remains unclear. Methods and results: EVs were separated from the supernatant of KLF2-overexpressing ECs by gradient centrifugation. Mice were repeatedly administered low-dose doxorubicin (DOX) and then received KLF2-EVs through an intravenous injection. Treatment with KLF2-EVs prevented doxorubicin-induced left ventricular dysfunction and reduced the recruitment of Ly6high Mo/Mø in the myocardium. We used flow cytometry to detect Ly6high monocytes in bone marrow and spleen tissues and to elucidate the mechanisms underlying this beneficial effect. KLF2-EVs increased the retention of Ly6Chigh monocytes in the bone marrow but not in the spleen tissue. KLF2-EVs also significantly downregulated C–C chemokine receptor 2 (CCR2) protein expression in cells from the bone marrow. Conclusions: EVs derived from KLF2-overexpressing ECs reduced cardiac inflammation and ameliorated left ventricular dysfunction in DCM mice by targeting the CCR2 protein to inhibit Ly6Chigh monocyte mobilization from the bone marrow. [ABSTRACT FROM AUTHOR]

Highlights: [•] Unsymmetrical tetrahydrofurfuryl carbonate was synthesized with high selectivity. [•] The K2CO3/ZrO2 catalyst exhibited the best performance in transesterification. [•] The surface carboxylate species rather than the basic sites were the active sites. [•] The K2CO3 supported on other TiO2 and Al2O3 cannot produce the carboxylate species. [Copyright &y& Elsevier]

• Kaolin is co-modified by calcination at varying temperatures and NaOH leaching. • Light tar and aromatics increase and the O content of tar reduces after catalysis. • Amorphous SiO 2 formation and desilication improve mesopores and acidity of kaolin. • Calcining kaolin at 1100 °C is most favorable for upgrading volatiles. Catalytic upgrading of coal pyrolysis volatiles is an effective approach to improve tar quality with its high-value utilization, and the use of inexpensive solid acid catalysts can reduce the cost of industrial applications. In this work, kaolin was chosen as the raw material for modification by calcination (950–1200 °C) and NaOH leaching to serve as a catalyst (ACK) for upgrading volatiles from Hami coal pyrolysis. The properties of ACK under different calcination temperatures and the distribution of pyrolysis products were characterized to investigate the relationship between ACK properties and catalytic effect. The addition of ACK significantly improved the tar quality, as demonstrated by an increase in light tar fraction from 40.1 wt% to 46.4–52.8 wt%, a reduction in O/C atomic ratio of 11.4 %–37.6 %, and an increase in aromatics selectivity from 18.3 % to 21.2 %–25.0 %. These improvements were attributed to the varying increases in the specific surface area and acid sites of kaolin, a consequence of the formation of differing amounts and locations of amorphous silica during calcination and subsequent desilication by NaOH. Both the specific surface area and acid sites of ACK showed a tendency to increase and then decrease with rising calcination temperature. The improvements in tar quality were intimately linked to the pore structure and acidity of ACK, with ACK1100 (1100 °C calcination followed by NaOH leaching) exhibiting the most promising tar upgrading performance due to its maximum acid sites and a high specific surface area second only to ACK1050. [ABSTRACT FROM AUTHOR]

