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
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Chem. Phys., 2014, 16, 6283-6293.
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3. N. Kotera, N. Tassali, P. Berthault, et al. Angew. Chem. Int. Ed. 2012, 51, 4100-4103.