4.8 Article

Thermal Atomization of Platinum Nanoparticles into Single Atoms: An Effective Strategy for Engineering High-Performance Nanozymes

期刊

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 44, 页码 18643-18651

出版社

AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c08581

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资金

  1. National Key R&D Program of China [2017YFA0205501, 2018YFA0702003]
  2. National Natural Science Foundation of China [82172087, 21890383, 21871159, 21962013, 51872008]
  3. Beijing Outstanding Young Scientists Projects [BJJWZYJH01-201910005018]
  4. Science and Technology Key Project of Guangdong Province of China [2020B010188002]
  5. Youth Innovation Promotion Association of Chinese Academy of Sciences [2018017]
  6. China Postdoctoral Science Foundation [2021T140018]
  7. Postdoctoral Fellowship of Peking-Tsinghua Center for Life Sciences

向作者/读者索取更多资源

A novel and efficient strategy was reported to access high-performance nanozymes by atomizing platinum nanoparticles into single atoms, leading to dramatically enhanced enzymatic performance. The engineered single-atom Pt nanozyme exhibited remarkable catalytic activity and kinetics, far exceeding traditional Pt nanoparticle nanozymes.
Although great progress has been made in artificial enzyme engineering, their catalytic performance is far from satisfactory as alternatives of natural enzymes. Here, we report a novel and efficient strategy to access high-performance nanozymes via direct atomization of platinum nanoparticles (Pt NPs) into single atoms by reversing the thermal sintering process. Atomization of Pt NPs into single atoms makes metal catalytic sites fully exposed and results in engineerable structural and electronic properties, thereby leading to dramatically enhanced enzymatic performance. As expected, the as-prepared thermally stable Pt single-atom nanozyme (PtTS-SAzyme) exhibited remarkable peroxidase-like catalytic activity and kinetics, far exceeding the Pt nanoparticle nanozyme. The following density functional theory calculations revealed that the engineered P and S atoms not only promote the atomization process from Pt NPs into PtTS-SAzyme but also endow single-atom Pt catalytic sites with a unique electronic structure owing to the electron donation of P atoms, as well as the electron acceptance of N and S atoms, which simultaneously contribute to the substantial enhancement of the enzyme-like catalytic performance of PtTS-SAzyme. This work demonstrates that thermal atomization of the metal nanoparticle-based nanozymes into single-atom nanozymes is an effective strategy for engineering high-performance nanozymes, which opens up a new way to rationally design and optimize artificial enzymes to mimic natural enzymes.

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