Research status of membrane fouling mitigation by PAC in submerged PAC-AMBRs

doi:10.16085/j.issn.1000-6613.2022-0527

Abstract

Abstract:

The submerged powdered activated carbon-aerobic membrane bioreactors (PAC-AMBRs) are new wastewater treatment technology, which integrates PAC adsorption, microbial degradation, and membrane separation. This review focuses on the previously published research on the mechanism of directly adding PAC to the submerged PAC-AMBRs system to alleviate membrane fouling in the past 20 years. The membrane fouling mitigation mechanism of sludge flocs and dissolved organic matters by PAC is analyzed comprehensively. The effects of PAC dosage and replenishment rate on membrane fouling are discussed. It is concluded that the fouling mitigation by PAC is a comprehensive process. The cake layer formed by sludge flocs with PAC as a carrier had a loose structure and strong pressure resistance. It not only effectively reduces the cake resistance but also is used as a self-forming dynamic membrane, intercepting dissolves organic matter and suspends microorganisms and reducing membrane fouling. Dissolved organic matter is removed through the synergistic effect of PAC adsorption and/or microbial degradation on PAC, reducing membrane fouling and improving permeate flux. Regular discharge and supplement of a certain amount of PAC can improve the efficiency of fouling alleviation.

Key words: powdered activated carbon, aerobic membrane bioreactor, adsorption, microbial degradation, fouling

摘要：

浸没式粉末活性炭-好氧膜生物反应器（powdered activated carbon-aerobic membrane bioreactors，PAC-AMBRs）是一种利用PAC吸附性、微生物降解性和膜分离特性的新型废水处理技术。本文重点分析了近20年来浸没式PAC-AMBRs系统直接投加PAC缓解膜污染机制的研究成果，探讨了PAC通过对污泥絮体和溶解性有机物的综合影响缓解膜污染的机制，分析了PAC投加量和补充率对膜污染的影响。通过分析可知PAC缓解膜污染是一个综合作用的结果。以PAC为载体形成的污泥絮体在膜表面形成结构疏松和抗压性强的滤饼层，不仅能有效降低滤饼层阻力（cake resistance，R_c），还可以作为自成型动态膜截留溶解性有机物和悬浮微生物等来减少此类污染物造成的膜污染。PAC通过吸附和/或表面附着的微生物降解溶解性有机物的协同作用降低其造成的过滤阻力。定期排出和补充一定量的PAC可以提高缓解膜污染的效率。

关键词: 粉末活性炭, 好氧膜生物反应器, 吸附, 微生物降解, 膜污染

CLC Number:

X703

LIU Yajuan. Research status of membrane fouling mitigation by PAC in submerged PAC-AMBRs[J]. Chemical Industry and Engineering Progress, 2023, 42(1): 457-468.

刘雅娟. 浸没式PAC-AMBRs系统中PAC缓解膜污染的研究进展[J]. 化工进展, 2023, 42(1): 457-468.

Figures/Tables 5

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膜材料、形式与膜孔径	PAC平均粒径或范围/μm	PAC投加量 /g·L^-1	初始絮状污泥粒径 /μm	PAC辅助形成的污泥絮体粒径/μm	膜污染控制效果	参考文献
PVDF平板膜 MWCO^①=140kDa	76~88	0.75	56.0	84	R_t和R_c分别降低17.5%和24.0%	[42]
聚乙烯中空纤维膜膜孔径0.1μm	150~250	1	—	401	R_t和R_c分别降低16.0%和18.4%	[30]
陶瓷平板膜膜孔径100nm	149	20	48	69±6	过滤周期延长1.5倍平均膜污染速率降低33%	[34]
尼龙滤网膜孔径30μm	8~35	2	98.6	150	过滤周期延长2.5倍	[31]
PVDF平板膜膜孔径0.2μm	125~150	1.2	47.0	56	R_t和R_c分别降低43.9%和53.9% 过滤周期延长1.8倍	[33]
外层尼龙滤网膜孔径75μm	29.4	1	26.1	60.6	稳定水通量提高25%	[35]
PVDF平板膜膜孔径0.1μm	15	0.5	72.2	69.8	临界通量提高19%	[38]
聚丙烯腈中空纤维膜膜孔径0.5μm	14.88±3.93 67.60±2.70	5 5	30.20±0.50	38.15±1.52 90.05±0.52	过滤周期延长5.7倍过滤周期延长9.4倍	[43]
聚乙烯中空纤维膜膜孔径0.1μm	28.64		3.6	6.7 8	过滤周期延长1.7倍过滤周期延长2.5倍	[44]
氯化聚乙烯平板膜膜孔径0.4μm	100~250	1	45	62	连续运行110d后， TMP降低9.3%	[45]
聚醚砜膜膜孔径0.05μm	75	2	70.6	84.7~86.5	运行145d的水通量提高 1.5~2.8倍	[46]
聚丙烯腈中空纤维膜膜孔径0.5μm	24.5	1 3 5	133.9	67.9 55.5 38.2	TMP增高速率降低98.8% TMP增高速率降低99.1% TMP增高速率降低99.3%	[3]

