Taler G, Eliav U, Navon G
Sackler Faculty of Exact Sciences, Tel Aviv University, Tel Aviv, 69978, Israel.
J Magn Reson. 1999 Dec;141(2):228-38. doi: 10.1006/jmre.1999.1853.
The application of multiple quantum filtered (MQF) NMR to the identification and characterization of the binding of ligands containing quadrupolar nuclei to proteins is demonstrated. Using relaxation times measured by MQF NMR multiple binding of boric acid and borate ion to ferri and ferrocytochrome c was detected. Borate ion was found to have two different binding sites. One of them was in slow exchange, k(diss) = 20 +/- 3 s(-1) at 5 degrees C and D(2)O solution, in agreement with previous findings by (1)H NMR (G. Taler et al., 1998, Inorg. Chim. Acta 273, 388-392). The triple quantum relaxation of the borate in this site was found to be governed by dipolar interaction corresponding to an average B-H distance of 2.06 +/- 0.07 A. Other, fast exchanging sites for borate and boric acid could be detected only by MQF NMR. The binding equilibrium constants at these sites at pH 9.7 were found to be 1800 +/- 200 M(-1) and 2.6 +/- 1.5 M(-1) for the borate ion and boric acid, respectively. Thus, detection of binding by MQF NMR proved to be sensitive to fast exchanging ligands as well as to very weak binding that could not be detected using conventional methods.
本文展示了多量子滤波(MQF)核磁共振技术在鉴定和表征含四极核配体与蛋白质结合方面的应用。通过MQF核磁共振测量弛豫时间,检测到硼酸和硼酸根离子与高铁和亚铁细胞色素c的多重结合。发现硼酸根离子有两个不同的结合位点。其中一个处于慢交换状态,在5℃的D₂O溶液中,解离常数k(diss) = 20 ± 3 s⁻¹,这与之前¹H NMR的研究结果一致(G. Taler等人,1998年,《无机化学学报》273,388 - 392)。发现该位点硼酸根的三重量子弛豫受偶极相互作用支配,对应的平均B - H距离为2.06 ± 0.07 Å。其他硼酸根和硼酸的快速交换位点只能通过MQF NMR检测到。在pH 9.7时,这些位点硼酸根离子和硼酸的结合平衡常数分别为1800 ± 200 M⁻¹和2.6 ± 1.5 M⁻¹。因此,MQF NMR检测结合被证明对快速交换配体以及传统方法无法检测到的非常弱的结合都很敏感。