Knowledge graph-derived feed efficiency analysis via pig gut microbiota.

Feed efficiency (FE) is essential for pig production, has been reported to be partially explained by gut microbiota. Despite an extensive body of research literature to this topic, studies regarding the regulation of feed efficiency by gut microbiota remain fragmented and mostly confined to disorganized or semi-structured unrestricted texts. Meanwhile, structured databases for microbiota analysis are available, yet they often lack a comprehensive understanding of the associated biological processes. Therefore, we have devised an approach to construct a comprehensive knowledge graph by combining unstructured textual intelligence with structured database information and applied it to investigate the relationship between pig gut microbes and FE. Firstly, we created the pgmReading knowledge base and the domain ontology of pig gut microbiota by annotating, extracting, and integrating semantic information from 157 scientific publications. Secondly, we created the pgmPubtator by utilizing PubTator to expand the semantic information related to microbiota. Thirdly, we created the pgmDatabase by mapping and combining the ADDAGMA, gutMGene, and KEGG databases based on the ontology. These three knowledge bases were integrated to form the Pig Gut Microbial Knowledge Graph (PGMKG). Additionally, we created five biological query cases to validate the performance of PGMKG. These cases not only allow us to identify microbes with the most significant impact on FE but also provide insights into the metabolites produced by these microbes and the associated metabolic pathways. This study introduces PGMKG, mapping key microbes in pig feed efficiency and guiding microbiota-targeted optimization.

Cu(I) Complexes Catalyzed the Dehydrogenation of N-Heterocycles.

A copper-catalyzed method for the dehydrogenation of various nitrogen-containing heterocycles to furnish quinolines and indoles has been developed. A range of 1,2,3,4-tetrahydroquinolines underwent dehydrogenation by employing 2 mol % of copper complex Cat 3 as a catalyst and using O2 as an oxidant at 120 °C in 1,2-dichlorobenzene to afford the desired quinolines. The method enables the dehydrogenation of a variety of indolines in the presence of 2 mol % of copper complex Cat 2, using 10 mol % of TEMPO as an additive and O2 as an oxidant under room temperature in tetrahydrofuran to furnish indoles in high yields. Mechanistic studies suggested that the dehydrogenative activity is ascribed to the formation of a copper(II) active species from copper(I) complexes oxidized by O2, which was proved by high-resolution mass spectrometry (HRMS). The copper-catalyzed dehydrogenation reaction proceeds via a superoxide radical anion (·O2-) as proved by electron paramagnetic resonance (EPR) spectrometry. In situ infrared spectroscopy revealed that the dihydroquinoline intermediate was formed in the dehydrogenation of 1,2,3,4-tetrahydroquinolines.

Highly asymmetric aldol reaction of isatins and ketones catalyzed by chiral bifunctional primary-amine organocatalyst on water.

Herein, we have reported an environmentally friendly asymmetric aldol reaction between isatins and ketones catalyzed by double-hydrogen-bonded primary amine organocatalysts on water under mild conditions. Enantioenriched 3-hydroxy-2-oxindoles were obtained in high yields (up to 99%) and excellent stereoselectivities (up to 99 : 1 dr and 99% ee) under optimal conditions. Furthermore, the model reaction involving isatin and cyclohexanone was successfully scaled to 10 mmol with no reduction in yield or stereoselectivity. In addition, the catalyst was recovered via simple filtration and was subsequently reused on water, which highlights its good application potential.

Unveiling the Electrocatalytic Activity of the GdBa0.5Sr0.5Co2-xCuxO5+δ (x ≥ 1) Oxygen Electrodes for Solid Oxide Cells.

The A-site cation-ordered GdBa0.5Sr0.5Co2-xCuxO5+δ (GBSCC) double perovskites are evaluated regarding the development of high-performance oxygen electrodes for reversible solid oxide cells (rSOCs). The aims are to maximally decrease the content of toxic and expensive cobalt by substitution with copper while at the same time improving or maintaining the required thermomechanical and electrocatalytic properties. Studies reveal that compositions with 1 ≤ x ≤ 1.15 are particularly interesting. Their thermal and chemical expansions are decreased, and sufficient transport properties are observed. Complementary density functional theory calculations give deeper insight into oxygen defect formation in the considered materials. Chemical compatibility with La0.8Sr0.2Ga0.8Mg0.2O3-δ (LSGM) and Ce0.9Gd0.1O2-δ (GDC) solid electrolytes is evaluated. It is documented that the GdBa0.5Sr0.5Co0.9Cu1.1O5+δ oxygen electrode enables obtaining very low electrode polarization resistance (Rp) values of 0.017 Ω cm2 at 850 °C as well as 0.111 Ω cm2 at 700 °C, which is lower in comparison to that of GdBa0.5Sr0.5CoCuO5+δ (respectively, 0.026 and 0.204 Ω cm2). Systematic distribution of relaxation times analyses allows studies of the electrocatalytic activity and distinguishing elementary steps of the electrochemical reaction at different temperatures. The rate-limiting process is found to be oxygen atom reduction, while the charge transfer at the electrode/electrolyte interface is significantly better with LSGM. The studies also allow elaborating on the catalytic role of the Ag current collector as compared with Pt. The electrodes manufactured using materials with x = 1 and 1.1 permit reaching high power outputs, exceeding 1240 mW cm-2 at 850 °C and 1060 mW cm-2 at 800 °C, for the LSGM-supported cells, which can also work in the electrolysis mode.

