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Pyridinium 1,4-zwitterionic thiolates were applied to a formal [3 + 2] annulation reaction with modified activated alkynes, affording various tetrasubstituted thiophenes with aryl, alkenyl, alkyl or silyl group at the special position. The structural modification of alkyne substrates enabled the synthesis of diverse thiophenes to be achieved using the pyridinium 1,4-zwitterionic thiolates as the sulfur-containing building blocks. This approach is metal-free and catalyst-free.

We consider Monge-Ampere equations with the right hand side function close to a positive constant and from a function class that is larger than any Holder class and smaller than the Dini-continuous class. We establish an upper bound for the modulus of continuity of the solution's second derivatives. This bound depends exponentially on a quantity similar to but larger than the Dini semi-norm. We establish explicit bounds regarding the shape of the sequence of shrinking sections, hence revealing the nature of such exponential dependence.

Thanasimus substriatus (Gebler) (Coleoptera: Cleridae) is an important predator of bark beetles (Scolytidae) and has been used in China for the biological control of the larch bark beetle, Ips subelongatus Motschulsky, and the spruce bark beetle, Ips typographus L. In this study, the number, external morphology, and distribution of antennal sensilla of T. substriatus were determined using scanning electron microscopy. The capitate antennae of both sexes consist of the scape, pedicel, and 9 flagellomeres. Two types of sensilla chaetica (SC1 and SC2), 2 types of sensilla trichodea (ST1 and ST2), 3 types of sensilla basiconica (SB1, SB2, SB3), and Böhm's bristles (BB) were identified according to the morphology and fine structure of each type of sensilla in both sexes. No differences in shape, structure, sensilla distribution, and typology were observed between the sexes. The density of sensilla was greater on the last 3 than on the first 8 segments. SC1 and SC2 occurred on all antennal segments in both sexes. SB1 were located only on the last 5 segments of the antennae. SB2 and SB3 were found only on the last 3 segments of the antennae and were absent on the first 8 segments in both sexes. ST1 and ST2 were absent from the scape and pedicel. BB only occurred on the scape and pedicel. The distal antennal sensilla of T. substriatus had notably more sensilla than proximal ones in type and number, indicating this is the main area to detect environmental stimuli for feeding or oviposition.

In August 2018, a remarkable polynya was observed off the north coast of Greenland, a perennial ice zone where thick sea ice cover persists. In order to investigate the formation process of this polynya, satellite observations, a coupled ice-ocean model, ocean profiling data, and atmosphere reanalysis data were applied. We found that the thinnest sea ice cover in August since 1978 (mean value of 1.1 m, compared to the average value of 2.8 m during 1978−2017) and the modest southerly wind caused by a positive North Atlantic Oscillation (mean value of 0.82, compared to the climatological value of −0.02) were responsible for the formation and maintenance of this polynya. The opening mechanism of this polynya differs from the one formed in February 2018 in the same area caused by persistent anomalously high wind. Sea ice drift patterns have become more responsive to the atmospheric forcing due to thinning of sea ice cover in this region.

With the outstanding mechanical properties, van der Waals (vdW) materials have attracted extensive attention in the research of straintronics in the past decade. In this perspective, we first review the recent progresses of the straintronics with vdW materials based on three different lattice deformation modes, i.e., in-plane strain, out-of-plane strain, and heterostrain. Then we discuss the current technique challenges in this field, and finally provide our perspectives on future research directions for both fundamental physics and electronic applications.

The synthesis of two kinds of five-membered organosulfur heterocycles (i.e., 1,4,2-oxathiazoles and 1,3,4-thiadiazoles) from α-enolic dithioesters with active 1,3-dipoles (nitrile oxides and nitrilimines) generated in situ was achieved under mild reaction conditions. This transformation further expands the synthetic application of α-enolic dithioesters as the sulfur-containing building blocks.

Cross-dehydrogenative coupling reactions provide a method to construct new chemical bonds by direct C–H activation without any pre-functionalization. Compared to functionalization of a C–H bond α- to ether oxygen, α- to carbonyl, or at a benzylic position, functionalization of unactivated hydrocarbons is difficult and often requires high temperatures, a transition-metal catalyst, or a superstoichiometric quantity of volatile, toxic, and explosive tert-butylhydroperoxide. Here, a cross-dehydrogenative C–O coupling reaction of N-hydroxyphthalimide with unactivated alkanes, nitriles, ethers, and thioethers has been realized by using iodobenzene diacetate as the radical initiator. The current protocol enables efficient functionalization of unactivated hydrocarbons and nitriles through inert C(sp3)–H bond activation under mild reaction conditions. O-substituted NHPI derivatives are generated in good yields under metal-free conditions. Robust and selective C–H functionalisation of alkanes remains a challenge. Here, iodine(III) mediates the radical coupling of N-hydroxyphthalimide and unactivated C(sp3)–H bonds in a range of cyclic and acyclic alkanes.

This paper considers screening of adaptive interventions or adaptive treatment strategies embedded in a sequential multiple assignment randomized trial (SMART). As a SMART typically consists of numerous adaptive interventions, inferential procedures based on pairwise comparisons of all interventions may suffer substantial loss in efficiency after accounting for multiplicity. We propose simultaneous confidence intervals that compare the values of interventions of interest to that of the unknown best intervention by generalizing the method in Edwards and Hsu (1983). The multiple comparison with the best (MCB) intervals are applied as screening tool: an intervention with MCB interval excluding zero will be declared as inferior to the true best at a pre-specified confidence level, and hence excluded from further exploration. Simulation studies show that the proposed method outperforms the multiple comparison procedures based on Bonferroni’s correction in terms of width of confidence intervals for estimation. The method is applied to analyze data from the CODIACS trial in patients with depression.

