化工进展 ›› 2021, Vol. 40 ›› Issue (1): 505-514.DOI: 10.16085/j.issn.1000-6613.2020-0548
煤化工废水中酚类物质、氨氮的处理方法研究进展
刘兴社(
), 刘永军(), 刘喆, 李鹏飞, 刘磐
- 西安建筑科技大学环境与市政工程学院，西北水资源与环境生态教育部重点实验室，陕西 西安 710055
-
收稿日期:2020-04-09出版日期:2021-01-05发布日期:2021-01-12 -
通讯作者:刘永军 -
作者简介:刘兴社（1992—），男，博士研究生，研究方向为煤化工废水无害化处理理论与技术。E-mail：xingsheliu@163.com 。 -
基金资助:国家自然科学基金(51978559);陕西省重点研发计划(2019ZDLSF05-06)
Research progress on treatment methods of phenolic substances and ammonia nitrogen in coal chemical wastewater
Xingshe LIU(), Yongjun LIU(), Zhe LIU, Pengfei LI, Pan LIU
- School of Environmental and Municipal Engineering, Xi’an University of Architecture and Technology, Key Laboratory of Northwest Water Resource, Environment and Ecology of Ministry of Education, Xi’an 710055, Shaanxi, China
-
Received:2020-04-09Online:2021-01-05Published:2021-01-12 -
Contact:Yongjun LIU
摘要：
煤化工废水是一种典型的有毒、难降解性工业废水。经预处理后的废水中仍含有大量的有毒有害物质，其中氨氮、酚类物质是典型的代表，氨氮含量在200mg/L左右，酚类物质含量占COD值的40%以上，浓度高达1000mg/L。如果对这些高毒性的物质不加处理或处理深度不够，则对环境和生命都会造成极大的危害。因此，酚类物质、氨氮的有效处理是实现煤化工废水无害化处理以及绿色可持续发展的关键。本综述主要从酚类物质处理技术与工艺、氨氮处理技术与工艺两个方面梳理了国内外煤化工废水中酚类物质、氨氮的处理现状，也全面分析了各种技术与工艺的优缺点。使该领域的研究人员以更加科学的方法了解煤化工废水中酚类物质、氨氮处理技术与工艺的研究现状和发展趋势。最后，探讨了未来煤化工废水中酚类物质、氨氮处理的发展前景。
中图分类号:
引用本文
刘兴社, 刘永军, 刘喆, 李鹏飞, 刘磐. 煤化工废水中酚类物质、氨氮的处理方法研究进展[J]. 化工进展, 2021, 40(1): 505-514.
Xingshe LIU, Yongjun LIU, Zhe LIU, Pengfei LI, Pan LIU. Research progress on treatment methods of phenolic substances and ammonia nitrogen in coal chemical wastewater[J]. Chemical Industry and Engineering Progress, 2021, 40(1): 505-514.
表1 三种煤气化废水水质[6] (mg/L)
| 项目 | 鲁奇工艺 | 德士古工艺 | 壳牌工艺 |
|---|---|---|---|
| 氨氮 | 3500~9000 | 1300~2700 | 9000 |
| COD | 3500~23000 | 200~760 | 200~300 |
| 甲酸化合物 | 无 | 100~1200 | 无 |
| 苯酚 | 1500~5500 | <10 | 20 |
| 氰化物 | 1~40 | 10~30 | 50 |
| 焦油 | <500 | 无 | 10~20 |
表1 三种煤气化废水水质[6] (mg/L)
| 项目 | 鲁奇工艺 | 德士古工艺 | 壳牌工艺 |
|---|---|---|---|
| 氨氮 | 3500~9000 | 1300~2700 | 9000 |
| COD | 3500~23000 | 200~760 | 200~300 |
| 甲酸化合物 | 无 | 100~1200 | 无 |
| 苯酚 | 1500~5500 | <10 | 20 |
| 氰化物 | 1~40 | 10~30 | 50 |
| 焦油 | <500 | 无 | 10~20 |
表2 活性污泥脱氮技术
| 处理工艺 | 主要的运行条件 | 进水水质 | 去除率 | 参考文献 |
|---|---|---|---|---|
单步活性 污泥法 | 水力停留时间96.1h | NH3-N 504~2340mg·L-1，COD 807~3275mg·L-1，酚110~350mg·L-1 | COD 75%、酚98% | Vazquez等[ |
