A “best-of-both-worlds” van der Waals (vdW) density functional is constructed, seamlessly supplementing the strongly constrained and appropriately normed (SCAN) meta-generalized gradient ...approximation for short- and intermediate-range interactions with the long-range vdW interaction from rVV10 , the revised Vydrov–van Voorhis nonlocal correlation functional. The resultant SCAN+rVV10 is the only vdW density functional to date that yields excellent interlayer binding energies and spacings, as well as intralayer lattice constants in 28 layered materials. Its versatility for various kinds of bonding is further demonstrated by its good performance for 22 interactions between molecules; the cohesive energies and lattice constants of 50 solids; the adsorption energy and distance of a benzene molecule on coinage-metal surfaces; the binding energy curves for graphene on Cu(111), Ni(111), and Co(0001) surfaces; and the rare-gas solids. We argue that a good semilocal approximation should (as SCAN does) capture the intermediate-range vdW through its exchange term. We have found an effective range of the vdW interaction between 8 and 16 Å for systems considered here, suggesting that this interaction is negligibly small at the larger distances where it reaches its asymptotic power-law decay.
Recently, we reported that some dairy cows could produce high amounts of milk with high amounts of protein (defined as milk protein yield MPY) when a population was raised under the same nutritional ...and management condition, a potential new trait that can be used to increase high-quality milk production. It is unknown to what extent the rumen microbiome and its metabolites, as well as the host metabolism, contribute to MPY. Here, analysis of rumen metagenomics and metabolomics, together with serum metabolomics was performed to identify potential regulatory mechanisms of MPY at both the rumen microbiome and host levels.
Metagenomics analysis revealed that several Prevotella species were significantly more abundant in the rumen of high-MPY cows, contributing to improved functions related to branched-chain amino acid biosynthesis. In addition, the rumen microbiome of high-MPY cows had lower relative abundances of organisms with methanogen and methanogenesis functions, suggesting that these cows may produce less methane. Metabolomics analysis revealed that the relative concentrations of rumen microbial metabolites (mainly amino acids, carboxylic acids, and fatty acids) and the absolute concentrations of volatile fatty acids were higher in the high-MPY cows. By associating the rumen microbiome with the rumen metabolome, we found that specific microbial taxa (mainly Prevotella species) were positively correlated with ruminal microbial metabolites, including the amino acids and carbohydrates involved in glutathione, phenylalanine, starch, sucrose, and galactose metabolism. To detect the interactions between the rumen microbiome and host metabolism, we associated the rumen microbiome with the host serum metabolome and found that Prevotella species may affect the host's metabolism of amino acids (including glycine, serine, threonine, alanine, aspartate, glutamate, cysteine, and methionine). Further analysis using the linear mixed effect model estimated contributions to the variation in MPY based on different omics and revealed that the rumen microbial composition, functions, and metabolites, and the serum metabolites contributed 17.81, 21.56, 29.76, and 26.78%, respectively, to the host MPY.
These findings provide a fundamental understanding of how the microbiome-dependent and host-dependent mechanisms contribute to varied individualized performance in the milk production quality of dairy cows under the same management condition. This fundamental information is vital for the development of potential manipulation strategies to improve milk quality and production through precision feeding. Video Abstract.
Palladium diselenide (PdSe2), a thus far scarcely studied group‐10 transition metal dichalcogenide has exhibited promising potential in future optoelectronic and electronic devices due to unique ...structures and electrical properties. Here, the controllable synthesis of wafer‐scale and homogeneous 2D PdSe2 film is reported by a simple selenization approach. By choosing different thickness of precursor Pd layer, 2D PdSe2 with thickness of 1.2–20 nm can be readily synthesized. Interestingly, with the increase in thickness, obvious redshift in wavenumber is revealed by Raman spectroscopy. Moreover, in accordance with density functional theory (DFT) calculation, optical absorption and ultraviolet photoemission spectroscopy (UPS) analyses confirm that the PdSe2 exhibits an evolution from a semiconductor (monolayer) to semimetal (bulk). Further combination of the PdSe2 layer with Si leads to a highly sensitive, fast, and broadband photodetector with a high responsivity (300.2 mA W−1) and specific detectivity (≈1013 Jones). By decorating the device with black phosphorus quantum dots, the device performance can be further optimized. These results suggest the as‐selenized PdSe2 is a promising material for optoelectronic application.
