Abstract:
Single-atom nanozymes (SANZs) have emerged as new media for enhancing chemodynamic therapy (CDT) to achieve desirable enzyme-like effects and excellent nanoscale specificity. However, non-optimal adsorption of Fenton-like reaction intermediates prevents SANZs from exerting kinetic activity and hinders the CDT effect. Herein, we demonstrate that heteroatom-doped Co single-atom nanozymes (SACNZs) with intrinsic charge transfer exhibit peroxidase-like properties and significantly improve the ability of CDT to treat Staphylococcus aureus-infected wounds. Density functional theory calculations showed that the S-induced charge transfer effect regulated the electronic distribution of the central metal more efficiently than P, thereby lowering the energy levels for the generation of OH and increasing the catalytic effect. Polyvinylpyrrolidone-modified SACNZs showed effects consistent with this theory in both in vitro antibacterial and in vivo ward management assays. This study systematically investigated the relationship between heteroatom-doping and the catalytic activity of metal centres, opening a new perspective for the application of CDT.
摘要:
单原子纳米酶(SANZ)已成为增强化学动力学疗法(CDT)的新介质,以实现理想的酶样效应和出色的纳米级特异性。然而,类Fenton反应中间体的非最佳吸附阻止了SANZ发挥动力学活性并阻碍了CDT效应。在这里,我们证明了具有固有电荷转移的杂原子掺杂的Co单原子纳米酶(SACNZs)具有过氧化物酶样特性,并显着提高了CDT治疗金黄色葡萄球菌感染伤口的能力。密度泛函理论计算表明,S引起的电荷转移效应比P更有效地调节中心金属的电子分布,从而降低了生成OH的能量水平并增加了催化作用。聚乙烯吡咯烷酮修饰的SACNZ在体外抗菌和体内病房管理测定中均显示出与该理论一致的作用。本研究系统地研究了杂原子掺杂与金属中心催化活性之间的关系,为CDT的应用开辟了新的视角。