Realizing Near Infrared Mechanoluminescence Switch in LAGO:Cr Based on Oxygen Vacancy.

Mechanoluminescence (ML) materials are featured with the characteristic of "force to light" in response to external stimuli, which have made great progress in artificial intelligence and optical sensing. However, how to effectively enable ML in the material is a daunting challenge. Here, a Lu3 Al2 Ga3 O12 :Cr3+ (LAGO: Cr3+ ) near infrared (NIR) ML material peaked at 706 nm is reported, which successfully realizes the key to unlock ML by the lattice-engineering strategy Ga3+ substitution for Al3+ to "grow" oxygen vacancy (Ov ) defects. Combined with thermoluminescence measurements, the observed ML is due to the formation of defect levels and the ML intensity is proportional to it. It is confirmed by X-ray photoelectron spectroscopy and electron paramagnetic resonance that such a process is dominated by Ov , which plays a crucial role in turning on ML in this compound. In addition, potential ML emissions from 4 T2 and 2 E level transitions are discussed from both experimental and theoretical aspects. This study reveals the mechanism of the change in ML behavior after cation substitution, and it may have important implications for the practical application of Ov defect-regulated turn-on of ML.

Ratiometric mechanoluminescence in single Pr3+ -activated LiGa5 O8.

Mechanoluminescence (ML) materials have found potential applications in information storage, anti-counterfeiting, and stress sensing. Conventional stress sensing based on absolute ML intensity is prone to significant mistakes owing to the unpredictability of measurement surroundings. However, implementing a ratiometric ML sensing technique may considerably ameliorate this issue. In this study, a single activator-doped gallate material (LiGa5 O8 :Pr3+ ) is proposed to determine the relationship between the ML intensity and the change in local positional symmetry that occurs when the material is subjected to stress. The sensing reliability of the ML intensity ratio under different factors (Force; Content; Thickness and Materials) is systematically analyzed, where the factor that has the greatest effect on the proportional ML is the concentration, with the ML intensity asymmetry ratio decreasing from 1.868 to 1.300 varying concentration at constant stress. The colour-resolved visualization of stress sensing is further realized, which opens a new path for a ratiometric ML-based strategy to improve the reliability of stress sensing.

Anionic Regulation toward Bi3+ Selective Occupation for Full-Spectrum White Light Emission.

An activator's selective occupation of a host is of great significance for designing high-quality white light-emitting diode phosphors, while achieving a full-spectrum single-phase white light emission phosphor is challenging. In this study, a boron phosphate solid-solution Na2Y2(BO3)2-x(PO4)xO:0.005 Bi3+ (NYB2-xPxO:0.005 Bi3+) white phosphor was designed by selectively occupying Bi3+ activators in the mixed anionic groups. The substitutes of the anionic unit (BO3)3- by the (PO4)3- unit are supposed to force part of the Bi3+ ion to enter the Na lattice site, which produces an intense orange-red emission peaked at 590 nm. In parallel, spectral tuning from blue to white light and an internal quantum efficiency of 56.42% was obtained, and the thermal stabile luminescence intensity remains at 94.2% of the initial intensity after four heating-cooling cycles from 30 to 210 °C (luminescent intensity is 83.6% of room temperature (RT) at 150 °C, with excellent thermal stability and recovery performance). Finally, an excellent color rendering index (Ra = 90.8 and R9 = 85) was demonstrated for white light-emitting diode devices using only an NYB1.5P0.5O:0.005 Bi3+ phosphor and a near-ultraviolet (n-UV) 365 nm LED chip. This work delves into the different selective occupancy of Bi3+ ions and explores a new avenue for the design of phosphors for full-spectrum white light emission.

Transparent Microcomposite Films Based on a Ce-Doped Li6Gd(BO3)3 Scintillator for Radiation Detection.

