Reduction of Punch-Sticking Propensity of Celecoxib by Spherical Crystallization via Polymer Assisted Quasi-Emulsion Solvent Diffusion.

Punch-sticking during tablet compression is a common problem for many active pharmaceutical ingredients (APIs), which renders tablet formulation development challenging. Herein, we demonstrate that the punch-sticking propensity of a highly sticky API, celecoxib (CEL), can be effectively reduced by spherical crystallization enabled by a polymer assisted quasi-emulsion solvent diffusion (QESD) process. Among three commonly used pharmaceutical polymers, poly(vinylpyrrolidone) (PVP), hydroxypropyl cellulose (HPC), and hydroxypropyl methylcellulose (HPMC), HPMC was the most effective in stabilizing the transient emulsion during QESD and retarding the coalescence of emulsion droplets and the initiation of CEL crystallization. These observations may arise from stronger intermolecular interactions between HPMC and CEL, consistent with solution 1H NMR analyses. SEM and X-ray photoelectron spectroscopy confirmed the presence of a thin layer of HPMC on the surfaces of spherical particles. Thus, the sticking propensity was significantly reduced because the HPMC coating prevents direct contact between CEL and the punch tip during tablet compression.

Reduced Punch Sticking Propensity of Acesulfame by Salt Formation: Role of Crystal Mechanical Property and Surface Chemistry.

Powder adhesion or sticking onto punches is one of the outstanding issues in pharmaceutical tablet manufacturing. We show in this work that, at comparable particle sizes, the acesulfame potassium exhibited pronouncedly reduced propensity to punch sticking than acesulfame. Detailed analyses revealed strong correlation between sticking propensity and crystal mechanical properties and surface chemistry. The free acid was highly plastic with high cohesive strength, while the salt form was brittle. During compaction, surfaces of acesulfame in contact with the punch face are abundant in electronegative functional groups, while those of the salt consist of mainly hydrophobic groups. Thus, acesulfame underwent stronger interactions with the electron-deficient punch. Consequently, the strikingly different onset and severity of sticking propensity between the two solid forms of acesulfame could be clearly explained based on their different crystal mechanical properties and surface characteristics. By providing molecular insight into the outstanding problem of punch sticking in tablet manufacturing, this work expands the list of pharmaceutical applications of crystal engineering.

Association of Thyroid Function With the Estimated Glomerular Filtration Rate in a Large Chinese Euthyroid Population.

BACKGROUND/AIMS: We aimed to explore whether thyroid function within a normal range is associated with the estimated glomerular filtration rate (eGFR) and the incidence of chronic kidney disease (CKD) in a large Chinese population. METHODS: We conducted a cross-sectional study that included 10,859 euthyroid individuals who underwent an annual regular health checkup in Jiangsu Province Official Hospital between August 2012 and August 2013. We measured the thyroid-stimulating hormone (TSH), free triiodothyronine (FT3) and free thyroxine (FT4) levels using a Roche modular analytics E170 and then calculated the eGFR using the Chinese modified Modification of Diet in Renal Disease (CMDRD) equation. RESULTS: In multiple linear regression models, TSH was negatively associated with eGFR after adjusting for confounding factors (ß = -0.072, P = 1.994×10-22). The significance remained in both males and females. No significant association was observed between FT4 and eGFR. In the logistic regression model, we did not observe significant associations of TSH or FT3 with CKD. Participants in the highest quartile of FT4 versus the lowest quartile (reference) had an increased risk of CKD (OR = 1.763, P = 0.012). The risk of CKD was more pronounced in females with the highest quartile of FT4 (OR = 2.424, P = 0.029). CONCLUSION: Our findings suggest that TSH is associated with eGFR in euthyroid individuals and that higher FT4 is associated with an increased risk of CKD. More cohort studies are warranted to confirm whether the association is causal.

High Detectivity Graphene-Silicon Heterojunction Photodetector.

