Research Online Research Online Impacts of redox-mediator type on trace organic contaminants Impacts of redox-mediator type on trace organic contaminants degradation by laccase: Degradation efficiency, laccase stability degradation by laccase: Degradation efficiency, laccase stability and effluent t
Research Online Research Online Impacts of redox-mediator type on trace organic contaminants Impacts of redox-mediator type on trace organic contaminants degradation by laccase: Degradation efficiency, laccase stability degradation by laccase: Degradation efficiency, laccase stability and effluent t
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发表时间：
2019
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通讯作者：
Bradley Ashe
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作者：
Bradley Ashe
本研究比较了7种氧化还原介导化合物，即1-羟基苯并三唑（HBT）、N-羟基邻苯二甲酰亚胺（HPI）、2，2，6，6-四甲基-1-哌啶氧基（克里思）、紫尿酸（VA）、丁香醛（SA）、香草醛（VA）和2，2 ′-连氮双（3-乙基苯并噻唑啉-6-磺酸）二铵盐（ABTS）遵循不同的氧化途径，用于降解痕量有机污染物（TrOC）。这些氧化还原介质进行了研究，以改善降解的四个TrOC显示耐降解的粗漆酶从白腐真菌Pleumorostreatus。ABTS和VA实现了酚类化合物的最高降解（即，羟苯酮和五氯苯酚），而非酚类化合物（即，敌百虫和莠去津）最好使用VA或HBT去除。这意味着非酚类化合物被由NeOH型介质产生的自由基物质更有效地去除（即，VA和HBT），而酚类化合物的去除可能更多地取决于介体产生的自由基的稳定性和氧化还原电位，而与类型无关。值得注意的是，酶的稳定性受到NeOH型介质的极大影响，但其快速降解能力弥补了这一点。总的来说，VA和HBT（NeOH型）似乎是最好的介质，用于增强所选化合物的降解，而不会在流出物中引起显着的毒性。本研究比较了7种氧化还原介导化合物，即1- 28羟基苯并三唑（HBT）、N-羟基邻苯二甲酰亚胺（HPI）、2，2，6，6-四甲基-1-29哌啶氧基（克里思）、紫尿酸（VA）、丁香醛（SA）、香草醛（VA）和2，2 ′-30连氮基双（3-乙基苯并噻唑啉-6-磺酸）二铵盐（ABTS）遵循31种不同的氧化途径，用于降解痕量有机污染物（TrOCs）。研究了这32种氧化还原介体对四种TrOC（即，氧苯酮、五氯苯酚、萘普生和莠去津）的改进降解，所述四种TrOC表现出对从白腐真菌糙皮侧耳收获的粗漆酶的降解34的抗性。一系列的筛选35测试表明，ABTS，VA和HBT是最有效的介质降解的36个选定的TrOC。ABTS和VA实现了酚类化合物37的最高降解（即，羟苯酮和五氯苯酚），而非酚类化合物（即，萘啶38和莠去津）最好使用VA或HBT去除。这意味着非酚类化合物39被N-OH型介体40产生的自由基物质更有效地去除（即，VA和HBT），而酚类化合物的去除可能更多地取决于介体产生的自由基的稳定性和氧化还原电位，而与类型无关。值得注意的是，酶的稳定性受到N-OH型介体的极大影响，但其快速降解能力补偿了酶的稳定性。总体而言，VA和HBT（N-OH型）似乎是增强所选化合物降解的最佳介质，而不会在流出物中引起显著毒性。
Abstract This study compares the effectiveness of seven redox-mediating compounds namely, 1-hydrozybenzotriazole (HBT), N-hydroxyphthalimide (HPI), 2,2,6,6-Tetramethyl-1-piperidinyloxy (TEMPO), violuric acid (VA), syringaldehyde (SA), vanillin (VA), and 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) diammonium salt (ABTS), which follow distinct oxidation pathways, for the degradation of trace organic contaminants (TrOCs). These redox-mediators were investigated for improved degradation of four TrOCs showing resistance to degradation by crude laccase from the white-rot fungus Pleurotus ostreatus. ABTS and VA achieved the highest degradation of the phenolic compounds (i.e., oxybenzone and pentachlorophenol), whereas the non-phenolic compounds (i.e., naproxen and atrazine) were best removed using VA or HBT. This implies that the non-phenolic compounds are more effectively removed by the radical species generated by the NeOH type mediators (i.e., VA and HBT), while removal of the phenolic compounds may depend more on the stability and the redox potential of the radicals generated from the mediator, irrespective of the type. Notably, enzyme stability was greatly affected by the NeOH type mediators but it was compensated by their rapid degradation capacity. Overall, VA and HBT (NeOH type) appear to be the best mediators for enhanced degradation of the selected compounds without causing significant toxicity in the effluent. Abstract 27 This study compares the effectiveness of seven redox-mediating compounds namely, 1- 28 hydrozybenzotriazole (HBT), N-hydroxyphthalimide (HPI), 2,2,6,6-Tetramethyl-1- 29 piperidinyloxy (TEMPO), violuric acid (VA), syringaldehyde (SA), vanillin (VA), and 2,2′- 30 azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) diammonium salt (ABTS), which follow 31 distinct oxidation pathways, for the degradation of trace organic contaminants (TrOCs). These 32 redox-mediators were investigated for improved degradation of four TrOCs, namely, 33 oxybenzone, pentachlorophenol, naproxen and atrazine, which showed resistance to degradation 34 by crude laccase harvested from the white-rot fungus Pleurotus ostreatus . A series of screening 35 tests showed that ABTS, VA and HBT were the most efficient mediators for degradation of the 36 selected TrOCs. ABTS and VA achieved the highest degradation of the phenolic compounds 37 ( i.e., oxybenzone and pentachlorophenol), whereas the non-phenolic compounds ( i.e., naproxen 38 and atrazine) were best removed using VA or HBT. This implies that the non-phenolic 39 compounds are more effectively removed by the radical species generated by the N-OH type 40 mediators ( i.e., VA and HBT), while removal of the phenolic compounds may depend more on 41 the stability and the redox potential of the radicals generated from the mediator, irrespective of 42 the type. Notably, enzyme stability was greatly affected by the N-OH type mediators but it was 43 compensated by their rapid degradation capacity. Overall, VA and HBT (N-OH type) appear to 44 be the best mediators for enhanced degradation of the selected compounds without causing 45 significant toxicity in the effluent.