[Display omitted] • ZIF-8 derived ZnO@NC can anchor Ru nanoparticles to create Ru-O-Zn interface. • Ru/ZnO@NC achieved complete conversion and 99.2% GVL yield in LA hydrogenation. • Ru/ZnO@NC achieved excellent reaction activity with a TOF of 6032 h−1 at 40 °C. • Reaction mechanism of LA hydrogenation to GVL has been revealed by DFT calculation. • Ru-O-Zn interface can remarkably decline activation energy of rate-determining step. Highly efficient synthesis of valuable γ-valerolactone (GVL) by levulinic acid (LA) hydrogenation is of interest for biomass refinery, but it suffers from great challenge to design highly active Ru-based catalyst at low temperature. ZIF-8 derived ZnO@NC nanocomposite can firmly anchor Ru nanoparticles to create strong Ru-ZnO interfacial structure, as revealed by characterization techniques and DFT calculations. By optimizing Ru content and ZnO particle size, Ru/ZnO@NC achieved excellent reaction activity with a turnover frequency (TOF) of 6032 h−1 at low temperature of 40 °C, which is never reported before. After etching the accessible ZnO, the TOF value was significantly declined to 125 h−1 on Ru/ZnO@NC-HF owing to the lack of effective Ru-ZnO interface. DFT calculation results demonstrate that the Ru-ZnO interfacial structure can facilitate the activation of intermediate CH 3 CHOCH 2 CH 2 COOH* and remarkably decline the activation energy barrier of rate-determining step (CH 3 CHOCH 2 CH 2 COOH + H = HPA) from 1.28 eV to 0.82 eV, thus leading to excellent activity of LA hydrogenation at low temperature. [ABSTRACT FROM AUTHOR]

Abstract: The conversion of propanoic acid under high hydrogen pressure has been studied over zirconia-supported monometallic Ru and bimetallic Ru–Mo catalysts. The cleavage of C–C bond of propanoic acid to methane and ethane is improved and the formation of Cnation products (propanol and propane) is decreased with increasing the temperature. Upon addition of Mo, both the overall activity and the C–C bond cleavage selectivity decrease while the selectivity of Cnation increases. With increase of Mo contents, the C–C bond cleavage reaction is significantly inhibited, especially at high temperature. This is also confirmed by the DRIFTS of propanoic acid, showing that the propanoyl intermediate species on Ru–Mo bimetal catalysts is more difficult to dissociate to CO compared with Ru monometal catalyst. Based on H2-TPR, CO-FTIR and DRIFTS of propanoic acid characterizations, the reaction mechanisms and the resulting selectivity towards the possible reaction paths (C–C bond cleavage/Cnation) are discussed in terms of the formation of Ru–MoO x and the stability and variety of propanoyl intermediate species occurring on the Ru–Mo bimetal catalysts. It is suggested that the interaction of Ru and MoO x species and the formation of Ru–MoO x interface are the important factors for the decrease in the TOF of propanoic acid and the C–C bond cleavage selectivity. [Copyright &y& Elsevier]

Abstract: For the aqueous-phase hydrodeoxygenation (APHDO) of carboxylic acids over the Ru/C, Ru/ZrO2 and Ru/Al2O3 catalysts, the Cnation and C–C bond cleavage reactions were studied by collecting reaction kinetics data and the measures of DRIFTS. The C–C bond cleavage was improved at high temperature and with high metal loadings. The acidic supports in combination with Ru metal can favor the Cnation of carboxyl. The C–C bond cleavage derived from the decarbonylation of acyl on the catalyst was studied by the measures of DRIFTS. The APHDO and DRIFTS results demonstrated that the C–C bond cleavage was favored in the order of Ru/C>Ru/ZrO2 >Ru/Al2O3. The catalysts were characterized by multiple methods (H2-TPR, NH3-TPD, CO-FTIR and DRIFTS of propanoic acid). It is concluded that the effect of support on the reaction routes may be attributed to these factors of catalysts, i.e., surface acidity, metal–support interaction and electronic state of Ru species. [Copyright &y& Elsevier]

Abstract: The reactivity of biomass-derived diethyl succinate and its main reaction intermediates was separately investigated in a fixed-bed reactor over CuO/ZnO catalyst, and some interesting results were obtained. Ethyl 4-hydroxybutyl succinate as an intermediate of diethyl succinate hydrogenation reaction was first detected, and it could be converted to 1,4-butanediol or polyesters. Additionally, propanol and butanol are mainly derived from 1,4-butanediol rather than gamma-butyrolactone. A comprehensive reaction pathway for the hydrogenation of diethyl succinate is proposed, which is significant for the design of new catalytic formulations. A CuO/ZnO+HY admixed catalyst exhibiting excellent performance was prepared according to the proposed reaction pathway. [ABSTRACT FROM AUTHOR]

