Covalent functionalization of Ti3C2T MXene flakes with Gd-DTPA Complex for Stable and Biocompatible MRI Contrast Agent
Covalent functionalization of Ti3C2T MXene flakes with Gd-DTPA Complex for Stable and Biocompatible MRI Contrast Agent
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DOI：
10.1016/j.cej.2022.136939
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发表时间：
2022-05
影响因子：
15.1
通讯作者：
Viktoria Neubertova;O. Guselnikova;Y. Yamauchi;A. Olshtrem;S. Rimpelová;E. Čižmár;M. Orendáč;J. Duchoň;L. Volfová;J. Lančok;V. Herynek;P. Fitl;P. Ulbrich;L. Jelínek;Patrik Schneider;J. Košek;P. Postnikov;Z. Kolská;V. Svorcik;S. Chertopalov;O. Lyutakov
中科院分区：
文献类型：
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作者：
Viktoria Neubertova;O. Guselnikova;Y. Yamauchi;A. Olshtrem;S. Rimpelová;E. Čižmár;M. Orendáč;J. Duchoň;L. Volfová;J. Lančok;V. Herynek;P. Fitl;P. Ulbrich;L. Jelínek;Patrik Schneider;J. Košek;P. Postnikov;Z. Kolská;V. Svorcik;S. Chertopalov;O. Lyutakov
MXene 是医疗应用的绝佳候选者，包括正电子发射断层扫描、计算机断层扫描和磁共振成像 (MRI) 等诊断方法。然而，MXene 在生物成像中的应用受到其普遍抗磁性的限制。 MXene 可以使用铁磁或顺磁化合物和纳米颗粒进行功能化，以开发高效的生物成像工具。与之前发表的基于静电相互作用的方法相比，共价方法可以增强 MXene 的稳定性并防止自聚集和降解。这项工作提出用螯合剂二乙烯三胺五乙酸 (DTPA) 对 Ti3C2T 薄片进行共价功能化，并进一步与 Gd3+ 离子络合。开发的功能化程序为 T1-MR 成像的本质抗磁 Ti3C2T 薄片提供了顺磁响应。此外，我们观察到磁弛豫时间对薄片浓度的明显依赖性，这使我们能够估计空间分辨的薄片分布。 MXene 的共价修饰策略可提供表面保护，防止磷酸盐缓冲盐水和血清中的氧化，同时提高细胞相容性。此外，与静电化学吸附相比，Gd3+离子的螯合可以防止泄漏。我们展示了 MXene-Gd 的高度光热转换效率，预计未来在光热治疗中的应用。这项工作不仅通过引入 MRI 对比，还通过开发 MXene 的共价功能化策略，拓宽了 MXene 的生物应用。
MXenes are an excellent candidate for medical applications, including diagnostic approaches such as positron emission tomography, computed tomography, and magnetic resonance imaging (MRI). However, the utilization of MXenes for bioimaging is restricted by their commonly diamagnetic nature. MXenes can be functionalized using ferromagnetic or paramagnetic compounds and nanoparticles to develop efficient bioimaging tools. In contrast to previously published approaches based on electrostatic interactions, covalent approaches could enhance MXene stability and prevent self-aggregation with degradation. This work proposes covalent functionalization of Ti3C2T flakes with a chelating agent diethylenetriaminepentaacetic acid (DTPA) and further complexing with Gd3+ions. The developed functionalization procedure provides a paramagnetic response to the intrinsically diamagnetic Ti3C2T flakes for T1-MR imaging. Moreover, we observed the apparent dependency of magnetic relaxation time on the flake concentration, which enabled us to estimate the spatially resolved flake distribution. The covalent decoration strategy for MXene led to surface protection against oxidation in phosphate buffer saline and blood serum, accompanied by increased cytocompatibility. Moreover, chelation of Gd3+ions prevented leaking compared with electrostatic chemisorption. We demonstrated a high degree of photothermal conversion efficiency of MXene-Gd, anticipating future application in photothermal therapy. This work broadens the bioapplication of MXenes, not only by introducing an MRI contrast but also by developing covalent functionalization strategies for MXenes.