Selective extraction of semiconducting carbon nanotubes is a key step in the production of high-performance, solution-processed electronics. Here, we describe the ability of a supramolecular sorting polymer to selectively disperse semiconducting carbon nanotubes from five commercial sources with diameters ranging from 0.7 to 2.2 nm. The sorting purity of the largest-diameter nanotubes (1.4 to 2.2 nm; from Tuball) was confirmed by short channel measurements to be 97.5%. Removing the sorting polymer by acid-induced disassembly increased the transistor mobility by 94 and 24% for medium-diameter and large-diameter carbon nanotubes, respectively. Among the tested single-walled nanotube sources, the highest transistor performance of 61 cm/V·s and on/off ratio >10 were realized with arc discharge carbon nanotubes with a diameter range from 1.2 to 1.7 nm. The length and quality of nanotubes sorted from different sources is compared using measurements from atomic force microscopy and Raman spectroscopy. The transistor mobility is found to correlate with the G/D ratio extracted from the Raman spectra.
Particle size is a key parameter that must be measured to ensure reproducible production of cellulose nanocrystals (CNCs) and to achieve reliable performance metrics for specific CNC applications. Nevertheless, size measurements for CNCs are challenging due to their broad size distribution, irregular rod-shaped particles, and propensity to aggregate and agglomerate. We report an interlaboratory comparison (ILC) that tests transmission electron microscopy (TEM) protocols for image acquisition and analysis. Samples of CNCs were prepared on TEM grids in a single laboratory, and detailed data acquisition and analysis protocols were provided to participants. CNCs were imaged and the size of individual particles was analyzed in 10 participating laboratories that represent a cross section of academic, industrial, and government laboratories with varying levels of experience with imaging CNCs. The data for each laboratory were fit to a skew normal distribution that accommodates the variability in central location and distribution width and asymmetries for the various datasets. Consensus values were obtained by modeling the variation between laboratories using a skew normal distribution. This approach gave consensus distributions with values for mean, standard deviation, and shape factor of 95.8, 38.2, and 6.3 nm for length and 7.7, 2.2, and 2.9 nm for width, respectively. Comparison of the degree of overlap between distributions for individual laboratories indicates that differences in imaging resolution contribute to the variation in measured widths. We conclude that the selection of individual CNCs for analysis and the variability in CNC agglomeration and staining are the main factors that lead to variations in measured length and width between laboratories.
We present the conducting polymer poly (3,4-ethylenedioxythiophene) (PEDOT) doped with an algal-derived glycan extract, Phycotrix™ [xylorhamno-uronic glycan (XRU84)], as an innovative electrically conductive material capable of providing beneficial biological and electrical cues for the promotion of favorable wound healing processes. Increased loading of the algal XRU84 into PEDOT resulted in a reduced surface nanoroughness and interfacial surface area and an increased static water contact angle. PEDOT-XRU84 films demonstrated good electrical stability and charge storage capacity and a reduced impedance relative to the control gold electrode. A quartz crystal microbalance with dissipation monitoring study of protein adsorption (transferrin, fibrinogen, and collagen) showed that collagen adsorption increased significantly with increased XRU84 loading, while transferrin adsorption was significantly reduced. The viscoelastic properties of adsorbed protein, characterized using the ΔD/Δf ratio, showed that for transferrin and fibrinogen, a rigid, dehydrated layer was formed at low XRU84 loadings. Cell studies using human dermal fibroblasts demonstrated excellent cell viability, with fluorescent staining of the cell cytoskeleton illustrating all polymers to present excellent cell adhesion and spreading after 24 h.
Vat photopolymerization (VP) is an advanced additive manufacturing (AM) platform that enables production of intricate 3D monoliths that are unattainable with conventional manufacturing methods. In this work, modification of amorphous poly(arylene ether sulfone)s (PSU) allows for VP printing. Post-polymerization telechelic functionalization with acrylate functionality yielded photocrosslinkable PSUs across a molecular weight range. 1 H NMR spectroscopy confirms chemical composition and quantitative acrylate functionalization. Addition of diphenyl-(2,4,6-trimethylbenzoyl)phosphine oxide (TPO) photoinitiator to 30 wt% PSU solutions in NMP provides a photocurable composition. However, subsequent photorheological studies elucidate rapid photodegradation of the polysulfone main chain, which is especially apparent in high M n (15 kg mol −1 ) PSU formulations. UV-light intensity and wavelength range are altered to reduce degradation while allowing for efficient crosslinking. The addition of 0.5 wt% of avobenzone photoblocker produces an ill-defined structure with 6 kg mol −1 PSU. For higher molecular weights (>12 kg mol −1 ), solutions with a low molar mass reactive diluent, i.e., trimethylolpropane triacrylate, enable the printing of an organogel with a storage modulus (>10 5 Pa) sufficient for vat photopolymerization. Employing multicomponent solutions provide well-defined parts with complex geometries through vat photopolymerization.
Glioblastoma (GBM) is the most common and aggressive primary adult brain tumor in the US. The current treatment regimen for GBM still retains an alarmingly poor prognosis, with median survival of only 14.6 months. Failure to generate more effective treatment strategies is due to the infiltrative nature of GBM tumor cells, which hinders complete surgical resection, and cellular heterogeneity within GBM tumors, with a sub-population of glioma stem cells (GSCs) resistant to irradiation treatment and chemotherapeutic agents including temozolomide. As a result, all treated GBM patients will experience tumor recurrence, highlighting the need for novel approaches in targeting such refractory tumor cell populations to successfully treat GBM tumors and prevent recurrence. Using super resolution localization microscopy, we have identified that increased interaction of connexin43 (Cx43) with microtubules in GSCs confers tumorigenic behavior to these cells. We employed a Cx43 mimetic peptide named JM2 (juxtamembrane 2) that encompasses the microtubule binding sequence of the Cx43 carboxy-terminus. This peptide drug efficiently and specifically disrupts the interaction of Cx43 with microtubules and limits GSC survival, proliferation, and migration, without affecting normal human astrocytes. Next, we implemented the therapeutic strategy of JM2 encapsulation within biodegradable polymeric nanoparticles (NPs) to reduce administration frequency and patient discomfort, and increase peptide stability and activity. We confirmed sustained release of JM2 from these poly(lactic-co-glycolic) acid biodegradable NPs, and JM2 bioactivity through disruption of Cx43 interaction with microtubules. Administration of JM2-NPs inhibits GSC-derived neurosphere formation in vitro and patient GBM-derived organoid growth ex vivo. Finally, using an orthotopic xenograft brain tumor mouse model, we demonstrate in vivo that JM2-NPs significantly decrease the number of GSCs within brain tumors, and inhibit the formation of highly invasive GBM tumors. Our findings on generation of JM2-NPs to target GSC survival lays the foundation for future clinical trials in newly diagnosed GBM patients.
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