两步活性 污泥法 | 第一好氧池停留时间为98h，第二好氧池停留时间为86h，循环比率为2 | NH3-N 123~296mg·L-1，COD 922~1980mg·L-1，酚133~293mg·L-1 | NH3-N99.2%、酚98.9%、COD90.7% | Vazquez等[ |
三步活性 污泥法 | 反硝化池水力停留时间为15.4h，第一好氧池水力停留时间为98h，第二好氧池水力停留时间为86h | COD 800~1870mg·L-1，酚100~221mg·L-1， NH3-N 133~348mg·L-1 | 氨氮、酚类物质、COD、总氮的去除率分别可达90%、99%、63%、90%。 | Mara?ón等[ |
表2 活性污泥脱氮技术
| 处理工艺 | 主要的运行条件 | 进水水质 | 去除率 | 参考文献 |
|---|---|---|---|---|
单步活性 污泥法 | 水力停留时间96.1h | NH3-N 504~2340mg·L-1，COD 807~3275mg·L-1，酚110~350mg·L-1 | COD 75%、酚98% | Vazquez等[ |
两步活性 污泥法 | 第一好氧池停留时间为98h，第二好氧池停留时间为86h，循环比率为2 | NH3-N 123~296mg·L-1，COD 922~1980mg·L-1，酚133~293mg·L-1 | NH3-N99.2%、酚98.9%、COD90.7% | Vazquez等[ |
三步活性 污泥法 | 反硝化池水力停留时间为15.4h，第一好氧池水力停留时间为98h，第二好氧池水力停留时间为86h | COD 800~1870mg·L-1，酚100~221mg·L-1， NH3-N 133~348mg·L-1 | 氨氮、酚类物质、COD、总氮的去除率分别可达90%、99%、63%、90%。 | Mara?ón等[ |
表3 同步硝化反硝化脱氮技术
| 处理工艺 | 主要的实验条件 | 进水水质 | 去除率 | 参考文献 |
|---|---|---|---|---|
| 固定生物膜法 | 载体材料为聚乙烯，填充率为50% | NH3-N 166~684mg·L-1，COD 1400~1980mg·L-1，酚38~90mg·L-1 | NH3-N 46%、酚78%、COD 49% | Rava等[ |
| A2/O-MBR | 总水力停留时间为40h，反应器运行500d | NH3-N 49~488mg·L-1，COD 1182~3310mg·L-1，TN 110~617mg·L-1 | NH3-N 99.5%，COD 89.8%，TN 71.5% | Zhao等[ |
| 限氧曝气-SBBR | 溶解氧浓度4.5~0.35mg·L-1 | NH3-N 80~125mg·L-1，COD 600~1000mg·L-1 | NH3-N 76.91%，TN 70.23% | Ma等[ |
| MBBR | 悬浮载体为直径10mm的聚乙烯圆柱形材料，其密度约为0.97g·cm-3，填充率约50%。溶解氧控制在5mg·L-1左右，温度为33℃左右 | NH3-N 182~259mg·L-1，COD 1712~2340mg·L-1，酚94~146mg·L-1 | NH3-N 93%，COD 81%，酚89% | Li等[ |
表3 同步硝化反硝化脱氮技术
| 处理工艺 | 主要的实验条件 | 进水水质 | 去除率 | 参考文献 |
|---|---|---|---|---|
| 固定生物膜法 | 载体材料为聚乙烯，填充率为50% | NH3-N 166~684mg·L-1，COD 1400~1980mg·L-1，酚38~90mg·L-1 | NH3-N 46%、酚78%、COD 49% | Rava等[ |
| A2/O-MBR | 总水力停留时间为40h，反应器运行500d | NH3-N 49~488mg·L-1，COD 1182~3310mg·L-1，TN 110~617mg·L-1 | NH3-N 99.5%，COD 89.8%，TN 71.5% | Zhao等[ |
| 限氧曝气-SBBR | 溶解氧浓度4.5~0.35mg·L-1 | NH3-N 80~125mg·L-1，COD 600~1000mg·L-1 | NH3-N 76.91%，TN 70.23% | Ma等[ |
| MBBR | 悬浮载体为直径10mm的聚乙烯圆柱形材料，其密度约为0.97g·cm-3，填充率约50%。溶解氧控制在5mg·L-1左右，温度为33℃左右 | NH3-N 182~259mg·L-1，COD 1712~2340mg·L-1，酚94~146mg·L-1 | NH3-N 93%，COD 81%，酚89% | Li等[ |
表4 短程硝化脱氮技术
| 处理工艺 | 主要的实验条件 | 进水水质 | 去除率 | 参考文献 |
|---|---|---|---|---|
