Heterogeneous Microtesla SABRE Enhancement of 15N NMR Signals

Heterogeneous Microtesla SABRE Enhancement of 15N NMR Signals
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DOI:
10.1002/anie.201705014
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发表时间:
2017-08-21
影响因子:
16.6
通讯作者:
Goodson, Boyd M.
Goodson, Boyd M.
中科院分区:
化学1区
文献类型:
--
作者:
Kovtunov, Kirill V.;Kovtunova, Larisa M.;Goodson, Boyd M.

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研究了在非均相催化和微磁场条件下,通过可逆交换信号放大(SABRE)实现的异核超极化。将[IrCl(COD)(IMES)],[IMES=1,3-双(2,4,6-三甲基苯基),咪唑-2-亚甲基;COD=环辛二烯]催化剂固定在经胺键修饰的二氧化硅颗粒上,得到了一种有效的多相SABRE(HET-SABRE)催化剂,该催化剂用于证明在9.4T下,N-15-吡啶中的N-15-核磁共振信号在磁屏蔽内仲氢鼓泡后增加了约100倍。从催化剂分离后的上清液中没有观察到N-15核磁共振增强,这与XPS表征一起支持了多相催化条件下SABRE的影响这一事实。这项技术可以进一步发展为通过具有超极化异核自旋的SABRE来生产无催化剂试剂,因此在生物医学核磁共振和核磁共振应用中具有广阔的前景。
The hyperpolarization of heteronuclei via signal amplification by reversible exchange (SABRE) was investigated under conditions of heterogeneous catalysis and microtesla magnetic fields. Immobilization of [IrCl(COD)(IMes)], [IMes=1,3-bis(2,4,6-trimethylphenyl), imidazole-2-ylidene; COD=cyclooctadiene] catalyst onto silica particles modified with amine linkers engenders an effective heterogeneous SABRE (HET-SABRE) catalyst that was used to demonstrate a circa 100-fold enhancement of N-15 NMR signals in N-15-pyridine at 9.4 T following parahydrogen bubbling within a magnetic shield. No N-15 NMR enhancement was observed from the supernatant liquid following catalyst separation, which along with XPS characterization supports the fact that the effects result from SABRE under heterogeneous catalytic conditions. The technique can be developed further for producing catalyst-free agents via SABRE with hyperpolarized heteronuclear spins, and thus is promising for biomedical NMR and MRI applications.