A graphene/n-type silicon (n-Si) heterojunction has been demonstrated to exhibit strong rectifying behavior and high photoresponsivity, which can be utilized for the development of high-performance photodetectors. However, graphene/n-Si heterojunction photodetectors reported previously suffer from relatively low specific detectivity due to large dark current. Here, by introducing a thin interfacial oxide layer, the dark current of graphene/n-Si heterojunction has been reduced by two orders of magnitude at zero bias. At room temperature, the graphene/n-Si photodetector with interfacial oxide exhibits a specific detectivity up to 5.77 × 10(13) cm Hz(1/2) W(-1) at the peak wavelength of 890 nm in vacuum, which is highest reported detectivity at room temperature for planar graphene/Si heterojunction photodetectors. In addition, the improved graphene/n-Si heterojunction photodetectors possess high responsivity of 0.73 A W(-1) and high photo-to-dark current ratio of ≈10(7) . The current noise spectral density of the graphene/n-Si photodetector has been characterized under ambient and vacuum conditions, which shows that the dark current can be further suppressed in vacuum. These results demonstrate that graphene/Si heterojunction with interfacial oxide is promising for the development of high detectivity photodetectors.

All carbon coaxial supercapacitors based on hollow carbon nanotube sleeve structure.

All carbon coaxial supercapacitors based on hollow carbon nanotube (CNT) sleeve structure are assembled and tested. The key advantage of the structure is that the inner core electrode is variable from CNT sleeve sponges, to CNT fibers, reduced graphene oxide fibers, and graphene woven fabrics. By changing core electrodes from sleeve sponges to CNT fibers, the electrochemical performance has been significantly enhanced. The capacitance based on sleeve sponge + CNT fiber double the capacitances of double-sleeve sponge supercapacitors thanks to reduction of the series and internal resistances. Besides, the coaxial sleeve structure possesses many other features, including high rate capacitance, long cycle life, and good flexibility.

Fabrication and oil adsorption of carbon nanotube/polyvinylpyrrolidone surface composite.

It needs to assemble the industrial CNT powders into macroscopic porous surface composite to utilize the surface properties of CNTs, as well as to prevent them entering into environments. We demonstrate a method to fabricate the surface composites from CNTs and polyvinylpyrrolidone (PVP) by electrospinning, where CNTs distribute firmly and mainly on the surface PVP nanofibers. The CNTs/PVP surface composites have high pore volume of 10 cc/g and remarkable CNTs load of 98%. Thus the surface composites show high oil adsorption capacity of 0.9~1.1 g/cm3. It can absorb more oil than commercial sponges due to the surface composite swells after absorbing oil. It shows attractive potential application of the CNT/PVP surface composite in oil spill cleanup.

Colloidal antireflection coating improves graphene-silicon solar cells.

Carbon nanotube-Si and graphene-Si solar cells have attracted much interest recently owing to their potential in simplifying manufacturing process and lowering cost compared to Si cells. Until now, the power conversion efficiency of graphene-Si cells remains under 10% and well below that of the nanotube-Si counterpart. Here, we involved a colloidal antireflection coating onto a monolayer graphene-Si solar cell and enhanced the cell efficiency to 14.5% under standard illumination (air mass 1.5, 100 mW/cm(2)) with a stable antireflection effect over long time. The antireflection treatment was realized by a simple spin-coating process, which significantly increased the short-circuit current density and the incident photon-to-electron conversion efficiency to about 90% across the visible range. Our results demonstrate a great promise in developing high-efficiency graphene-Si solar cells in parallel to the more extensively studied carbon nanotube-Si structures.

A Low-Complexity Beamformer for Ultrasound Imaging Based on Sub-Beamformer and Multi-Apodization With Cross-Correlation.