| 颗粒活性炭-短程脱氮技术 | 颗粒活性炭填充率25%；DO为4~6mg·L-1 | NH3-N 130.4~173.3mg·L-1，COD 1328.8~1807.3mg·L-1 | 总氮的去除率68.8%~75.8% | Zhao等[ |
| 粉末活性炭-短程脱氮技术 | 粉末活性炭投加量1g·L，HRT为24h，DO为4mg·L-1 | NH3-N 154mg·L-1，COD 1350mg·L-1，总酚420mg·L-1 | NH3-N86.89%，COD 85.8%，总氮75.54% | Zhao等[ |
表4 短程硝化脱氮技术
| 处理工艺 | 主要的实验条件 | 进水水质 | 去除率 | 参考文献 |
|---|---|---|---|---|
| 颗粒活性炭-短程脱氮技术 | 颗粒活性炭填充率25%；DO为4~6mg·L-1 | NH3-N 130.4~173.3mg·L-1，COD 1328.8~1807.3mg·L-1 | 总氮的去除率68.8%~75.8% | Zhao等[ |
| 粉末活性炭-短程脱氮技术 | 粉末活性炭投加量1g·L，HRT为24h，DO为4mg·L-1 | NH3-N 154mg·L-1，COD 1350mg·L-1，总酚420mg·L-1 | NH3-N86.89%，COD 85.8%，总氮75.54% | Zhao等[ |
表5 酚类物质的处理技术
| 处理工艺 | 主要的实验条件 | 进水水质 | 去除率 | 参考文献 |
|---|---|---|---|---|
| 高温上流式厌氧污泥床 | pH 7.1~7.9，温度55℃±2℃，HRT 24h，运行天数120d | 总酚570mg·L-1，COD 2900mg·L-1，BOD5 875mg·L-1 | TPH 50%~60%，COD 50%~55% | Wang等[ |
| 外循环厌氧反应器 | HRT 50h，pH>8，外循环比1∶3 | 总酚750~850mg·L-1，COD 3200~3500mg·L-1，NH4-N 250~300mg·L-1， pH 8.0~9.5 | 酚类物质可得到有效去除 | Jia等[ |
| 投加共基质的强化厌氧技术 | 甲醇投加浓度为500mg COD/L | 总酚600mg·L-1 | TPH 72% | Wang等[ |
| 微电解-生物反应器（MEBR） | 第1运行阶段：运行时间90d，HRT 24h，pH 6.2，分阶段增加曝气量，最大量为3.5mg·L-1。第2运行阶段：运行时间90d，pH 6.2，DO 0.5mg·L-1 | 总酚309~351mg·L-1，COD 1700~2100mg·L-1，100~120mg·L-1 | COD和酚类化合物得到高效去除 | Ma等[ |
| 厌氧-好氧间歇工艺 | 66次的循环处理，HRT（厌氧24h、好氧48h和厌氧48h、好氧48h） | 总酚850~950mg·L-1，COD 3800~4400mg·L-1，氨氮230~300mg·L-1 | 77种有机污染物几乎完全的去除 | Ji等[ |
| 酚降解菌强化生物法 | pH 7~7.5，温度35℃，DO 2~4mg·L-1，运行天数30d | 总酚355.4~403.6mg·L-1，COD 2580.7~2710.9mg·L-1，氨氮182.1~259.0mg·L-1 | 膜生物反应器可抵抗进水浓度为750mg·L-1的酚类化合物 | Fang等[ |
| 酚降解菌强化生物接触氧化池 | pH 7~7.2，HRT 36h，DO 0.5~1mg·L-1 | 总酚355.4~403.6mg·L-1，COD 2580.7~2710.9mg·L-1，氨氮182.1~259.0mg·L-1 | TPH 80%，COD 78%，氨氮25% | Fang等[ |
| 芬顿氧化 | pH 7.8，处理时间60min，Fe2+=300mg·L-1，H2O2=4000mg·L-1 | 酚244mg·L-1，COD 1140mg·L-1 | 酚86%，COD 99.5% | Gü?lü等[ |
表5 酚类物质的处理技术
| 处理工艺 | 主要的实验条件 | 进水水质 | 去除率 | 参考文献 |
|---|---|---|---|---|
| 高温上流式厌氧污泥床 | pH 7.1~7.9，温度55℃±2℃，HRT 24h，运行天数120d | 总酚570mg·L-1，COD 2900mg·L-1，BOD5 875mg·L-1 | TPH 50%~60%，COD 50%~55% | Wang等[ |
| 外循环厌氧反应器 | HRT 50h，pH>8，外循环比1∶3 | 总酚750~850mg·L-1，COD 3200~3500mg·L-1，NH4-N 250~300mg·L-1， pH 8.0~9.5 | 酚类物质可得到有效去除 | Jia等[ |
| 投加共基质的强化厌氧技术 | 甲醇投加浓度为500mg COD/L | 总酚600mg·L-1 | TPH 72% | Wang等[ |
