Bi-Directional H-Bonding Modulated Soft/Hard Polyethylene Glycol-Polyaniline Coated Si-Anode for High-Performance Li-Ion Batteries.

Ultrahigh-capacity silicon (Si) anodes are essential for the escalating energy demands driven by the booming e-transportation and energy storage field. However, their practical applications are strictly hampered by their intrinsically low electroconductivity, sluggish Li-ion diffusion, and undesirably large volume change. Herein, a high-performance Si anode, comprised of a modulated soft/hard coating of polyethylene glycol (PEG) (as Li-ion conductor) and polyaniline (PANI) (as electron conductor) on the surface of Si nanoparticles (NPs) through H-bonding network, is introduced. In this design, the abundant ─OH groups of soft PEG allow it to uniformly cover Si NPs while the hard PANI binds to PEG through its ─N─H group, thus constructing a tight connectin between Si and PEG-PANI (PP). Consequently, the elastic PP allows Si@PP to accommodate the huge volume expansion while possessing fine electronic/ionic conductivity. Therefore, the Si@PP anode exhibits a high initial Coulombic efficiency of 90.5% and a stable capacity of 1871 mAh g-1 after 100 cycles at 1 A g-1 with a retention of 85.7%. Additionally, the Si@PP anode also demonstrates a high areal capacity of 3.01 mAh cm-2 after 100 cycles at 0.5 A g-1 . This work reveals a scalable interface design of multi-layer multifunctional coatings for high-performance electrode materials in next-generation Li-ion batteries.

Light-oriented 3D printing of liquid crystal/photocurable resins and in-situ enhancement of mechanical performance.

Additive manufacturing technology has significantly impacted contemporary industries due to its ability to generate intricate computer-designed geometries. However, 3D-printed polymer parts often possess limited application potential, primarily because of their weak mechanical attributes. To overcome this drawback, this study formulates liquid crystal/photocurable resins suitable for the stereolithography technique by integrating 4'-pentyl-4-cyanobiphenyl with a photosensitive acrylic resin. This study demonstrates that stereolithography facilitates the precise modulation of the existing liquid crystal morphology within the resin. Furthermore, the orientation of the liquid crystal governs the oriented polymerization of monomers or prepolymers bearing acrylate groups. The products of this 3D printing approach manifest anisotropic behavior. Remarkably, when utilizing liquid crystal/photocurable resins, the resulting 3D-printed objects are approximately twice as robust as those created using commercial resins in terms of their tensile, flexural, and impact properties. This pioneering approach holds promise for realizing autonomously designed structures that remain elusive with present additive manufacturing techniques.

Study on the Mass Spectrometry Fragmentation Patterns for Rapid Screening and Structure Identification of Ketamine Analogues in Illicit Powders.

Ketamine analogues have been emerging in recent years and are causing severe health and social problems worldwide. Ketamine analogues use 2-phenyl-2-aminocyclohexanone as the basic structure and achieve physiological reactions similar to or even more robust than the prototype of ketamine by changing the substituents on the benzene ring (R1 and R2) and amine group (RN1). Therefore, the mass spectrometry (MS) fragmentation pathways and fragments of ketamine analogues have certain regularity. Eight ketamine analogues are systematically investigated by GC-QTOF/MS and LC-Q-Orbitrap MS/MS with the positive mode of electrospray ionization. The MS fragmentation patterns of ketamine analogues are summarized according to high-resolution MS data. The α-cleavage of carbon bond C1-C2 in the cyclohexanone moiety and further losses of CO, methyl radical, ethyl radical and propyl radical are the characteristic fragmentation pathways of ketamine analogues in EI-MS mode. The loss of H2O or the sequential loss of RN1NH2, CO and C4H6 are the distinctive fragmentation pathways of ketamine analogues in ESI-MS/MS mode. Moreover, these MS fragmentation patterns are first introduced for the rapid screening of ketamine analogues in suspicious powder. Furthermore, the structure of the ketamine analogue in suspicious powder is 2-(Methylamino)-2-(o-tolyl)cyclohexan-1-one, which is further confirmed by NMR. This study contributes to the identification of the chemical structure of ketamine analogues, which can be used for the rapid screening of ketamine analogues in seized chemicals.

Recent Progress of Self-Supported Metal Oxide Nano-Porous Arrays in Energy Storage Applications.