A large amount of light crude oils have been found within 4000 to 7000 m deep strata of Cambrian, Ordovician, and Silurian reservoirs in the Tarim Basin, NW China. To enhance the understanding of parental materials of deep oils, a set of high-quality source rocks from the Yuertusi Formation in well Luntan 1 (maximum drilling depth of 8882 m) was studied in terms of their sedimentary condition and mechanism of organic matter enrichment. Total organic carbon (TOC) content, carbon isotope of kerogen (δ13Cker), and major and trace elements of the rocks from the Sinian Qigebulake, Cambrian Yuertusi, and Xiaoerbulake Formations in well Luntan 1 were analysed. The results showed that the δ13Cker value of the Yuertusi Formation barely changed with an average of -31.19‰. High TOC contents accompanied by enrichments of the bioessential trace elements, such as cadmium, chromium, copper, nickel, and zinc, occurred in the lower part of the Yuertusi Formation. Excess barium (Baxs) and phosphorus concentrations revealed high primary productivity during the deposition of the Yuertusi Formation. Moreover, variations in the enrichment factors of molybdenum, uranium, and vanadium and molybdenum-uranium covariation pattern indicated suboxic-anoxic conditions in the Qigebulake Formation, anoxic-euxinic conditions in the Yuertusi Formation, and suboxic-oxic conditions in the Xiaoerbulake Formation. The TOC contents were significantly correlated with the paleoproductivity and paleoredox parameters, indicating that high productivity and reducing conditions jointly controlled the organic matter accumulation and preservation in well Luntan 1.

In this paper, we introduce the concept of l-order and conjecture that the l-order of hazard rate vectors of components implies the likelihood ratio order of parallel systems. We prove this conject...

An efficient annulation reaction of aurone-derived α,β-unsaturated imines and activated terminal alkynes mediated by triethylamine is described, which enables the facile synthesis of 1,4-dihydrobenzofuro[3,2-b]pyridines in high yields. When the nucleophile of triethylamine was replaced with triphenylphosphine, another class of 1,4-dihydrobenzofuro[3,2-b]pyridines tethered with an additional acrylate motif were obtained instead. These two types of 1,4-dihydrobenzofuro[3,2-b]pyridines could be aromatized in the presence of DBU to afford benzofuro[3,2-b]pyridines, which could also be accessed via a one-pot procedure.

HighlightsAERMOD and SCIPUFF were employed to back-calculate farm-level PM10 emission rates based on inverse modeling.Both AERMOD and SCIPUFF did not capture the diurnal and seasonal variations of farm-level PM10 emission rates.AERMOD modeling results were affected by wind speed, with higher wind speed leading to higher emission rates.Higher numbers of receptors and PM10 measurements with greater time resolution may be recommended in the future.Abstract. Air pollutant emissions from animal feeding operations (AFOs) have become a serious concern for public health and ambient air quality. Particulate matter with aerodynamic equivalent diameter less than or equal to 10 µm (PM10) is one of the major air pollutants emitted from AFOs. To assess the impacts of PM10 emissions from AFOs, knowledge about farm-level PM10 emission rates is needed but is challenging to obtain through field measurements. The inverse dispersion modeling approach provides an alternative way to estimate farm-level PM10 emission rates. In this study, two dispersion models, AERMOD and SCIPUFF, were employed to back-calculate farm-level PM10 emission rates based on hourly PM10 concentration measurements at four downwind locations in the vicinity of a commercial egg production farm in the southeast U.S. Onsite meteorological data were simultaneously recorded using a 10 m weather tower to facilitate the dispersion modeling. The modeling results were compared with PM10 emission measurements from two layer houses on the farm. Single-area source, double-area source, and double-volume source were used in AERMOD, while only single-point source was used in SCIPUFF. The inverse modeling results indicated that both SCIPUFF and AERMOD did not capture the diurnal and seasonal variations of the farm-level PM10 emission rates. In addition, the AERMOD modeling results were affected by wind speed, and higher emission rates may be predicted at higher wind speeds. The single-point source for SCIPUFF, the plume rise simplification for AERMOD, and insufficient concentration measurement resolution in response to temporal changes in wind direction may have added uncertainties to the modeling results. The results of this study suggest that more receptors covering more representative downwind locations should be considered in future modeling for farm-level emissions assessment. Moreover, ambient data collection with greater time resolution (e.g., less than one hour) is recommended to capture diurnal and seasonal patterns more rigorously. Only in this way can researchers achieve a better understanding of the effectiveness of inverse dispersion modeling for estimation of pollutant emission rates. Keywords: AERMOD, Animal feeding operations, Egg production, Farm-level emission rate, Inverse dispersion modeling, PM10, SCIPUFF.

A facile access to thiazolidin-4-ones from α-enolic dithioesters and α-halohydroxamates in situ derived active 1,3-dipolar aza-oxyallyl cations was achieved under mild conditions. These five-membered heterocycles with Z-exocyclic double bonds and diverse substituents can be readily obtained via a regio- and stereoselective formal [3+2] cycloaddition pathway.