Scintillators are widely used for high-energy radiation detection. Hybrid inorganic-organic composite scintillators with high light yields, high light decay rates, excellent stability, and low costs are in great demand. Here, we report a novel scintillator composed of Ce-doped Li6Gd(BO3)3 (LGBO) microphosphors (MPs) and polymethyl methacrylate for X-ray and thermal neutron detection. The Ce-doped LGBO MPs, fabricated using a facile high-temperature solid-state reaction method, exhibit intense blue light at 416 nm under X-ray and UV excitation and have a high photoluminescence quantum yield of ∼63%. More importantly, the composite scintillator based on these MPs has excellent transparency and luminescence intensity. The luminescence integral intensity of composite scintillators is superior to that of commercial CsI:Na under X-ray excitation, and the light yield under thermal neutron irradiation is 21,000 photons/thermal neutron. The scintillation decay time is found to be below 600 ns. The neutron-gamma signal discrimination and neutron detection efficiency of the composite scintillators are acceptable for practical application. There is an excellent separation between neutron and background events. It represents significant improvements in scintillator performances, especially for reliable thermal neutron scintillators that are likely to improve the data qualities of scientific instruments, including charge-coupled device-based imagers and Anger logic-based position-sensitive detectors in neutron user facilities.

Human epididymis protein 4: a novel predictor of ischemic cardiomyopathy.

BACKGROUND: The prognostic value of human epididymis protein 4 (HE4) in patients with ischemic cardiomyopathy (ICM) is unknown. METHODS: A total of 103 patients with ICM were prospectively enrolled in this study from Hunan Provincial People's Hospital between February 2019 and June 2019. All patients were tested for HE4 levels at baseline and follow-up. Endpoints of the study included cardiovascular death and heart failure-related hospitalization. RESULTS: A total of 96 patients with ICM were included for analysis. After a mean follow-up period of 263 (153-313) days, cardiovascular events were observed in 45 patients. Serum HE4 levels in patients with events were significantly higher than those in patients without events [188.70 (113.35-326.82) pmol/L versus 92.90 (61.50-123.20) pmol/L, P < 0.001]. Multivariate Cox regression analysis revealed that HE4 [χ2: 9.602, hazard ratio (HR): 1.003, 95% confidence interval (CI): 1.001-1.005, P = 0.002] and age [χ2: 4.55, HR: 1.044, 95% CI: 1.003-1.085, P = 0.033] were independent predictors of events. After adjusting for age and sex, the risk of events in patients with HE4 > 100.2 pmol/L was higher than that in patients with HE4 ≤ 100.2 pmol/L [HR: 3.372, 95% CI: 1.409-8.065, P < 0.001]. CONCLUSION: HE4 is an independent predictor of cardiovascular death and heart failure-related rehospitalization in patients with ICM.

Photoreduction properties of novel Z-scheme structured Sr0.8La0.2(Ti1-δ 4+Ti δ 3+)O3/Bi2MoO6 composites for the removal of Cr(vi).

Novel Z-scheme structured Sr0.8La0.2(Ti1-δ 4+Ti δ 3+)O3/Bi2MoO6 (LSTBM) composites were prepared via a facile two-step solvothermal method. Several characterization techniques were employed to investigate the phases, microstructures, compositions, valence states, oxygen vacancies, surface oxygen absorption, energy band structures and lifetime of photoproduced carriers. It was found that the lifetime and transfer of the photoproduced carriers of LSTBM were better than those of Bi2MoO6 (BMO) and Sr0.8La0.2(Ti1-δ 4+Ti δ 3+)O3 (LSTO). The LSTBM with a molar ratio of BMO/(LSTO + BMO) = 0.07 (denoted as LSTBM7) showed 1.9 and 3.1 times removal rates than those for BMO and LSTO, respectively. Importantly, the built-in electric field in the heterojunction of LSTBM and Ov-s, especially in Ov-s on the higher-Fermi-level side of the heterojunction, had co-played roles in prolonging the lifetime and improving the transfer of photogenerated carriers. The photoproduced e- played a dominant role in reducing Cr(vi) to Cr(iii) and the produced Cr(iii) tends to form Cr(OH)3 and adsorb onto the surface of the photocatalyst to decrease the nucleation energy. The possible reduction route for Cr(vi) to Cr(iii) over LSTBM7 was figured out. This study implies that inducing Ov-s on the higher-Fermi-level side of the Z-scheme heterojunction is a more effective route for separating the photogenerated electrons and holes and improving the transfer of photogenerated carriers.