膜材料、形式与膜孔径	PAC平均粒径或范围/μm	PAC投加量 /g·L^-1	初始絮状污泥粒径 /μm	PAC辅助形成的污泥絮体粒径/μm	膜污染控制效果	参考文献
PVDF平板膜 MWCO^①=140kDa	76~88	0.75	56.0	84	R_t和R_c分别降低17.5%和24.0%	[42]
聚乙烯中空纤维膜膜孔径0.1μm	150~250	1	—	401	R_t和R_c分别降低16.0%和18.4%	[30]
陶瓷平板膜膜孔径100nm	149	20	48	69±6	过滤周期延长1.5倍平均膜污染速率降低33%	[34]
尼龙滤网膜孔径30μm	8~35	2	98.6	150	过滤周期延长2.5倍	[31]
PVDF平板膜膜孔径0.2μm	125~150	1.2	47.0	56	R_t和R_c分别降低43.9%和53.9% 过滤周期延长1.8倍	[33]
外层尼龙滤网膜孔径75μm	29.4	1	26.1	60.6	稳定水通量提高25%	[35]
PVDF平板膜膜孔径0.1μm	15	0.5	72.2	69.8	临界通量提高19%	[38]
聚丙烯腈中空纤维膜膜孔径0.5μm	14.88±3.93 67.60±2.70	5 5	30.20±0.50	38.15±1.52 90.05±0.52	过滤周期延长5.7倍过滤周期延长9.4倍	[43]
聚乙烯中空纤维膜膜孔径0.1μm	28.64		3.6	6.7 8	过滤周期延长1.7倍过滤周期延长2.5倍	[44]
氯化聚乙烯平板膜膜孔径0.4μm	100~250	1	45	62	连续运行110d后， TMP降低9.3%	[45]
聚醚砜膜膜孔径0.05μm	75	2	70.6	84.7~86.5	运行145d的水通量提高 1.5~2.8倍	[46]
聚丙烯腈中空纤维膜膜孔径0.5μm	24.5	1 3 5	133.9	67.9 55.5 38.2	TMP增高速率降低98.8% TMP增高速率降低99.1% TMP增高速率降低99.3%	[3]