| 微电解-生物反应器（MEBR） | 第1运行阶段：运行时间90d，HRT 24h，pH 6.2，分阶段增加曝气量，最大量为3.5mg·L-1。第2运行阶段：运行时间90d，pH 6.2，DO 0.5mg·L-1 | 总酚309~351mg·L-1，COD 1700~2100mg·L-1，100~120mg·L-1 | COD和酚类化合物得到高效去除 | Ma等[ |
| 厌氧-好氧间歇工艺 | 66次的循环处理，HRT（厌氧24h、好氧48h和厌氧48h、好氧48h） | 总酚850~950mg·L-1，COD 3800~4400mg·L-1，氨氮230~300mg·L-1 | 77种有机污染物几乎完全的去除 | Ji等[ |
| 酚降解菌强化生物法 | pH 7~7.5，温度35℃，DO 2~4mg·L-1，运行天数30d | 总酚355.4~403.6mg·L-1，COD 2580.7~2710.9mg·L-1，氨氮182.1~259.0mg·L-1 | 膜生物反应器可抵抗进水浓度为750mg·L-1的酚类化合物 | Fang等[ |
| 酚降解菌强化生物接触氧化池 | pH 7~7.2，HRT 36h，DO 0.5~1mg·L-1 | 总酚355.4~403.6mg·L-1，COD 2580.7~2710.9mg·L-1，氨氮182.1~259.0mg·L-1 | TPH 80%，COD 78%，氨氮25% | Fang等[ |
| 芬顿氧化 | pH 7.8，处理时间60min，Fe2+=300mg·L-1，H2O2=4000mg·L-1 | 酚244mg·L-1，COD 1140mg·L-1 | 酚86%，COD 99.5% | Gü?lü等[ |
表6 在MEBR反应器中进水和出水的有机物组成[44]
| 有机化合物 | 进水 | 出水 | 有机化合物 | 进水 | 出水 |
|---|---|---|---|---|---|
| phenol | 12.09① | ND② | naphthalene,1,3-dimethyl | 2.65 | ND |
| p-cresol | 15.12 | 2.16 | quinoline | 0.62 | ND |
| phenol,4-ethyl | 3.19 | ND | furan,3-phenyl | 3.08 | ND |
| phenol,2,6-dimethyl | 5.39 | ND | 5-hydroxyindole | 0.34 | 2.45 |
| phenol,3,4-dimethyl | 3.45 | ND | 2-hydroxypyridine | ND | 1.87 |
| phenol,3-ethy | 9.04 | 1.02 | undecane | 0.27 | 0.31 |
| 1-naphthalenol,2-methyl | 2.84 | ND | hexadecane | 0.81 | 0.11 |
| phenol,2-(1-methylethyl)- | 0.44 | ND | pentadecane | 1.38 | 0.97 |
| phenol,4-bis(1,1-dimethylethyl)- | 1.51 | 2.12 | phthalic acid, isobutyl 4-octyl ester | ND | 10.76 |
| phenol,3,5-dimethyl | 2.71 | 0.13 | 4-chlorobutyric acid,3,4-dimethylphenyl | ND | 6.12 |
| phenol,2-[(trimethylsilyl)oxy] | 0.89 | 1.32 | phthalic acid,6-ethyl-3-octyl butyl ester | ND | 10.35 |
| indole | 1.84 | ND | hydroxybutanedioic acid | ND | 7.61 |
| 6-methyl-4-indanol | 1.25 | ND | propanoic acid,anhydride | ND | 4.11 |
| benzene,1-ethyl-4-methoxy | 0.27 | ND | heptanoic acid | ND | 6.16 |
| naphthalene | 2.87 | ND | others | 27.95 | 42.43 |
表6 在MEBR反应器中进水和出水的有机物组成[44]
| 有机化合物 | 进水 | 出水 | 有机化合物 | 进水 | 出水 |
|---|---|---|---|---|---|
| phenol | 12.09① | ND② | naphthalene,1,3-dimethyl | 2.65 | ND |
| p-cresol | 15.12 | 2.16 | quinoline | 0.62 | ND |
| phenol,4-ethyl | 3.19 | ND | furan,3-phenyl | 3.08 | ND |
| phenol,2,6-dimethyl | 5.39 | ND | 5-hydroxyindole | 0.34 | 2.45 |