Abstract: Vapor-phase hydrogenolysis of ethyl lactate to 1,2-propanediol was performed over a series of SiO2 supported metal (Fe, Co, Ni, Ru, and Pd) catalysts in a fixed-bed reactor. Among them, the Co/SiO2 and Cu/SiO2 catalysts exhibit promising performance, and the Co/SiO2 were more active than the traditional copper catalysts under mild conditions. Effects of support, metal loading and preparation method were investigated to optimize the performance of the Co-based catalysts. Over the optimal catalyst (a 10wt.% Co/SiO2 catalyst prepared via rotary evaporation drying method), the 1,2-propanediol selectivity was in excess of 98% at 90.2% lactate conversion, 2.5MPa and 160°C. The cobalt catalysts were characterized by X-ray diffraction (XRD) and temperature programmed reduction by H2 (H2-TPR) and temperature programmed desorption of H2 (H2-TPD). Interestingly, a quasi-linear correlation is observed between the average reaction rate and the percentage of bulk-like Co3O4 phase precursors, suggesting that the metallic cobalt from the bulk-like Co3O4 phase precursor is more active than that from the cobalt surface support species. The emerging technologies for production of low-cost lactate ester, make this high-yield route a sustainable benign process for 1,2-propanediol. [Copyright &y& Elsevier]

Background: Danon disease (DD) is a rare x-linked dominant multisystemic disorder with a clinical triad of severe cardiomyopathy, skeletal myopathy, and mental retardation. It is caused by a defect in the lysosomal-associated membrane protein-2 (LAMP2) gene, which leads to the formation of autophagic vacuoles containing glycogen granule deposits in skeletal and cardiac muscle fibers. So far, more than 50 different mutations in LAMP2 have been identified. Case presentation: Here, we report an 18-year-old male patient who was hospitalized for heart failure. Biopsy of the left lateral femoral muscle revealed scattered autophagic vacuoles in the muscle fibers with increased glycogen. Next generation sequencing (NGS) was used to detect gene mutations of the proband sample and a novel frameshift mutation (c.1052delG) has been identified in exon 8 of LAMP2, which leads to truncation of the protein. Conclusion: We found a novel frameshift mutation, a hemizygous mutation (c.1052delG) in exon 8 of LAMP2, identified as presenting the hypertrophic cardiomyopathy (HCM) phenotype. Genetic analysis is the gold standard for the diagnosis of DD and is essential to determine appropriate treatment strategies and to confirm the genetic risk of family members. [ABSTRACT FROM AUTHOR]

• Hydrogen bonds significantly influence structure of solid products in direct coal liquefaction. • Benzene is a stronger OH-π hydrogen bonds acceptor compared to tetralin. • Benzene promotes lengthening of O–H bonds in when hydrogen bonds are formed. • Benzene promotes decomposition of –OH and generation of aryl ether bonds in direct coal liquefaction. Hydrogen bonds play a crucial role in thermal conversion of low rank coal, especially direct coal liquefaction (DCL) because of their wealthy abundance and great influence on generation of light products. Relative distribution of hydrogen bonds was evaluated with in-situ diffuse reflectance infrared Fourier transformation (DRIFT), while visualization analysis of hydrogen bonds (OH-π in particular) between coal and solvents were performed using density functional theory (DFT) and reduced density gradient (RDG) analysis. In terms of their effects, DCL experiments of demineralized Yunnan lignite (DeYN) with/without addition of benzene at 200, 250 and 300 °C were carried out, and oxygen-containing functional groups were investigated by solid-state 13C NMR and in-situ DRIFT. Relative content of OH-π hydrogen bonds increased with temperature rising. Benzene is the stronger hydrogen bonds acceptor compared to tetralin (THN). Conclusions drawn from DCL experiments are consistent with DFT calculations. To be specific, benzene with mass concentration of 2% promotes cleavage of O–H bonds, carboxyl groups and the generation of aryl ether bonds, and the differences caused by benzene are intensified when DCL temperature rises. [ABSTRACT FROM AUTHOR]