Visible-Light-Driven Organocatalytic Alkoxylation of Benzylic C-H Bonds.

A variety of strategies for direct alkoxylation of the benzyl C-H bond have been developed toward the construction of benzyl ethers. The light-induced benzyl C-H bond alkoxylation provides an alternative strategy for the synthesis of these important intermediates. The photocatalyzed alkoxylation of the benzyl C-H bond has dominated by metal-catalyzed methods. Herein, we reported a light-driven organocatalytic approach for alkoxylation of the benzyl C-H bond by the use of 9,10-dibromoanthracene as a photocatalyst and employing N-fluorobenzenesulfonimide as an oxidant. This reaction proceeds at room temperature and is capable of converting a variety of alkyl biphenyl and coupling partners, including a variety of alcohol and carboxylic acid, as well as peroxide, to the desired products under 400 nm light irradiation.

Highly enantioselective one-pot sequential synthesis of valerolactones and pyrazolones bearing all-carbon quaternary stereocentres.

Highly enantiopure and bioactive δ-valerolactones and pyrazolones, bearing α-all-carbon quaternary stereocentres, were successfully and sequentially prepared via a one-pot procedure starting from readily available, inexpensive materials, catalysed by a new chiral squaramide under mild reaction conditions. An organocatalytic Michael reaction afforded the valerolactones, while a one-pot Michael-hydrazinolysis-imidization cascade yielded the pyrazolones. This procedure is economically efficient and environmentally benign.

Micro/Nano Na3V2(PO4)3/N-Doped Carbon Composites with a Hierarchical Porous Structure for High-Rate Pouch-Type Sodium-Ion Full-Cell Performance.

Polyanion-type Na3V2(PO4)3 (NVP) is an overwhelmingly attractive cathode material for sodium-ion batteries (SIBs) because of its high structural stability and fast Na+ mobility. However, its practical application is strongly plagued by either nanoscale particle size or poor rate performance. Herein, a micro/nanocomposite NVP cathode with a hierarchical porous structure is proposed to solve the problem. The microscale NVP material assembled by interconnected nanoflakes with N-doped carbon coating that is capable of simultaneously providing fast carrier transmission dynamics and outstanding structural integrity exhibits precedent sodium-storage behavior. It delivers a superior rate capability (79.1 mAh g-1 at 200C) and excellent long-life cycling (capacity retention of 73.4% after 10 000 cycles at 100C). Remarkably, a pouch-type sodium-ion full cell consisting of the as-obtained NVP cathode and a hard carbon anode demonstrates the gravimetric energy density as high as 212 Wh kg-1 and an exceptional rate performance (71.8 mAh g-1 at 10C). Such structural design of fabricating micro/nanocomposite electrode materials is expected to accelerate the practical applications of SIBs for large-scale energy storage.

Unveiling the Interface Structure of the Exsolved Co-Fe Alloy Nanoparticles from Double Perovskite and Its Application in Solid Oxide Fuel Cells.

Exsolution of catalytic nanoparticles (NPs) from perovskites has arisen as a flexible method to develop high-performance functional materials with enhanced durability for energy conversion and catalytic synthesis applications. Here, we unravel the interface structure of the in situ exsolved alloy nanoparticles from the double perovskite substrate on the atomic scale. The results show that the Co-Fe alloy NPs exsolved topologically from the {100} facets terminations of the Sr2FeMo0.65Co0.35O6-δ (SFMC) double perovskite along ⟨100⟩ directions exhibiting the same orientation and identical crystal structure. The lattice planes of these two phases align and insert into each other at the interface, forming a smooth and continuous coherent connection. The presence of moiré patterns at the interface confirms the topological exsolution mechanism. The coherent interface can significantly reduce the interfacial energy and therefore stabilize the exsolved nanoparticles. Therefore, excellent and stable electrochemical performance of the NP-decorated SFMC perovskite is observed as the anode for solid oxide fuel cells. Our contribution promotes a fundamental understanding of the interface structure of the in situ exsolved alloy nanoparticles from perovskite substrate.

