Статья

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

Yuanjun ChenDepartment of Chemistry, Tsinghua University, Beijing 100084, ChinaPeixia WangInstitute of Molecular Medicine, College of Future Technology, Peking University, Beijing 100871, ChinaHaigang HaoCollege of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021, ChinaJuanji HongExperimental Center of Advanced Materials, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing 100081, ChinaHaijing LiBeijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, ChinaShufang JiDepartment of Chemistry, Tsinghua University, Beijing 100084, ChinaAng LiBeijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing 100024, ChinaRui GaoCollege of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021, ChinaJuncai DongBeijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, ChinaXiaodong HanBeijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing 100024, ChinaMinmin LiangExperimental Center of Advanced Materials, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing 100081, ChinaDingsheng WangDepartment of Chemistry, Tsinghua University, Beijing 100084, ChinaYadong LiDepartment of Chemistry, Tsinghua University, Beijing 100084, China

2021en

ABI

Аннотация

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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Идентификаторы

DOI: 10.1021/jacs.1c08581

Цитирования и источники

Цитирований: 2Использованных источников: 0

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