| phenol,3,4-dimethyl | 3.45 | ND | 2-hydroxypyridine | ND | 1.87 |
| phenol,3-ethy | 9.04 | 1.02 | undecane | 0.27 | 0.31 |
| 1-naphthalenol,2-methyl | 2.84 | ND | hexadecane | 0.81 | 0.11 |
| phenol,2-(1-methylethyl)- | 0.44 | ND | pentadecane | 1.38 | 0.97 |
| phenol,4-bis(1,1-dimethylethyl)- | 1.51 | 2.12 | phthalic acid, isobutyl 4-octyl ester | ND | 10.76 |
| phenol,3,5-dimethyl | 2.71 | 0.13 | 4-chlorobutyric acid,3,4-dimethylphenyl | ND | 6.12 |
| phenol,2-[(trimethylsilyl)oxy] | 0.89 | 1.32 | phthalic acid,6-ethyl-3-octyl butyl ester | ND | 10.35 |
| indole | 1.84 | ND | hydroxybutanedioic acid | ND | 7.61 |
| 6-methyl-4-indanol | 1.25 | ND | propanoic acid,anhydride | ND | 4.11 |
| benzene,1-ethyl-4-methoxy | 0.27 | ND | heptanoic acid | ND | 6.16 |
| naphthalene | 2.87 | ND | others | 27.95 | 42.43 |
表7 从煤化工废水中分离出的降解酚类污染物的优势菌
| 微生物 | 底物 | 降解性能 | 微生物来源 | 参考文献 |
|---|---|---|---|---|
| Diaphorobacter P2 | 苯酚 | 4d内可完全生化降解约1/2（412.3mg·L-1）焦化原水中的酚类物质 | 分离于焦化废水 | Meng等[ |
| Pseudomonas sp. | 邻二甲苯 | 在邻二甲苯浓度高达2500mg·L-1时，对其的去除率在30h内可达到73% | 分离于受焦化废水污染的土壤中 | Chen等[ |
| Comamonas testosterone | 苯酚 | 对苯酚具较高耐受力达到2000mg·L-1、且在48h内可将初始浓度为1000mg·L-1的苯酚完全降解 | 分离于焦化废水厂的活性污泥中 | Chen等[ |
| Tropicalis strain K11 | 苯酚 | 初始浓度为125mg·L-1的苯酚去除率可达80% | 分离于焦化废水厂的活性污泥中 | Karim等[ |
| Debaryomyces sp. | 苯酚 | 在适宜的条件下，500mg·L-1的苯酚可在32h时内完全降解 | 分离于煤气化废水 | Jiang等[ |
| Klebsiella sp. | 苯酚、4-甲基苯酚以及 3,5-二甲基苯酚和间苯二酚 | 该菌株形成的膜生物反应器可抵抗进水浓度为750mg·L-1的酚类化合物 | 分离于煤气化废水 | Fang等[ |
表7 从煤化工废水中分离出的降解酚类污染物的优势菌
| 微生物 | 底物 | 降解性能 | 微生物来源 | 参考文献 |
|---|---|---|---|---|
| Diaphorobacter P2 | 苯酚 | 4d内可完全生化降解约1/2（412.3mg·L-1）焦化原水中的酚类物质 | 分离于焦化废水 | Meng等[ |
| Pseudomonas sp. | 邻二甲苯 | 在邻二甲苯浓度高达2500mg·L-1时，对其的去除率在30h内可达到73% | 分离于受焦化废水污染的土壤中 | Chen等[ |
| Comamonas testosterone | 苯酚 | 对苯酚具较高耐受力达到2000mg·L-1、且在48h内可将初始浓度为1000mg·L-1的苯酚完全降解 | 分离于焦化废水厂的活性污泥中 | Chen等[ |
| Tropicalis strain K11 | 苯酚 | 初始浓度为125mg·L-1的苯酚去除率可达80% | 分离于焦化废水厂的活性污泥中 | Karim等[ |
| Debaryomyces sp. | 苯酚 | 在适宜的条件下，500mg·L-1的苯酚可在32h时内完全降解 | 分离于煤气化废水 | Jiang等[ |
| Klebsiella sp. | 苯酚、4-甲基苯酚以及 3,5-二甲基苯酚和间苯二酚 | 该菌株形成的膜生物反应器可抵抗进水浓度为750mg·L-1的酚类化合物 | 分离于煤气化废水 | Fang等[ |
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