Correction: N-Primary-amine tetrapeptide-catalyzed highly asymmetric Michael addition of aliphatic aldehydes to maleimides.

Correction for 'N-Primary-amine tetrapeptide-catalyzed highly asymmetric Michael addition of aliphatic aldehydes to maleimides' by Zhi-Hong Du et al., Org. Biomol. Chem., 2020, 18, 6899-6904, DOI: 10.1039/D0OB01457E.

N-Primary-amine tetrapeptide-catalyzed highly asymmetric Michael addition of aliphatic aldehydes to maleimides.

The highly asymmetric Michael addition reaction between maleimides and aliphatic aldehydes catalyzed by low-loading ß-turn tetrapeptides with excellent yields and enantioselectivities at room temperature was reported. α-Branched and α-unbranched aldehydes both are suitable nucleophiles. N-Aryl, alkyl and hydrogen maleimides all are well tolerated and led to high yields and enantioselectivities. The transformation can be enlarged to the gram scale without decrease in the yield and enantioselectivity. Furthermore, the succinimides were converted into γ-lactams and γ-lactones, showing good practicality of this work. Some reaction intermediates in the proposed reaction mechanism can be captured with the HR-MS method.

Peptide-Catalyzed Highly Asymmetric Cross-Aldol Reaction of Aldehydes to Biomimetically Synthesize 1,4-Dicarbonyls.

ß-Turn tetrapeptides were demonstrated to catalyze asymmetric aldol reaction of α-branched aldehydes and α-carbonyl aldehydes, i.e. glyoxylates and α-ketoaldehydes, to biomimetically synthesize acyclic all-carbon quaternary center-bearing 1,4-dicarbonyls in high yield and excellent enantioselectivity under mild conditions. The spatially restricted environment of the tetrapeptide warrants high enantioselectivity and yield with broad substrates. Using this protocol, (R)-pantolactone, the key intermediate of vitamin B5, was readily accessed in a practical, efficient, and environmentally benign process from inexpensive starting materials.

Characterization of the physical properties of electron-beam-irradiated white rice and starch during short-term storage.

Electron-beam irradiation (EBI) is a cold sterilization technology used in the irradiation processing of food, including rice. Herein, the effects of EBI on the swelling power, color, pasting, and sensory properties of white rice after short-term storage were analyzed. Samples were electron-beam irradiated at 0, 2, 4, 6, or 8 kGy and stored at 25 °C or 37 °C for up to 75 days. Results showed that swelling power and major pasting viscosities (including peak, breakdown, and setback viscosities) at both storage temperatures decreased with increased irradiation dose. Negative correlations were also observed between the major viscosities of pasting properties and irradiation dose at both storage temperatures. During sensory evaluation, extremely low scores for rice hardness, appearance, taste, and overall acceptability were obtained for rice subjected to high EBI dose (>4 kGy). However, rice stored at 37 °C showed lower performance than rice at 25 °C in terms of the abovementioned parameters. By contrast, the sensory properties at irradiation doses between 2 and 4 kGy were better than those of the control group at both storage temperatures. All these findings indicated the potential of low-dose (<4 kGy) EBI as pretreatment for improving the quality of white rice during storage.

Superior High-Rate and Ultralong-Lifespan Na3V2(PO4)3@C Cathode by Enhancing the Conductivity Both in Bulk and on Surface.

Na3V2(PO4)3 has shown great promise in next-generation cathode materials for sodium-ion batteries owning to its fast Na+ diffusion in the three-dimensional open NASICON framework and high theoretical energy density. However, Na3V2(PO4)3 suffers from undesirable rate performance and unstable cyclability arising from low electronic conductivity. Herein, we propose a facile approach for significantly enhancing the electrochemical properties of Na3V2(PO4)3 by Ti doping at V site and constructing nanoparticle@carbon core-shell nanostructure. This material design provides fast electron conduction network within the whole active particles because of the mixed valence Ti4+/3+ in bulk and highly conductive carbon shell on the surface. Lattice doping and carbon coating reduce the electrode polarization and facilitate the electrode reaction kinetics, while the nanostructure enhances the ionic conduction by shortening the diffusion distance and offers sufficient contact of active particles with organic electrolyte. The multiple synergetic effects enable a superior electrochemical performance. The optimized Na3V1.9Ti0.1(PO4)3@C cathode shows a high specific capacity (116.6 mAh g-1 at 1C), an unprecedented rate performance (93.4 mAh g-1 at 400C), and an exceptional long-term high-rate cycling stability (capacity retention of 69.5% after 14 000 cycles at 100C, corresponding to 0.0002% decay per cycle).

