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Development of copper based material systems for generating nitric oxide to control nitrifying bacterial biofilms

机译:用于产生一氧化氮以控制硝化细菌生物膜的铜基材料系统的开发

摘要

Biofilms, which are bacteria cells aggregates that exist within a matrix of extracellular polymeric substances, are known to cause problems in industrial water systems. In order to prevent biofilm formation and pathogens occurrence, disinfectants such as chloramine are usually added into the water. However, chloramine addition has been shown to trigger the growth of nitrifying biofilms which subsequently accelerate chloramine decay. Therefore, a new antibiofilm agent, namely nitric oxide (NO), is investigated for nitrifying biofilm control.Herein, NO was generated from catalytic reduction of nitrite in the presence of a copper(II) complex catalyst embedded in a poly(vinyl chloride) (PVC) matrix. Ascorbic acid was added into the solution as a reducing agent to aid the formation of the active copper(I) species that will react with nitrite to generate NO. The copper-nitrite-ascorbic acid combination showed enhanced NO generation compared to that generated in the presence of nitrite-ascorbic acid alone, and subsequently, enhanced biofilm suppression was observed. The catalytically generated NO was also found to be effective in dispersing pre-formed biofilm, with simultaneous biofilm cells killing observed when a high concentration of nitrite-ascorbic acid was used. An alternative reducing agent, namely Fe2+, was investigated for the potential to mediate reduction of copper(II) complex for generating NO. The amount of NO generated was found to be highly dependent on Fe speciation in different pH and buffer composition. Nonetheless, the NO generated in phosphate buffer pH 6 is still capable of dispersing pre-formed nitrifying biofilms, thus suggesting the robustness of NO-mediated biofilm dispersal. In the last part of the study, an iron complex, namely FeDTTCT, was synthesised and immobilised into PVC with the copper catalyst. The iron complex was found to facilitate copper(II)/copper(I) redox cycling, subsequently enabling NO generation from nitrite. Importantly, the mixed metal system exhibited a non-toxic antibiofilm activity, whereby biofilm formation was suppressed and bacterial growth was confined to the free-floating planktonic phase. These thus imply that the mixed metal system was capable of converting nitrite endogenously produced by nitrifying bacteria to NO, hence eliminating the need to add a reducing agent and NO precursor in solution form into the system.
机译:众所周知,生物膜是细菌细胞聚集体,存在于细胞外聚合物质的基质中,会在工业用水系统中引起问题。为了防止生物膜的形成和病原体的发生,通常将诸如氯胺的消毒剂添加到水中。然而,已表明添加氯胺会触发硝化生物膜的生长,从而加速氯胺的衰减。因此,研究了一种新的抗生物膜剂,即一氧化氮(NO),用于控制生物膜的硝化作用。 (PVC)矩阵。将抗坏血酸作为还原剂添加到溶液中,以帮助形成能与亚硝酸盐反应生成NO的活性铜(I)物种。与仅存在亚硝酸盐-抗坏血酸的情况相比,亚硝酸铜-抗坏血酸的铜组合物显示出增强的NO产生,随后观察到生物膜抑制作用增强。还发现催化产生的NO在分散预先形成的生物膜中是有效的,当使用高浓度的亚硝酸抗坏血酸时,观察到同时的生物膜细胞被杀死。研究了另一种还原剂,即Fe2 +,具有介导还原铜(II)络合物生成NO的潜力。发现在不同的pH和缓冲液组成中,NO的生成高度依赖于Fe的形态。尽管如此,在磷酸盐缓冲液pH 6中产生的NO仍然能够分散预先形成的硝化生物膜,因此表明NO介导的生物膜分散的稳定性。在研究的最后一部分,合成了铁配合物FeDTTCT,并用铜催化剂将其固定在PVC中。发现该铁络合物促进铜(II)/铜(I)的氧化还原循环,随后使亚硝酸盐生成NO。重要的是,混合金属系统表现出无毒的抗生物膜活性,从而抑制了生物膜的形成并将细菌的生长限制在自由漂浮的浮游阶段。因此,这意味着该混合金属系统能够将细菌硝化产生的内源性亚硝酸盐转化为NO,从而消除了向该系统中添加还原剂和NO前体溶液形式的需求。

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