OBJECTIVE: This paper proposes an ultrasound imaging algorithm based on sub-beamformer and multi-apodization with cross-correlation (SUB-MAX), aiming to achieve high resolution close to the minimum variance (MV) beamforming with low complexity and to enhance image contrast while maintaining background quality. METHODS: The output of two (N/2)-element DAS beamformers with asymmetric phase centers is subtracted, resulting in a large drop in the main-lobe amplitude, while the sidelobe maintains a relatively high amplitude level. Inspired by this characteristic, the coefficients with opposite trends compared with the subtracted output are obtained and fused with the normalized cross-correlation (NCC) weighting matrix acquired by using multi-pair received apodization, the proposed SUB-MAX obtains a new weighting matrix to weight the output of the DAS beamformer. RESULTS: For ats_wire point targets, the average full-width at half-maximum (FWHM) of SUB-MAX compared with DAS, DMAS, CF, and MAX decreases by 52.7%, 43.5%, 33.3%, and 52.7%, respectively. For geabr_0 cysts, the average contrast ratio (CR) of SUB-MAX compared with DAS, MV, DMAS, and CF increases by 57.7%, 86.8%, 2.5%, and 14.4%, respectively. Experiments on rat_tumor dataset also indicate that SUB-MAX has a superior comprehensive imaging performance. CONCLUSION: The experimental results indicate that the superior comprehensive imaging performance of the proposed SUB-MAX is expected to be suitable for real-time imaging systems due to its non-reliance on covariance matrix inversion.

Controllable synthesis of spongy carbon nanotube blocks with tunable macro- and microstructures.

Macroscopic carbon nanotubes (CNTs) with uniform structures are in great demand for use in composites and environmental materials. Here we demonstrate the controlled synthesis of spongy CNT blocks with isotropic properties and flexible, freestanding structures. The formation mechanism of the isotropic CNT sponges is discussed, based on its open-ended structure and initial formation in the vapor phase. The microstructure of the CNT sponges can be tuned by changing the flow rate of the carrier gas, resulting in CNT sponges with diameters ranging from 30.2 to 47.8 nm and wall thicknesses from 7 to 16 nm. The bulk density (5-25 mg cm(-3)), mechanical strength of the CNT sponges, and filling rate of ferromagnetic catalyst in the CNT sponges can also be modulated by controlling the supply rate of the carbon source, suggesting potential applications in mechanical energy absorption and environmental materials.

Suppression of the coffee-ring effect by self-assembling graphene oxide and monolayer titania.

The in situ self-assembly of two types of typical two-dimensional (2D) nanomaterials (i.e., graphene oxide (GO) and monolayer titania (TO)) is realized using a simple drop-casting method. Within the as-prepared hybrid films, the GO and TO nanosheets arrange alternately into a lamellar structure. Notably, the hybridization of GO and TO suppresses the formation of coffee-rings when drop-cast, which is attributed to the strong interactions between the GO and TO nanosheets. Finally, the mechanism for the in situ hybridization of these two types of nanosheets into heterogeneous lamellar films and the suppression of the coffee-ring effect are discussed. These results demonstrate the potential applications of drop-cast hybrid films for high-quality membrane deposition from liquid phases.

Flexible all solid-state supercapacitors based on chemical vapor deposition derived graphene fibers.

Flexible all-solid-state supercapacitors based on graphene fibers are demonstrated in this study. Surface-deposited oxide nanoparticles are used as pseudo-capacitor electrodes to achieve high capacitance. This supercapacitor electrode has an areal capacitance of 42 mF cm(-2), which is comparable to the capacitance for fiber-based supercapacitors reported to date. During the bending and cycling of the fiber-based supercapacitor, the stability could be maintained without sacrificing the electrochemical performance, which provides a novel and simple way to develop flexible, lightweight and efficient graphene-based devices.

Urinary Nickel Was Associated with the Prevalence of Diabetes: Results from NHANES.

The study aimed to investigate the association between nickel exposure and the presence of diabetes (DM). The participants were analyzed from the National Health and Nutrition Examination Surveys (NHANES) 2017-2018. Urinary nickel exposure was measured using inductively coupled-plasma mass spectrometry. DM was diagnosed based on the WHO standards. The association between nickel and DM or fasting glucose was examined using multivariable linear regression models and logistic regression models. A total of 1899 participants (933 men and 966 women) were included in our study, of whom 342 (18.0%) were diagnosed with DM. There was a significant positive association between nickel level and DM (OR: 1.27, 95%CI: 1.04-1.56) after adjusting for potential confounding factors. Comparing with the lowest quartile, the highest quartile independently increased a 0.66-fold higher risk of DM (OR: 1.66, 95%CI: 1.13-2.44]). In addition, nickel exposure was independently related to the level of fasting glucose. The exposure to nickel was associated with a higher risk of DM in general population.

