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通过亚硫酸盐介导的铁氧化还原循环促进细胞外聚合物中芳香族氨基酸的靶向转化,实现污泥固液分离。

Promotion of aromatic amino acids of extracellular polymeric substance targeted transformation via sulfite mediated iron redox cycling in sludge solid-liquid separation.

机构信息

Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing 210096, China.

School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan 430074, China.

出版信息

Water Res. 2024 Nov 15;266:122369. doi: 10.1016/j.watres.2024.122369. Epub 2024 Sep 1.

Abstract

Highly hydrophilic extracellular polymeric substance (EPS) with gel-like structure seriously plagues the development of sludge deep dewatering. Oxysulfur radicals-based oxidation driven by iron-bearing mineral proposes a promising strategy for effective EPS decomposition. However, the transformation and involved interaction mechanisms of aromatic proteins are still controversial due to the complex EPS structure. Herein, sulfite mediated siderite (denoted as Fe(II)/S(IV)) was developed for targeted transformation aromatic amino acids in EPS oxidation to strengthen sludge solid-liquid separation. The enhanced sludge dewaterability were benefited from the Fe(II)/S(IV) bonded interaction assisted by Fe/Fe as redox interface that facilitating the release of intracellular bound water via diminish the hydrophily and bind strength with solid protons. The amide region nitrogen of aromatic amino acids (especially tyrosine and tryptophan) originating from EPS presented looser structure and lower spatial site resistance, which were attributed to the exposure of hydrophobic sites in amino groups after Fe(II)/S(IV) treatment. Furthermore, the effective decline of aromatic amino acids in inner layer-EPS (loosely bound EPS and tightly bound EPS) was directed from Fe-N targeted interaction by triggering a series of sulfate-based radical chain reactions. The good correlation between electron transfer amount (R = 0.926) and Fe-N (R = 0.925) with bonding interaction demonstrated that the complexation of aromatic amino acids with Fe sites on siderite/sulfite via Fe-N bonds, accounting for efficient sludge solid-liquid separation. This study deepens the understanding of sludge organic matter targeted transformation and provides a tactic for iron-based conditioning of sludge.

摘要

高度亲水的胞外聚合物(EPS)具有凝胶状结构,严重阻碍了污泥深度脱水的发展。含铁矿物驱动的氧硫自由基氧化为有效分解 EPS 提供了一种很有前途的策略。然而,由于 EPS 结构复杂,芳香族蛋白质的转化和涉及的相互作用机制仍存在争议。本文中,亚硫酸盐介导的菱铁矿(记为 Fe(II)/S(IV)) 被开发用于靶向转化 EPS 氧化中的芳香族氨基酸,以增强污泥固液分离。增强的污泥脱水性能得益于 Fe/Fe 作为氧化还原界面的 Fe(II)/S(IV)键合相互作用,通过减少与固体质子的亲水性和结合强度,促进细胞内结合水的释放。源自 EPS 的芳香族氨基酸(特别是酪氨酸和色氨酸)的酰胺区域氮呈现出较松散的结构和较低的空间位阻,这归因于 Fe(II)/S(IV)处理后氨基中疏水区位的暴露。此外,内层-EPS(松散结合 EPS 和紧密结合 EPS)中芳香族氨基酸的有效减少是通过触发一系列基于硫酸盐的自由基链式反应,由 Fe-N 靶向相互作用引起的。电子转移量(R = 0.926)与 Fe-N(R = 0.925)之间的良好相关性表明,芳香族氨基酸与菱铁矿/亚硫酸盐上的 Fe 位点通过 Fe-N 键络合,这解释了污泥固液分离的高效性。本研究深化了对污泥有机物靶向转化的认识,并为基于铁的污泥调理提供了一种策略。

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