Mechanistic and kinetic insights into size-dependent activity in ultra-small Pt/CNTs nanozymes during antibacterial process
Mechanistic and kinetic insights into size-dependent activity in ultra-small Pt/CNTs nanozymes during antibacterial process
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DOI：
10.1016/j.arabjc.2022.104238
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发表时间：
2022-09
影响因子：
6
通讯作者：
Jie Yang;Xiaofeng Ren;Xiaoyu Zhang;Xiaozhe Wang;Rong Zhang;Peirong Bai;Baojie Du;Liping Li
中科院分区：
文献类型：
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作者：
Jie Yang;Xiaofeng Ren;Xiaoyu Zhang;Xiaozhe Wang;Rong Zhang;Peirong Bai;Baojie Du;Liping Li
在类酶催化反应中，纳米粒子的尺寸效应一直是影响纳米酶催化活性的重要因素。此外，具有可控尺寸和电子结构的纳米酶的合成是一个巨大的挑战，这限制了对其结构-性质关系的内在本质的系统探索和实际应用。在这项工作中，我们提出了一种新的策略，通过原子层沉积来调节铂(0.55%∼到2.81%nm)的尺寸，以精确地定制铂基纳米酶。在类过氧化物酶反应和抗菌过程中观察到了尺寸依赖的电子和动力学效应，揭示了本征活性对铂纳米颗粒大小的火山型依赖关系，发现最佳的铂纳米颗粒尺寸约为1.69 nm。动力学研究、XPS分析和多种纳米酶表征相结合的结果表明，具有合适尺寸的铂纳米粒子与底物具有良好的亲和力，这与铂纳米粒子表面较高的Pt0/Pt2+比例有关，这有利于获得优异的催化性能和抗菌活性。我们的工作为深入理解纳米酶在抗菌过程中的尺寸依赖催化机理提供了见解。
In enzyme-like catalytic reactions, the size effect of nanoparticles has been an essential yet unclear factor for the catalytic activity of nanozymes. Moreover, the synthesis of nanozymes with controllable size and electronic structures represents a grand challenge, which limits the systemic exploration the underlying nature of their structure–property relations and practical application. In this work, we proposed a novel strategy to regulate the size of Pt (0.55 ∼ 2.81 nm) by atomic layer deposition for precisely tailoring Pt-based nanozymes. The size-dependent electronic and kinetic effects have been observed for the peroxidase-like reaction and antibacterial process, revealing a volcano-type dependence of intrinsic activity on Pt nanoparticle sizes, and the optimum Pt nanoparticle size was found to be ca. 1.69 nm. A combination of kinetic study and XPS analyses, as well as multiple nanozyme characterizations, demonstrates that Pt nanoparticles with an appropriate size contribute to proper affinity to the substrates, relating to a high ratio of Pt0/Pt2+on the surface of Pt nanoparticles, which is beneficial to obtain the excellent catalytic performance and antibacterial activity. Our work provides insights for an in-depth understanding size-dependent catalytic mechanism of nanozymes during antibacterial processes.