A Molecular Imaging Approach to Mercury Sensing Based on Hyperpolarized 129Xe Molecular Clamp Probe
Qianni Guo1, Qingbin Zeng1, Weiping Jiang1, Xiaoxiao Zhang1, Qing Luo1, and Xin Zhou1

1Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan, China, People's Republic of

Synopsis

Mercury contamination is widespread and arises from a variety of natural sources.We propose the use of hyperpolarized 129Xe nuclear magnetic resonance (NMR) spectroscopy for the sensitive detection of Hg2+ ions in aqueous solution.We develop a biosensor whose molecular structure is like a clamp. When interact with Hg2+ in aqueous solution, the molecular structure of the biosensor could be changed as a clamp from “open” to “closed”. This molecular structure change causes the distance between the two cryptophane cages of the biosensor become closer, and the electron cloud of them overlapped. As a result, comparing with normal downfield chemical shifts of the reported xenon biosensors formetallic ions, the Xe caged in the cryptophane moiety shows a upfield chemical shift change from 66.5 ppm to 66.1 ppm. Images were obtained using a CSI method preciously used for clinical MRI.

Contamination with heavy metal ions may have severe effects on human health and the environment. Mercury contamination is widespread and arises from a variety of natural sources. 1 In the reported small-molecule sensors, only a few compounds can selectively detect Hg2+ ion in aqueous solutions. Herein we propose the use of hyperpolarized 129Xe magnetic resonance image (MRI) for the sensitive detection of Hg2+ ions in aqueous solution. To achieve this goal, we develop a biosensor whose molecular structure is like a clamp. The biosensor is developed using dipyrrolylquinoxaline as the basic molecular clamp scaffold, pyrrole and the hydrazone as the recognition site, and cryptophane as the 129Xe NMR signal reported moiety. 2, 3 When interact with Hg2+ in aqueous solution, the molecular structure of the biosensor could be changed as a clamp from "open" to "closed". This molecular structure change causes the distance between the two cryptophane cages of the biosensor become closer, and the electron cloud of them overlapped. As a result, comparing with normal downfield chemical shifts of the reported xenon biosensors formetallic ions, the Xe caged in the cryptophane moiety shows a upfield chemical shift change from 66.5 ppm to 66.1 ppm (Δ=38.6 Hz). Images were obtained using a CSI method preciously used for clinical MRI. (Fig. 1).

Acknowledgements

No acknowledgement found.

References

1. P. Mazumdar, D. Das, A. Misra, et al. Phys. Chem. Chem. Phys., 2014, 16, 6283-6293.

2. L. Wang, X-J. Zhu, W-Y. Wong, et al. Dalton. Trans. 2005, 3235-3240.

3. N. Kotera, N. Tassali, P. Berthault, et al. Angew. Chem. Int. Ed. 2012, 51, 4100-4103.

Figures

Fig. 1 (i) 129Xe NMR spectra and MRI of the clamp biosensor on the addition of Hg2+. (ii) The molecular structure change and electron cloud overlap diagram of the biosensor as a molecular clamp from "open" to "closed" when binding with Hg2+.



Proc. Intl. Soc. Mag. Reson. Med. 24 (2016)
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