Increased Th17 activation and gut microbiota diversity are associated with pembrolizumab-triggered tuberculosis.

INTRODUCTION: A hypersensitivity response akin to immune reconstitution inflammatory syndrome (IRIS) has been proposed as a mechanism responsible for anti-PD-1 therapy-induced tuberculosis. IRIS is associated with enhanced activation of IL-17A-expressing CD4 + T cells (Th17). Gut microbiota is thought to be linked to pulmonary inflammation through the gut-lung axis. MATERIALS AND METHODS: We used ImmuCellAI to investigate the T cell population in lung cancer and tuberculosis samples. Then, we applied flow cytometry to monitor the expression levels of the Th17 cell activation marker CD38 in the peripheral blood of a patient experiencing adverse events, including tuberculosis, in response to pembrolizumab. The gut microbiome was examined by 16S rRNA sequencing to examine the alterations caused by pembrolizumab. RESULTS: The percentage of Th17 cells was increased in both lung cancer and tuberculosis. FACS analysis showed that pembrolizumab induced substantial CD38 expression in Th17 cells. The patient's fecal samples showed that the diversity of the gut microbiota was significantly increased in response to the pembrolizumab cycle. One enriched genus was Prevotella, which has previously been linked to lung inflammation and Th17 immune activation. DISCUSSION: The observed Th17 activation in our patient was consistent with a role of Th17-mediated IRIS in pembrolizumab-triggered tuberculosis. Pembrolizumab might trigger airway inflammation with a Th17 phenotype through microbiota interactions in the gut-lung axis.

On-line immobilized trypsin microreactor for evaluating inhibitory activity of phenolic acids by capillary electrophoresis and molecular docking.

Phenolic acids, which are important aromatic secondary metabolites, are widely distributed in plant foods. In this study, a simple, economical and fast on-line immobilized trypsin microreactor was developed for evaluating the inhibitory activity of phenolic acids by capillary electrophoresis. The Michaelis-Menten constant (Km) of immobilized trypsin was determined as 0.99 mM, and the half-maximal inhibitory concentration (IC50) and inhibition constant (Ki) of benzamidine were measured as 3.39 and 1.68 mM, respectively. Then, the developed strategy was applied to investigate the inhibitory activity of six phenolic acids on trypsin. The results showed that gallic acid, caffeic acid and ferulic acid had high inhibitory activity at concentration of 150 µM. Molecular docking results illustrated that gallic acid, caffeic acid and ferulic acid can interact indirectly with the catalytic and substrate-binding sites of trypsin. The developed strategy is an effective tool for evaluating inhibitory activity of phenolic acids on trypsin.

Cupric ion functionalized polydopamine coated magnetic microspheres as solid-phase adsorbent for the extraction of purines in plasma.

In this paper, Cu2+ functionalized Fe3O4@polydopamine core-shell (Fe3O4@PDA@Cu2+) magnetic microspheres were prepared by the chelation between Cu2+ and catechol of polydopamine surface. The synthetic magnetic adsorbent was characterized by Fourier transform infrared spectroscopy, energy dispersive X-ray spectroscopy, vibrating sample magnetometry, thermogravimetric analysis, scanning electron microscope and transmission electron microscopy. Four purines include guanine, adenine, hypoxanthine and xanthine were selected as model compounds to evaluate the applicability of this adsorbent. Several parameters that effected the extraction efficiency, such as extraction time, adsorbent amount, solution pH, ionic strength, eluent type, concentration of eluent and eluent time, were investigated. Under the optimized conditions, good linearity was obtained with correlation coefficients between 0.9983 and 0.9999 for the four analytes, and their LOD and LOQ were 0.42-2.15 ng/mL and 1.41-6.50 ng/mL, respectively. Meanwhile, the RSDs of intra-day and inter-day precision were in the range of 1.43%-5.55% and 4.56%-7.01%, respectively. The spiked recoveries of four purines in real sample were 70.01%-102.42%, indicating this proposed method might have potential applications for the analysis of purines in real samples. In addition, the developed method was used to monitor the concentrations of adenine in rat plasma at different time points after intragastric administration.