Urban residents are suffering from serious thermal stress resulting from urban heat island and global warming. Investigators have explored several methods to address this issue. Vegetation, especially trees, were found to play a vital part in urban environments. It produces a cooling effect by reducing temperature and radiation levels. To find thermal performances of trees in detail, this study physically measured two urban parks during August 2019 in a satellite city of China regarding their thermal environments relevant to tree planting indices. There were three planting indices used, sky view factor, leaf area index and enclosure area. Through associating them with thermal indicators by linear regression, all of the indices were confirmed to have significant thermal effects. Every 0.1 increase in sky view factor resulted in an increase of 1°C air temperature, 0.16 m/s air velocity, 40 W/m2 solar radiation level and 1.6°C mean radiant temperature. Same effects were found in nearly 0.4 leaf area index decrease and approximately 20 m2 enclosure area increase. These results provide very optimistic directions for future urban forestry planning and landscaping.

The synthesis of 3,4-dihydro-2H-1,3-thiazines from α-enolic dithioesters and 1,3,5-triazinanes has been achieved via a formal (3 + 3) annulation reaction under thermal conditions, where 1,3,5-triazinanes were utilized as three-atom synthons. This transformation is catalyst-free and additive-free.

A novel compound zoanone A (1), together with eight new alkaloids, 3β,14α-dihydroxy-28-deoxyzoanthenamine (2), 7α-hydroxy-28-deoxyzoanthenamine (3), 3α-hydroxyzoanthenamine (4), 7β-hydroxyzoanthena...

The effect of doping different contents of Ni on the thermal stability of Cu(Ni) alloy films has been investigated. Cu(Ni) films with different Ni contents were deposited on SiO2/Si substrates by magnetron sputtering, then annealed in vacuum at 350°C to 650°C for 0.5 h. X-ray diffraction analysis and resistance measurements revealed that high-resistance copper silicide was formed after annealing at 450°C for the Cu(Ni, 1.66 at.%) and Cu(Ni, 9.16 at.%) samples. However, no copper silicide was observed for Cu(Ni, 3.59 at.%) even after annealing at 650°C. Transmission electron microscopy provided evidence for a ∼ 25-nm self-formed barrier layer at the Cu/SiO2 interface with Cu(Ni, 3.59 at.%). The failure to form a diffusion barrier for the Cu(Ni, 1.66 at.%) sample resulted from its low Ni doping concentration, which was insufficient to produce such a self-formed layer during annealing. The barrier failure was caused by grain refinement due to the increased Ni content, providing diffusion channels for atom diffusion. The results clearly suggest that addition of an appropriate amount of Ni can improve the thermal stability of Cu(Ni)/SiO2/Si interconnect structure materials.

Snow and ice were monitored by thermistor-string-based Snow and Ice Mass Balance Array (SIMBA) in Lake Orajärvi in northern Finland. An existing automatic SIMBA-algorithm was further developed to derive air/snow, snow/ice and ice/water interfaces based on the SIMBA environment temperature (ET) profiles. The identified interfaces agreed with in situ observations made in 2011/12 winter season. The method was capable to identify upward-moving snow/ice interface that was also visible from SIMBA heating temperature (HT) profiles, which responds to differences in the thermal diffusivities of air, snow, ice and water. The SIMBA data obtained in winters 2017/18 and 2018/19 were used to investigate snow and ice mass balance. An upward-moving snow/ice interface was detected as a result of meteoric ice (snow ice and superimposed ice) formation. Snow contributed to granular lake ice formation up to 40–55% of the total ice thickness on the seasonal mean. Heavy snowfalls and low air temperature in early winter are favourable for granular ice formation. The seasonal mean snow depth on nearby land was 2.7–2.9 times of that on the lake. The estimation of freeboard from snow and ice mass-balance measurement is sensitive to the snow density. Accurate ice freeboard calculation is still a challenge.

Two reaction modes of pyridinium 1,4-zwitterionic thiolates with sulfenes generated in situ from alkanesulfonyl chlorides are described with DIPEA as the base. 3H-1,2-Dithiole 2,2-dioxides could be...

Interlayer interaction could substantially affect the electrical transport in transition metal dichalcogenides, serving as an effective way to control the device performance. However, it is still challenging to utilize interlayer interaction in weakly interlayer-coupled materials such as pristine MoS2 to realize layer-dependent tunable transport behavior. Here, we demonstrate that, by substitutional doping of vanadium atoms in the Mo sites of the MoS2 lattice, the vanadium-doped monolayer MoS2 device exhibits an ambipolar field effect characteristic, while its bilayer device demonstrates a heavy p-type field effect feature, in sharp contrast to the pristine monolayer and bilayer MoS2 devices, both of which show similar n-type electrical transport behaviors. Moreover, the electrical conductance of the doped bilayer MoS2 device is drastically enhanced with respect to that of the doped monolayer MoS2 device. Employing first-principle calculations, we reveal that such striking behaviors arise from the presence of electrical transport networks associated with the enhanced interlayer hybridization of S-3pz orbitals between adjacent layers activated by vanadium dopants in the bilayer MoS2, which is nevertheless absent in its monolayer counterpart. Our work highlights that the effect of dopant not only is confined in the in-plane electrical transport behavior but also could be used to activate out-of-plane interaction between adjacent layers in tailoring the electrical transport of the bilayer transitional metal dichalcogenides, which may bring different applications in electronic and optoelectronic devices.