Unveiling the effects of A-site substitutions on the oxygen ion migration in A2-xA'xNiO4+δ by first principles calculations.

The effects of A-site substitutions on the interstitial oxygen formation energy and the migration energy in layered A2-xA'xNiO4+δ (A = selected lanthanides, A' = Ba, Sr, Ca) are investigated by first principles calculations. The interstitial oxygen formation energy is negative, in the range of -4.81 eV to -3.45 eV, strongly supporting easiness of formation of the interstitial oxygen defects in the (A,A')O rock salt plane. The Pr2NiO4+δ compound shows the lowest formation energy, indicating the highest amount of interstitial oxygen. Doping with alkaline earth cations (A') increases the formation energy of the interstitial oxygen, which prefers to be located far away from the dopants. Nevertheless, Ca seems to be the best choice, due to relatively low formation energy. Calculations for the four kinds of diffusion paths allow it to be predicted that the oxygen transport in A2-xA'xNiO4+δ is governed by the interstitialcy mechanism in the ab plane, because of the significantly lower energy barriers for this mechanism. An interesting finding is achieved for A2NiO4+δ (A = Pr, Nd, Sm), for which the energy barriers for the interstitialcy transport are negative (-0.47 eV, -0.33 eV and -0.02 eV, respectively), implying that the transition state is more stable than the assumed initial state. A new structural configuration is proposed in this work, with the adjacent apical oxygen located at the adjacent interstitial site, which shows ca. 0.5 eV lower free energy than that of the initial model. This result provides a new understanding for the location of the interstitial and the adjacent apical oxygens from an energetic point of view and supports previously published experimental data. It is found that alkaline earth doping at the A-site deteriorates the interstitial oxygen diffusion in La2-xA'xNiO4.25 materials, but concerning overall transport properties, Ca seems to be a good dopant from an energetic point of view, when compared with Ba and Sr.

(101) Plane-Oriented SnS2 Nanoplates with Carbon Coating: A High-Rate and Cycle-Stable Anode Material for Lithium Ion Batteries.

Tin disulfide is considered to be a promising anode material for Li ion batteries because of its high theoretical capacity as well as its natural abundance of sulfur and tin. Practical implementation of tin disulfide is, however, strongly hindered by inferior rate performance and poor cycling stability of unoptimized material. In this work, carbon-encapsulated tin disulfide nanoplates with a (101) plane orientation are prepared via a facile hydrothermal method, using polyethylene glycol as a surfactant to guide the crystal growth orientation, followed by a low-temperature carbon-coating process. Fast lithium ion diffusion channels are abundant and well-exposed on the surface of such obtained tin disulfide nanoplates, while the designed microstructure allows the effective decrease of the Li ion diffusion length in the electrode material. In addition, the outer carbon layer enhances the microscopic electrical conductivity and buffers the volumetric changes of the active particles during cycling. The optimized, carbon coated tin disulfide (101) nanoplates deliver a very high reversible capacity (960 mAh g-1 at a current density of 0.1 A g-1), superior rate capability (796 mAh g-1 at a current density as high as 2 A g-1), and an excellent cycling stability of 0.5 A g-1 for 300 cycles, with only 0.05% capacity decay per cycle.

Organocatalytic Enantioselective Cross-Aldol Reaction of o-Hydroxyarylketones and Trifluoromethyl Ketones.

The enantioselective cross-aldol reaction between o-hydroxyacetophenones and trifluoromethyl ketones catalyzed by chiral thiourea organocatalysts is reported. Gram-scale synthesis of the cross-aldol product was carried out, with no decrease in the yield and enantioselectivity. Furthermore, the cross-aldol products thus prepared were used in the preparation of medicinally interesting 3,5-diaryl-5-trifluoromethyl-2-isoxazoline and ß-trifluoromethyl-ß-tertiary hydroxy acid ester with high yield and enantiopurity.

Reversible splenial lesion syndrome in children: Retrospective study and summary of case series.