The demand for high-performance and cost-effective energy storage solutions for mobile electronic devices and electric vehicles has been a driving force for technological advancements. Among the various options available, transitional metal oxides (TMOs) have emerged as a promising candidates due to their exceptional energy storage capabilities and affordability. In particular, TMO nanoporous arrays fabricated by electrochemical anodization technique demonstrate unrivaled advantages including large specific surface area, short ion transport paths, hollow structures that reduce bulk expansion of materials, and so on, which have garnered significant research attention in recent decades. However, there is a lack of comprehensive reviews that discuss the progress of anodized TMO nanoporous arrays and their applications in energy storage. Therefore, this review aims to provide a systematic detailed overview of recent advancements in understanding the ion storage mechanisms and behavior of self-organized anodic TMO nanoporous arrays in various energy storage devices, including alkali metal ion batteries, Mg/Al-ion batteries, Li/Na metal batteries, and supercapacitors. This review also explores modification strategies, redox mechanisms, and outlines future prospects for TMO nanoporous arrays in energy storage.

Screening strategy for ketamine-based new psychoactive substances using fragmentation characteristics from high resolution mass spectrometry.

Recreational designer drugs called new psychoactive substances (NPS) are emerging and pose enormous risks to public health. Detection of recently discovered or unreported NPS remains a huge challenge by using traditional targeted mass spectrometry methods. Here a novel screening strategy was developed to detect both known and novel analogs of NPS based on fragmentation characteristics from liquid chromatography-high resolution mass spectrometry (LC-HRMS). The HRMS fragmentation pathway of one selected NPS family was investigated to form a database containing predicted drugs as well as their mass characteristics. During the study, an unexpected substituent effect was found to distinguish geometric isomers. Seventy-eight seized samples were analyzed using this strategy, four ketamine-based NPS were detected and three of them were newly marketed. The substituent effect predicted the position of their phenylic substituent, the results were confirmed by NMR.

Chlorinated Narrow Bandgap Polymer Suppresses Non-Radiative Recombination Energy Loss Enabling Perylene Diimides-Based Organic Solar Cells Exceeding 10% Efficiency.

The scarcity of narrow bandgap donor polymers matched with perylene diimides (PDI)-based nonfullerene acceptors (NFAs) hinders improvement of the power conversion efficiency (PCE) value of organic solar cells (OSCs). Here, it is reported that a narrow bandgap donor polymer PDX, the chlorinated derivative of the famous polymer donor PTB7-Th, blended with PDI-based NFA boosts the PCE value exceeding 10%. The electroluminescent quantum efficiency of PDX-based OSCs is two orders of magnitude higher than that of PTB7-Th-based OSCs;therefore, the nonradiative energy loss is 0.103 eV lower. This is the highest PCE value for OSCs with the lowest energy loss using the blend of PTB7-Th derivatives and PDI-based NFAs as the active layer. Besides, PDX-based devices showed larger phase separation, faster charge mobilities, higher exciton dissociation probability, suppressed charge recombination, elevated charge transfer state, and decreased energetic disorder compared with the PTB7-Th-based OSCs. All these factors contribute to the simultaneously improved short circuit current density, open circuit voltage, and fill factor, thus significantly improving PCE. These results prove that chlorinated conjugated side thienyl groups can efficiently suppress the non-radiative energy loss and highlight the importance of fine-modifying or developing novel narrow bandgap polymers to further elevate the PCE value of PDI-based OSCs.

Novel Third Components with (Thio)barbituric Acid as the End Groups Improving the Efficiency of Ternary Solar Cells.

Developing novel third component is critical for the ternary organic solar cells (TOSCs). Herein, we design and synthesize two novel third components, MAZ-1 and MAZ-2, with 1,3-diethyl-2-thiobarbituric acid and 1,3-dimethylbarbituric acid as the weak electron withdrawing end groups, respectively. Both MAZ-1 and MAZ-2 could improve the photovoltaic performance of the binary OSCs based on D18:Y6 which exhibit the power conversion efficiency (PCE) of 17%, because the third components can optimize the phase separation, suppress the bimolecular recombination, and decrease the nonradiative energy loss in ternary blends. The PCE of the optimized TOSCs approaches 18% along with the simultaneous increase in open circuit voltage, short circuit current density, and fill factor by incorporating 10 wt % MAZ-1 and MAZ-2 in acceptors. This work enriches the building blocks for novel third components for achieving highly efficient TOSCs.

Total Synthesis of (-)-Rhodomollanol A.