A Fast Ice Prediction System (FIPS) was constructed and is the first regional land-fast sea-ice forecasting system for the Antarctic. FIPS had two components: (1) near-real-time information on the ice-covered area from MODIS and SAR imagery that revealed, tidal cracks, ridged and rafted ice regions; (2) a high-resolution 1-D thermodynamic snow and ice model (HIGHTSI) that was extended to perform a 2-D simulation on snow and ice evolution using atmospheric forcing from ECMWF: either using ERA-Interim reanalysis (in hindcast mode) or HERS operational 10-day predictions (in forecast mode). A hindcast experiment for the 2015 season was in good agreement with field observations, with a mean bias of 0.14 ± 0.07 m and a correlation coefficient of 0.98 for modeled ice thickness. The errors are largely caused by a cold bias in the atmospheric forcing. The thick snow cover during the 2015 season led to modeled formation of extensive snow ice and superimposed ice. The first FIPS operational service was performed during the 2017/18 season. The system predicted a realistic ice thickness and onset of snow surface melt as well as the area of internal ice melt. The model results on the snow and ice properties were considered by the captain of R/VXuelongwhen optimizing a low-risk route for on-ice transportation through fast ice to the coastal Zhongshan Station.

We examine the relative effect of warming events (storms) and snow cover on thermodynamic growth of Arctic sea ice in winter. We use a 1-D snow and ice thermodynamic model to perform sensitivity experiments. Observations from the winter period of the Norwegian young sea ICE (N-ICE2015) campaign north of Svalbard are used to initiate and force the model. The N-ICE2015 winter was characterized by frequent storm events that brought pulses of heat and moisture, and a thick snow cover atop the sea ice (0.3–0.5 m). By the end of the winter, sea-ice bottom growth was negligible. We show that the thermodynamic effect of storms to the winter sea-ice growth is controlled by the amount of snow on sea ice. For 1.3 m initial ice thickness, the decrease in ice growth caused by the warming events ranged from −1.4% (for 0.5 m of snow) to −7.5% (for snow-free conditions). The decrease in sea-ice growth caused by the thick snow (0.5 m) was more important, ranging from −17% (with storms) to −23% (without storms). The results showcase the critical role of snow on winter Arctic sea-ice growth.

Gaussian boson sampling is an alternative model for demonstrating quantum computational supremacy, where squeezed states are injected into every input mode, instead of applying single photons as in the case of standard boson sampling. Here by analyzing numerically the computational costs, we establish a lower bound for achieving quantum computational supremacy for a class of Gaussian boson-sampling problems. Specifically, we propose a more efficient method for calculating the transition probabilities, leading to a significant reduction of the simulation costs. Particularly, our numerical results indicate that one can simulate up to 18 photons for Gaussian boson sampling at the output subspace on a normal laptop, 20 photons on a commercial workstation with 256 cores, and about 30 photons for supercomputers. These numbers are significantly smaller than those in standard boson sampling, suggesting that Gaussian boson sampling could be experimentally-friendly for demonstrating quantum computational supremacy.

In recent years, the regional difference of residential solar panel adoption has raised the concern on energy justice and also elicited a fundamental question on how the distribution of access to s...

To realize energy conservation and environmental protection, solar street lights have been widely used in urban areas in China. To reasonably and effectively utilize solar street lights, the original street lights must be located, and the solar street light potential must be assessed. The Jilin1-03B (JL1-3B) satellite provides next-generation nighttime light data with a high spatial resolution and in three spectral bands. Consequently, the street lights can be extracted from the nighttime light data. We used the road network dataset from the open street map with a specific buffer to extract the road area as a constraint region. Next, the grayscale brightness of JL1-3B images was obtained by integrating all the three bands to locate the street light by using a local maximum algorithm. Then, the values of the original three bands were utilized to classify the types of street lights as high-pressure sodium (HPS) lamps or light-emitting diode lamps. Finally, we simulated the replacement of all the HPS lamps with solar street lights and assessed the corresponding solar energy potential by using the digital surface model data and hourly cloud cover data through the SHORTWAVE-C model. The accuracy of location of the street lights was approximately 90%. Replacing an HPS lamp by one solar street light for 20 years can save 1.85 × 104 kWh of electrical energy, 7.41 t of standard coal, 5.03 t of C emissions, 18.47 t of CO2 emissions, 0.55 t of SO2 emissions, and 0.28 t of NOX emissions.

A phytochemical investigation of Aleurites moluccanus yielded one novel dinor-diterpenoid, aleuritin (1), along with a rare diterpenoid, aleuritone (2). Compound 1 has an unprecedented skeleton with a 6/6/5-fused tricyclic ring system. Compound 2 possesses a rare 6/6/5/3-fused tetracyclic skeleton, which is probably an artifact formed photochemically by the Norrish reaction. The structures of 1 and 2 were determined by spectroscopic methods (ECD, IR, mass, and NMR) and confirmed by single-crystal X-ray diffraction analyses. A plausible biogenetic pathway of 1 is proposed. Pharmacological study showed that these two compounds possessed mild in vitro anti-lymphangiogenic activity, which suppressed tube formation with IC50 values of 48.1 ± 1.8 and 34.2 ± 0.8 μg mL−1, respectively.

