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Single Atom Iron-Doped Graphic-Phase C3N4 Semiconductor Nanosheets for Augmented Sonodynamic Melanoma Therapy Synergy with Endowed Chemodynamic Effect
Advanced Science ( IF 14.3 ) Pub Date : 2023-06-06 , DOI: 10.1002/advs.202302579
Guiying Feng 1 , Hui Huang 2 , Min Zhang 1 , Zhuole Wu 1 , Dandan Sun 1 , Qiqing Chen 1 , Dayan Yang 1 , Yuanyi Zheng 3 , Yu Chen 2 , Xiangxiang Jing 1
Advanced Science ( IF 14.3 ) Pub Date : 2023-06-06 , DOI: 10.1002/advs.202302579
Guiying Feng 1 , Hui Huang 2 , Min Zhang 1 , Zhuole Wu 1 , Dandan Sun 1 , Qiqing Chen 1 , Dayan Yang 1 , Yuanyi Zheng 3 , Yu Chen 2 , Xiangxiang Jing 1
Affiliation
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Sonodynamic therapy (SDT) is a non-invasive therapeutic modality with high tissue-penetration depth to induce reactive oxygen species (ROS) generation for tumor treatment. However, the clinical translation of SDT is restricted seriously by the lack of high-performance sonosensitizers. Herein, the distinct single atom iron (Fe)-doped graphitic-phase carbon nitride (C3N4) semiconductor nanosheets (Fe-C3N4 NSs) are designed and engineered as chemoreactive sonosensitizers to effectively separate the electrons (e−) and holes (h+) pairs, achieving high yields of ROS generation against melanoma upon ultrasound (US) activation. Especially, the single atom Fe doping not only substantially elevates the separation efficiency of the e−-h+ pairs involved in SDT, but also can serve as high-performance peroxidase mimetic enzyme to catalyze the Fenton reaction for generating abundant hydroxyl radicals, therefore synergistically augmenting the curative effect mediated by SDT. As verified by density functional theory simulation, the doping of Fe atom significantly promotes the charge redistribution in the C3N4-based NSs, which improves their synergistic SDT/chemodynamic activities. Both the in vitro and in vivo assays demonstrate that Fe-C3N4 NSs feature an outstanding antitumor effect by aggrandizing the sono-chemodynamic effect. This work illustrates a unique single-atom doping strategy for ameliorating the sonosensitizers, and also effectively expands the innovative anticancer-therapeutic applications of semiconductor-based inorganic sonosensitizers.
中文翻译：
单原子铁掺杂图形相 C3N4 半导体纳米片用于增强声动力黑色素瘤治疗协同作用与赋予化学动力学效应
声动力疗法（SDT）是一种非侵入性治疗方式，具有高组织穿透深度，可诱导活性氧（ROS）产生以治疗肿瘤。然而，由于缺乏高性能声敏剂，SDT的临床转化受到严重限制。在此，独特的单原子铁（Fe）掺杂石墨相氮化碳（C 3 N 4）半导体纳米片（Fe-C 3 N 4 NS）被设计和工程化为化学活性声敏剂，以有效分离电子（e -）和空穴 (h + ) 对，在超声 (US) 激活后实现针对黑色素瘤的高产率 ROS 生成。特别是，单原子Fe掺杂不仅大幅提高了SDT中e - -h +对的分离效率，而且可以作为高性能过氧化物酶模拟酶催化Fenton反应产生丰富的羟基自由基，因此具有协同作用增强SDT介导的疗效。密度泛函理论模拟证实，Fe原子的掺杂显着促进了C 3 N 4基NSs中的电荷重新分布，从而提高了它们的协同SDT/化学动力学活性。体外和体内试验均表明，Fe-C 3 N 4 NSs 通过增强声化学动力学效应而具有出色的抗肿瘤作用。这项工作展示了一种改善声敏剂的独特单原子掺杂策略，并有效扩展了基于半导体的无机声敏剂的创新抗癌治疗应用。
更新日期：2023-06-06
中文翻译：
单原子铁掺杂图形相 C3N4 半导体纳米片用于增强声动力黑色素瘤治疗协同作用与赋予化学动力学效应
声动力疗法（SDT）是一种非侵入性治疗方式，具有高组织穿透深度，可诱导活性氧（ROS）产生以治疗肿瘤。然而，由于缺乏高性能声敏剂，SDT的临床转化受到严重限制。在此，独特的单原子铁（Fe）掺杂石墨相氮化碳（C 3 N 4）半导体纳米片（Fe-C 3 N 4 NS）被设计和工程化为化学活性声敏剂，以有效分离电子（e -）和空穴 (h + ) 对，在超声 (US) 激活后实现针对黑色素瘤的高产率 ROS 生成。特别是，单原子Fe掺杂不仅大幅提高了SDT中e - -h +对的分离效率，而且可以作为高性能过氧化物酶模拟酶催化Fenton反应产生丰富的羟基自由基，因此具有协同作用增强SDT介导的疗效。密度泛函理论模拟证实，Fe原子的掺杂显着促进了C 3 N 4基NSs中的电荷重新分布，从而提高了它们的协同SDT/化学动力学活性。体外和体内试验均表明，Fe-C 3 N 4 NSs 通过增强声化学动力学效应而具有出色的抗肿瘤作用。这项工作展示了一种改善声敏剂的独特单原子掺杂策略，并有效扩展了基于半导体的无机声敏剂的创新抗癌治疗应用。
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