Abstract
Developing artificial enzymes with the excellent catalytic performance of natural enzymes has been a long-standing goal for chemists. Single-atom catalysts with well-defined atomic structure and electronic coordination environments can effectively mimic natural enzymes. Here, we report an engineered FeN3P-centred single-atom nanozyme (FeN3P-SAzyme) that exhibits comparable peroxidase-like catalytic activity and kinetics to natural enzymes, by controlling the electronic structure of the single-atom iron active centre through the precise coordination of phosphorus and nitrogen. In particular, the engineered FeN3P-SAzyme, with well-defined geometric and electronic structures, displays catalytic performance that is consistent with Michaelis–Menten kinetics. We rationalize the origin of the high enzyme-like activity using density functional theory calculations. Finally, we demonstrate that the developed FeN3P-SAzyme with superior peroxidase-like activity can be used as an effective therapeutic strategy for inhibiting tumour cell growth in vitro and in vivo. Therefore, SAzymes show promising potential for developing artificial enzymes that have the catalytic kinetics of natural enzymes.
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The data supporting the findings of this study are available within the article and its Supplementary Information files. All other relevant source data are available from the corresponding authors upon reasonable request.
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Acknowledgements
This work was supported by the National Key R&D Program of China (2017YFA0205501, 2018YFA0702003), the National Natural Science Foundation of China (81722024, 21890383, 21871159, 21802076), the National Postdoctoral Program for Innovative Talents (BX20180160), the China Postdoctoral Science Foundation (2018M640113) and the Youth Innovation Promotion Association of the Chinese Academy of Sciences (2014078, 2018017). We thank the BL11B station at the Shanghai Synchrotron Radiation Facility and the 1W1B and 4B7A stations at the Beijing Synchrotron Radiation Facility.
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M.L., D.W., X.Y. and Y.L. conceived the idea, designed the research project and co-wrote the manuscript. S.J. designed the synthesis and controlled the experiments, collected and analysed the data and wrote the manuscript. B.J. carried out the performance experiments and analysed the data. H.H. and R.G. contributed to the computational results and wrote the manuscript. Y.C. contributed to characterizations of samples, as well as helped to analyse the data and write the manuscript. J.D. performed XAFS data analysis. Y.M. contributed to the computational results and contributed to the manuscript. Z.Z. contributed to synthesis of samples. W.C., H.L., S.L. and Y.W. helped to test the XAFS measurement of samples. R.Z., Q.L. and D.D. contributed to grouping nude mice, tumour xenogeneic transplants and tail vein injections. Q.Z. and L.G. performed the AC HAADF-STEM characterizations. All the authors commented on the manuscript and have given approval to the final version of the manuscript.
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Supplementary Figs. 1–48, Tables 1–6 and Notes 1–4.
Supplementary Data 1.
Atomic coordinates.
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Ji, S., Jiang, B., Hao, H. et al. Matching the kinetics of natural enzymes with a single-atom iron nanozyme. Nat Catal 4, 407–417 (2021). https://doi.org/10.1038/s41929-021-00609-x
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DOI: https://doi.org/10.1038/s41929-021-00609-x
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