Key Laboratory of Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, Chongqing University, Chongqing, China; Department of Environmental Engineering, Chongqing University, Chongqing, China.
Key Laboratory of Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, Chongqing University, Chongqing, China; Department of Environmental Engineering, Chongqing University, Chongqing, China.
Chemosphere. 2020 Jan;239:124779. doi: 10.1016/j.chemosphere.2019.124779. Epub 2019 Sep 7.
Laccase mediator system (LMS), a very attractive candidate for refractory organics biodegradation, harbors tremendous potential on industry application. However, the performance of LMS usually varies with the discrepancy of mediators and substrates in their chemical structures. Here, we adopt electrochemical analysis that is able to assess the degradation performance of various LMS on three different dyes by quantitative analysis of reaction outcome. Two mechanisms were suggested to explain the grafting of three mediators (1-Hydroxybenzotriazole, Violuric Acid and Acetosyringone), involving the transformation of proton or electron to produce active moieties, which subsequently react with target substrates. A thorough electrochemical insight into the redox features of mediators and its change in the presence of laccase and substrates were carried out using electrochemical analysis. The effectiveness of each kind of LMS on substrates was preliminarily evaluated by analyzing the change of the peak current and potential of mediators. The actual conversion rate of dyes was used to verify the analysis results, which confirms the important role of the stability of the oxidized form as well as their redox potential of the mediators in determining the mechanism of substrate oxidation. The application of electrochemical analysis in efficiency evaluation of LMS shed new light on effective selection of suitable mediators for degradation of refractory organics. It was therefore possible to prejudge the efficacy of LMS by analyzing the electrochemical parameters of target substances and mediators, which undoubtedly has broad further application prospects of LMS.
漆酶介体系统(LMS)作为一种很有前途的难降解有机物生物降解方法,在工业应用中具有巨大的潜力。然而,LMS 的性能通常因介体和底物在化学结构上的差异而有所不同。在这里,我们采用电化学分析方法,通过对反应结果进行定量分析,评估了三种不同染料的各种 LMS 的降解性能。提出了两种机制来解释三种介体(1-羟基苯并三唑、尿囊素和乙酰丁香酮)的接枝,涉及质子或电子的转化以产生活性部分,然后这些活性部分与目标底物反应。通过电化学分析,深入研究了介体的氧化还原特性及其在漆酶和底物存在下的变化。通过分析介体的峰电流和电位的变化,初步评估了每种 LMS 对底物的有效性。使用染料的实际转化率来验证分析结果,这证实了介体氧化形式的稳定性及其氧化还原电位在确定底物氧化机制中的重要作用。电化学分析在 LMS 效率评估中的应用为选择合适的介体来降解难降解有机物提供了新的思路。因此,通过分析目标物质和介体的电化学参数,可以预先判断 LMS 的效果,这无疑为 LMS 的进一步广泛应用提供了广阔的前景。