Wheat stripe rust can cause considerable yield losses, and genetic resistance is the most effective approach for controlling the disease. To identify the genomic regions responsible for Puccinia striiformis f. sp. tritici (Pst) resistance in a set of winter wheat strains mainly from southwestern China, and to identify DNA markers in these regions, we carried out a genome-wide association study (GWAS) of 120 China winter wheat accessions using single nucleotide polymorphism (SNP) markers from 90K wheat SNP arrays. In total, 16 SNP loci were significantly associated with wheat stripe rust in field and greenhouse trials. Of these, three distinctive SNPs on chromosomes 1B, 4A, and 6A were identified at a site in Mianyang in 2014, where the most prevalent wheat stripe rust races since 2009 have been V26 (G22-9, G22-14). This suggests that the three SNP loci were linked to the new quantitative trait loci (QTL)/genes resistant to the V26 races. Germplasm with immunity to Pst is a good source of stripe rust resistance for breeding, and after further validation, SNPs closely linked to resistance QTLs/genes could be converted into user-friendly markers and facilitate marker-assisted selection to improve wheat stripe rust resistance. Electronic supplementary material The online version of this article (10.1007/s13353-019-00533-8) contains supplementary material, which is available to authorized users.

Exosomes are endogenous vesicles of cells, and can be used as important biomarkers for cancers. In this work, we developed a sensitive and reliable SERS sensor for simultaneous detection of multiple cancer-related exosomes. The SERS detection probes were made of bimetallic SERS-active nanotags, gold-silver-silver core-shell-shell nanotrepangs (GSSNTs), which were composed of bumpy surface nanorod (gold nanotrepang, GNT) cores and bilayer silver shells, and decorated with linker DNAs, which were complementary to the aptamer targeting exosomes. Three kinds of SERS detection probes were designed via the adoption of different Raman reporter molecules and linker DNAs. The capture probes were prepared by modifying specific aptamers of the target exosomes on magnetic beads (MBs). In the absence of target exosomes, SERS detection probes were coupled with MBs via specific DNA hybridization for use as aptamer-based SERS sensors. In the presence of target exosomes, the aptamer specifically recognized and captured the exosomes, and GSSNTs were subsequently released into the supernatant. Therefore, attenuated SERS signals were detected on the MBs, indicating the presence of target exosomes. The proposed aptamer-based SERS sensor is expected to be a facile and sensitive method for the multiplex detection of cancer biomarkers and has potential future applications in clinical diagnosis.

A [3+2] cascade cyclization reaction of pyridinium 1,4-zwitterionic thiolates and activated allenes has been developed, which allows facile access to a library of tetrasubstituted thiophenes with great variety under thermal conditions.

Arctic landfast sea ice (LFSI) represents an important quasi-stationary coastal zone. Its evolution is determined by the regional climate and bathymetry. This study investigated the seasonal cycle and interannual variations of LFSI along the northwest coast of Kotelny Island. Initial freezing, rapid ice formation, stable and decay stages were identified in the seasonal cycle based on application of the visual inspection approach (VIA) to MODIS/Envisat imagery and results from a thermodynamic snow/ice model. The modeled annual maximum ice thickness in 1995–2014 was 2.02 ± 0.12 m showing a trend of −0.13 m decade−1. Shortened ice season length (−22 d decade−1) from model results associated with substantial spring (2.3°C decade−1) and fall (1.9°C decade−1) warming. LFSI break-up resulted from combined fracturing and melting, and the local spatiotemporal patterns of break-up were associated with the irregular bathymetry. Melting dominated the LFSI break-up in the nearshore sheltered area, and the ice thickness decreased to an average of 0.50 m before the LFSI disappeared. For the LFSI adjacent to drift ice, fracturing was the dominant process and the average ice thickness was 1.56 m at the occurrence of the fracturing. The LFSI stages detected by VIA were supported by the model results.

Switchable ring-contractive extrusion reactions of 2,5-dihydro-1,4,5-thiadiazepine S-oxides are described, which allow expedient access to pyridazines under thermal conditions or pyrazoles under Le...

Photoinduced phosphonation of aryl triflates with trialkyl phosphites via a tandem single-electron-transfer, C-O bond cleavage and Arbuzov rearrangement process in the absence of transition-metal and external photosensitizer is reported herein. The protocol features good functional group compatibility and mild reaction conditions, providing various aryl phosphates in good to high yields. Furthermore, this strategy allows the late-stage phosphonation of complex and biologically active compounds.

The bottom topography of ridged sea ice differs greatly from that of other sea-ice types. The form drag of ridge keels has an important influence on sea-ice drift and deformation. In this study, both laboratory experiment (LabE) and fluid dynamics numerical simulation (FDS) have been carried out for a physical ridge model in a tank to better understand the quantitative characteristics of the form drag. The LabEs covered both laminar and turbulent conditions. The local form drag coefficient of a keel, C-dw, varied with the keel depth h(w) and the slope angle alpha(w) in the turbulent regime. After validated by the LabE measurements, the FDSs were employed to extend the parameterization from the finite water depth to deep water. The results gave C-dw = 0.68 center dot ln (alpha(w)/7.8 degrees), R-2 = 0.998, 10 degrees = 0.01), the variation of the local form drag coefficient and its contribution to total drag coefficient were sensitive to the keel slope angle. Assuming the log-normal distribution for this angle, the average value of the local form drag coefficient was 0.75, recommended for sea-ice dynamic models.

