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      Hyperpolarized Xe NMR signal advancement by metal-organic framework entrapment in aqueous solution

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          Significance

          Hyperpolarized 129Xe NMR/MRI is a useful method for diagnosis of diseases of the respiratory system. However, the sensitive detection of specific compounds in blood remains a challenge because of the weak 129Xe signal in aqueous solution. We developed a way, Hyper-SAME, to promote the 129Xe signal in aqueous solution. The 129Xe signal intensity is four times beyond that of free 129Xe in water and 200 times better than the benchmark molecular cage, cryptophane-A, in its saturated aqueous solution. Additionally, the hyperpolarized 129Xe signal can be amplified further by combining Hyper-SAME with hyperpolarized 129Xe chemical exchange saturation transfer.

          Abstract

          We report hyperpolarized Xe signal advancement by metal-organic framework (MOF) entrapment (Hyper-SAME) in aqueous solution. The 129Xe NMR signal is drastically promoted by entrapping the Xe into the pores of MOFs. The chemical shift of entrapped 129Xe is clearly distinguishable from that of free 129Xe in water, due to the surface and pore environment of MOFs. The influences from the crystal size of MOFs and their concentration in water are studied. A zinc imidazole MOF, zeolitic imidazole framework-8 (ZIF-8), with particle size of 110 nm at a concentration of 100 mg/mL, was used to give an NMR signal with intensity four times that of free 129Xe in water. Additionally, Hyper-SAME is compatible with hyperpolarized 129Xe chemical exchange saturation transfer. The 129Xe NMR signal can be amplified further by combining the two techniques. More importantly, Hyper-SAME provides a way to make detection of hyperpolarized 129Xe in aqueous solution convenient and broadens the application area of MOFs.

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          Author and article information

          Journal
          Proc Natl Acad Sci U S A
          Proc. Natl. Acad. Sci. U.S.A
          pnas
          pnas
          PNAS
          Proceedings of the National Academy of Sciences of the United States of America
          National Academy of Sciences
          0027-8424
          1091-6490
          28 July 2020
          13 July 2020
          : 117
          : 30
          : 17558-17563
          Affiliations
          [1] aKey Laboratory of Magnetic Resonance in Biological Systems, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences-Wuhan National Laboratory for Optoelectronics, 430071 Wuhan, People’s Republic of China;
          [2] bKey Laboratory of Biomedical Polymers, Ministry of Education, College of Chemistry and Molecular Sciences, Wuhan University , 430072 Wuhan, People’s Republic of China;
          [3] c University of Chinese Academy of Sciences , 100049 Beijing, People’s Republic of China;
          [4] dState Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University , 200240 Shanghai, People’s Republic of China;
          [5] eThe Institute of Advanced Studies, Wuhan University , 430072 Wuhan, People’s Republic of China
          Author notes
          2To whom correspondence may be addressed. Email: qian-niguo@ 123456wipm.ac.cn , hdeng@ 123456whu.edu.cn , or xinzhou@ 123456wipm.ac.cn .

          Edited by Omar M. Yaghi, University of California, Berkeley, CA, and approved June 15, 2020 (received for review March 24, 2020)

          Author contributions: Q.G., H.D., and X. Zhou designed research; Q.Z. and B.B. performed research; Y. Yuan, Q.H., X.H., P.L., and X. Zhou contributed new reagents/analytic tools; Q.G., M.C., X. Zhang, Y. Yang, and M.L. analyzed data; and Q.G., H.D., and X. Zhou wrote the paper.

          1Q.Z. and B.B. contributed equally to this work.

          Author information
          https://orcid.org/0000-0001-6075-9690
          https://orcid.org/0000-0002-6112-0765
          https://orcid.org/0000-0003-2040-4291
          https://orcid.org/0000-0001-9858-2747
          https://orcid.org/0000-0003-3493-0655
          https://orcid.org/0000-0001-8458-5568
          https://orcid.org/0000-0002-9398-7996
          Article
          PMC7395552 PMC7395552 7395552 202004121
          10.1073/pnas.2004121117
          7395552
          32661173
          50d00ea3-212b-48c6-bbd3-89deeaa05c9c
          Copyright @ 2020

          Published under the PNAS license.

          History
          Page count
          Pages: 6
          Funding
          Funded by: National Natural Science Foundation of China (NSFC) 501100001809
          Award ID: 81625011
          Award ID: 91859206
          Award ID: 21921004
          Award Recipient : Hexiang Deng Award Recipient : Xin Zhou
          Funded by: National Natural Science Foundation of China (NSFC) 501100001809
          Award ID: 21971199
          Award Recipient : Hexiang Deng Award Recipient : Xin Zhou
          Funded by: National Key R&D Program of China
          Award ID: 2018YFA0704000
          Award Recipient : Hexiang Deng Award Recipient : Xin Zhou
          Categories
          Physical Sciences
          Chemistry

          signal advancement,MRI,NMR,MOFs,Hyper-CEST
          signal advancement, MRI, NMR, MOFs, Hyper-CEST

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