化工进展 ›› 2021, Vol. 40 ›› Issue (12): 6846-6858.DOI: 10.16085/j.issn.1000-6613.2021-0106
张钤1(), 崔敏华1,2,3(), 陈蕾1, 吴平1, 刘和1,2,3()
收稿日期:
2021-01-15
修回日期:
2021-03-01
出版日期:
2021-12-05
发布日期:
2021-12-21
通讯作者:
崔敏华,刘和
作者简介:
张钤(1996—),女,硕士研究生。E-mail:基金资助:
ZHANG Qian1(), CUI Minhua1,2,3(), CHEN Lei1, WU Ping1, LIU He1,2,3()
Received:
2021-01-15
Revised:
2021-03-01
Online:
2021-12-05
Published:
2021-12-21
Contact:
CUI Minhua,LIU He
摘要:
疏水性新兴污染物(hydrophobic emerging contaminants,HECs)具有环境危害大、分布范围广和处理难度高等特点,利用生物电化学系统(bioelectrochemical system,BES)实现HECs的降解和脱毒是当前研究热点。本文综述了BES降解转化HECs的研究现状,分析了影响BES去除HECs效果的关键因素,着重介绍了BES降解转化不同类型HECs(包括药物类、个人护理品类、卤代烃类和抗生素及抗性基因类)的效能,然后回顾了BES与其他技术(传统厌氧工艺、芬顿、复合湿地及光催化等)结合协同降解HECs的最新进展,最后在功能电极材料设计研发、HECs降解去除与安全转化的理论研究及工程化应用等方面进行了总结和展望,以期对该领域的研究人员提供一定的理论参考和技术支持,从而推进生物电化学技术在疏水性新兴污染物降解领域的应用和发展。
中图分类号:
张钤, 崔敏华, 陈蕾, 吴平, 刘和. 生物电化学技术降解疏水性新兴污染物的研究进展[J]. 化工进展, 2021, 40(12): 6846-6858.
ZHANG Qian, CUI Minhua, CHEN Lei, WU Ping, LIU He. A critical review of bioelectrochemical system in the degradation of hydrophobic emerging contaminants[J]. Chemical Industry and Engineering Progress, 2021, 40(12): 6846-6858.
处理方法 | 具体工艺/试剂 | 污染物种类 | 去除效果 | 优点 | 缺点 | 参考 文献 |
---|---|---|---|---|---|---|
好氧生物降解 | 传统活性污泥法 | 佳乐麝香 | 73%~96% | 降解、矿化程度高;成本低; 降解产物毒性一般小于母体污染物 | 降解周期长;可降解污染物种类少、具有局限性 | [ |
膜生物反应器 | 双氯酚酸 | 60%~80% | ||||
水解酸化-生物处理 | 环丙沙星 | 90% | [ | |||
厌氧生物降解 | 污泥厌氧消化 | 萘普生 | 80% | |||
麝香 | 50%~90% | [ | ||||
布洛芬 | 30%~60% | |||||
卡马西平 | 无明显降解 | |||||
化学氧化法 | β-FeOOH/Al2O3 | 布洛芬 | 100% | 降解/矿化程度高、效果稳定、反应过程容易控制 | 基建/运行成本高,二次污染重;中间降解产物生态毒性不稳定 | [ |
β-FeOOH/Al2O3 | 环丙沙星 | 100% | [ | |||
臭氧催化氧化 | Mg3Fe0.5Al | 双氯酚酸 | 73% | [ | ||
芬顿法 | FeS2 | 三氯生 | 90% | [ | ||
Fe3O4 | 卡马西平 布洛芬 | 86.26% 83.29% | [ | |||
Fe3O4 | 萘啶酸 | 60% | [ | |||
电离辐射 | 60Co(1.1KGy) | 布洛芬 | 100% | [ | ||
60Co(2.0KGy) | 双氯酚酸 | 100% | [ | |||