• Positive and negative interactions co-exist during co-pyrolysis process. • Positive interaction is mainly caused by the hydrogen supply of MLS. • Negative interaction is ascribed to the heat and mass transfer caused by MLS properties. • Activation energies of co-pyrolysis significantly decrease with MLS dosage increasing. Co-pyrolysis behaviors of MLS with Hami sub-bituminous coal (HM) were examined by a thermogravimetric analyzer coupled with a mass spectrometer and the kinetic characteristics were interpreted with simplified distributed activation energy model, aiming at understanding the co-pyrolysis characteristics and interactions between MLS and coal, and providing some useful guidance for the efficient utilize of MLS. Two special crucible reactors with or without a vertical baffle were made to investigate the interactions between MLS and HM during co-pyrolysis. Results show that the amount of C–H bonds in MLS is more abundant, but the oxygen-containing functional groups are less compared with HM. The pyrolysis reactivity of MLS is higher than that of HM, and that of blends increases with the MLS dosage increasing. The co-pyrolysis behaviors including weight loss, weight loss rate and the gas emission characteristics of MLS and HM in the two crucibles were compared, and it is found that the different results are related to pyrolysis temperature and MLS dosage. The role of promoting release of volatiles is mainly caused by the hydrogen supply from MLS and the opposite effect is mainly ascribed to the heat and mass transfer caused by low softening point and strong cohesiveness of MLS. In addition, the activation energies of co-pyrolysis of the blends significantly decrease with the increase of MLS dosage. [ABSTRACT FROM AUTHOR]

• Presenting an overview of MS in cosmetic analysis over the past two decades. • Detailed demonstration of current sample preparation and ionization techniques. • Offering a concise outlook on future development of MS in cosmetic analysis. Mass spectrometry (MS) is a crucial tool in cosmetic analysis. It is widely used for ingredient screening, quality control, risk monitoring, authenticity verification, and efficacy evaluation. However, due to the diversity of cosmetic products and the rapid development of MS-based analytical methods, the relevant literature needs a more systematic collation of information on this subject to unravel the true potential of MS in cosmetic analysis. Herein, an overview of the role of MS in cosmetic analysis over the past two decades is presented. The currently used sample preparation methods, ionization techniques, and types of mass analyzers are demonstrated in detail. In addition, a brief perspective on the future development of MS for cosmetic analysis is provided. [ABSTRACT FROM AUTHOR]

Flavonoids play important roles in root development and in its tropic responses, whereas the flavonoids-mediated changes of the global transcription levels during root growth remain unclear. Here, the global transcription changes in quercetin-treated rice primary roots were analyzed. Quercetin treatment significantly induced the inhibition of root growth and the reduction of H2O2 and O2− levels. In addition, the RNA-seq analysis revealed that there are 1243 differentially expressed genes (DEGs) identified in quercetin-treated roots, including 1032 up-regulated and 211 down-regulated genes. A gene ontology (GO) enrichment analysis showed that the enriched GO terms are mainly associated with the cell wall organization, response to oxidative stress, and response to hormone stimulus. The Kyoto Encyclopedia of Genes and Genomes (KEGG) enrichment pathway analysis showed that the enriched DEGs are involved in phenylpropanoid biosynthesis, glutathione metabolism, and plant hormone signal transduction. Moreover, the quercetin treatment led to an increase of the antioxidant enzyme activities of catalase (CAT), peroxidase (POD), and superoxide dismutase (SOD) in rice roots. Also, the quercetin treatment altered the DR5:GUS expression pattern in the root tips. All of these data indicated that the flavonoids-mediated transcription changes of genes are related to the genes involved in cell wall remodeling, redox homeostasis, and auxin signaling, leading to a reduced cell division in the meristem zone and cell elongation in the elongation zone of roots. [ABSTRACT FROM AUTHOR]