膜材料、形式与孔径	操作条件	PAC粒径与投加方式	PAC投加量 /g·L^-1	废水及其特征	有机物去除效率	膜污染控制效果	参考文献
PVDF平板膜，MWCO=140kDa	HRT=4d 恒流过滤 J=30LMH	75~80μm 一次性	0.75	市政污水处理厂二沉池出水，TOC=10.7mg/L	TOC：62.7%，TOC去除率提高3.9倍	膜过滤时间延长2倍，R_t降低17.4%	[42]
聚氯乙烯平板膜，膜孔径0.4μm	HRT=12h	— 一次性	4	煤气化废水， COD^①=2.27g/L	COD^①：93%，sEPS减少67.7%	过滤周期延长1.25倍，连续运行50d后，TMP下降34%	[64]
PVDF中空纤维膜，膜孔径0.2μm	恒流过滤 J=15LMH	<200目一次性	1	合成废水， COD=398mg/L	COD：95.4%，SMP降低62.2%	R_t和R_c分别降低2.0%和9.1%，膜污染速率降低12.6%~36.4%	[9]
			2		COD：95%，SMP减少69.4%	R_t和R_c分别降低5.1%和16.4%，膜污染速率降低16.1%~38.8%
			4		COD：94.3%，SMP减少50.6%	R_t和R_c分别降低4.7%和18.8%，膜污染速率降低7.1%~19.9%
陶瓷平板膜，膜孔径100nm	DO^②=1.5~2.5mg/L 恒流过滤 J=15LMH	149μm 定期	20	合成市政污水， COD=200~220mg/L	COD：（99.5±0.1）%，SMP和EPS降低77%和61%	过滤周期延长1.5倍，平均膜污染速率降低33%	[34]
氯化聚乙烯平板膜，膜孔径0.4μm	SRT=30h，HRT=19h SAD^③=1.5m³/(m²·h) 恒流过滤 J=8LMH	0.1~0.25mm 定期	1	化妆品废水， COD=9.6~10g/L	COD：（95.4±0.6）%，SMP减少6.9%	临界水通量增加25%，TMP降低	[45]
聚醚砜膜，膜孔径0.05μm	曝气速率=8~10L/min，恒压过滤 TMP=20kPa	75μm 一次性	2	化学法合成依托度酸制药废水，COD=18g/L	COD：85%~98%，sEPS减少28%~88%	运行145d的水通量提高1.5~2.8倍	[46]
PVDF中空纤维膜，膜孔径0.2μm	HRT=6h，曝气速率=120L/h，恒流过滤J=16LMH	— 一次性	0.75	校园生活污水 COD=428.4mg/L	COD：91.4%，混合液中COD减少5.9%	膜污染速率降低27.4%~91.3%	[52]
PVDF中空纤维膜，膜孔径0.2μm	HRT=6h，曝气速率=120L/h，恒流过滤J=16LMH	— 一次性	1.5	校园生活污水 COD=428.4mg/L	COD：91.8%，混合液中COD减少8.0%	膜污染速率降低3.4%~88.4%	[52]
氯化聚乙烯平板膜，膜孔径0.4μm	恒流过滤 J=17LMH	一次性	1	合成废水 COD=（1987±73）mg/L	COD：96%，SMP减少10%	过滤50mL废水的时间缩短15%	[68]
			3		SMP减少25%	过滤50mL废水的时间缩短40%
			5		SMP减少10%	过滤50mL废水的时间缩短10%
亲水性中空纤维膜，膜孔径0.1μm	曝气速率=5L/min 恒流过滤 J=42LMH	22~45μm（52%）一次性	10	合成废水 COD=9.09mg/L	COD：74.4%，UV₂₅₄去除率提高64%	过滤周期延长1.9倍，膜表面有机物含量减少26.3%	[67]
亲水性中空纤维膜，膜孔径0.1μm	曝气速率=5L/min 恒流过滤 J=42LMH	22~45μm（52%）一次性	40	合成废水 COD=9.09mg/L	COD：82.5%，UV₂₅₄去除率提高64%	过滤周期延长3倍膜表面有机物含量减少83.2%	[67]
PVDF中空纤维膜，膜孔径0.22μm	SRT=30d，HRT=2h 恒流过滤 J=20.02LMH	每天	2	湖水 COD＝7.31mg/L	COD：52.04%，TOC和UV₂₅₄去除率提高2.1和2.3倍	R_c降低47% R_irr降低20.4%	[69]
尼龙滤网，膜孔径30μm	HRT=7d，DO=2~4 mg/L 曝气速率=2.6~ 4.5L/min	31.9μm 一次性	2	酒精蒸馏废水 COD=（29.20~48.26）g/L	COD：41%，COD去除率提高1.5倍	临界通量提高近23% 无膜更换和清洗下的过滤时间延长8d	[71]
聚乙烯亲水膜，膜孔径0.1μm	HRT=2.4h 曝气强度 1000L/(m³·min) 恒流过滤速率=320m/d	— 一次性	40	经沉淀处理后的河水 TOC=（2.35±0.25）mg/L	TOC：71%，多糖和蛋白质去除率提高4.3%和2.2%~4.5%	50d内，TMP从初始值增加到50kPa的过滤周期减少25%	[70]
聚乙烯亲水膜，膜孔径0.1μm	HRT=2.4h 曝气强度 1000L/(m³·min) 恒流过滤速率=320m/d	— 一次性	40	生物过滤后的出水 TOC=（2.10±0.38）mg/L	TOC：66%，蛋白质去除率提高6.2%~6.7%	50d内，TMP从初始值增加到50kPa的过滤周期减少50%	[70]
微滤膜	HRT=2h 曝气强度=0.25m³/h 恒流过滤 J=16.6LMH	— 一次性	5	模拟微污染地表水 DOC=5.4~6.1mg/L	DOC：35%，UV₂₅₄去除率提高66.7%	TMP达到50kPa时的水通量为19LMH	[72]
			25		DOC：50%，UV₂₅₄去除率提高1.3倍	TMP达到50kPa时的水通量为18LMH
			50		DOC：75%，UV₂₅₄去除率提高1.8倍	TMP达到50kPa时的水通量为15.5LMH
			75		DOC：80%，UV₂₅₄去除率提高2倍	TMP达到50 kPa时的水通量为13LMH
聚醚酰亚胺中空纤维膜，膜孔径0.5μm	HRT=9.5h 曝气强度=0.5m³/h	定期	10	漂白浆厂废水 COD=1125mg/L	COD：88%	水通量提高60% 过滤阻力降低50%	[73]
PVDF中空纤维膜，膜孔径0.2μm	DO=2~4mg/L 恒流过滤 J=15LMH	定期	2	合成废水 COD=44g/L	COD：（97±2）%	过滤周期延长9.7%~51.2% 过滤阻力降低0.8%~45.3%	[74]