An asymmetric approach for the first total synthesis of (-)-rhodomollanol A, a highly oxidized diterpenoid, is described. The efficient synthetic strategy features three key transformations: (1) an oxidative dearomatization-induced (5 + 2) cycloaddition/pinacol-type 1,2-acyl migration cascade to build up the bicyclo[3.2.1]octane skeleton; (2) a retro-Dieckmann fragmentation/vinylogous Dieckmann cyclization cascade to assemble the bicyclo[3.3.0]octane subunit; and (3) a photo-Nazarov cyclization/intramolecular cycloetherification cascade to forge the 7-oxabicyclo[4.2.1]nonane core structure of the natural product.

Total Synthesis of (+)-Jatrophalactam.

The first asymmetric total synthesis of (+)-jatrophalactam was reported, which unambiguously determined the absolute configuration of the titled natural product. The key features entail a conformationally controlled cyclopropanation, a Meldrum's acid adduct-engaged macrolactam formation, and a Pd(II)-mediated oxidative cyclization.

Ladder-Type Nonacyclic Arene Bis(thieno[3,2-b]thieno)cyclopentafluorene as a Promising Building Block for Non-Fullerene Acceptors.

The ladder-type nonacyclic arene (bis(thieno[3,2-b]thieno)cyclopentafluorene (BTTF)) has been designed and synthesized through fusing thienothiophenes with the fluorene core from the synthon of dimethyl 9,9-dioctyl-2,7-bis(thieno[3,2-b]thiophen-2-yl)fluorene-3,6-dicarboxylate. With BTTF as the central donor unit, a novel acceptor-donor-acceptor (A-D-A) type non-fullerene small-molecule acceptor (BTTFIC) was prepared with 1,1-dicyanomethylene-3-indanones (IC) as the peripheral acceptor units. The energy level of the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) of BTTFIC locate at -5.56 and -3.95 eV, respectively, presenting a low optical band gap of 1.58 eV. Encouragingly, polymer solar cells based on the blends of BTTFIC with both the representative wide- and low-bandgap polymer donors (PBDB-T, 1.82 eV. PTB7-Th, 1.58 eV) offer power conversion efficiencies over 8 % (8.78±0.18 % for PBDB-T:BTTFIC and 8.18±0.29 % for PTB7-Th:BTTFIC). These results highlight the advantage of ladder-type BTTF on the preparation of nonfullerene acceptors with extended conjugated backbones.

Detection of myocardial enzymes, cardiac troponin T and hepatic and renal function in the diagnosis and treatment of severe pneumonia in children.

OBJECTIVE: To analyze the significance of myocardial enzymes, cardiac troponin T (cTnT) and hepatic and renal function in the treatment of severe pneumonia in children. METHODS: One hundred and twenty children with severe pneumonia who were admitted to the hospital between April 2015 and February 2017 were selected and included as a severe pneumonia group; 120 children with common pneumonia were included as a common pneumonia group; 100 healthy children were included as controls. The myocardial enzymes, cTnT and hepatic and renal function of patients in the three groups were detected and compared. The children with severe pneumonia were divided into a mild hypoxia group, a moderate hypoxia group and a severe hypoxia group according to arterial partial pressure of oxygen; the myocardial enzymes, hepatic and renal function and cTnT of the children in the three groups were compared. The correlations of partial pressure of blood oxygen with myocardial enzymes, hepatic and renal function and cTnT were analyzed. RESULTS: The levels of myocardial enzymes, hepatic and renal function and cTnT of the severe pneumonia group, common pneumonia group and control group declined, and the differences had statistical significance (P<0.05). The levels of myocardial enzymes, hepatic and renal function and cTnT were higher in the children with severe hypoxia. The partial pressure of blood oxygen was in a negative correlation with myocardial enzymes, hepatic and renal function and cTnT in the severe pneumonia group. CONCLUSION: Timely monitoring of myocardial enzymes, hepatic and renal function and cTnT has an extremely important role in the evaluation of children with severe pneumonia.

A Ladder-type Heteroheptacene 12H-Dithieno[2',3':4,5]thieno[3,2-b:2',3'-h]fluorene Based D-A Copolymer with Strong Intermolecular Interactions toward Efficient Polymer Solar Cells.