Abstract Circular RNAs (circRNAs) have recently been considered as key regulators in carcinogenesis. Nevertheless, the study of circRNAs involved in non-small cell lung cancer (NSCLC) remains largely unclear. In this study, we aim to explore the clinical significance, regulatory effect and mechanism of circ-FOXM1 in NSCLC. The results indicated that circ-FOXM1 overexpression was observed in NSCLC tissues and closely associated with lymph node invasion, higher TNM stage, and unfavorable prognosis. Furthermore, knockdown and ectopic expression of circ-FOXM1 significantly inhibited and promoted the growth, migration and invasion of NSCLC cells, respectively. Mechanistically, miR-1304-5p was discovered as a direct target of circ-FOXM1. Circ-FOXM1 upregulated the level of pancreatic progenitor cell differentiation and proliferation factor (PPDPF) and metastasis-associated in colon cancer 1 (MACC1) by sponging miR-1304-5p, thereby increasing the proliferation and invasion of NSCLC cells. Taken together, this work revealed that circ-FOXM1/miR-1304-5p/PPDPF/MACC1 signaling was essential for the development and progression of NSCLC. Highlights • Circ-FOXM1 is upregulated in NSCLC tissues and cell lines. • Circ-FOXM1 functions as an oncogene in NSCLC cells. • Circ-FOXM1 sponges miR-1304-5p to regulate PPDPF and MACC1 expression at post-transcriptional level. • The oncogenic role of circ-FOXM1 is dependent on its regulation of PPDPF and MACC1. [ABSTRACT FROM AUTHOR]

One‐step catalytic conversion of fructose to furfuryl alcohol (FOL) is not only a challenge task but also to open a new pathway for conversion of hexose into useful chemicals. The favorable yield (41.6 %) of FOL can be directly obtained from fructose over the tandem of HY zeolite and Pd/Al2O3. However, the Pd/montmorillonite (Pd/MMT) was deactivated for production of FOL. The proportion of available Pd active sites (i. e. facets, corners and edges) vary with different supports, and the strong metal support interaction (SMSI) plays the pivotal role on the catalytic performance. For Al2O3 support, exposure of Pd (111) plane allows the hydroxymethylfurfural (HMF) to bind on the Pd (111) surface via planar arrangement. In this stance, the aldehyde group of HMF is readily eliminated by decarbonylation. Conversely, for Pd/MMT, the decarbonylation is completely inhibited due to the HMF absorbs on corner sites in perpendicular orientation. The XPS studies indicate that the density electron of Pd nanoparticles (NPs) could be manipulated by various supports, and the electron‐donating effect of Al2O3 was observed. The collaborative effects between available sites and density electron of Pd are observed with respect to the different binding modes of HMF on the surface of Pd. The electronegative Pd NPs facilitate the decarbonylation of HMF as a consequence of the different adsorption strength between furan ring and aldehyde group. [ABSTRACT FROM AUTHOR]

Abstract Preheating stage is of significance for direct coal liquefaction process, especially for the low-rank coals, with high reactivity and suitable for direct coal liquefaction. Properties of solvents used in preheating stage could greatly affect structure of coal and conversion of its oxygen-containing functional groups. In this work, the preheating process of one Chinese Yunnan lignite (YN lignite) was conducted in tetralin (THN) and 1-methylnaphthalene (1-MN) to figure out the interactions between YN lignite and nonpolar aromatic solvents. In-situ diffuse reflectance infrared Fourier transformation (DRIFT) technique coupled with curve-fitting analysis and ion-exchange titration analysis and solid-state 13C NMR were used to investigate the structural changes of YN lignite when preheated in different solvents at different temperatures. Additionally, swelling ratio determination and density function theory (DFT) calculation were employed to evaluate the strength of interactions existing between YN lignite and THN or 1-MN. The results show that, the decrease of oxygen-containing functional groups and increase of aromaticity occur when YN lignite are preheated in THN and 1-MN, and these changes are intensified with temperature rising. Moreover, THN and 1-MN have different effects on variation of YN lignite, especially for phenolic hydroxyl groups, which are more likely to be decomposed in THN, while carboxyl groups break down more easily in 1-MN at 200–300 °C. DFT calculation and swelling ratio results show that stronger noncovalent interactions (OH π hydrogen bonds in particular) between THN and YN lignite result in weaker O H bond in phenolic hydroxyl groups and subsequently decomposition of more phenolic hydroxyl groups compared to 1-MN. [ABSTRACT FROM AUTHOR]

