期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 120, 期 22, 页码 12149-12156出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.6b04484
关键词
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资金
- NIH [1R21EB018014, 1R21EB020323]
- NSF [CHE-1416432, CHE-1416268]
- DOD [W81XWH-12-1-0159/BC112431, W81XWH-15-1-0271, W81XWH-15-1-0272]
- Exxon Mobil Knowledge Build
- NIH NIBIB [T32 EB001628]
- Gower summer research fellowship (SIUC)
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1416432] Funding Source: National Science Foundation
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1416268] Funding Source: National Science Foundation
Two synthetic strategies are investigated for the preparation of water-soluble iridium-based catalysts for NMR signal amplification by reversible exchange (SABRE). In one approach, PEGylation of a variant N-heterocyclic carbene provided a novel catalyst with excellent water solubility. However, while SABRE-active in ethanol solutions, the catalyst lost activity in >50% water. In a second approach, synthesis of a novel di-iridium complex precursor where the cyclooctadiene (COD) rings have been replaced by CODDA (1,2-dihydroxy-3,7-cyclooctadiene) leads to the creation of a catalyst [IrCl(CODDA)IMes] that can be dissolved and activated in water-enabling aqueous SABRE in a single step, without need for either an organic cosolvent or solvent removal followed by aqueous reconstitution. The potential utility of the CODDA catalyst for aqueous SABRE is demonstrated with the similar to(-)32-fold enhancement of H-1 signals of pyridine in water with only 1 atm of parahydrogen.
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