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Physical-chemical factors known to influence water exchange rates in EuDOTA-tetraamide complexes were used to design new paraCEST agents with record slow water exchange kinetics. The solution structure of the complexes as determined by analysis of lanthanide-induced paramagnetic shifts compared favorably to the structures determined by DTF calculations. In vitro CEST experiments demonstrated that these slow water exchange systems translated to optimal CEST imaging of one of the complexes in mouse kidneys.
EuDOTA-tetraamide complexes as paraCEST agents offer an attractive platform for designing biological sensors and responsive agents. The early versions of these agents showed low sensitivity at temperature and power levels suitable for in vivo applications partly due to non-optimal water exchange rates. Here we report two new EuDOTA derivatives having glutamyl-phosphonate side arms that display the slowest water exchange rates of any other paraCEST agent reported so far. The advantages of such systems are demonstrated experimentally both in vitro and in vivo and DFT calculations were performed to help understand the physical-chemical reasons for this interesting behavior.
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