膜材料、形式与孔径	操作条件	PAC粒径与投加方式	PAC投加量 /g·L^-1	废水及其特征	有机物去除效率	膜污染控制效果	参考文献
PVDF平板膜，MWCO=140kDa	HRT=4d 恒流过滤 J=30LMH	75~80μm 一次性	0.75	市政污水处理厂二沉池出水，TOC=10.7mg/L	TOC：62.7%，TOC去除率提高3.9倍	膜过滤时间延长2倍，R_t降低17.4%	[42]
聚氯乙烯平板膜，膜孔径0.4μm	HRT=12h	— 一次性	4	煤气化废水， COD^①=2.27g/L	COD^①：93%，sEPS减少67.7%	过滤周期延长1.25倍，连续运行50d后，TMP下降34%	[64]
PVDF中空纤维膜，膜孔径0.2μm	恒流过滤 J=15LMH	<200目一次性	1	合成废水， COD=398mg/L	COD：95.4%，SMP降低62.2%	R_t和R_c分别降低2.0%和9.1%，膜污染速率降低12.6%~36.4%	[9]
			2		COD：95%，SMP减少69.4%	R_t和R_c分别降低5.1%和16.4%，膜污染速率降低16.1%~38.8%
			4		COD：94.3%，SMP减少50.6%	R_t和R_c分别降低4.7%和18.8%，膜污染速率降低7.1%~19.9%
陶瓷平板膜，膜孔径100nm	DO^②=1.5~2.5mg/L 恒流过滤 J=15LMH	149μm 定期	20	合成市政污水， COD=200~220mg/L	COD：（99.5±0.1）%，SMP和EPS降低77%和61%	过滤周期延长1.5倍，平均膜污染速率降低33%	[34]
氯化聚乙烯平板膜，膜孔径0.4μm	SRT=30h，HRT=19h SAD^③=1.5m³/(m²·h) 恒流过滤 J=8LMH	0.1~0.25mm 定期	1	化妆品废水， COD=9.6~10g/L	COD：（95.4±0.6）%，SMP减少6.9%	临界水通量增加25%，TMP降低	[45]
聚醚砜膜，膜孔径0.05μm	曝气速率=8~10L/min，恒压过滤 TMP=20kPa	75μm 一次性	2	化学法合成依托度酸制药废水，COD=18g/L	COD：85%~98%，sEPS减少28%~88%	运行145d的水通量提高1.5~2.8倍	[46]
PVDF中空纤维膜，膜孔径0.2μm	HRT=6h，曝气速率=120L/h，恒流过滤J=16LMH	— 一次性	0.75	校园生活污水 COD=428.4mg/L	COD：91.4%，混合液中COD减少5.9%	膜污染速率降低27.4%~91.3%	[52]
PVDF中空纤维膜，膜孔径0.2μm	HRT=6h，曝气速率=120L/h，恒流过滤J=16LMH	— 一次性	1.5	校园生活污水 COD=428.4mg/L	COD：91.8%，混合液中COD减少8.0%	膜污染速率降低3.4%~88.4%	[52]
氯化聚乙烯平板膜，膜孔径0.4μm	恒流过滤 J=17LMH	一次性	1	合成废水 COD=（1987±73）mg/L	COD：96%，SMP减少10%	过滤50mL废水的时间缩短15%	[68]
			3		SMP减少25%	过滤50mL废水的时间缩短40%
			5		SMP减少10%	过滤50mL废水的时间缩短10%
亲水性中空纤维膜，膜孔径0.1μm	曝气速率=5L/min 恒流过滤 J=42LMH	22~45μm（52%）一次性	10	合成废水 COD=9.09mg/L	COD：74.4%，UV₂₅₄去除率提高64%	过滤周期延长1.9倍，膜表面有机物含量减少26.3%	[67]
亲水性中空纤维膜，膜孔径0.1μm	曝气速率=5L/min 恒流过滤 J=42LMH	22~45μm（52%）一次性	40	合成废水 COD=9.09mg/L	COD：82.5%，UV₂₅₄去除率提高64%	过滤周期延长3倍膜表面有机物含量减少83.2%	[67]
PVDF中空纤维膜，膜孔径0.22μm	SRT=30d，HRT=2h 恒流过滤 J=20.02LMH	每天	2	湖水 COD＝7.31mg/L	COD：52.04%，TOC和UV₂₅₄去除率提高2.1和2.3倍	R_c降低47% R_irr降低20.4%	[69]
尼龙滤网，膜孔径30μm	HRT=7d，DO=2~4 mg/L 曝气速率=2.6~ 4.5L/min	31.9μm 一次性	2	酒精蒸馏废水 COD=（29.20~48.26）g/L	COD：41%，COD去除率提高1.5倍	临界通量提高近23% 无膜更换和清洗下的过滤时间延长8d	[71]
聚乙烯亲水膜，膜孔径0.1μm	HRT=2.4h 曝气强度 1000L/(m³·min) 恒流过滤速率=320m/d	— 一次性	40	经沉淀处理后的河水 TOC=（2.35±0.25）mg/L	TOC：71%，多糖和蛋白质去除率提高4.3%和2.2%~4.5%	50d内，TMP从初始值增加到50kPa的过滤周期减少25%	[70]
聚乙烯亲水膜，膜孔径0.1μm	HRT=2.4h 曝气强度 1000L/(m³·min) 恒流过滤速率=320m/d	— 一次性	40	生物过滤后的出水 TOC=（2.10±0.38）mg/L	TOC：66%，蛋白质去除率提高6.2%~6.7%	50d内，TMP从初始值增加到50kPa的过滤周期减少50%	[70]
微滤膜	HRT=2h 曝气强度=0.25m³/h 恒流过滤 J=16.6LMH	— 一次性	5	模拟微污染地表水 DOC=5.4~6.1mg/L	DOC：35%，UV₂₅₄去除率提高66.7%	TMP达到50kPa时的水通量为19LMH	[72]
			25		DOC：50%，UV₂₅₄去除率提高1.3倍	TMP达到50kPa时的水通量为18LMH
			50		DOC：75%，UV₂₅₄去除率提高1.8倍	TMP达到50kPa时的水通量为15.5LMH
			75		DOC：80%，UV₂₅₄去除率提高2倍	TMP达到50 kPa时的水通量为13LMH
聚醚酰亚胺中空纤维膜，膜孔径0.5μm	HRT=9.5h 曝气强度=0.5m³/h	定期	10	漂白浆厂废水 COD=1125mg/L	COD：88%	水通量提高60% 过滤阻力降低50%	[73]
PVDF中空纤维膜，膜孔径0.2μm	DO=2~4mg/L 恒流过滤 J=15LMH	定期	2	合成废水 COD=44g/L	COD：（97±2）%	过滤周期延长9.7%~51.2% 过滤阻力降低0.8%~45.3%	[74]

