Nanoscale Catalysts for NMR Signal Enhancement by Reversible Exchange
| Autor: | Aaron M. Coffey, Eduard Y. Chekmenev, Fan Shi, Kevin W. Waddell, Boyd M. Goodson |
|---|---|
| Jazyk: | angličtina |
| Rok vydání: | 2015 |
| Předmět: |
chemistry.chemical_classification
inorganic chemicals 010405 organic chemistry Nanoparticle chemistry.chemical_element Polymer 010402 general chemistry 01 natural sciences Article 0104 chemical sciences Surfaces Coatings and Films Electronic Optical and Magnetic Materials Catalysis chemistry.chemical_compound General Energy chemistry Methacrylic acid Chemical engineering Pyridine Proton NMR Molecule Organic chemistry Iridium Physical and Theoretical Chemistry |
| Zdroj: | The Journal of Physical Chemistry. C, Nanomaterials and Interfaces |
| ISSN: | 1932-7455 1932-7447 |
| Popis: | Two types of nanoscale catalysts were created to explore NMR signal enhancement via reversible exchange (SABRE) at the interface between heterogeneous and homogeneous conditions. Nanoparticle and polymer comb variants were synthesized by covalently tethering Ir-based organometallic catalysts to support materials composed of TiO2/PMAA (poly(methacrylic acid)) and PVP (polyvinylpyridine), respectively, and characterized by AAS, NMR, and DLS. Following parahydrogen (pH2) gas delivery to mixtures containing one type of “nano-SABRE” catalyst particle, a target substrate, and ethanol, up to ∼(−)40-fold and ∼(−)7-fold 1H NMR signal enhancements were observed for pyridine substrates using the nanoparticle and polymer comb catalysts, respectively, following transfer to high field (9.4 T). These enhancements appear to result from intact particles and not from any catalyst molecules leaching from their supports; unlike the case with homogeneous SABRE catalysts, high-field (in situ) SABRE effects were generally not observed with the nanoscale catalysts. The potential for separation and reuse of such catalyst particles is also demonstrated. Taken together, these results support the potential utility of rational design at molecular, mesoscopic, and macroscopic/engineering levels for improving SABRE and HET-SABRE (heterogeneous-SABRE) for applications varying from fundamental studies of catalysis to biomedical imaging. |
| Databáze: | OpenAIRE |
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