期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 44, 页码 52395-52405出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c15717
关键词
nanozyme; magnetic nanoparticles; cascade reaction; magneto-heat modulation; cancer therapy
资金
- National Natural Science Foundation of China [31400663, 81771981, 82072063]
- Shaanxi Science and Technology Funds [2019KW-078, 2019JM-143]
- Shaanxi Province Funds for Distinguished Young Scholars [202031900097]
- Natural Science Basic Research Program of Shaanxi [2021JQ-438]
The study demonstrates a strategy for precise modulation of enzyme-nanozyme cascade reaction kinetics through remote magnetic stimulation. This approach allows for enhanced cascade activity and improved tumor inhibition in mice, showcasing promise for future biotechnology and synthetic biology applications.
Spatiotemporal regulation of multi-enzyme catalysis with stimuli is crucial in nature to meet different metabolic requirements but presents a challenge in artificial cascade systems. Here, we report a strategy for precise and tunable modulation of enzyme-nanozyme cascade reaction kinetics by remote magnetic stimulation. As a proof of concept, glucose oxidase (GOx) was immobilized onto a ferrimagnetic vortex iron oxide nanoring (Fe3O4 NR) functionalized with poly(ethylene glycol) of different molecular weights to construct a series of Fe3O4 NR@GOx with nanometer linking distances. The activities of GOx and the Fe3O4 NR nanozyme in these systems were shown to be differentially stimulated by Fe3O4 NR-mediated local heat in response to an alternating magnetic field (AMF), leading to modulated cascade reaction kinetics in a distancedependent manner. Compared to the free GOx and Fe3O4 NR mixture, Fe3O4 NR(D-2)@GOx with an optimum linking distance of 1 nm exhibits a superior kinetic match between GOx and the Fe3O4 NR nanozyme and over a 400-fold higher cascade activity under AMF exposure. This enables remarkable intracellular reactive oxygen species production and significantly improved tumor inhibition of AMF-stimulated Fe3O4 NR(D-2)@GOx in 4T1 tumor-bearing mice. The strategy reported here offers a straightforward new tool for fine-tuning multi-enzyme catalysis at the molecular level using magnetic stimuli and holds great promise for use in a variety of biotechnology and synthetic biology applications.
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