用于调节晶格和电子结构以增强压电催化治疗和铁死亡的掺杂工程,Advanced Materials

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用于调节晶格和电子结构以增强压电催化治疗和铁死亡的掺杂工程
Advanced Materials ( IF 27.4 ) Pub Date : 2023-07-12 , DOI: 10.1002/adma.202304262
Boshi Tian _{1,

2} , Ruixue Tian ₃ , Shaohua Liu ₂ , Yan Wang ₁ , Shili Gai ₁ , Ying Xie ₄ , Dan Yang ₁ , Fei He ₁ , Piaoping Yang ₁ , Jun Lin ₅

Affiliation

压电催化疗法在机械力作用下产生活性氧(ROS)，由于其深层组织穿透深度和较少的O 2 依赖性，在癌症治疗中的应用引起了广泛的_关注。然而，由于压电响应差、电子空穴对分离度低以及复杂的肿瘤微环境（TME），压电催化治疗效率受到限制。在此，通过掺杂工程构建了具有增强压电效应的可生物降解的多孔锰掺杂氧化锌（Mn-ZnO）纳米团簇。Mn掺杂不仅会引起晶格畸变以增加极化，而且会产生丰富的氧空位（O _V）来抑制电子空穴对的复合，从而在超声波照射下高效产生ROS。此外，由于Mn（II/III）的混合价态，Mn掺杂的ZnO表现出TME响应的多酶模拟活性和谷胱甘肽（GSH）消耗能力，进一步加剧了氧化应激。密度泛函理论计算表明，由于O _V的存在，Mn 掺杂可以提高 Mn-ZnO 的压电催化性能和酶活性。受益于ROS生成和GSH消耗能力的增强，Mn-ZnO可以显着加速脂质过氧化物的积累并灭活谷胱甘肽过氧化物酶4（GPX4）以诱导铁死亡。这项工作可能为探索新型压电声敏剂用于肿瘤治疗提供新的指导。

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Doping Engineering to Modulate Lattice and Electronic Structure for Enhanced Piezocatalytic Therapy and Ferroptosis

Piezocatalytic therapy, which generates reactive oxygen species (ROS) under mechanical force, has garnered extensive attention for its use in cancer therapy owing to its deep tissue penetration depth and less O₂-dependence. However, the piezocatalytic therapeutic efficiency is limited owing to the poor piezoresponse, low separation of electron–hole pairs, and complicated tumor microenvironment (TME). Herein, a biodegradable, porous Mn-doped ZnO (Mn–ZnO) nanocluster with enhanced piezoelectric effect is constructed via doping engineering. Mn-doping not only induces lattice distortion to increase polarization but also creates rich oxygen vacancies (O_V) for suppressing the recombination of electron–hole pairs, leading to high-efficiency generation of ROS under ultrasound irradiation. Moreover, Mn-doped ZnO shows TME-responsive multienzyme-mimicking activity and glutathione (GSH) depletion ability owing to the mixed valence of Mn (II/III), further aggravating oxidative stress. Density functional theory calculations show that Mn-doping can improve the piezocatalytic performance and enzyme activity of Mn–ZnO due to the presence of O_V. Benefiting from the boosting of ROS generation and GSH depletion ability, Mn–ZnO can significantly accelerate the accumulation of lipid peroxide and inactivate glutathione peroxidase 4 (GPX4) to induce ferroptosis. The work may provide new guidance for exploring novel piezoelectric sonosensitizers for tumor therapy.

更新日期：2023-07-12

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