60Co(5.0KGy) | 氯贝酸 | 100% | [ | |||
60Co(20Gy) | 4-壬基酚 | 100% | [ | |||
吸附法 | 颗粒活性炭 | 双氯酚酸、三氯生 布洛芬 | 10%~68% | 系统简单,不形成有毒中间产物;处理方法成本基建及设备投资少,稳定性高,能耗低 | 污染物没有进一步降解转化,仍存在介质中 | [ |
粉状活性炭(PAC) | 卡马西平 | 60% | ||||
AmberliteXAD-4 | 双氯酚酸 | 92.80% | ||||
磁性树脂W150 | 呋喃西林 | 180mg·g-1 | ||||
矿物 | 双氯酚酸 | 37.5%~95.9% | ||||
膜分离法 | 微滤-颗粒活性炭-纳滤 | 疏水性PPCPs | 45%~80% | 操作简单,污染物去除率高,占用空间小 | 易造成膜孔隙堵塞污染 | [ |
超滤-纳滤 | 磺胺甲唑、 双氯芬酸 | 70% |
表1 常见HECs处理工艺效果以及优缺点比较
处理方法 | 具体工艺/试剂 | 污染物种类 | 去除效果 | 优点 | 缺点 | 参考 文献 |
---|---|---|---|---|---|---|
好氧生物降解 | 传统活性污泥法 | 佳乐麝香 | 73%~96% | 降解、矿化程度高;成本低; 降解产物毒性一般小于母体污染物 | 降解周期长;可降解污染物种类少、具有局限性 | [ |
膜生物反应器 | 双氯酚酸 | 60%~80% | ||||
水解酸化-生物处理 | 环丙沙星 | 90% | [ | |||
厌氧生物降解 | 污泥厌氧消化 | 萘普生 | 80% | |||
麝香 | 50%~90% | [ | ||||
布洛芬 | 30%~60% | |||||
卡马西平 | 无明显降解 | |||||
化学氧化法 | β-FeOOH/Al2O3 | 布洛芬 | 100% | 降解/矿化程度高、效果稳定、反应过程容易控制 | 基建/运行成本高,二次污染重;中间降解产物生态毒性不稳定 | [ |
β-FeOOH/Al2O3 | 环丙沙星 | 100% | [ | |||
臭氧催化氧化 | Mg3Fe0.5Al | 双氯酚酸 | 73% | [ | ||
芬顿法 | FeS2 | 三氯生 | 90% | [ | ||
Fe3O4 | 卡马西平 布洛芬 | 86.26% 83.29% | [ | |||
Fe3O4 | 萘啶酸 | 60% | [ | |||
电离辐射 | 60Co(1.1KGy) | 布洛芬 | 100% | [ | ||
60Co(2.0KGy) | 双氯酚酸 | 100% | [ | |||
60Co(5.0KGy) | 氯贝酸 | 100% | [ | |||
60Co(20Gy) | 4-壬基酚 | 100% | [ | |||
吸附法 | 颗粒活性炭 | 双氯酚酸、三氯生 布洛芬 | 10%~68% | 系统简单,不形成有毒中间产物;处理方法成本基建及设备投资少,稳定性高,能耗低 | 污染物没有进一步降解转化,仍存在介质中 | [ |
粉状活性炭(PAC) | 卡马西平 | 60% | ||||
AmberliteXAD-4 | 双氯酚酸 | 92.80% | ||||
磁性树脂W150 | 呋喃西林 | 180mg·g-1 | ||||
矿物 | 双氯酚酸 | 37.5%~95.9% | ||||
膜分离法 | 微滤-颗粒活性炭-纳滤 | 疏水性PPCPs | 45%~80% | 操作简单,污染物去除率高,占用空间小 | 易造成膜孔隙堵塞污染 | [ |
超滤-纳滤 | 磺胺甲唑、 双氯芬酸 | 70% |
分类 | 名称 | 分子式 | 辛醇-水分配系数 lgKow | 分子量 | 结构式 | 浓度水平/ng·L-1 | 国家/地区 |
---|---|---|---|---|---|---|---|
药品及 个人护理用品 | 阿奇霉素① | C38H72N2O12 | 4.02 | 749 | 47~82 | 加拿大[ | |
克拉霉素① | C38H69NO13 | 3.16 | 748 | 89~231 | 加拿大[ | ||
双氯芬酸② | C14H10Cl2O2 | 4.51 | 296 | 147~320 | 上海[ | ||
