Abstract
Developing artificial nanomaterial systems that can convert external stimuli to achieve nanoscale self-sustainable motion (for example, self-rotation), and simultaneously integrate and deploy the spatial localization of multiple active sites to unravel the intraparticle diffusion patterns of molecules, is of great importance for green synthetic chemistry. Here we show a paddle-like self-stirring mesoporous silica nanoreactor system with separated chambers and controllable proximity of active sites. The nanoreactors are designed by encapsulating magnetic Fe3O4 (~20 nm) in the first chamber, and meantime, Au and Pd nanocrystals are spatially isolated in different domains. Such a nanoreactor generates nanoscale rotation under the rotating magnetic fields and exhibits an order of magnitude activity enhancement in the cascade synthesis of 5,6-dimethylphenanthridinium (96.4% selectivity) compared with conventional macro-stirring. Meanwhile, we quantitatively uncovered the rotation-induced enhancement in sequential and reverse transfer of reactive intermediates, consequently revealing the relevance of self-rotation and proximity effects in controlling the catalytic performance.
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Data supporting the findings of this study are available within the article and the associated Supplementary Information section. Source data are provided with this paper.
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Acknowledgements
This work was supported by the National Key R&D Program of China (2018YFA0209401) (D.Z.), the National Natural Science Foundation of China (22088101 (D.Z.), 21733003 (D.Z.), 51961145403 (D.Z.) and 22375107 (Y.M.)), the Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (22JC1410200) (D.Z.) and the National Natural Science Foundation of China (62227815) (J.L.). This publication was made possible by the Inner Mongolia Natural Science Foundation Youth Fund (2023QN02013) (Y.M.) and the Young Science and Technology Talent Program (NJYT24068) (Y.M.). The statements made herein are solely the responsibility of the authors. We wish to thank Q. He and the Electron Microscopy Centre of Inner Mongolia University for the microscopy and microanalysis of our specimens.
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Contributions
D.Z. and Y.M. contributed to the conception and writing of the paper. J. Liu, Z.L. and H.Z. helped edit and discuss the paper. Y.M. and P.G. performed all material syntheses, characterizations, data collection and analysis. J. Li, A.W., B.M., J.J., Y.A. and W.Z. assisted P.G. for the synthesis of materials and the data collection and analysis. S.G., X.P., Z.L. and Y.-L.Z. performed the simulation of the rotation of nanoreactors. J. Li, X.L. and L.D. involved in partial nano-stirring paddle data and analysis. H.Z. helped conduct catalytic experiments and data analysis. Y.M., P.G. and B.M. contributed equally to this work. All authors read and commented on the paper.
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Nature Nanotechnology thanks Jun Chen, Yusuke Yamauchi and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Supplementary information
Supplementary Information
Table of contents, Supplementary methods, Figs. 1–50 and Tables 1 and 2.
Supplementary Video 1
Concept video of planetary cascade nanoreactors.
Supplementary Video 2
Parallel stirring of nanopaddle-containing droplets.
Supplementary Video 3
The motion trajectories of nano-stirring paddles.
Supplementary Video 4
Planetary group patterns of the nano-stirring paddles with different concentrations.
Supplementary Video 5
Simulation of the effect of rotation on molecular mixing.
Supplementary Video 6
Degradation of MB under nano-stirring.
Supplementary Video 7
The stirring of solution by nano-stirring paddle.
Supplementary Video 8
The influence of macro-stirring on intermediate diffusion.
Supplementary Video 9
The influence of nano-stirring (nanoreactor 1) on intermediate diffusion.
Supplementary Video 10
Diffusion paths of intermediates between two adjacent nanoreactors.
Supplementary Video 11
The influence of nano-stirring (nanoreactor 2) on intermediate diffusion.
Supplementary Video 12
The influence of nano-stirring (nanoreactor 3) on intermediate diffusion.
Supplementary Data
Source data for supplementary figures.
Source data
Source Data Fig. 2
Statistical source data Fig. 2f.
Source Data Fig. 3
Statistical source data Fig. 3a,b,d–g.
Source Data Fig. 4
Statistical source data Fig. 4d–f,h–j.
Source Data Fig. 5
Statistical source data Fig. 5c–e.
Source Data Fig. 6
Statistical source data Fig. 6c,d,f,j.
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Ma, Y., Guo, P., Ma, B. et al. Paddle-like self-stirring nanoreactors with multi-chambered mesoporous branches for enhanced dual-dynamic cascade reactions. Nat. Nanotechnol. 20, 897–906 (2025). https://doi.org/10.1038/s41565-025-01915-2
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DOI: https://doi.org/10.1038/s41565-025-01915-2
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