膜材料、形式与孔径	操作条件	PAC投加方式	PAC投加量 /g·L^-1	被处理废水类型	废水COD 含量/mg·L^-1	COD去除效率/%	膜污染控制效果	参考文献
PVDF板式膜，膜孔径0.1μm	HRT=3.3h 曝气强度=6m³/h 恒压过滤TMP=0.1MPa	一次性	1	微污染地表水	2.91	38.1	运行第30d的水通量提高10.5%	[75]
			2	微污染地表水	2.86	61.3	运行第30d的水通量提高5.3%
			3	微污染地表水	3.03	26	运行第30d的水通量降低15.3%
聚乙烯中空纤维膜，膜孔径0.4μm	HRT=100h 曝气强度=4m³/h	一次性	1.5	皮革厂废水	4051	81.6	膜污染速率降低，碱洗后TMP降低42.9%，酸清后TMP降低5%	[76]
聚乙烯中空纤维膜，膜孔径0.4μm	HRT=100h 曝气强度=4m³/h	一次性	3	皮革厂废水	4051	79.5	膜污染速率降低，碱洗后TMP降低60%，酸清后TMP降低40%	[76]
聚氯乙烯中空纤维膜，膜孔径10nm	HRT=20min 恒流过滤 J=20LMH	定期	0.003	微污染水	1.92±0.84	24.8	运行35d后的TMP降低13%	[77]
聚醚砜平板膜，膜孔径150kDa	HRT=20h 曝气强度=20m³/h 恒流过滤 J=300L/h	定期	0.5	果汁加工厂废水	4004±698	－	膜污染速率降低65.9%	[78]