This study reports on the wafer‐area synthesis of a high‐quality 2D palladium diselenide (PdSe2) layer through a simple selenization method. Both experimental analysis and theoretical simulation reveal that the PdSe2 film exhibits a gradual transition from a semiconductor (monolayer) to semimetal (bulk). Further combination of PdSe2 with Si leads to a fast and sensitive broadband photodiode, with a high responsivity and specific detectivity.
In this study, bentonite-supported nZVI (B-nZVI) was used as a catalyst to activate H2O2 for atrazine (ATZ) degradation in the presence of FeS2. Results indicated that ATZ degradation by B-nZVI/H2O2 ...process was significantly enhanced when FeS2 was introduced, and nearly 98% of ATZ was degraded by B-nZVI/FeS2/H2O2 process within 60 min under the optimum conditions. ATZ degradation of B-nZVI/FeS2/H2O2 process was much higher than the sum of B-nZVI and FeS2/H2O2 processes. The presence of HCO3−, PO43− and F− exhibited significant negative effects on the ATZ degradation, whereas both Cu2+ and Ni2+ exhibited positive effects on that. Both citric acid (CA) and ethylenediaminetetraacetic acid (EDTA) with lower concentration enhanced ATZ degradation rate, but significant suppression effects on that with higher concentration. The degradation of ATZ and 2,4-Dichlorophenol (2,4-DCP) could be simultaneously achieved in B-nZVI/FeS2/H2O2 process under certain conditions. High soluble Fe2+ induced an excellent decomposition of H2O2 by B-nZVI and FeS2. OH was dominant radical, and contributed to nearly 86% of the overall ATZ removal. A total of five intermediate products of ATZ were identified, and ATZ degradation was achieved via de-alkylation and hydroxylation processes. An enhanced reaction mechanism for ATZ degradation by B-nZVI/FeS2/H2O2 process was proposed, and B-nZVI/FeS2/H2O2 process exhibited an excellect catalytic performance within four successive runs.
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•ATZ degradation by B-nZVI/H2O2 process was enhanced in the presence of FeS2.•High Fe2+ was favorable to H2O2 decomposition by B-nZVI/FeS2/H2O2 process.•OH was dominant radical, and contributed to 86.1% of the overall ATZ removal.•Possible pathways of ATZ degradation were proposed based on intermediate products.•Enhanced mechanism for ATZ degradation by B-nZVI/FeS2/H2O2 process was proposed.
A large nonlinear optical (NLO) coefficient and a wide band gap are two crucial but contradictory parameters that are difficult to achieve simultaneously in a single infrared (IR) NLO compound. A ...salt‐inclusion chalcogenide (SIC), LiLiCs2ClGa3S6 (1), was prepared that presents a nanosized tunnel framework constructed from monotype chalcogenide tetrahedra. Highly oriented covalent GaS4 tetrahedra in the host lead to a moderate second harmonic generation response (0.7 AgGaS2), and ionic guests effectively broaden the band gap to the widest value (4.18 eV) among all IR NLO chalcogenides, thereby achieving a remarkable balance between NLO efficiency and band gap.
The salt‐inclusion chalcogenide LiLiCs2ClGa3S6 is presented, which features a 3D framework composed of Ga3S6 nanosized tunnels. Introduction of an ionic guest to the covalent chalcogenide host produces a material with a moderate nonlinear optical (NLO) coefficient and an ultrawide band gap (Eg). These characteristics are promising for the development of infrared (IR) NLO materials.
Group‐10 layered transitional metal dichalcogenides including PtS2, PtSe2, and PtTe2 are excellent potential candidates for optoelectronic devices due to their unique properties such as high carrier ...mobility, tunable bandgap, stability, and flexibility. Large‐area platinum diselenide (PtSe2) with semiconducting characteristics is far scarcely investigated. Here, the development of a high‐performance photodetector based on vertically aligned PtSe2‐GaAs heterojunction which exhibits a broadband sensitivity from deep ultraviolet to near‐infrared light, with peak sensitivity from 650 to 810 nm, is reported. The Ilight/Idark ratio and responsivity of photodetector are 3 × 104 and 262 mA W−1 measured at 808 nm under zero bias voltage. The response speed of τr/τf is 5.5/6.5 µs, which represents the best result achieved for Group‐10 TMDs based optoelectronic device thus far. According to first‐principle density functional theory, the broad photoresponse ranging from visible to near‐infrared region is associated with the semiconducting characteristics of PtSe2 which has interstitial Se atoms within the PtSe2 layers. It is also revealed that the PtSe2/GaAs photodetector does not exhibit performance degradation after six weeks in air. The generality of the above good results suggests that the vertically aligned PtSe2 is an ideal material for high‐performance optoelectronic systems in the future.
