Single-atom nanozymes (SAzymes) are emerging natural enzyme mimics and have attracted much attention in the biomedical field. SAzymes with Metal─N sites designed on carbon matrixes are currently the mainstream in research. It is of great significance to further expand the types of SAzymes to enrich the nanozyme library. Single-atom alloys (SAAs) are a material in which single-atom metal sites are dispersed onto another active metal matrix, and currently, there is limited research on their enzyme-like catalytic performance. In this work, a biodegradable PtPd SAA is fabricated via a simple galvanic replacement strategy, and for the first time reveals its intrinsic enzyme-like catalytic performance including catalase-, oxidase-, and peroxidase-like activities, as well as its photodynamic effect. Experimental characterizations demonstrate that the introduction of single-atom Pt sites contributes to enhancing the affinity of PtPd single-atom alloy nanozyme (SAAzyme) toward substrates, thus exhibiting boosted catalytic efficiency. In vitro and in vivo experiments demonstrate that PtPd SAAzyme exhibits a photo-controlled therapeutic effect, with a tumor inhibition rate of up to 100%. This work provides vital guidance for opening the research direction of SAAs in enzyme-like catalysis.
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http://dx.doi.org/10.1002/smll.202309704 | DOI Listing |
J Phys Chem Lett
May 2024
Engineering Research Center of Advanced Functional Material Manufacturing of Ministry of Education, School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, PR China.
Single-atom alloy (SAA) catalysts exhibit unique and excellent catalytic properties in heterogeneous hydrogenation/dehydrogenation reactions. A thorough understanding of the microscopic surface processes is essential to improve the catalytic performance. Here, from a new perspective of the temperature-programmed desorption (TPD) spectra of hydrogen (H) on two common SAA surfaces, Pt@Cu(111) and Pd@Cu(111), we reveal and confirm the key influence of H atoms attached to Pt/Pd dopants, i.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
March 2024
Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, 361021, China.
Monoatomic dispersion of precious metals on the surface of CeO nanocrystals is a highly practical approach for dramatically reducing the usage of precious metals while exploiting the unique properties of single-atom catalysts. However, the specific atomic sites for anchoring precious metal atoms on the CeO support and underlying chemical mechanism remain partially unknown. Herein, we show that the terminal hydroxyls on the (100) surface are the most stable sites for anchoring Ag atoms on CeO , indicating that CeO nanocubes are the most efficient substrates to achieve monoatomic dispersion of Ag.
View Article and Find Full Text PDFAcc Chem Res
February 2023
Department of Chemical and Petroleum Engineering, University of Pittsburgh, 3700 O'Hara Street, Pittsburgh, Pennsylvania15261, United States.
ConspectusMultimetallic nanoparticles (NPs) have highly tunable properties due to the synergy between the different metals and the wide variety of NP structural parameters such as size, shape, composition, and chemical ordering. The major problem with studying multimetallic NPs is that as the number of different metals increases, the number of possible chemical orderings (placements of different metals) for a NP of fixed size explodes. Thus, it becomes infeasible to explore NP energetic differences with highly accurate computational methods, such as density functional theory (DFT), which has a high computational cost and is typically applied to up to a couple of hundred metal atoms.
View Article and Find Full Text PDFJ Chem Phys
November 2022
Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, People's Republic of China.
Revealing the effect of external applied potential on the reaction mechanism and product selectivity is of great significance in electrochemical studies. In this work, the grand canonical density functional theory method was applied to simulate the explicit electrocatalytic process of oxygen evolution reaction and electrochemical ozone production due to the O product sensitivity toward the applied potential. Over the Pt/Pd single atom embedded on B/N co-doped graphene (Pt/Pd-BNC) surface, crossover points of O/O selectivity inversion were predicted to be 1.
View Article and Find Full Text PDFSmall Methods
July 2022
Key Laboratory for Magnetism and Magnetic Materials of the Ministry of Education, School of Physical Science & Technology, Lanzhou University, Lanzhou, 730000, P. R. China.
Single-atom catalysts (SACs) with a maximum atom utilization efficiency have received growing attention in heterogeneous catalysis. The supporting substrate that provides atomic-dispersed anchoring sites and the local electronic environment in these catalysts is crucial to their activity and stability. Here, inspired by N-doped graphene substrate, the role of N is explored in transition metal nitrides for anchoring single metal atoms toward single-atom catalysis.
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