Extraction of nucleobases, nucleosides and nucleotides by employing a magnetized graphene oxide functionalized with hydrophilic phytic acid and titanium(IV) ions.

A magnetite@graphene oxide nanocomposite was first coated with polyethylenimine and then modified with phytic acid and titanium(IV) ions. The high loading with Ti(IV) and the good hydrophilicity of PEI and PA result in a material that can be applied to the efficient extraction of highly polar nucleobases, nucleosides and nucleotides. The physicochemical properties of the composite were investigated by scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, water contact angle measurements, thermogravimetric analysis, and vibrating sample magnetometry. A series of parameters that affect extraction and elution under the conditions of immobilized metal affinity chromatography (IMAC) and hydrophilic interaction liquid chromatography (HILIC) were examined. The analytes were eluted from the nanocomposites using 10 mM trisodium phosphate as the elution solution in the IMAC mode, and 50% methanol-water as elution solution in the HILIC mode. Figures of merit include (a) an intra-day precision of 0.1-1.0% in the IMAC mode; (b) an intra-day precision of 0.4%-0.8% in the HILIC mode; (c) detection limits between 1.8-2.8 ng mL-1 in the IMAC mode; and (d) detection limits of 4.0-10.5 ng mL-1 in the HILIC mode. The method was applied to the extraction of the nucleotides cytidine-5'-monophosphate (CMP), uridine-5'-monophosphate (UMP), guanosine-5'-monophosphate (GMP), and adenosine-5'-monophosphate (AMP), and the nucleobases and nucleosides hypoxanthine, adenosine, cytosine, inosine and cytidine from Cordyceps sinensis, Lentinus edodes and plasma samples. Graphical abstract Schematic presentation of the workflow for the extraction of nucleobases, nucleosides and nucleotides using phytic acid-Ti(IV) functionalized magnetite@graphene oxide nanocomposites under two distinct modes.

Effect of (Tb+Y)/Al ratio on Microstructure Evolution and Densification Process of (Tb0.6Y0.4)3Al5O12 Transparent Ceramics.

(Tb0.6Y0.4)3Al5O12 transparent ceramics were successfully fabricated by solid-state reactive sintering using Tb4O7, Y2O3, and α-Al2O3 powders as raw materials. The effect of (Tb+Y)/Al ratio on microstructure evolution and densification process was investigated in detailed. The results showed that the grain growth kinetics were significantly affected by (Tb+Y)/Al ratio. Al-rich and Tb-rich phases appeared in part of the samples of different ratios. Particularly, excess aluminum increased the diffusing process, leading to a higher densification rate, while samples with excess terbium ratios displayed a smaller grain size and lower relative density. The optical quality was highly related to the amount of the secondary phase produced by different (Tb+Y)/Al ratios. Finally, (Tb0.6Y0.4)3Al5O12 transparent ceramics have been fabricated through pre-sintering in vacuum, followed by hot isostatic sintering (HIP), and the best transmittance of sample with a 4 mm thickness was approximately 78% at 1064 nm.

Photocatalytic properties of a new Z-scheme system BaTiO3/In2S3 with a core-shell structure.

