期刊
ANALYTICAL CHEMISTRY
卷 89, 期 13, 页码 7190-7194出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.7b01363
关键词
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资金
- National Science Foundation (NSF) [CHE-1153159, CHE-1508707, CHE-1048804]
- Arnold and Mabel Beckman Foundation
- Max Planck Society
- Jonsson Comprehensive Cancer Center Foundation at UCLA
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1508707] Funding Source: National Science Foundation
Parahydrogen-induced polarization (PHIP) is a method for enhancing NMR sensitivity. The pairwise addition of parahydrogen in aqueous media by heterogeneous catalysts can lead to applications in chemical and biological systems. Polarization enhancement can be transferred from H-1 to C-13 for longer lifetimes by using zero field cycling. In this work, water-dispersible N-acetylcysteine- and l-cysteine-stabilized palladium nanoparticles are introduced, and carbon polarizations up to 2 orders of magnitude higher than in previous aqueous heterogeneous PHIP systems are presented. (PC)-C-13 values of 1.2 and 0.2% are achieved for the formation of hydroxyethyl propionate from hydroxyethyl acrylate and ethyl acetate from vinyl acetate, respectively. Both nanoparticle systems are easily synthesized in open air, and TEM indicates an average size of 2.4 +/- 0.6 nm for NAC@Pd and 2.5 +/- 0.8 nm for LCys@Pd nanoparticles with 40 and 25% ligand coverage determined by thermogravimetric analysis, respectively. As a step toward biological relevance, results are presented for the unprotected amino acid allylglycine upon aqueous hydrogenation of propargylglycine.
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