基于导电材料强化抗生素胁迫厌氧消化的研究进展

doi:10.16085/j.issn.1000-6613.2022-0707

摘要/Abstract

摘要：

厌氧消化是处理含抗生素有机废物的常用技术手段，但高浓度抗生素会抑制厌氧微生物菌群活性，从而干扰厌氧消化效能和抗生素自身降解效率。近年来，导电材料强化含抗生素有机废物厌氧消化取得了良好效果，有机废物资源回收效率得到进一步提升。本文从抗生素使用现状和对厌氧消化代谢过程的影响出发，讨论了抗生素在厌氧消化中的迁移转化机制，重点阐述了铁基和碳基导电材料在抗生素胁迫厌氧消化系统中的应用及生化作用机理。研究表明：通过富集功能性微生物、强化微生物种间电子传递以及削减厌氧消化系统中的抗生素和抗生素抗性基因，导电材料可以提升厌氧消化产甲烷效能、降低抗生素污染的环境风险。最后，从构建生物信息网络、开发优化新型材料和处理多元污染物方面对导电材料强化技术的发展方向进行了展望。

关键词: 厌氧消化, 抗生素, 导电材料, 种间电子传递, 产甲烷菌

Abstract:

Anaerobic digestion (AD) is a conventional technique in antibiotic organic waste treatment. However, high concentration of antibiotics might threaten the activity of microbial community, thus weakening the anaerobic digestion performance and antibiotics degradation. In recent years, anaerobic digestion of organic waste containing antibiotics via conductive materials (CM) addition has been enhanced, and the efficiency of organic resources recovery has been further improved. Based on the current consumption of antibiotic and their effects on AD progress, the review analyzed the antibiotics removal mechanism in AD, and especially emphasized the application and mechanism of iron-based and carbon-based materials on improving antibiotic-stressed AD performance. The results indicated that CM could improve the performance of AD and reduce environmental risks by enhancing interspecies electron transfer, enriching functional microorganisms, and decreasing antibiotics and antibiotic resistance genes in the AD system. Finally, the future directions of conductive materials strengthening technology were discussed from the construction of biological information network, the development and optimization of new material, and the application in multi-pollutant treatment.

Key words: anaerobic digestion, antibiotic, conductive materials, direct interspecies electron transfer, methanogens

中图分类号:

祝佳欣, 朱雯喆, 徐俊, 谢靖, 王文标, 谢丽. 基于导电材料强化抗生素胁迫厌氧消化的研究进展[J]. 化工进展, 2023, 42(2): 1008-1019.

ZHU Jiaxin, ZHU Wenzhe, XU Jun, XIE Jing, WANG Wenbiao, XIE Li. Enhancement of anaerobic digestion under antibiotics stress via conductive materials application: A review[J]. Chemical Industry and Engineering Progress, 2023, 42(2): 1008-1019.

图/表 6

表1 常见抗生素的分类、结构特点、抗菌机理及用途[2, 8-10, 16-19]