Abstract Tris (2-chloroethyl) phosphate (TCEP) is a typical phosphate flame retardant. Its potential adverse health effects have recently aroused concern. We investigated the seasonal variations of TCEP concentrations in the raw, finished and tap water samples from two drinking water treatment plants (DWTPs) in China, and evaluated the cytotoxicity and apoptosis/necrosis of organic extracts (OEs) in water samples. We enriched TCEP and OEs in water samples by solid-phase extraction method. The TCEP concentrations in water samples were determined by gas chromatography–mass spectrometry. Normal human liver cell line L02 was treated with OEs in the water samples, and then the cytotoxicity and apoptosis/necrosis were measured by 3-(4, 5-dimethyithiazol-2-yl)-2,5-diphenyl-tetrazolium bromide assay and flow cytometry, respectively. The results showed that cytotoxicities of OEs in raw water samples from both DWTPs in summer and winter were stronger than those in spring and autumn, cytotoxicity of OEs in finished and tap water samples from both DWTPs in summer and autumn were stronger than those in spring and winter. In all seasons, the maximal concentrations (100 mL water/mL cell culture) of OEs in the raw water samples from both DWTPs induced late apoptosis/necrosis. The reasons for seasonal variations of TCEP in water samples and potential toxic effects of other pollutants in the water samples need to be further investigated. Graphical abstract Unlabelled Image [ABSTRACT FROM AUTHOR]

Abstract The tautomer distributions of d ‑fructose, a popular model compound for biorefinery, in various lower alcohols and DMSO‑ d 6 (ROHs/DMSO‑ d 6) mixtures at 298 K were investigated by quantitative 13C NMR. The tautomer distributions of d ‑fructose in ethanol/DMSO‑ d 6 and methanol/DMSO‑ d 6 with different volume ratios of alcohols to DMSO‑ d 6 were also examined. For these normal alcohols (methanol, ethanol, n ‑propanol and n ‑butanol)/DMSO‑ d 6 , the tautomer distribution of d ‑fructose in methanol/DMSO‑ d 6 exhibited the shortest equilibration time (46 h) and the lowest concentration of β‑furanose (39.0%) at equilibrium. The fraction of fructofuranose (α‑furanose and β‑furanose) at equilibrium and time needed to reach equilibrium in branched chain alcohols/DMSO‑ d 6 obey the following order: 2‑propanol/DMSO‑ d 6 (62.2%, 320 h) > tert ‑butanol/DMSO‑ d 6 (61.6%, 307 h) > 2‑butanol/DMSO‑ d 6 (60.6%, 216 h) > isobutanol/DMSO‑ d 6 (57.8%, 134 h). For the diols/DMSO‑ d 6 , the time for the tautomer distribution of d ‑fructose to reach the equilibrium was found to be: 1,4‑butanediol/DMSO‑ d 6 (113 h) > 1,2‑propanediol/DMSO‑ d 6 (38 h) > ethylene glycol/DMSO‑ d 6 (36 h). For ethanol/DMSO‑ d 6 and methanol/DMSO‑ d 6 with respectively different volume ratios, the experimental results showed that the high concentration of ethanol or methanol increases the conversion rate of tautomers. Graphical abstract Unlabelled Image Highlights • Tautomer distributions of d ‑fructose in ROHs/DMSO‑ d 6 were investigated by 13C qNMR. • The effects of volumetric ratios between ethanol or methanol and DMSO‑ d 6 on tautomerization of d ‑fructose were examined. • Significant differences in the tautomer distributions of d ‑fructose in lower alcohols/DMSO‑ d 6 have been observed. • High concentration of ethanol or methanol increases the conversion rate of tautomers. [ABSTRACT FROM AUTHOR]

