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@ARTICLE{Adelabu:306517,
author = {I. Adelabu and J. Gyesi and M. R. H. Chowdhury and C.
Oladun and S. Nantogma and G. Foren and A. Samoilenko and J.
Ettedgui and R. E. Swenson and M. C. Krishna and P. TomHon
and T. Theis and H. de Maissin and A. Schmidt$^*$ and B. M.
Goodson and S. Scofield and L. Stilgenbauer and M.
Sadagurski and E. Y. Chekmenev},
title = {{M}ultidimensional p{H}-{T}emperature {M}apping of
{SABRE}-{SHEATH} 13{C} {H}yperpolarization of
[1-13{C}]{P}yruvate.},
journal = {The journal of physical chemistry / B},
volume = {nn},
issn = {1520-6106},
address = {Washington, DC},
publisher = {Americal Chemical Society},
reportid = {DKFZ-2025-02582},
pages = {nn},
year = {2025},
note = {epub},
abstract = {Hyperpolarized [1-13C]pyruvate has emerged as a
next-generation molecular probe for in vivo metabolic flux
imaging in deep tissue. This molecular contrast agent is now
under evaluation in over 50 clinical trials, according to
clinicaltrials.gov. Hyperpolarized [1-13C]pyruvate is
produced through dissolution dynamic nuclear polarization
(d-DNP) for clinical research use. This remarkable
hyperpolarization technique is regarded as expensive (>2 M
equipment cost) and slow (1 h production). One alternative
hyperpolarization technique called Signal Amplification By
Reversible Exchange (SABRE) in SHield Enables Alignment
Transfer to Heteronuclei (SABRE-SHEATH) has recently
garnered substantial attention for production of
hyperpolarized [1-13C]pyruvate quickly (in 1 min) and
inexpensively (<$20K equipment). It has been successfully
demonstrated in vivo for metabolic imaging of cancer. This
technique relies on the simultaneous chemical exchange of
parahydrogen, acting as a source of nuclear spin order, and
[1-13C]pyruvate on a Ir-IMes polarization transfer catalyst
at ∼0.4 μm magnetic field. The SABRE catalyst forms two
kinds of complexes with parahydrogen-derived hydrides,
pyruvate, and dimethyl sulfoxide, acting as a critically
important coligand; however, only the complex that binds
pyruvate in an equatorial position can release
hyperpolarized [1-13C]pyruvate into the solution to enable
bulk HP [1-13C]pyruvate production for use in molecular
imaging and other applications. Here, we investigate the
interplay of pH and temperature with the SABRE-SHEATH
hyperpolarization of [1-13C]pyruvate. Temperature and pH
modulate this process in remarkable and complementary ways,
greatly affecting pyruvate exchange and 13C relaxation
dynamics. The overall process is optimal at pH (methanol) of
6.5-7.7 and a temperature of 6 °C: indeed, the
catalyst-bound pyruvate exhibits high 13C polarization
levels in excess of 25\%. The 13C polarization results are
additionally supported by 13C relaxation dynamics at a
polarization field of 0.4 microtesla. These results provide
deeper understanding of the SABRE-SHEATH process and pave
the way to further improve the efficiency of the
hyperpolarization technique.},
cin = {FR01},
ddc = {530},
cid = {I:(DE-He78)FR01-20160331},
pnm = {899 - ohne Topic (POF4-899)},
pid = {G:(DE-HGF)POF4-899},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:41273337},
doi = {10.1021/acs.jpcb.5c05015},
url = {https://inrepo02.dkfz.de/record/306517},
}