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1.
J Am Chem Soc ; 146(21): 14587-14592, 2024 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-38716882

RESUMO

The ability to controllably move gaseous ions is an essential aspect of ion-based spectrometry (e.g., mass spectrometry and ion mobility spectrometry) as well as materials processing. At higher pressures, ion motion is largely governed by diffusion and multiple collisions with neutral gas molecules. Thus, high-pressure ion optics based on electrostatics require large fields, radio frequency drives, complicated geometries, and/or partially transmissive grids that become contaminated. Here, we demonstrate that low-power standing acoustic waves can be used to guide, block, focus, and separate beams of ions akin to electrostatic ion optics. Ions preferentially travel through the static-pressure regions ("nodes") while neutral gas does not appear to be impacted by the acoustic field structure and continues along a straight trajectory. This acoustic ion manipulation (AIM) approach has broad implications for ion manipulation techniques at high pressure, while expanding our fundamental understanding of the behavior of ions in gases.

2.
Langmuir ; 39(5): 1786-1792, 2023 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-36701245

RESUMO

The interpretation of color change in sensors and tests can be linked to incorrect conclusions if the intrinsic color changes are not accounted for. In this work, we study the intrinsic color change associated with the process of embedding nanoparticles in a polymer to create nanocomposite films. We present a safer, faster method to coat silver nanoparticles with silica and employ a seven-factor Plackett-Burman design to identify critical factors in the synthesis. Silver nanodisks with increasing thicknesses of the silica shell showed a decreasing sensitivity of their localized surface plasmon resonance (LSPR) toward changes in the refractive index surrounding the nanoparticle. A color shift of up to 72 nm was observed when bare nanoparticles were embedded in poly(vinyl alcohol), but no color change was perceived when nanoparticles were coated with a 25-nm-thick silica shell. Understanding the origin of color changes intrinsic to the preparation of polymeric nanocomposites aids in the design and correct use of plasmonic sensors.

3.
ACS Omega ; 6(35): 22589-22602, 2021 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-34514231

RESUMO

A synthetic strategy yielded polyelectrolytes and polyampholytes with tunable net charge for complexation and protein binding. Organocatalytic ring-opening polymerizations yielded aliphatic polycarbonates that were functionalized with both carboxylate and ammonium side chains in a post-polymerization, radical-mediated thiol-ene reaction. Incorporating net charge into the polymer architecture altered the chain dimensions in phosphate buffered solution in a manner consistent with self-complexation and complexation behavior with model proteins. A net cationic polyampholyte with 5% of carboxylate side chains formed large clusters rather than small complexes with bovine serum albumin, while 50% carboxylate polyampholyte was insoluble. Overall, the aliphatic polycarbonates with varying net charge exhibited different macrophase solution behaviors when mixed with protein, where self-complexation appears to compete with protein binding and larger-scale complexation.

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