The selective synthesis of furfural or hydroxymethylfurfural (HMF) from fructose on single catalyst (Beta zeolite, Hβ) is challenging task. However, in this study, selectivity of Hβ zeolite was discovered easily to tune by solvent effects. Strong solvent effects on the selectivity of fructose conversion were observed in different manners depending on the solvent used. It was shown that the coordinated state of framework aluminum, induced by solvent effects, has a major impact on the selectivity. The solvents with amide group were discovered to induce the reversible tetrahedral-octahedral framework aluminum transformation, but the configuration of aluminum was no influenced by other solvents such as γ-butyrolactone (GBL). Compared with other solvents, the GBL was not able to enhance turnover frequency (TOF) value of reaction but also suppress the degradation of furfural. Interestingly, a considerable yield of furfural (50.25%) was obtained combined with tetrahedral and octahedral framework aluminum active sites in GBL, while high selectivity of HMF (83.3%) was achieved in presence of single tetrahedral framework aluminum over Hβ in NMP. [ABSTRACT FROM AUTHOR]

• Introduction of Sn leads to an increase in Lewis acidity of ZSM-5. • Enhanced Lewis acidity facilitates Diels-Alder reaction during co-feeding methanol with 2-methylfuran. • Hierarchical Sn-MFI shows fine aromatics selectivity and catalytic stability. • Individual conversion of methanol is partly inhibited during co-reaction with 2-methylfuran. • Cycloaddition of furans with alkene is the rate-determining step for Diels-Alder reaction. It is of great interest to explore sustainable routes for producing aromatics from renewable biomass resources. Herein, co-aromatization of 2-methylfuran (2-MF) with methanol was investigated at 500 °C over the hierarchical Sn-containing ZSM-5 zeolites. The results demonstrated that the Sn-containing samples showed higher aromatics selectivity than the Sn-free counterpart, due to that the increase of Lewis acidic sites caused by Sn incorporation contributed to Diels-Alder (DA) reaction of 2-MF with alkenes. The Sn-containing ZSM-5 was modified by the alkaline treatment to form hierarchical structure. The newly formed mesopores facilitated the mass transport and promoted coke tolerance capacity, thus greatly improving aromatics selectivity and catalytic stability. In addition, the route of aromatics formation were detailed by isotopic experiment and theoretical calculations. The results showed that the individual conversion of 2-MF, alkene/aromatics methylations and DA reaction might co-occur during co-feeding of 13C-methanol with 2-MF, while the individual conversion of 13C-methanol reaction seems to be partly inhibited. The theoretical calculations disclosed that the cycloaddition of furans with alkene was the rate-determining step for aromatics formation via the DA route. [ABSTRACT FROM AUTHOR]

Tris (2-chloroethyl) phosphate (TCEP) has been widely used as a plasticizer and flame retardant. TCEP as a potential carcinogen is often detected in the occupational and nature environments. To investigate effects of TCEP on human hepatocytes, we assessed cell growth rate, cellular membrane integrity, senescence-associated β-galactosidase (SA-β-Gal) activity and analyzed expression of regulators involved in the p53-p21 Waf1/Cip1 -Rb pathway in TCEP-treated L02 cells. The results showed TCEP increased the percentage of SA-β-Gal positive cells, decreased IL-6 levels, down-regulated the regulators of p38MAPK-NF-κB pathways, but up-regulated the regulators of p21 Waf1/Cip1 -Rb pathway in L02 cells. Furthermore, we measured the SA-β-Gal activity and expression of regulators involved in the p53-p21 Waf1/Cip1 -Rb pathway in L02 −p53 cells and p53-null Hep3B cells. Similar results were found in L02 −p53 cells and Hep3B cells. The findings demonstrated that TCEP induced senescence-like growth arrest via the p21 Waf1/Cip1 -Rb pathway in a p53-independent manner, without activation of the IL-6/IL6R, p38MAPK-NF-κB pathways in hepatocytes. [ABSTRACT FROM AUTHOR]

