Production, isolation, and shipment of clinically relevant quantities of astatine-211: A simple and efficient approach to increasing supply.

The alpha emitter astatine-211 (211At) is a promising candidate for cancer treatment based on Targeted Alpha (α) Therapy (TAT). A small number of facilities, distributed across the United States, are capable of accelerating α-particle beams to produce 211At. However, challenges remain regarding strategic methods for shipping 211At in a form adaptable to advanced radiochemistry reactions and other uses of the radioisotope. PURPOSE: Our method allows shipment of 211At in various quantities in a form convenient for further radiochemistry. PROCEDURES: For this study, a 3-octanone impregnated Amberchrom CG300M resin bed in a column cartridge was used to separate 211At from the bismuth matrix on site at the production accelerator (Texas A&M) in preparation for shipping. Aliquots of 6 M HNO3 containing up to ≈2.22 GBq of 211At from the dissolved target were successfully loaded and retained on columns. Exempt packages (<370 MBq) were shipped to a destination radiochemistry facility, University of Texas MD Anderson Cancer Center, in the form of a convenient air-dried column. Type A packages have been shipped overnight to University of Alabama at Birmingham. MAIN FINDINGS: Air-dried column hold times of various lengths did not inhibit simple and efficient recovery of 211At. Solution eluted from the column was sufficiently high in specific activity to successfully radiolabel a model compound, 4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)aniline (1), with 211At. The method to prepare and ship 211At described in this manuscript has also been used to ship larger quantities of 211At a greater distance to University of Alabama at Birmingham. PRINCIPAL CONCLUSIONS: The successful proof of this method paves the way for the distribution of 211At from Texas A&M University to research institutions and clinical oncology centers in Texas and elsewhere. Use of this simple method at other facilities has the potential increase the overall availability of 211At for preclinical and clinical studies.

Focused Ion Beam-Prepared Transmission Electron Microscopy Examination of Atmospheric Chemical Vapor-Infiltrated Silicon Carbide Morphology.

Silicon carbide (SiC)-based ceramic matrix composites (CMCs) are utilized for their refractory properties in the aerospace industry. The composition and structure of these materials are crucial to maintaining the strength, toughness, oxidation, and creep resistances that are desired of silicon carbide. This work analyzes the chemical composition of the matrix in batches of SiC/SiC (silicon carbide fiber-reinforced silicon carbide matrix) minicomposites that are processed by chemical vapor infiltration of the BN interphase and SiC matrix on single Hi-Nicalon Type S fiber tows using a range of processing parameters. The analysis was performed here to investigate the potential causes of variation in matrix tensile strength in the various batches of minicomposites. Six different morphologies present in the silicon carbide matrix were observed: smooth, nodular, rough nodular, bumpy, nucleated, and plate-like. It was found that high-matrix tensile strength minicomposite batches contained solely the smooth morphology, while low-matrix tensile strength minicomposite batches contained a variety of other morphologies. FIB/TEM was used to study the atomic and crystal character of each individual morphology. Smooth SiC is oriented by the (111) planes and is primarily SiC, while the other morphologies are randomly oriented and contain significant oxygen. These results match the tensile strength tests, which pointed to smooth SiC as the strongest matrix material.

Magnetic Nanoparticles with Surface Nanopockets for Highly Selective Antibody Isolation.

Monoclonal antibodies (mAbs) are key components of revolutionary disease immunotherapies and are also essential for medical diagnostics and imaging. The impact of cost is illustrated by a price >$200,000 per year per patient for mAb-based cancer therapy. Purification represents a major issue in the final cost of these immunotherapy drugs. Protein A (PrA) resins are widely used to purify antibodies, but resin cost, separation efficiency, reuse, and stability are major issues. This paper explores a synthesis strategy for low-cost, reusable, stable PrA-like nanopockets on core-shell silica-coated magnetic nanoparticles (NPs) for IgG antibody isolation. Mouse IgG2a, a strong PrA binder, was used as a template protein, first attaching it stem-down onto the NP surface. The stem-down orientation of IgG2a on the NP surface before polymerization is critical for designing the films to bind IgGs. Following this, 1-tetraethoxysilane and four organosilane monomers with functional groups capable of mimicking binding interactions of proteins with IgG antibody stems were reacted to form a thin polymer coating on the NPs. After blocking nonspecific binding sites, removal of the mouse IgG2a provided nanopockets on the core-shell NPs that showed binding characteristics for antibodies remarkably similar to PrA. Both smooth and rough core-shell NPs were used, with the latter providing much larger binding capacities for IgGs, with an excellent selectivity slightly better than that of commercial PrA magnetic beads. This paper is the first report of IgG-binding NPs that mimic PrA selectivity. These nanopocket NPs can be used for at least 15 regeneration cycles, and cost/use was 57-fold less than a high-quality commercial PrA resin.

Catalytic manganese oxide nanostructures for the reverse water gas shift reaction.

Understanding the fundamental structure-property relationships of nanomaterials is critical for many catalytic applications as they comprise of the catalyst designing principles. Here, we develop efficient synthetic methods to prepare various MnO2 structures and investigate their catalytic performance as applied to the reverse Water Gas Shift (rWGS) reaction. We show that the support-free MnO derived from MnO2 1D, 2D and 3D nanostructures are highly selective (100% CO2 to CO), thermally stable catalysts (850 °C) and differently effective in the rWGS. Up to 50% conversion is observed, with a H2/CO2 feed-in ratio of 1 : 1. From both experiments and DFT calculations, we find the MnO2 morphology plays a critical role in governing the catalytic behaviors since it affects the predominant facets exposed under reaction conditions as well as the intercalation of K+ as a structural building block, substantially affecting the gas-solid interactions. The relative adsorption energy of reactant (CO2) and product (CO), ΔE = Eads(CO2) -Eads(CO), is found to correlate linearly with the catalytic activity, implying a structure-function relationship. The strong correlation found between Eads(CO2) -Eads(CO), or more generally, Eads(R) -Eads(P), and catalytic activity makes ΔE a useful descriptor for characterization of efficient catalysts involving gas-solid interactions beyond the rWGS.

Trends in Solid Adsorbent Materials Development for CO2 Capture.

A recent report from the United Nations has warned about the excessive CO2 emissions and the necessity of making efforts to keep the increase in global temperature below 2 °C. Current CO2 capture technologies are inadequate for reaching that goal, and effective mitigation strategies must be pursued. In this work, we summarize trends in materials development for CO2 adsorption with focus on recent studies. We put adsorbent materials into four main groups: (I) carbon-based materials, (II) silica/alumina/zeolites, (III) porous crystalline solids, and (IV) metal oxides. Trends in computational investigations along with experimental findings are covered to find promising candidates in light of practical challenges imposed by process economics.