Shallow-water delta sandstones in lacustrine basin are widely a concern due to their petroleum exploration potential. However, characteristics such as small thickness, multi-genesis, and multi-stage limit their successful exploration. Here, we present a comprehensive seismic sedimentological research on shallow-water delta in the first member of the Cretaceous Yaojia Formation of Changling area in southern Songliao Basin. The target strata can be divided into 1 third-order sequence and three system tracts. Interpretations of typical stratal slices which were extracted from each system tract indicate that the distributary channel type shallow-water delta is mainly developed in Changling area, two subfacies such as shallow-water delta plain and shallow-water delta front; five main sand bodies such as distributary channel, abandon distributary channel, subaqueous distributary channel, mouth bar, and distal bar are further identified. The type and shape of the sand body are closely related to the degree of sheet modification. Meandering distributary channel, multilevel branching dendritic channel, and lobate subaqueous distributary channel develop at the delta plain, the proximal and distal of the delta front respectively. The study shows that sedimentary characteristics and sedimentary model study based on seismic sedimentology theory provide a powerful theoretical support for lateral reservoir prediction of thin distributary channel type shallow-water lacustrine delta sandstones.

Hot carrier (HC) cooling is a critical photophysical process that significantly influences the optoelectronic performance of hybrid perovskite-based devices. The hot carrier extraction at the device interface is very challenging because of its ultrashort lifetime. Here, ultrafast transient reflectance spectroscopy measurements and time-domain

Eleven new secondary metabolites [kuroshines H-J (1-3), 27-methyl glycinate zoanthenamine (4), 27-hydroxyzoanthenamine (5), 27-methyl glycinate kuroshine A (6), 27-hydroxykuroshine A (7), 3β-hydroxy-28-deoxyzoanthenamine (8), 14α-hydroxy-28-deoxyzoanthenamine (9), 27-hydroxy-28-deoxyzoanthenamine (10), and kuroshine K (11)], along with seven known compounds (12-18), were isolated from the zoantharian Zoanthus vietnamensis. The structures of all isolated components were elucidated by spectroscopic data (IR, MS, NMR, and UV), especially 2D NMR analyses. The relative configurations of 1 and 2 were confirmed by using single-crystal X-ray crystallography. Compounds 1-3 were found to have an unprecedented ether linkage between C-15 and C-28, while the unusual substituent methyl glycinate, attached at C-27 in compounds 4 and 6, was found for the first time in zoanthamine-type alkaloids. The anti-lymphangiogenic activities of 17 isolated compounds were evaluated. Compounds 4, 5, and 10 exerted promising anti-lymphangiogenic functions by reducing cell growth and tube formation of human lymphatic endothelial cells (LECs). In addition, the structure-activity relationships of the isolated alkaloids against lymphangiogenesis of LECs are discussed.

Fine particulate matter (i.e., PM2.5) has gained extensive attention owing to its adverse effects. The impacts of PM2.5 may vary in time and space due to the spatiotemporal variations of PM2.5 number size distribution and chemical compositions. This research analyzed the latest PM2.5 chemical compositions measurements with an aim to better understand the dynamic changes of PM2.5 in response to emission reductions due to the new regulations. The particulate measurements from the Southeastern Aerosol Research and Characterization (SEARCH) network between 2001 and 2016 were analyzed for the spatiotemporal variations of PM2.5 and inorganic PM2.5 (iPM2.5 = SO42− + NH4+ + NO3−) chemical compositions in the Southeastern United States (U.S.). It was discovered that PM2.5 and iPM2.5 mass concentrations exhibited significant downward trends in 2001–2016. Both PM2.5 and iPM2.5 mass concentrations were higher at urban and inland sites than rural/suburban and coastal sites. The higher iPM2.5 concentrations at agricultural sites were attributed to the influences of ammonia (NH3) emissions from animal feeding operations (AFOs). The iPM2.5 was the dominant contributor to PM2.5 in 2001–2016 at the coastal sites, whereas organic carbon matter (OCM) was the major contributor to PM2.5 after 2011 at the inland sites. Our data analysis suggests that significant decrease of PM2.5 concentrations is attributed to the reductions in nitrogen oxides (NOx) and sulfur dioxide (SO2) emissions in 2001–2016. Findings from this research provide insights into the development of effective PM2.5 control strategies and assessment of air pollutants exposure.

By combining femtosecond transient reflectance (TR) spectroscopy and density functional theory (DFT) calculations, we reveal the impact of the length of the organic linkers (HOC2H4NH3+ and C6H5C2H4...

In drilling engineering, it is extremely challenging to drill a prescribed wellbore over several thousand meters. One of the main difficulties arises from accurately predicting and controlling the directional drilling performance, caused by the complex nonlinear dynamics of the slender drilling assembly and its interactions with the surrounding rocks. Nowadays, the simplified analytical geometry method, which has been adopted as the industry standard, can merely offer a rough estimation of the drilling direction, while the high-accuracy finite element method is computationally inefficient. This study is intended to provide a straightforward prediction of the drilling direction for a long drilling distance accurately and efficiently by proposing a dynamical simulation method based on the flexible multibody approach. Three techniques were adopted to achieve the critical objective of the paper. First, an Arbitrary Lagrangian–Eulerian formulation was used to provide a new approach to balance the efficiency and accuracy. Additionally, it can perfectly simulate the realistic drilling operation that drill pipes are continuously added to the drill string one by one through dynamically inserting new beam elements into the existing model. Second, the whole drill string and its interaction with the wellbore were all considered to carry out a high-fidelity simulation. Finally, the bit–rock interaction model was introduced to offer a straightforward way of evaluating the steerability of drilling assemblies. The presented method and model were validated by the consistency between the simulated wellbore trajectory and the in-field experimental data and are ready to be applied in drilling tools design, real-time drilling simulation, and drilling direction control.