It's highly desired to design and fabricate an effective Z-scheme photo-catalyst with excellent charge transfer and separation, and a more negative conduction band edge (E CB) than O2/·O2 - (-0.33 eV) and a more positive valence band edge (E VB) than ·OH/OH- (+2.27 eV) which provides high-energy redox radicals. Herein, we firstly designed and synthesized a core-shell-heterojunction-structured Z-scheme system BaTiO3@In2S3 (BT@IS, labelled as BTIS) through a hydrothermal method, where commercial BT was used as the core and In(NO3)3·xH2O together with thioacetamide as the precursor of IS was utilized as the shell material. In this system, the shell IS possesses a E CB of -0.76 eV and visible-light-response E g of 1.92 eV, while the core BT possesses a E VB of 3.38 eV, which is well suited for a Z-scheme. It was found that the as-prepared BTIS possesses a higher photocatalytic degradation ability for methyl orange (MO) than commercial BT and the as-prepared IS fabricated by the same processing parameters as those of BTIS. Holes (h+) and superoxide radicals (·O2 -) were found to be the dominant active species for BTIS. In this work, the core-shell structure has inhibited the production of ·OH because the shell IS has shielded the OH- from h+. It is assumed that if the structure of BTIS is a composite, not a core-shell structure, ·OH could be produced during photocatalysis, and therefore a higher photocatalytic efficiency would be obtained. This current work opens a new pathway for designing Z-scheme photocatalysts and offers new insight into the Z-scheme mechanism for applications in the field of photocatalysis.

Evaluation of thrombin inhibitory activity of catechins by online capillary electrophoresis-based immobilized enzyme microreactor and molecular docking.

An online capillary electrophoresis (CE)-based thrombin (THR) immobilized enzyme microreactor (IMER) method was established to screen THR inhibitors in this study. S-2366 was used as chromogenic substrate for determination of THR activity and other kinetic constants. After continuously run for 50 times, the prepared IMER could still remain 89% of the initial immobilized enzyme activity. The Michaelis-Menten constant (Km) of immobilized THR was measured as 0.514 mmol/L and the half-maximal inhibitory concentration (IC50) and inhibition constant (Ki) of argatroban on THR were determined as 78.07 and 26.53 nmol/L, respectively, which indicated that CE-based THR IMER was successfully established and could be applied to screen THR inhibitors. Then the prepared IMER was used to investigate the inhibitory potency on THR of four main catechins in green tea including epicatechin (EC), epigallocatechin (EGC), epicatechin gallate (ECG), and epigallocatechin gallate (EGCG). The results showed that ECG and EGCG had good THR inhibition activity and their inhibition rates at concentration of 200 µmol/L were 53.2 ±â€¯3.8% and 55.8 ±â€¯2.6%, respectively, which was in consistent with the results of microplate reader assay. Additionally, molecular docking results showed that the benzopyran groups of ECG and EGCG were inserted into the THR active pocket and interacted with residues LYS60F, TRP60D, TRY60A, IEU99, GLY216, HIS57 and SER195, but EC and EGC did not. Therefore, the developed CE-based THR IMER is reliable method for measuring THR inhibitory activity of natural inhibitors.

Preparation and photocatalytic properties of porous C and N co-doped TiO2 deposited on brick by a fast, one-step microwave irradiation method.

A one-step microwave irradiation method was used to deposit carbon and nitrogen co-doped TiO2 ((C, N)-TiO2) on commercial brick ((C, N)-TiO2/brick). The as-prepared samples were characterized by X-ray diffraction, ultraviolet-visible (UV-vis) diffuse reflectance spectroscopy, photoluminescence spectroscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy (SEM). A selective technique was also used to investigate the concentration of hydroxyl radicals during UV-vis irradiation of the Methyl Orange solution with the as-prepared samples. The C and N dopants enhanced visible light absorption and provided a longer lifetime for the photo-generated electron-hole pairs. The SEM images showed that the as-prepared sample is porous. The dark adsorption and photodegradation test for (C, N)-TiO2/brick showed good photodegradation and good recyclability. The best photodegradation rate was 94% after 2hr. The maximum degradation rate was maintained even after the 6th cycle. The good photocatalytic properties are attributed to the enhanced visible light absorption, enhanced pollutant adsorption arising from the porous structure of the (C, N)-TiO2 thin film, and longer lifetime of the photo-generated electron-hole pairs. (C, N)-TiO2/brick should have potential commercial applications in photodegradation processes because of its low cost, good photodegradation, and excellent recyclability.