Molecular complexes of drug combinations: A review of cocrystals, salts, coamorphous systems and amorphous solid dispersions.

As the advancements in the medical technology and healthcare develop through the years, combinational therapy has evolved to be an important treatment modality in many disease settings, including cancer, cardiovascular disease and infectious diseases. In an effort to alleviate "pill burden" and improve patient compliance, fixed dose combinations (FDCs) have been developed to be used as effective therapeutics. Among all FDCs, the category of drug-drug molecular complexes has been proven an efficient methodology in designing and treating diseases, with many drugs being approved. Among all drug-drug molecular complexes, drug-drug cocrystals, salts, coamorphous systems and solid dispersions have been successfully developed and many have been approved by the FDA. In this review, we dwell deeply into the molecular mechanisms behind the different types of drug-drug molecular complexes, including the key functional groups involved in the intermolecular interactions, the applications of each category of molecular complexes, as well as the advantages and challenges thereof. This comprehensive review provides useful insights into the practical design and manufacture of drug-drug molecular complexes and points out the future direction for the development of new advantageous combinational therapies that benefit more patients.

Controllable growth of triangular hexagonal boron nitride domains on copper foils by an improved low-pressure chemical vapor deposition method.

We demonstrate an improved low-pressure chemical vapor deposition method to fabricate hexagonal boron nitride (h-BN) domains of a few layers (one-four layers) from ammonia borane by adding a small quartz tube to stabilize the gas flow over the copper substrate and reducing the growing rate of h-BN. The h-BN grows freely and spontaneously to form triangular domains on the Cu (100) plane. The triangular domains are prone to be parallel to each other on the copper substrate. The h-BN domains grow by extending in the normal direction of the triangle and form a large thin film by joining together. Both the size and coverage rate on Cu foils are well controlled by tuning the amount of ammonia borane.

Topology evolution of graphene in chemical vapor deposition, a combined theoretical/experimental approach toward shape control of graphene domains.

Morphology control of thin film relies on understanding multiple ongoing processes during deposition and growth. To reveal the shape evolution of graphene domains on copper surfaces in chemical vapor deposition (CVD), a combinative study is performed on the CVD growth of graphene on copper surfaces. To identify the factors that influence the adsorption and diffusion of carbon atoms and further determine the domain shape, simulations based on kinetic Monte Carlo techniques are carried out. The results reveal the dependence of the graphene domain shapes on the crystalline orientation of the underlying copper substrate surfaces.

Preparation of highly oxidized nitrogen-doped carbon nanotubes.

A method for the preparation of highly oxidized nitrogen-doped carbon nanotubes (N-CNTs) from KMnO(4) + H(2)SO(4) solution is described. The atomic ratio of C/O in oxidized N-CNTs is as low as 1.2. The x-ray photoelectron spectroscopy results show that about 75% of the carbon atoms are oxidized and bound to oxygen-containing functional groups. The oxidation reaction mainly occurs at the outer sidewalls, which destroys the graphene stack to an sp(3)-rich structure and helps to preserve the tubular structure of the inner N-CNTs. The oxidized N-CNTs show an energy gap of ~2.1 eV.

Wire-supported CdSe nanowire array photoelectrochemical solar cells.

Previous fiber-shaped solar cells are based on polymeric materials or dye-sensitized wide band-gap oxides. Here, we show that efficient fiber solar cells can be made from semiconducting nanostructures (e.g. CdSe) with smaller band-gap as the light absorption material. We directly grow a vertical array of CdSe nanowires uniformly around a core metal wire and make the device by covering the top of nanowires with a carbon nanotube (CNT) film as the porous transparent electrode. The CdSe-CNT fiber solar cells show power conversion efficiencies of 1-2% under AM 1.5 illumination after the nanowires are infiltrated with redox electrolyte. We do not use a secondary metal wire (e.g. Pt) as in conventional fiber-shaped devices, instead, the end part of the CNT film is condensed into a conductive yarn to serve as the secondary electrode. In addition, our CdSe nanowire-based photoelectrochemical fiber solar cells maintain good flexibility and stable performance upon rotation and bending to large angles.

