Eriksson Shannon L, Mammen Mathew W, Eriksson Clark W, Lindale Jacob R, Warren Warren S
Department of Chemistry, Duke University, Durham, NC 27708, United States; School of Medicine, Duke University, Durham, NC 27708, United States.
Department of Physics, Duke University, NC 27708, United States.
J Magn Reson. 2022 Sep;342:107282. doi: 10.1016/j.jmr.2022.107282. Epub 2022 Aug 5.
Signal Amplification By Reversible Exchange (SABRE) and the heteronuclear variant, X-SABRE, increase the sensitivity of magnetic resonance techniques using order derived from reversible binding of para-hydrogen. One current limitation of SABRE is suboptimal polarization transfer over the lifetime of the complex. Here, we demonstrate a multiaxial low-field pulse sequence which allows optimal polarization build-up during a low-field "evolution" pulse, followed by a high-field "mixing" pulse which permits proton decoupling along an orthogonal axis. This preserves the singlet character of the hydrides while allowing exchange to replenish the ligands on the iridium catalyst. This strategy leads to a 2.5-fold improvement over continuous field SABRE SHEATH experimentally which was confirmed with numerical simulation.
通过可逆交换实现信号放大(SABRE)以及异核变体X-SABRE,利用对氢可逆结合产生的有序性提高了磁共振技术的灵敏度。SABRE目前的一个局限性是在复合物的寿命期间极化转移不够理想。在此,我们展示了一种多轴低场脉冲序列,该序列允许在低场“演化”脉冲期间实现最佳极化积累,随后是一个高场“混合”脉冲,该脉冲允许质子沿正交轴去耦。这在保留氢化物单重态特征的同时,允许交换以补充铱催化剂上的配体。通过数值模拟证实,该策略在实验上比连续场SABRE SHEATH提高了2.5倍。