Evaluation of interactions between RAW264.7 macrophages and small molecules by capillary electrophoresis.

In this study, the affinity interactions between RAW 264.7 macrophages and three small molecules including naringin, oleuropein and paeoniflorin were evaluated by affinity capillary electrophoresis (ACE), partial filling affinity capillary electrophoresis (PFACE) and frontal analysis capillary electrophoresis (FACE), respectively. The result indicated that ACE (varying concentrations of cell suspension were filled in the capillary as receptor) may not be suitable for the evaluation of interactions between cell and small molecules due to the high viscosity of cell suspension; PFACE can qualitatively evaluate the interaction, but the difference in viscosity between RAW264.7 suspension and buffer effects on the liner relationship between filling length and injection time, which makes the calculation of binding constant difficult. Furthermore, based on the PFACE results, naringin showed stronger interaction with macrophages than the other two molecules; taking advantage of the aggregation phenomenon of cell induced by electric field, FACE was successfully used to determine the stoichiometry (n = 5×109 ) and binding constant (Kb = 1×104 L/mol) of the interaction between RAW264.7 and naringin.

Design and simple synthesis of composite Bi12TiO20/Bi4Ti3O12 with a good photocatalytic quantum efficiency and high production of photo-generated hydroxyl radicals.

Hybrid Bi12TiO20/Bi4Ti3O12 composites with different Bi : Ti molar ratios were successfully fabricated using a one-step solid-state calcination. These samples were characterized using X-ray diffraction, specific surface area analysis, scanning electron microscopy, high-resolution microscopy, selected-area electron diffraction, X-ray photoelectron spectroscopy, UV-vis diffuse reflection spectroscopy, photoluminescence analyses, and photocurrent and electrochemical impedance spectroscopy. Some specified techniques were also used to investigate the photocatalytic properties and the formation of radical species under UV-vis irradiation. The composites provide an efficient pathway for photo-produced electrons and holes to diffuse and transfer to the exterior of the particles for photodegradation, because of the good contact between hybrid Bi12TiO20 and Bi4Ti3O12. Therefore, the hybrid Bi12TiO20/Bi4Ti3O12 can prolong the carrier lifetime as compared to any individual material (Bi12TiO20 or Bi4Ti3O12). In particular, the hybrid Bi12TiO20/Bi4Ti3O12 composite with a Bi : Ti ratio of 12 : 6 had the longest photo-generated carrier lifetime and produced the maximum amount of hydroxyl radicals during UV-vis irradiation; therefore, it demonstrated the best photo-catalytic properties. A Z-scheme mechanism was proposed to explain the hydroxyl radical yield and photodegradation.

Evaluation of affinity interaction between small molecules and platelets by open tubular affinity capillary electrochromatography.

In this paper, an open tubular affinity capillary electrochromatography (OT-ACEC) was developed by physical adsorption of rabbit platelets on the inner surface of capillary. The interactions between small molecules include adenosine diphosphate (ADP) (positive control), protocatechuic acid (negative control) and seven natural products (salvianolic acid B, salvianic acid A sodium, hydroxysafflor yellow A, ferulic acid, chlorogenic acid, sinapic acid, caffeic acid) and platelets were evaluated by their retention factors and binding constants obtained based on peak-shift assay. Then, the activities of anti-platelet aggregation induced by thrombin (THR), ADP and arachidonic acid (AA) for those small molecules (except ADP) were evaluated by turbidimetric method. The results indicate that: (i) ADP, a platelet aggregation inducer, had strong interaction with platelet, while protocatechuic acid that had no inhibition on platelet aggregation behaved no specific interaction; (ii) there was a positive correlation between the anti-platelet aggregation activities of small molecules and their interactions with platelet, generally those compounds with higher binding constants with platelet exhibited higher activities. Therefore, the OT-ACEC method developed in the present study can be a potential method to evaluate affinity interactions between small molecules and platelets, so as to predict the biological activities such as anti-platelet aggregation for the small molecules.