Nepenthes plants are regarded as a kind of Traditional Chinese Medicine for several diseases but its anticancer activity remain unclear. The subject of this study is to evaluate the antiproliferation effects on oral cancer cells by Nepenthes plants using ethyl acetate extract of Nepenthes adrianii x clipeata (EANA). Cell viability was detected using MTS assay. Its detailed mechanisms including cell cycle, apoptosis, oxidative stress, and DNA damage were explored by flow cytometry or western blotting. For 24 hours EANA treatment, five kinds of oral cancer cells (CAL 27, Ca9-22, OECM-1, HSC-3, and SCC9) show IC50 values of cell viability ranging from 8 to 17 μg/mL but the viability of normal oral cells (HGF-1) remains over 80%. Subsequently, CAL 27 and Ca9-22 cells with high sensitivity to EANA were chosen to investigate the detailed mechanism. EANA displays the time course and concentration effects for inducing apoptosis based on flow cytometry (subG1 and annexin V analyses) and western blotting [cleaved poly (ADP-ribose) polymerase (c-PARP)]. Oxidative stress and DNA damage were induced by EANA treatments in oral cancer cells through reactive oxygen species (ROS), mitochondrial membrane potential disruption, mitochondrial superoxide, and γH2AX. All these changes of EANA treatments in oral cancer cells were reverted by the ROS scavenger N-acetylcysteine pretreatment. Therefore, EANA induces preferential killing, apoptosis, and DNA damage against oral cancer cells through oxidative stress.

Pd:LaFe0.9Mg0.1O3 is researched as a acetone sensor with high response. The response of sensor expose to 10, 20, 50, 100, 200, 500, 1000 ppb is 1.15, 1.24, 1.45, 1.72, 1.98, 2.57 and 3.28 at 180 °C at normal atmospheric pressure, respectively. This sensor can detect extreme low limit of acetone gas as 10 ppb. The response of sensor under light is also measured, the result indicate that the optimum temperature is reduced and the response at this optimum temperature is promoted. The sensor show excellent selectivity to acetone gas among mixed composition. Experiments prove that since its extreme low detecting limit to acetone gas, the sensor can be used to preliminary judge that if person is diabetic.

The realization of strong magnetoelectric (ME) coupling for efficiently controlling of magnetism is urgently needed but still a significant challenge. Based on first-principle calculations and effective Hubbard models, we demonstrated that the polar charges and locality of edge states in hexagonal BN nanoribbons (BNNRs) play key roles in the behavior of edge magnetism M. By applying a transverse electric field, the magnetism in both zigzag and armchair edges can be regulated sufficiently. In particular, the magnetic on/off switches can be realized in armchair edges, it is robust against various edge decorations including hydrogenation, fluoridation and hydroxylation. Furthermore, uniaxial tensile strains can also produce significant magnetic modulation in Z-BNNRs, which stem from the piezoelectricity. All these suggest that h-BNNRs are ideal platforms for ME coupling researching and promising candidates for functional spintronics application.

Carbon-coated VBO3 on graphene sheets (VBO3/C@G) composite synthesized by freeze-drying method is presented as anode material for lithium-ion batteries. In the final material, VBO3 nanoparticles, which are uniformly coated by amorphous carbon, are either adhered to the surface of graphene sheets or covered by graphene sheets. The amorphous carbon and graphene not only prevent the growth of VBO3 nanoparticles but also provide an excellent conductive 3D network, which is beneficial for the battery performance. The material delivers an initial charge capacity of 787 mAh g−1 at 0.1 C and maintains 697 mAh g−1 after 100 cycles at 0.1 C. It also exhibits an excellent rate performance with a charge capacity of 609 mAh g−1 at 10 C.

VBO3 nanoparticles on graphene sheets (VBO3@G) composite is synthesized by a freeze-drying method as anode material for lithium-ion batteries. After optimization of sintering temperature, reduced graphene oxide (rGO) forms a 3D-framework and VBO3 nanoparticles are adhered to the surface of rGO uniformly. The graphene sheets not only assist the formation of nanoparticles, but also provide an excellent conductive 3D network. It is found that the composite shows a good cycling performance with an initial charge capacity of 779 mAh g−1 at 0.1 C and maintains 610 mAh g−1 after 100 cycles. It also exhibits an excellent rate performance with charge capacities of 592 mAh g−1 at 5 C and 442 mAh g−1 at 10 C.