氯贝酸① | C10H11ClO3 | 2.57 | 214 | 7.4~51.3 | 上海[ | ||
布洛芬② | C13H18O2 | 3.97 | 206 | 480 | 意大利[ | ||
卡马西平② | C15H12N2O | 2.47 | 236 | 0.1~8.5 44.6~118 | 北京[ 长江流域 | ||
三氯生② | C12H7Cl3O2 | 4.71 | 289 | 5.74~105 | 东江[ | ||
三氯卡班② | C13H9ClN2O | 4.90 | 315 | 4.11~71.8 | 东江[ | ||
萘普生② | C14H14O3 | 3.18 | 230 | 6.32~145 | 美国[ | ||
苯扎贝特 | C19H20ClNO4 | 4.25 | 362 | 72.1 | 美国[ | ||
氯霉素② | C11H12Cl2N2O5 | 1.14 | 323 | 93~1178 | 河北[ | ||
吲哚美辛① | C19H16ClNO4 | 4.27 | 358 | 83~979 | 长江 流域[ | ||
内分泌干扰物 | 邻苯二甲酸二(2-乙基)己酯 | C24H38O4 | 7.60 | 391 | 61 | 全国 平均值[ | |
酞酸二丁酯 | C16H22O4 | 4.50 | 278 | 284 | 长江 上游[ | ||
双酚A② | C15H16O2 | 3.32 | 228 | 26.2 | 黄河口[ | ||
壬基酚 | C15H24O | 5.99 | 220 | 60~730 | 全国[ |
表2 常见HECs基本信息及浓度分布
分类 | 名称 | 分子式 | 辛醇-水分配系数 lgKow | 分子量 | 结构式 | 浓度水平/ng·L-1 | 国家/地区 |
---|---|---|---|---|---|---|---|
药品及 个人护理用品 | 阿奇霉素① | C38H72N2O12 | 4.02 | 749 | 47~82 | 加拿大[ | |
克拉霉素① | C38H69NO13 | 3.16 | 748 | 89~231 | 加拿大[ | ||
双氯芬酸② | C14H10Cl2O2 | 4.51 | 296 | 147~320 | 上海[ | ||
氯贝酸① | C10H11ClO3 | 2.57 | 214 | 7.4~51.3 | 上海[ | ||
布洛芬② | C13H18O2 | 3.97 | 206 | 480 | 意大利[ | ||
卡马西平② | C15H12N2O | 2.47 | 236 | 0.1~8.5 44.6~118 | 北京[ 长江流域 | ||
三氯生② | C12H7Cl3O2 | 4.71 | 289 | 5.74~105 | 东江[ | ||
三氯卡班② | C13H9ClN2O | 4.90 | 315 | 4.11~71.8 | 东江[ | ||
萘普生② | C14H14O3 | 3.18 | 230 | 6.32~145 | 美国[ | ||
苯扎贝特 | C19H20ClNO4 | 4.25 | 362 | 72.1 | 美国[ | ||
氯霉素② | C11H12Cl2N2O5 | 1.14 | 323 | 93~1178 | 河北[ | ||
吲哚美辛① | C19H16ClNO4 | 4.27 | 358 | 83~979 | 长江 流域[ | ||
内分泌干扰物 | 邻苯二甲酸二(2-乙基)己酯 | C24H38O4 | 7.60 | 391 | 61 | 全国 平均值[ | |
酞酸二丁酯 | C16H22O4 | 4.50 | 278 | 284 | 长江 上游[ | ||
双酚A② | C15H16O2 | 3.32 | 228 | 26.2 | 黄河口[ | ||
壬基酚 | C15H24O | 5.99 | 220 | 60~730 | 全国[ |
污染物种类 | 污染物名称 | 污染物浓度 | 反应装置 类型 | 输出电压 (MFC) | 外加电压(MEC) | 电极材料 | 降解 周期 | 降解 效率/% | 参考 文献 |
---|---|---|---|---|---|---|---|---|---|