抗生种类		结构特点	抗菌机理	主要用途
抗生种类		结构特点	抗菌机理	临床	养殖	农业
β-内酰胺类
	青霉素	含有β-内酯胺环	抑制细胞壁中黏肽合成酶，对动物毒性低	√	√
	头孢菌素	含有β-内酯胺环	抑制细胞壁中黏肽合成酶，对动物毒性低	√	√
四环素类
	金霉素	具有并四苯基	抑制蛋白质合成，阻断肽链的延长	√	√
	土霉素			√	√	√
	强力霉素			√	√
	四环素			√	√
喹诺酮类
	环丙沙星	具有相似4-喹诺酮母核	抑制细菌DNA旋转酶或拓扑异构酶活性	√
	诺氟沙星			√	√
	恩诺沙星			√	√
	氧氟沙星			√
大环内酯类
	阿奇霉素	具有不少于12个碳原子的内酯环	核糖体水平上抑制细菌蛋白质合成	√	√
	红霉素			√	√
	克拉霉素			√
	罗红霉素			√	√
磺胺类
	磺胺嘧啶	具有对氨基苯磺酰胺结构	阻止细菌的二氢叶酸合成	√	√
	磺胺甲𫫇唑			√	√
	磺胺甲嘧啶			√	√
	磺胺二甲嘧啶			√	√
林可酰胺类
	林可霉素	含有氨基酸和糖苷部分，并通过肽键相连	与50S核糖体亚基结合，阻止原核翻译	√	√
	克林霉素	含有氨基酸和糖苷部分，并通过肽键相连	与50S核糖体亚基结合，阻止原核翻译	√
多肽类
	黏杆菌素	由肽键将各氨基酸结合成锁链状	抑制细菌的生长和繁殖	√	√
	杆菌肽	由肽键将各氨基酸结合成锁链状	抑制细菌的生长和繁殖	√	√
酰胺醇类
	氯霉素	由对硝基苯基、丙二醇与二氯乙酰胺组成	抑制细菌70S核糖体与50S亚基结合及肽酰基转移酶和肽链延伸，干扰蛋白质合成	√	√
	甲砜霉素	由对硝基苯基、丙二醇与二氯乙酰胺组成	抑制细菌70S核糖体与50S亚基结合及肽酰基转移酶和肽链延伸，干扰蛋白质合成		√
氨基糖苷类
	链霉素	由氨基糖与氨基环醇组成	抑制蛋白质合成，对厌氧菌不具有抗菌作用	√		√
	卡那霉素			√
	庆大霉素			√	√
	新霉素			√	√

图1 抗生素厌氧消化文献统计分析图（2001年至今）

表2 抗生素对厌氧消化效能的影响

种类		浓度	底物	甲烷产量/%	挥发性脂肪酸变化情况	微生物相对丰度变化	参考文献
四环素类
	四环素	20mg/L	合成废水	-31.3	丙酸累积浓度260mg/L	Porphyromonas pogonae^③(+5.6%)、 Proteiniphilum acetatigenes^③(+0.3%)、 Syntrophobacter wolinii^④(-0.09%)、 Methanomassiliicoccus^⑥(+0.1%)	[26]
	金霉素	28mg/L	猪粪	-27.8	TVFA^①产量+88.8%	Methanosaetaceae^⑤、 Methanosarcinaceae spp.^⑦减少	[36]
	氯四环素	40mg/L	丁酸钠	-40.4	丁酸降解速率-44.2%	Syntrophomonas^④表现出耐受性、Tepidanaerobacter^④被抑制	[37]
大环内酯类
	红霉素	25mg/L	污泥	-40.6	乙酸、丙酸和丁酸分别累积0.9倍、0.3倍和2.5倍	—^②	[28]
	红霉素	500mg/L	红霉素	+13.0	—	Sedimentibacter^③(+33%)、 Methanosarcina^⑦(+2800%)	[30]
	克拉霉素	1000mg/ kg TSS	污泥	—	乙酸、丙酸和丁酸降解速率分别减少-28.0%、9.3%和-15.5%	水解发酵菌+0.64%、 Gammaproteobacteria^④(-2.1%)	[38]
林可酰胺类
	林可霉素(LCM)	25mg/L	污泥	-29.4	丁酸累积6.2倍	—	[28]
	林可霉素(LCM)	1000mg/L	葡萄糖	+20.8	LCM浓度≥200mg/L，乙酸和丙酸显着积累	—	[29]
磺胺类
	磺胺甲𫫇唑(SMX)	25mg/L	短链脂肪酸	-35.8	当SMX由250mg/L增加到1000mg/L，丙酸和丁酸利用率分别减少41.0%和30.3%	—	[34]
	磺胺二甲嘧啶	500mg/kg	污泥	+5.0～9.1	—	Methanosaetaceae^⑤(-9.6%)、Methanosarcinaceae^⑦(-19.0%)	[27]
喹诺酮类
	环丙沙星（CIP）	0.5~50mg/L	葡萄糖、肉提取物、蛋白胨	-4.8~32.0	50mg/L CIP出现丙酸积累	Syntrophobacter^④、Methanosaeta^⑤减少	[39]
	诺氟沙星	0.5mmol/L	—	-77.4	理论总挥发性脂肪酸(TVFA) -61.2%	Methanosaeta^⑤(-22.7%)、 Methanobacterium^⑥(-1.3%)、 Methanoculleus^⑥(+10.4%)	[40]
	诺氟沙星	500mg/kg	污泥	-11.3	—	Methanosaetaceae^⑤(-9.4%)、 Methanosarcinaceae^⑦(-39.9%)	[27]
	恩诺沙星	8mg/kg TS	鸡粪	+15.3	TVFA+5.9%	Methanosaeta^⑤(-12.6%)、 Methanobrevibacter^⑥(+48.6%)	[41]

