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Supramolecule self-assembly synthesis of amyloid phenylalanine-Cu fibrils with laccase-like activity and their application for dopamine determination

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Abstract

Laccases are multicopper proteins for dioxygen-involved oxidation of a broad spectrum of organic compounds. I Novel amyloid-like phenylalanine-Cu (F-Cu(II)) fibrils were developed, which were obtained via supramolecular self-assembly of Cu2+ and phenylalanine (F) under basic condition. The obtained amyloid-like fibrils represented highly periodic structure, of which the lattice unit was constructed via alternating hydrophobic (aromatic environment) and hydrophilic (both hydrogen bonding and Cu(II) coordination) interactions. Relative to natural laccases, the amyloid-like F-Cu(II) architecture exhibited comparable substrate affinity (Michaelis constant, Km = 0.75 mM) and higher catalytic efficiency (kcat/Km = 773.33 × 10−3 g−1 min−1L). Moreover, it exhibited remarkable tolerances in pH (4 ~ 10), temperature (room temperature ~ 200 ℃), organic solvent, and long-term storage (> 15 days). These stabilities were superior among the reported nature and artificial laccases, presenting a more promising candidate in various chemo- or bio-applications. In addition, F-Cu(II) fibrils could catalyze the oxidation of dopamine (DA) to a brown product, in which a new absorption band at 470 nm was observed. Based on this, a simple colorimetric assay for the detection of DA could be performed.

Graphical abstract

We reported a novel amyloid-like phenylalanine-Cu fibrils, in which F-Cu+ complex can mimick the T1 site of natural laccase to oxidize the substrates. Then electrons transferred to F-Cu2+ complex via N-H···O=C hydrogen binding pathway. Finally, the dioxygen was transformed to water though radical reaction.

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Acknowledgements

The authors acknowledge the assistance of JLICT Center of Characterization and Analysis.

Funding

This study received financial support from the Jilin Scientific and Technological Development Program (CN) (No. YDZJ202101ZYTS174).

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Authors and Affiliations

  1. College of Materials Science and Engineering, Jilin Institute of Chemical Technology, Jilin, 132022, China

    Mengxuan Liu, Jian-Hang Yin, Chengwu Lan, Lei Meng & Na Xu

  2. College of Chemistry and Pharmaceutical Engineering, Jilin Institute of Chemical Technology, Jilin, 132022, China

    Jian-Hang Yin

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  1. Mengxuan Liu
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Correspondence to Lei Meng or Na Xu.

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Liu, M., Yin, JH., Lan, C. et al. Supramolecule self-assembly synthesis of amyloid phenylalanine-Cu fibrils with laccase-like activity and their application for dopamine determination. Microchim Acta 189, 98 (2022). https://doi.org/10.1007/s00604-022-05194-9

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