The SnO2 film deposited at room temperature (RT) on the substrate of Pt/Ti/SiO2/Si is nano-crystallized, which exhibits room temperature ferromagnetism (FM) due to the oxygen vacancies of SnO2 film. The bipolar and multilevel resistive switching (RS) can be observed in the Ta/SnO2/Pt devices, where SnO2 film was deposited at RT. The Ta/SnO2/Pt device has a large ON/OFF ratio (27000) and multilevel RS, which is of great significance for high-density data storage applications. The saturation magnetization of Ta/SnO2/Pt/Ti/SiO2/Si (Ta/SnO2/Pt device) is almost the same as SnO2/Pt/Ti/SiO2/Si, which implies that the influence of Ta top electrodes on the saturation magnetization of Ta/SnO2/Pt/Ti/SiO2/Si is much less. The Ta/SnO2/Pt device shows the non-volatile and reversible saturation magnetization modulation between low resistance state (LRS) and high resistance state (HRS), which results from the formation/rupture of oxygen vacancy filaments. The saturation magnetization at LRS is higher than that at HRS. In addition, the saturation magnetization also enhances with an increase the magnitude of positive DC sweeping voltage. Without DC loop current, the saturation magnetization of Ta/SnO2/Pt increases with an application of positive electric field and drops again with an application of certain negative electric field. The saturation magnetization of Ta/SnO2/Pt can be reversibly modulated in non-volatile by only electric voltage without DC loop current. Such modulation of Ms by only electric voltage without loop DC current is connected with the change in Vo+ density in a certain range of SnO2 films.

A general and efficient protocol was developed for the synthesis of polysubstituted pyridines from propargyl amines and unsaturated carbonyl compounds through a tandem condensation/alkyne isomerization/6 pi 3-azatriene electrocyclization sequence. This process was found to be applicable to a wide range of readily available substrates (30 examples, up to 95 % yield) and could be readily performed on a preparative (20 g) scale. By taking advantage of this method for late-stage pyridine incorporation, we successfully completed the collective total synthesis of suveoline, norsuveoline, and macrophylline.

Erythromycin is necessary in medical treatment and known to be biosynthesized with propionyl-CoA as direct precursor. Oversupply of propionyl-CoA induced hyperpropionylation, which was demonstrated as harmful for erythromycin synthesis in Saccharopolyspora erythraea. Herein, we identified three propionyl-CoA synthetases regulated by propionylation, and one propionyl-CoA synthetase SACE_1780 revealed resistance to propionylation. A practical strategy for raising the precursor (propionyl-CoA) supply bypassing the feedback inhibition caused by propionylation was developed through two approaches: deletion of the propionyltransferase AcuA, and SACE_1780 overexpression. The constructed Δ acuA strain presented a 10% increase in erythromycin yield; SACE_1780 overexpression strain produced 33% higher erythromycin yield than the wildtype strain NRRL2338 and 22% higher erythromycin yield than the industrial high yield Ab strain. These findings uncover the role of protein acylation in precursor supply for antibiotics biosynthesis and provide efficient post-translational modification-metabolic engineering strategy (named as PTM-ME) in synthetic biology for improvement of secondary metabolites.

Secondary inorganic fine particulate matter (iPM2.5) constitutes a significant amount of the atmospheric PM2.5. The formation of secondary iPM2.5 is characterized by thermodynamic equilibrium gas-particle partitioning of gaseous ammonia (NH3) and aerosol ammonium (NH4+). To develop effective strategies for controlling atmospheric PM2.5, it is essential to understand the responses of secondary iPM2.5 to different precursor gases. In southeastern North Carolina, the amount of NH3 is in excess to fully neutralize acidic gases (i.e., NH3-rich conditions). NH3-rich conditions are mainly attributed to the significant NH3 emissions in the region, especially from the large amounts of animal feeding operation (AFO). To gain a better understanding of the impact of NH3 on the formation of secondary iPM2.5 in this area, the responses of iPM2.5 to precursor gases under different ambient conditions were investigated based upon three-year monitoring data of the chemical components in iPM2.5, gaseous pollutants, and meteorological conditions. The gas ratio (GR) was used to assess the degree of neutralization via NH3, and ISORROPIA II model simulation was used to examine the responses of iPM2.5 to changes in the total NH3, the total sulfuric acid (H2SO4), and the total nitric acid (HNO3). It was discovered that under different ambient temperature and humidity conditions, the responses of iPM2.5 to precursor gases vary. In general, iPM2.5 responds nonlinearly to the total NH3 but linearly to the total H2SO4 and the total HNO3. In NH3-rich regions, iPM2.5 is not sensitive to changes in the total NH3, but it is very sensitive to changes in the total H2SO4 and/or the total HNO3. Reducing the total H2SO4, as opposed to the total HNO3 or the total NH3, leads to a significant reduction in iPM2.5 and is thus a more effective strategy for decreasing the concentration of iPM2.5. This research provides insight into controlling and regulating PM2.5 in NH3-rich regions.

We developed a novel fluorescence labelling method to track exosome internalization pathways in cells by confocal microscopy. The proposed method allows evaluation and comparison of the uptake pathways of exosomes originating from different cells, which would offer the potential for understanding the functions of exosomes in intercellular communication and their applications in drug delivery.

An efficient synthetic approach for the spiro-linked [7-5-6-5] all-carbon tetracyclic core derivatives of logeracemin A, a unique dimeric calyciphylline A-type alkaloid, from the known methyl cyclohept-1-ene carboxylate was described. The synthesis features a bioinspired successive Michael/double aldol/dehydration reaction sequence, which might indicate the possibility of a more efficient alternative biosynthetic pathway of logeracemin A.