4.7 Article

Basis for Sensitive and Selective Time-Delayed Luminescence Detection of Hydroxyl Radical by Lanthanide Complexes

期刊

INORGANIC CHEMISTRY
卷 52, 期 16, 页码 9390-9398

出版社

AMER CHEMICAL SOC
DOI: 10.1021/ic4009569

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资金

  1. National Science Foundation [1151665]
  2. NIH-CBITG [GM 08700]
  3. Department of Chemistry of the University of Minnesota
  4. Division Of Chemistry
  5. Direct For Mathematical & Physical Scien [1151665] Funding Source: National Science Foundation

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Molecular probes for the detection of hydroxyl radical (HO center dot) by time-delayed luminescence spectroscopy directly in water at neutral pH with high sensitivity and selectivity are presented. The bimolecular probes consist of a lanthanide complex with open coordination sites and a reactive pre-antenna composed of an aromatic acid or amide; the latter binds to and sensitizes terbium emission upon hydroxylation by HO center dot. These probes exhibit long luminescence lifetimes compatible with time-delayed measurements that remove interfering background fluorescence from the sample. Six different reactive pre-antenna (benzoate, benzamide, isophthalate, isophthalamide, trimesate, and trimesamide) and two different terbium complexes [Tb-(1,4,7,10-tetraazacyclododecane-1,4,7-tris(acetic acid)) (Tb-DO3A) and Tb-(1,4,7,10-tetraazacyclododecane-1,7-bis(acetic acid)) (Tb-DO2A)] were evaluated. Of these the trimesamide/Tb-DO3A system enables the most sensitive detection of HO center dot with an about 1000-fold increase in metal-centered time-delayed emission upon hydroxylation of the pre-antenna to 2-hydroxytrimesamide. Excellent selectivity for both the trimesamide/Tb-DO3A and trimesate/Tb-DO3A systems over other reactive oxygen and nitrogen species are observed. Notably, the increase in metal-centered luminescence intensity is not associated with a decrease in the hydration number (q) of Tb-DO3A, suggesting that the antenna is interacting with the lanthanide via a second sphere coordination environment or that coordination by the antenna occurs by displacement of one or more of the carboxylate arms of DO3A. Formation of a weak ternary complex Tb-DO3A center dot hydroxytrimesamide was confirmed by temperature-dependent titration and a decrease in K-app with increasing temperature.

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