Strong and reversible modulation of carbon nanotube-silicon heterojunction solar cells by an interfacial oxide layer.

Deposition of nanostructures such as carbon nanotubes on Si wafers to make heterojunction structures is a promising route toward high efficiency solar cells with reduced cost. Here, we show a significant enhancement in the cell characteristics and power conversion efficiency by growing a silicon oxide layer at the interface between the nanotube film and Si substrate. The cell efficiency increases steadily from 0.5% without interfacial oxide to 8.8% with an optimal oxide thickness of about 1 nm. This systematic study reveals that formation of an oxide layer switches charge transport from thermionic emission to a mixture of thermionic emission and tunneling and improves overall diode properties, which are critical factors for tailoring the cell behavior. By controlled formation and removal of interfacial oxide, we demonstrate oscillation of the cell parameters between two extreme states, where the cell efficiency can be reversibly altered by a factor of 500. Our results suggest that the oxide layer plays an important role in Si-based photovoltaics, and it might be utilized to tune the cell performance in various nanostructure-Si heterojunction structures.

Achieving high efficiency silicon-carbon nanotube heterojunction solar cells by acid doping.

Various approaches to improve the efficiency of solar cells have followed the integration of nanomaterials into Si-based photovoltaic devices. Here, we achieve 13.8% efficiency solar cells by combining carbon nanotubes and Si and doping with dilute HNO(3). Acid infiltration of nanotube networks significantly boost the cell efficiency by reducing the internal resistance that improves fill factor and by forming photoelectrochemical units that enhance charge separation and transport. Compared to conventional Si cells, the fabrication process is greatly simplified, simply involving the transfer of a porous semiconductor-rich nanotube film onto an n-type crystalline Si wafer followed by acid infiltration.

The clinical characteristics of Chinese elderly patients with different durations of type 2 diabetes mellitus.

Aims: To explore the clinical characteristics among elderly (aged ≥60 years) patients with type 2 diabetes (T2DM) of different durations. Methods: Clinical characteristics were investigated in 3840 elderly T2DM patients according to their different durations of diabetes (< 1 year, 1~5 years, 5~10 years, and ≥ 10 years). Kruskal-Wallis and Dunn tests were used to assess the differences among groups for continuous variables. The chi-square and post hoc tests were carried out for dichotomous variables. The logistic regression was adopted to investigate the relationships between various durations of diabetes and the control rates of achieving the control targets for T2DM as well as diabetic vascular complications. Results: There were 972, 896, 875 and 1097 patients with a duration of diabetes of <1, 1~5, 5~10 and ≥10 years, respectively. In logistic regression models adjusted for age, sex, education, BMI, smoking and family history of diabetes, elderly T2DM patients with a duration of diabetes of ≥10 years were more likely to reach the comprehensive control targets for TC (ORTC = 1.36, 95% CI =1.14-1.63), LDL-C (ORLDL-C = 1.39, 95% CI =1.17-1.66), TG (ORTG = 1.76, 95% CI =1.46-2.12) and BMI (ORBMI = 1.82, 95% CI =1.52-2.18). Elderly T2DM patients with a duration of diabetes of 1~5 years were more likely to achieve the HbA1c control target (ORHbA1c = 1.92, 95% CI = 1.59-2.31) than elderly T2DM patients with a duration of diabetes of <1 year. Furthermore, in elderly T2DM patients with a duration of diabetes of 5~10 years or ≥ 10 years, the duration of diabetes was positively associated with diabetic macrovascular complications (coronary heart disease and peripheral artery disease). In elderly T2DM patients with a duration of diabetes of over 10 years, the duration of diabetes was associated with diabetes kidney disease (all P < 0.05). Conclusions: It is worth noting that the clinical characteristics of elderly patients with type 2 diabetes in different durations of diabetes are different.