期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 133, 期 43, 页码 17370-17374出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja2057924
关键词
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资金
- Japan Society for the Promotion of Science (JSPS)
- JST CREST
- Natural Science Foundation of China [20902055]
- Grants-in-Aid for Scientific Research [09F09259, 20111008] Funding Source: KAKEN
A novel amphiphilic Tb3+ complex (TbL+) having anionic bis(pyridine) arms and a hydrophobic alkyl chain is developed. It spontaneously self-assembles in water and gives stable vesicles that show sensitized luminescence of Tb3+ ions at neutral pH. This TbL+ complex is designed to show coordinative unsaturation, i.e., water molecules occupy some of the first coordination spheres and are replaceable upon binding of phosphate ions. These features render TbL+ self-assembling receptor molecules which show increase in the luminescence intensity upon binding of nucleotides. Upon addition of adenosine triphosphate (ATP), significant amplification of luminescent intensity was observed. On the other hand, ADP showed moderately increased luminescence and almost no enhancement was observed for AMP. Very interestingly, the increase in luminescence intensity observed for ATP and ADP showed sigmoidal dependence on the concentration of added nucleotides. It indicates positive cooperative binding of these nucleotides to TbL+ complexes preorganized on the vesicle surface. Self-assembly of amphiphilic Tb3+ receptor complexes provides nanointerfaces which selectively convert and amplify molecular information of high energy phosphates linked by phosphoanhydride bonds into luminescence intensity changes.
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