OBJECTIVE: To describe clinical features of reversible splenial lesion syndrome (RESLES) in children. METHODS: Retrospectively analyzed clinical features of RESLES in children and compared differences between severe and non-severe group, classified by clinical global impression-scale; summarized clinical features of children with mild encephalitis/encephalopathy with a reversible splenial lesion (MERS) from case series. RESULTS: 16 episodes of RESLES occurring in 15 Chinese children were analyzed, with 13 episodes having MERS and 3 episodes with epilepsy. 10 episodes were associated with various pathogens including rotavirus (n=5), adenovirus (n=1), influenza A (n=1), mycoplasma (n=2), and jejunum campylobacter (n=1). The common neurological symptoms included seizure, behavioral changes, altered consciousness and motor deterioration. The lesions of splenium of corpus callosum (SCC), extra-SCC (n=2) or extra-CC (n=1) showed T2-weight and FLAIR hyper-intensity, with the corresponding reduced diffusion. All had complete resolution of radiological changes except 1 episode with small residual. 8 episodes had EEG abnormalities, while elevated white blood count, increased hs-CRP, and hyponatremia were commonly revealed. 7 episodes were given steroid plus therapy, while 3 episodes were treated with antiepileptic drugs. Compared with non-severe group, the number of patients with altered consciousness, EEG abnormalities, motor deterioration, or extra-SCC lesions in severe group was significantly increased. The patients in severe group tended to need longer hospital stay interval. No case caused neurological sequelae, except 1 patient in severe group with recurrent episode and extra-CC lesions having intellectual disability (ID). Five pediatric MERS case series were summarized, including 67 episodes (40 male and 27 female; age ranging 10 m∼13y) from 65 patients, with 33 episodes in Japan, 27 in China, and 7 in Caucasian Australian children, and all patients have a good prognosis except 1 patient with ID (current study). CONCLUSION: Although RESLES in children tend to be a good outcome, the prognosis of patient in severe group, especially with extra-CC lesions, might have neurological sequelae.

MoS2 Nanosheets Vertically Grown on Graphene Sheets for Lithium-Ion Battery Anodes.

A designed nanostructure with MoS2 nanosheets (NSs) perpendicularly grown on graphene sheets (MoS2/G) is achieved by a facile and scalable hydrothermal method, which involves adsorption of Mo7O24(6-) on a graphene oxide (GO) surface, due to the electrostatic attraction, followed by in situ growth of MoS2. These results give an explicit proof that the presence of oxygen-containing groups and pH of the solution are crucial factors enabling formation of a lamellar structure with MoS2 NSs uniformly decorated on graphene sheets. The direct coupling of edge Mo of MoS2 with the oxygen from functional groups on GO (C-O-Mo bond) is proposed. The interfacial interaction of the C-O-Mo bonds can enhance electron transport rate and structural stability of the MoS2/G electrode, which is beneficial for the improvement of rate performance and long cycle life. The graphene sheets improve the electrical conductivity of the composite and, at the same time, act not only as a substrate to disperse active MoS2 NSs homogeneously but also as a buffer to accommodate the volume changes during cycling. As an anode material for lithium-ion batteries, the manufactured MoS2/G electrode manifests a stable cycling performance (1077 mAh g(-1) at 100 mA g(-1) after 150 cycles), excellent rate capability, and a long cycle life (907 mAh g(-1) at 1000 mA g(-1) after 400 cycles).

High-Performance Anode Material Sr2FeMo0.65Ni0.35O6-δ with In Situ Exsolved Nanoparticle Catalyst.

A metallic nanoparticle-decorated ceramic anode was prepared by in situ reduction of the perovskite Sr2FeMo0.65Ni0.35O6-δ (SFMNi) in H2 at 850 °C. The reduction converts the pure perovksite phase into mixed phases containing the Ruddlesden-Popper structure Sr3FeMoO7-δ, perovskite Sr(FeMo)O3-δ, and the FeNi3 bimetallic alloy nanoparticle catalyst. The electrochemical performance of the SFMNi ceramic anode is greatly enhanced by the in situ exsolved Fe-Ni alloy nanoparticle catalysts that are homogeneously distributed on the ceramic backbone surface. The maximum power densities of the La0.8Sr0.2Ga0.8Mg0.2O3-δ electrolyte supported a single cell with SFMNi as the anode reached 590, 793, and 960 mW cm(-2) in wet H2 at 750, 800, and 850 °C, respectively. The Sr2FeMo0.65Ni0.35O6-δ anode also shows excellent structural stability and good coking resistance in wet CH4. The prepared SFMNi material is a promising high-performance anode for solid oxide fuel cells.