Ladder-type electron-donating units for D-A copolymers applied in polymer solar cells usually comprise multiple tetrahedral carbon bridges bonded with out-of-plane alkyl chains for desirable solubility for device processing. However, molecular packing of resultant copolymers in the solid state and charge transport within devices are also impeded in spite of with multiple fused aromatic backbones. To mitigate this issue, a structurally well-defined ladder-type electron-donating heteroheptacene, 12H-dithieno[2',3':4,5]thieno[3,2-b:2',3'-h]fluorene (DTTF) with an extended conjugated backbone and a single tetrahedral carbon bridge attached with two bulky alkyl chains was designed and synthesized. The copolymerization of DTTF with 4,7-bis(4-hexylthiophen-2-yl)benzo[c][1,2,5]thiadiazole (DTBT) afforded a soluble D-A copolymer (PDTTF-DTBT) with a medium optical band gap of 1.72 eV and low-lying HOMO level at -5.36 eV. PDTTF-DTBT unprecedentedly exhibits strong intermolecular stacking ability and presents preferential face-on orientation on both ZnO and PEDOT:PSS layers. The improved packing order and appropriate phase separation of both the copolymer and PC71BM in the bulk heterojunction blend on the ZnO layer over on the PEDOT:PSS layer lead to much improved power conversion efficiency of ∼8.2% in the inverted solar cell device, among the highest for reported ladder-type D-A copolymers. The research demonstrates that it is an effective method to incorporate a single tetrahedral carbon bridge to the molecular center of a ladder-type heteroacene with heavily extended π-conjugation to prepare D-A copolymers toward highly efficient PSCs.

[Longitudinal surveillance of intestinal nematodiasis in Yinghu Village of Wujiang City].

OBJECTIVE: To understand the epidemic dynamics of intestinal nematodiasis in Wujiang City. METHOD: The residents of Yinghu Village of Wujiang City were investigated with Kato-Katz technique for the infections of intestinal nematodes, and the persons with the infections were administered with anthelmintics and they also received the health education. RESULTS: Of the 5 757 residents, 147 persons were infected with intestinal nematodes, with the average infection rate of 2.55%. The infection rates of hookworm, Ascaris lumbricoides and Tricuris trichiura were 1.96%, 0.49% and 0.24%, respectively. The repeated infection rate was 20.30%, that was 10.36 times higher than the new infection rate (1.96%). CONCLUSIONS: There are still regions and populations with high infection rates of intestinal nematodes in Wujiang City where the intestinal nematodiasis has been controlled. Therefore, it is necessary to strengthen the monitoring, prevention and control work.

[T lymphocytes with chimeric receptor induce carcinoembryonic antigen-positive specific gastric carcinoma cells apoptosis].

OBJECTIVE: To develop a method to generate T lymphocytes that identify tumor specific carcinoembryonic antigen (CEA), and induce anti-tumor response such as apoptosis. METHODS: Peripheral blood samples were collected from 10 healthy persons and peripheral blood mononuclear cells (PBMCs) were isolated. 1, then CD8(+) T cells were isolated from the PBMCs by magnetic activated cell sorting (MACS) using magnetic beads-conjugated anti-CD8 monoclonal antibodies. Then the recombinant vector anti-CEA-scFv-CD3zeta-pcDNA3.0 was transfected into the CD8(+) T cells by lipofectamine 2000 and T lymphocytes with chimeric receptor were generated and cultivated. The T lymphocytes' activation was assessed by detecting the expression of CD69, an early signal of T cell activation. Human gastric carcinoma cells of the lines HGC-27 (CEA(+)) and SGC-7901 (CEA(-)) were cocultivated with the T lymphocytes with chimeric receptor. Flow cytometry (FCM) with annexin V-FITC/PI double staining was used to detect the expressions of annexin V, a signal of cell apoptosis, so as to observe the apoptosis of the gastric carcinoma cells. T cells activated by phytohemagglutinin (PHA) were used as positive controls, and T cells transfected with blank vector pcDNA3.0 were used as negative controls. RESULTS: T lymphocytes with chimeric receptor directed towards CEA(+) gastric carcinoma cells were generated. 12 and 24 hours after the co-culture of these T cells and HCG-27 cells, the CD69 expression rates were 40.5% +/- 3.4% and 48.3% +/- 2.8% respectively. However, the CD69 expression rates of the HGC-27 and SGC-7901 cells transfected with the T lymphocytes transfected with blank vector were both 0%. FCM showed that the apoptotic rates of the CEA(+) gastric tumor HGC-27 cells was 47.8% +/- 4.2%, significantly higher than that of the CEA(-) gastric tumor SGC-7901 cells (18.7% +/- 2.8%, P < 0.05). CONCLUSION: T lymphocytes with chimeric receptor targeting CEA specifically identify CEA positive gastric carcinoma cells and promote the apoptosis thereof, thus providing a promising method of cellular immunotherapy for gastric carcinomas.