疏水性药品 及个人护理 用品 | 三氯生 | 10mg·L-1 | AD-MFC | (420±40)mV | — | 碳毡(9×9cm2) | 8天 | 100 | [ |
三氯生 | 1mg·L-1 | MFC | 60mV | — | 碳刷(5.9×6.9cm2) | 48h | 94 | [ | |
氯霉素 | 50mg·L-1 | MFC | >50mV | — | 碳毡(3×3cm2) | 12h | 84 | [ | |
氯霉素 | 20mg·L-1 | 电辅助厌氧系统 | — | 0~2V | 石墨板 | 1天 | 53~88 | [ | |
双氯芬酸 | 10mg·L-1 | CF-MFC | 0.51V | Ru/Fe-碳毡 | 2天 | 76 | [ | ||
卤代烃类 化合物 | 对氯硝基苯 | 40~120mg·L-1 | BES | — | 0.2~0.8V | 碳刷(3×3cm2) | 55h | >80 | [ |
二氯硝基苯 | 100mg·L-1 | MEC | — | 1.5V | 碳毡(200×70mm2) | 24h | 91 | [ | |
多氯联苯 | (20.2±4.0)mg·kg-1 | BES | — | 1.5、2.2、3.0V | 碳毡 | 24h | 40~60 | [ | |
2,4-二氯酚 | 100mg·L-1 | BES | — | 保持恒电流密度50mA/cm2 | Pd/MWNTs气体 扩散电极 | 2h | >79 | [ | |
对氟硝基苯 | 0.4mmol·L-1 | BES | — | 0~1.4V | 石墨电极 | 10h | 0~100 | [ | |
对硝基酚 | 0.93~6.77mol·m-3·d-1 | UASB–BES | — | 1.2V | 碳毡(5×3cm2) | 9h | 100 | [ |
表3 BES去除典型HECs的参数设置及降解效率
污染物种类 | 污染物名称 | 污染物浓度 | 反应装置 类型 | 输出电压 (MFC) | 外加电压(MEC) | 电极材料 | 降解 周期 | 降解 效率/% | 参考 文献 |
---|---|---|---|---|---|---|---|---|---|
疏水性药品 及个人护理 用品 | 三氯生 | 10mg·L-1 | AD-MFC | (420±40)mV | — | 碳毡(9×9cm2) | 8天 | 100 | [ |
三氯生 | 1mg·L-1 | MFC | 60mV | — | 碳刷(5.9×6.9cm2) | 48h | 94 | [ | |
氯霉素 | 50mg·L-1 | MFC | >50mV | — | 碳毡(3×3cm2) | 12h | 84 | [ | |
氯霉素 | 20mg·L-1 | 电辅助厌氧系统 | — | 0~2V | 石墨板 | 1天 | 53~88 | [ | |
双氯芬酸 | 10mg·L-1 | CF-MFC | 0.51V | Ru/Fe-碳毡 | 2天 | 76 | [ | ||
卤代烃类 化合物 | 对氯硝基苯 | 40~120mg·L-1 | BES | — | 0.2~0.8V | 碳刷(3×3cm2) | 55h | >80 | [ |
二氯硝基苯 | 100mg·L-1 | MEC | — | 1.5V | 碳毡(200×70mm2) | 24h | 91 | [ | |
多氯联苯 | (20.2±4.0)mg·kg-1 | BES | — | 1.5、2.2、3.0V | 碳毡 | 24h | 40~60 | [ | |
2,4-二氯酚 | 100mg·L-1 | BES | — | 保持恒电流密度50mA/cm2 | Pd/MWNTs气体 扩散电极 | 2h | >79 | [ | |
对氟硝基苯 | 0.4mmol·L-1 | BES | — | 0~1.4V | 石墨电极 | 10h | 0~100 | [ | |
对硝基酚 | 0.93~6.77mol·m-3·d-1 | UASB–BES | — | 1.2V | 碳毡(5×3cm2) | 9h | 100 | [ |
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