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Monitoring enzymatic degradation of emerging contaminants using a chip-based robotic nano-ESI-MS tool
Analytical and Bioanalytical Chemistry ( IF 3.8 ) Pub Date : 2017-11-17 , DOI: 10.1007/s00216-017-0729-4
Lara F. Stadlmair , Thomas Letzel , Johanna Graßmann

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.

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Graphical abstract

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



中文翻译:

使用基于芯片的机器人纳米ESI-MS工具监测新兴污染物的酶促降解

到目前为止,对能够降解各种新出现的污染物(CEC)的酶的知识是有限的,这尤其是由于缺乏快速的筛选方法。因此,已经开发出使用与质谱联用的基于芯片的机器人纳米电喷雾电离系统的小型化高通量设置,以快速筛选与环境相关的CEC的酶促反应。研究了三种漆酶,两种酪氨酸酶和两种过氧化物酶转化十种药物和苯并三唑的能力。对乙酰氨基酚最易受到辣根过氧化物酶(HRP),云母Trametes versicolor(LccTV)漆酶和双孢蘑菇(Agriaris bisporus)酪氨酸酶的酶促转化的影响(TyrAB)。双氯芬酸和甲芬那酸是通过HRP和LccTV转化的,而索他洛尔仅适合于HRP转化。苯并三唑,卡马西平,加巴喷丁,美托洛尔,普力米酮,磺胺甲恶唑和文拉法辛在本研究中仍然有效。此处获得的结果强调,酶是高度选择性的催化剂,在使用快速监控技术以找到合适的酶系统方面需要付出更多的努力。尽管详细讨论了方法上的局限性,但自动化工具仍可对各种酶促反应进行常规在线筛选,以识别可降解CEC的潜在酶。

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图形概要

基于芯片的机器人纳米ESI-MS工具,可快速监测与环境相关的新兴污染物的酶促降解

更新日期:2017-11-17
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