This work shows the large‐area growth of high‐quality vertically aligned PtSe2, and its application to photodetectors based on PtSe2‐GaAs heterojunctions which exhibit a broadband sensitivity to illumination ranging from deep ultraviolet to near‐infrared light, with a peak sensitivity in the region from 650 to 810 nm. The high‐performance broadband photodetector will develop the next‐generation 2D Group‐10 materials based optoelectronic devices.
Tumor associated macrophages (TAMs) are considered with the capacity to have both negative and positive effects on tumor growth. The prognostic value of TAM for survival in patients with solid tumor ...remains controversial.
We conducted a meta-analysis of 55 studies (n = 8,692 patients) that evaluated the correlation between TAM (detected by immunohistochemistry) and clinical staging, overall survival (OS) and disease free survival (DFS). The impact of M1 and M2 type TAM (n = 5) on survival was also examined.
High density of TAM was significantly associated with late clinical staging in patients with breast cancer risk ratio (RR) = 1.20 (95% confidence interval (CI), 1.14-1.28) and bladder cancer RR = 3.30 (95%CI, 1.56-6.96) and with early clinical staging in patients with ovarian cancer RR = 0.52 (95%CI, 0.35-0.77). Negative effects of TAM on OS was shown in patients with gastric cancer RR = 1.64 (95%CI, 1.24-2.16), breast cancer RR = 8.62 (95%CI, 3.10-23.95), bladder cancer RR = 5.00 (95%CI, 1.98-12.63), ovarian cancer RR = 2.55 (95%CI, 1.60-4.06), oral cancer RR = 2.03 (95%CI, 1.47-2.80) and thyroid cancer RR = 2.72 (95%CI, 1.26-5.86),and positive effects was displayed in patients with colorectal cancer RR = 0.64 (95%CI, 0.43-0.96). No significant effect was showed between TAM and DFS. There was also no significant effect of two phenotypes of TAM on survival.
Although some modest bias cannot be excluded, high density of TAM seems to be associated with worse OS in patients with gastric cancer, urogenital cancer and head and neck cancer, with better OS in patients with colorectal cancer.
Biodegradable plastics, as alternatives to conventional plastics, are increasingly used, but their interactions with organic pollutants are still unknown. In this study, the sorption and desorption ...behaviors on a type of biodegradable plastic−poly(butylene adipate co-terephtalate) (PBAT) were investigated, and at the same time two types of conventional plastics−polyethylene (PEc and PEv) and polystyrene (PS) were used for comparison. Phenanthrene (PHEN) was chosen as one of representative organic pollutants. Results indicated that the sorption and desorption capacities of PBAT were not only higher than those of the other types of microplastics, but also higher than those of carbonaceous geosorbents. The surface area normalized results illustrated that sorption and desorption of the microplastics were positively correlated with their abundance of rubbery subfraction. The sorption kinetic results showed that the sorption rates of PBAT and PEc were higher than PEv and PS. The effects of water chemistry factors including salinity, dissolved organic matter and Cu2+ ion on the sorption process displayed the same trend, but the degrees of influence on the four microplastics differed. The degrees of influence were mainly dependent on the abundance of rubbery subfraction for microplastics. These findings indicate that the biodegradable poly(butylene adipate co-terephtalate) microplastics are actually stronger vectors than the conventional microplastics, and crystallization characteristics of the microplastics have great influences on the vector effect.
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•Biodegradable microplastics sorbed/desorbed more PHEN than conventional ones.•Sorption/desorption capacities depended on the content of rubbery subfraction.•Plastic additives didn't alter the microplastics adsorption process.•High salinity and low DOM strengthen the sorption of PHEN onto microplastics.
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