论文总字数：21973字

摘 要

随着生产和使用量的增加，具有长半衰期、高化学惰性和皮肤渗透性的双酚S（4,4'-Sulfonyldiphenol，BPS）在环境样品中检出频率不断增加，严重危害了生态环境和人体健康。作为难降解有机污染物的主要处理技术，生物降解技术在BPS去除方面的研究较少。做为一项新一代的生物反应器，生物电化学体系（BESs）微生物菌种可做为在厌氧条件下将有机污染物转变成为能量。电极做为生物电化学体系中至关重要的核心，其性能是决定体系性能的主要因素，因此它是依托于生物电化学的基本原理，利用腐植酸（HA）改性生物阳极，研究改性阳极作用下BPS 的厌氧生物降解特征，深入分析腐植酸增进 BPS 降解效率的机制

本论文研究中，构建了对照系统（CC-BES）和HA改性-生物电化学系统（HA-BES）。根据BPS降解效率、中间代谢产物以及微生物群落分析，归纳出HA在生物电化学系统中对BPS降解的影响，并表征反应前后HA分子的变化。利用0.05 g、0.1 g、0.15 g HA对阳极进行修饰改性，研究改性阳极对BPS厌氧生物降解的影响。结果显示， 0.05 g HA 改性阳极作用下BPS的降解效率由对照系统的31.07%提高至62.24%。微生物群落分析发现HA的改性都对微生物群落结构产生了影响。与难降解有机物降解相关的Tolumonas在HA-BES系统中富集。同时对反应前后电极上HA进行表征，HA中羧基和羟基的谱带发生变化，推测HA可能通过表面基团调变来提高BPS生物降解效率。

关键词：腐植酸，生物电化学系统，双酚S，厌氧降解

Study on bioelectrochemical anaerobic degradation of bisphenol S by humic acid

Abstract

With the increase of production and usage, the detection frequency of 4,4'-Sulfonyldiphenol(BPS) with long half-life and high chemical inertias and skin permeability in environmental samples is increasing.It seriously harms the ecological environment and human health. As the main treatment technology for refractory organic pollutants, biodegradation technology has little research on the removal of BPS.Bioelectrochemical system(BESs) is a new type of bioreactor, which can convert organic pollutants into energy by using microorganisms under anaerobic conditions.As the key and core of the bioelectrochemical system, electrode performance is the key factor determining the system performance. Therefore, based on the principle of bioelectrochemistry, humic acid (HA) was used to modify the biological anode to study the anaerobic biodegradation characteristics of BPS under the action of the modified anode, and the mechanism of humic acid promoting the degradation efficiency of BPS was analyzed.

In this study, control system (CC-BES) and HA modified-bioelectrochemical system (HA-BES) were constructed.Based on the analysis of BPS degradation efficiency, intermediate metabolites, microbial community,and the influence of HA on BPS degradation in the BES were summarized, and the changes of HA molecules before and after the reaction were characterized.The anodes were modified with 0.05g, 0.1g and 0.15g HA to study the effect of the modified anodes on the anaerobic biodegradation of BPS.It revealed that the degradation efficiency of BPS under the action of 0.05 g HA modified anode was increased from 31.07% in the control system to 62.24% by the completion. Analysis of the microbial community revealed that HA modification has an effect on the structure of the microbial community.Tolumonas, which is related to the degradation of refractory organic compounds, was enriched in the HA-BES system.At the same time, HA was characterized on the electrodes before and after the reaction, and the spectral bands of the carboxyl and hydroxyl groups in HA changed. It was speculated that HA might improve the biodegradation efficiency of BPS through surface group modulation.

Key Words:Humic acid，Bioelectrochemical system,BPS,Anaerobic degradation

目录

摘要 Ⅰ

Abstract Ⅱ

第一章 文献综述 1

1.1双酚S概述 1

1.1.1双酚S理化性质 1

1.1.2双酚S作用机制及危害 2

1.1.3双酚S去除技术 2

1.2. 生物电化学系统概述 3

1.2.1基本原理 3

1.2.2应用现状 3

1.3腐植酸研究现状 4

1.3.1腐植酸理化性质 4

1.3.2腐植酸作用机制 4

1.4课题研究内容 5

1.4.1课题研究意义与目的 5

1.4.2研究内容 5

第二章 生物电化学系统构建 6

2.1电极制备 6

2.2构建方法 6

2.3分析方法 7

2.3.1功率密度分析 7

2.3.2循环伏安分析 7

2.4微生物的培养及接种 8

2.5生物电化学系统的启动与运行 8

第三章 腐植酸强化双酚S厌氧降解的研究 9

3.1引言 9

3.2实验仪器与试剂 10

3.3分析与计算方法 12

3.3.1双酚S的检测与分析 12

3.3.2微生物多样性分析 12

3.3.3傅里叶红外光谱分析 12

3.4结果与讨论 13

3.4.1降解效率分析 13

3.4.2降解途径分析 14

3.4.3电化学分析 15

3.4.4微生物多样性分析 16

3.4.5腐植酸表征分析 17

3.5本章小结 18

第四章 结论与展望 19

4.1结论 19

4.2展望 19

参考文献 20

致谢 24

第一章 文献综述

1.1双酚S概述

1.1.1双酚S理化性质

双酚S(BPS)，其化学方程式为C₁₂H₁₀O₄S，全名叫4，4’-二羟基二苯砜，是双酚A(BPA)的结构类似物。它是一类纯白色针状晶状体,具备耐温性、低毒性和耐光性。它可溶解于 烃的衍生物、醇、异丙醇、丙酮、2-乙基己醇和乙腈，微溶解于芳香烃，微溶解于乙酸乙酯 和甲基异丁基酮，不溶解于甲苯和水。相对于别的酚类化合物，BPS的酸性更强。BPS 现阶段被用来作为BPA的同类产品，主要用来作为固色剂、皮革制品鞣剂、电镀液添加剂 、抽空染剂高温染色分散剂、树脂阻燃剂，农药杀虫剂中间体、染料和添加剂中间体等。双酚S的其他理化性质如表1所示。

表1-1 双酚S的基本理化性质

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