Being a suitable way for achieving the maximum efficiency of atoms, the atomically dispersed metals are playing an ever-increasingly important role in bridging heterogeneous and homogeneous catalysis. It is extremely challenging for dispersing metals in atomic-scales as the applicable high-loading catalysts for industry. The reducible and defective supports or metal surfaces are commonly chosen for anchoring the metals. We here report that atomically-dispersed but high-loading (15 wt%) metals were achieved by covalent-bonding to irreducible SiO 2 (though silanol groups) which is realized by a simple urea hydrolysis assistant hydrothermal-deposition method. The Cu O Si bonding tailors the structural and electronic states of catalyst by maximum of atom efficiency and tuning electronic effects. The intrinsic performance of C O hydrogenation was thus boosted by one- to two- orders-of-magnitude in comparison with impregnated and precipitated catalysts. The choices of metals include Cu, Zn, Ni, Co and Mn, showing potentials for a category of applied materials. [ABSTRACT FROM AUTHOR]

Two kinds of typical mineral-derived Cu/ZnO catalysts consisting of aurichalcite and zincian malachite were introduced for furfural hydrogenation to furfuryl alcohol (FOL) and 2-methylfuran (2-MF) in a fixed-bed reactor. Under proper reaction conditions, high yields of FOL (above 99 %) and 2-MF (94.5 %) could be obtained over the aurichalcite Cu/ZnO catalyst (AC-CZ), whereas the best yield of 2-MF was only 76.9 % (0.5 h−1) over the zincian malachite Cu/ZnO catalyst (ZM-CZ). The normalized productivity of 2-MF was 43.5 mol kgCu−1 h−1 and 17.4 mol kgCu−1 h−1 for AC-CZ and ZM-CZ, respectively (LHSV=1.5 h−1). The catalysts were characterized by XRD analysis, Raman spectra, CO IR spectroscopy, H2 temperature-programmed reduction, N2O titration, NH3 temperature-programmed desorption, and X-ray photoelectron spectroscopy. The far better performance of AC-CZ in furfural hydrogenation was ascribed to its higher dispersion of copper species, superior copper surface area, better surface acidity distribution, and stronger Cu0-ZnO synergy. In addition, the surface acidity of the catalysts seemed to have a higher influence on 2-MF production than the Cu surface area, but the optimal balance of both factors still needs to be investigated systematically. [ABSTRACT FROM AUTHOR]

Doping B 2 O 3 to an Ag/SiO 2 catalyst notably improves its activity as well as its stability for the vapor-phase hydrogenation of dimethyl oxalate (DMO) to methyl glycolate (MG). [Display omitted] • 96.1% yield to MG was achieved over Ag-B 2 O 3 /SiO 2 under 180 °C and 0.5 MPa H 2. • Addition of B 2 O 3 can promote the dispersion and stability of Ag NPs on SiO 2 support. • Addition of B 2 O 3 favors the formation of Ag centers with electron-deficient state. • The strong interaction between Ag and boron promotes the activity of the catalysts. A highly active and stable catalyst for the hydrogenation of dimethyl oxalate (DMO) to methyl glycolate (MG) had been developed. The Ag-B 2 O 3 /SiO 2 catalysts were prepared by impregnation method with boric acid (H 3 BO 3). The properties and the structures of the catalysts were fully characterized by BET, XRD, H 2 -TPR, NH 3 -TPD, FTIR, XPS and TEM. Compared with Ag/SiO 2 catalyst, the Ag-B 2 O 3 /SiO 2 catalyst exhibited significantly enhanced catalytic performance and high stability for the hydrogenation of DMO to MG under relatively milder reaction conditions (180 °C, 0.5 MPa). A high yield of 96.1% for MG was achieved over Ag-B 2 O 3 /SiO 2 catalyst, while the yield of MG was only 54.3% over Ag/SiO 2 catalyst. The excellent catalytic performance for Ag-B 2 O 3 /SiO 2 catalyst was attributed to the introduction of B 2 O 3. The addition of B 2 O 3 to Ag/SiO 2 catalyst favored the formation of highly dispersed Ag centers with electron-deficient state, which can strongly bind and activate the ester and acyl groups of DMO in the hydrogenation processes. Besides its effectiveness, the catalyst showed an excellent stability which can be performed for 264 h under the reaction conditions of 180 °C, 0.5 MPa H 2 and the weight space velocity of 0.2 h−1. [ABSTRACT FROM AUTHOR]