表3 导电材料强化抗生素厌氧消化效能

材料	基质	投加量	甲烷产量	初始抗生素浓度	抗生素去除率	参考文献
零价铁	污泥	0.8g/L 1g/L 1.2g/L	+20.2% +80.9% +47.3%	20μg/L^①	磺胺甲𫫇唑：+21.1% 磺胺嘧啶：+56.0%	[56]
零价铁	猪粪	15g/L	+4.7%（37℃） +3.9%（55℃）	—^②	抗生素抗性基因（ARGs）还原+33.3%（37℃）	[11]
纳米零价铁	葡萄糖	Fe∶VS=0.5	+441.0%	80mg/L	四环素：+3.7%	[57]
纳米零价铁	模拟废水	1g/L	+200%以上	50mg/L	氯霉素：+52.7%	[58]
纳米零价铁（NZVI）+ 活性炭（AC）	模拟废水	1.06g NZVI/L、1.24g AC/L	—	100mg/L	环丙沙星：+5.0%	[59]
磁铁矿	葡萄糖	0.1~5g/L	+15.7%～28.9%	100mg/L	四环素：+6.3%～40.4%	[60]
纳米磁铁矿	污泥	20mmol/L	—	50mg/L	环丙沙星+35%～77%	[61]
碳纳米管	乙醇	0.1g/L	产率-3.8%	1mmol/L	环丙沙星：+2%	[48]
生物炭	养殖废水	0.5g/L	—	100μg/L^②	磺胺甲𫫇唑：+28.8%～33.1%；磺胺嘧啶：+39.4%～61.2%；磺胺二甲嘧啶：+44.4%～61.2%	[62]
石墨烯气凝胶	氯霉素	0.5g/L	—	50mg/L	氯霉素：+51.6%^③	[63]

表4 厌氧消化中与铁有关的反应

反应式	ΔG/kJ·mol^-1	参考文献
$8 H + + 4 F e 0 + C O 2 → C H 4 + 4 F e 2 + + 2 H 2 O$	-136	[69]
$F e 0 + 2 H 2 O → H 2 + F e 2 + + 2 O H -$	-5.02	[70]
$4 F e 0 + 8 H + → 4 F e 2 + + 4 H 2$	+3.5	[71]
$4 H 2 + C O 2 → C H 4 + 2 H 2 O$	-139	[71]
$8 F e 2 + + C O 2 + 8 H + → 8 F e 3 + + C H 4 + 2 H 2 O$	+774	[71]

表4 厌氧消化中与铁有关的反应

反应式	ΔG/kJ·mol^-1	参考文献
$8 H + + 4 F e 0 + C O 2 → C H 4 + 4 F e 2 + + 2 H 2 O$	-136	[69]
$F e 0 + 2 H 2 O → H 2 + F e 2 + + 2 O H -$	-5.02	[70]
$4 F e 0 + 8 H + → 4 F e 2 + + 4 H 2$	+3.5	[71]
$4 H 2 + C O 2 → C H 4 + 2 H 2 O$	-139	[71]
$8 F e 2 + + C O 2 + 8 H + → 8 F e 3 + + C H 4 + 2 H 2 O$	+774	[71]

图2 导电材料强化抗生素胁迫厌氧消化的作用机理

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