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Monitoring enzymatic degradation of emerging contaminants using a chip-based robotic nano-ESI-MS tool

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Abstract

Up to now, knowledge of enzymes capable of degrading various contaminants of emerging concern (CEC) is limited, which is especially due to the lack of rapid screening methods. Thus, a miniaturized high-throughput setup using a chip-based robotic nanoelectrospray ionization system coupled to mass spectrometry has been developed to rapidly screen enzymatic reactions with environmentally relevant CECs. Three laccases, two tyrosinases, and two peroxidases were studied for their ability to transform ten pharmaceuticals and benzotriazole. Acetaminophen was most susceptible to enzymatic conversion by horseradish peroxidase (HRP), laccase from Trametes versicolor (LccTV), and a tyrosinase from Agaricus bisporus (TyrAB). Diclofenac and mefenamic acid were converted by HRP and LccTV, whereas sotalol was solely amenable to HRP conversion. Benzotriazole, carbamazepine, gabapentin, metoprolol, primidone, sulfamethoxazole, and venlafaxine remained persistent in this study. The results obtained here emphasize that enzymes are highly selective catalysts and more effort is required in the use of fast monitoring technologies to find suitable enzyme systems. Despite the methodological limitations discussed in detail, the automated tool provides a routine on-line screening of various enzymatic reactions to identify potential enzymes that degrade CECs.

A chip-based robotic nano-ESI-MS tool to rapidly monitor enzymatic degradation of environmentally relevant emerging contaminants

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Acknowledgements

The authors would like to thank AB Enzyme GmbH for the supply of two laccases and one tyrosinase. Furthermore, the authors thank Frank Porbeck (Advion BioSciences) for his assistance with the TriVersa NanoMate® system and various chips free of charge. The authors also gratefully thank the master’s students Rebecca Feind, Janine Storms, and Anastasia Vavelidou for their lab assistance and dedicated work.

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Correspondence to Johanna Graßmann.

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This research did not receive any specific grant from funding agencies in the public, commercial, or not-for profit sector. We, the authors, declare that we have no competing interests. All authors are aware of and accept responsibility for this manuscript.

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Stadlmair, L.F., Letzel, T. & Graßmann, J. Monitoring enzymatic degradation of emerging contaminants using a chip-based robotic nano-ESI-MS tool. Anal Bioanal Chem 410, 27–32 (2018). https://doi.org/10.1007/s00216-017-0729-4

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