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DNA-directed enzyme immobilization on Fe3O4 modified with nitrogen-doped graphene quantum dots as a highly efficient and stable multi-catalyst system

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Abstract

The exploration of new tactics for manufacturing artificial immobilized multi-enzyme systems based on enzyme cascades has recently attracted considerable interest because of the urgent need for multi-enzyme catalysts and the high cost of free enzymes. Because of the inevitable limitations of native enzymes such as instability and storage issues, the development of nanozyme–enzyme cascades is needed. A versatile strategy was developed for fabricating an efficient multi-catalyst system by immobilizing glucose oxidase (GOx) on ferriferous oxide nanocomposites functionalized with nitrogen-doped graphene quantum dots (Fe3O4@N-GQDs) through DNA-directed immobilization. The Fe3O4@N-GQDs acted as a carrier for the natural enzyme and showed high peroxidase activity which enabled an enzyme cascade that included GOx to be set up. This multi-catalyst system showed great catalytic activity, reversibility and operational stability. The surfaces of GOx-targeted magnetic nanoparticles were regenerated by mild dehybridization of DNA. The Michaelis constant (Km) and maximum initial velocity (Vmax) of the multi-catalyst system were 1.069 mM and 11.2 × 10−8 M s−1, respectively, which are considerably better than the corresponding values for adsorbed and free bienzyme combinations. The increased bioactivity of the multi-catalyst system is ascribed to the satisfactory peroxidase-like activity of Fe3O4@N-GQDs, the enzyme–promoting effect of the QDs and enhancement by DNA-directed immobilization. Because of the diverse range of possible nanozyme–enzyme combinations and high efficiency of this approach, this work provides a novel pathway for the manufacturing of synthetic enzyme catalyst systems, which have great potential in the field of biotechnology.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant No. 21675008) and the National Key Research and Development Program of China: Studies and applications of NQI technologies of graphene and related materials (No. 2016YFF0204303).

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  1. Beijing Key Laboratory of Environmentally Harmful Chemical Analysis, College of Science, Beijing University of Chemical Technology, Beijing, 100029, People’s Republic of China

    Hao Shen, Jiayi Song, Ye Yang, Ping Su & Yi Yang

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  1. Hao Shen
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  2. Jiayi Song
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Correspondence to Ping Su or Yi Yang.

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Shen, H., Song, J., Yang, Y. et al. DNA-directed enzyme immobilization on Fe3O4 modified with nitrogen-doped graphene quantum dots as a highly efficient and stable multi-catalyst system. J Mater Sci 54, 2535–2551 (2019). https://doi.org/10.1007/s10853-018-2992-y

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