腐殖酸含量对污泥厌氧发酵过程产CH_4效率的影响
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摘要
污泥中含有的HA(腐殖酸)会对厌氧发酵过程产生影响.为探究ρ(HA)对厌氧发酵产CH_4效率的影响规律,开展了ρ(HA)为0、200、300和400 mg/L(依次记为T0、T1、T2、T3处理)的中温厌氧发酵模拟试验,检测和分析了φ(CH_4)、累计CH_4产量与产生动力学特征,以及ρ(HA)与累计CH_4产量之间的相关性.结果表明:各处理发酵过程的pH在6. 9～7. 9之间变化,并且HA对pH变化具有减缓作用; T1处理的φ(CH_4)峰值为66. 7%,高于T0处理的61. 5%,但随着ρ(HA)的进一步增加,φ(CH_4)峰值逐渐下降为62. 0%(T2处理)和60. 0%(T3处理);采用修正Gompertz方程对累计CH_4产量的拟合结果表明,HA对厌氧发酵的产CH_4潜能呈抑制作用,且随ρ(HA)的增加,该抑制作用更加明显,T0、T1、T2和T3处理的最大累计CH_4产量分别为441. 1、432. 1、397. 1和253. 5 m L;相关性分析结果显示,ρ(HA)与累计CH_4产量呈负相关,随着ρ(HA)的增加,累计CH_4产量逐渐降低.研究显示,HA对污泥厌氧发酵产CH_4过程呈抑制作用,ρ(HA)较低时可提高沼气中的φ(CH_4)峰值.
Humic acid(HA) in the sludge affects the anaerobic fermentation process. In order to investigate the effect of HA content on the methanogenic efficiency of anaerobic fermentation,mesophilic anaerobic fermentation tests of HA content 0,200,300,400 mg/L(recorded as T0,T1,T2,T3 systems) were conducted. The methane content,cumulative methane yield and production dynamics,as well as the correlation between methane yield and HA content were analyzed. The results showed that the pH in anaerobic fermentation systems with HA changed from 6. 9 to 7. 9. HA had buffering function on the change of pH value. The peak of methane content in T1 treatment was 66. 7%,which was higher than 61. 5% of T0. However,with the increase of HA content,the peak of methane content decreased to 62. 0%(T2 system) and 60. 0%(T3 system). The modified Gompertz equation was used to fit the cumulative methane yield and the results showed that HA inhibited the theoretical methane production of anaerobic fermentation. The inhibition efficiency was more significant with increasing HA,and the theoretical methanogenic potential of T0,T1,T2 and T3 systems were 441. 1,432. 1,397. 1 and253. 5 m L,respectively. The correlation analysis showed that the HA content and cumulative methane yield were negatively correlated. The cumulative methane yield gradually decreased with increasing HA. Therefore,HA inhibited methane production during sludge anaerobic fermentation,and the peak of methane content in the biogas increased when the HA content was low.
Humic acid(HA) in the sludge affects the anaerobic fermentation process. In order to investigate the effect of HA content on the methanogenic efficiency of anaerobic fermentation,mesophilic anaerobic fermentation tests of HA content 0,200,300,400 mg/L(recorded as T0,T1,T2,T3 systems) were conducted. The methane content,cumulative methane yield and production dynamics,as well as the correlation between methane yield and HA content were analyzed. The results showed that the pH in anaerobic fermentation systems with HA changed from 6. 9 to 7. 9. HA had buffering function on the change of pH value. The peak of methane content in T1 treatment was 66. 7%,which was higher than 61. 5% of T0. However,with the increase of HA content,the peak of methane content decreased to 62. 0%(T2 system) and 60. 0%(T3 system). The modified Gompertz equation was used to fit the cumulative methane yield and the results showed that HA inhibited the theoretical methane production of anaerobic fermentation. The inhibition efficiency was more significant with increasing HA,and the theoretical methanogenic potential of T0,T1,T2 and T3 systems were 441. 1,432. 1,397. 1 and253. 5 m L,respectively. The correlation analysis showed that the HA content and cumulative methane yield were negatively correlated. The cumulative methane yield gradually decreased with increasing HA. Therefore,HA inhibited methane production during sludge anaerobic fermentation,and the peak of methane content in the biogas increased when the HA content was low.
引文
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[5]张仙梅,云斯宁,杜玉凤,等.微晶化磷钾矿粉催化牛粪厌氧消化试验[J].农业机械学报,2016,47(5):183-190.ZHANG Xianmei,YUN Sining,DU Yufeng,et al. Application of microcrystalline phosphate or potassium powder in anaerobic digestion of cattle manure as functional catalysts[J].Transactions of the Chinese Society for Agricultural Machinery,2016,47(5):183-190.
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[8] ZHANG Wanli,XING Wanli,LI Rundong. Real-time recovery strategies for volatile fatty acid-inhibited anaerobic digestion of food waste for methane production[J]. Bioresource Technology,2018,265:82-92.
[9] YANG Yuning,LI Huan,LI Jinyi. Variation in humic and fulvic acids during thermal sludge treatment assessed by size fractionation,elementary analysis,and spectroscopic methods[J].Frontiers of Environmental Science&Engineering,2014,8(6):854-862.
[10]郝晓地,周鹏,曹亚莉.污水处理中腐殖质的来源及其演变过程[J].环境工程学报,2017,11(1):1-11.HAO Xiaodi,ZHOU Peng,CAO Yali. Origins and evolution processes of humic substances in wastewater treatment[J].Chinese Journal of Environmental Engineering,2017,11(1):1-11.
[11] AKIO I,TAKEHIKO F,KAZUO M,et al. Characterization of dissolved organic matter in effluents from wastewater treatment plants[J].Water Research,2002,36(4):859-870.
[12] POLAK J,BARTOSZEK M,SUKOWSKI W W. Comparison of some spectroscopic and physico-chemical properties of humic acids extracted from sewage sludge and bottom sediments[J]. Journal of Molecular Structure,2009,924:309-312.
[13] JASONK K,PAMELAB W,JPATRICK M.Humic acids as electron acceptors in wetland decomposition[J]. Soil Biology&Biochemistry,2009,41(7):1518-1522.
[14] YAP S D,ASTALS S,LU Y,et al. Humic acid inhibition of hydrolysis and methanogenesis with different anaerobic inocula[J].Waste Management,2018,80:130-136.
[15] LI Huan,LI Youkang,JIN Yiying,ZOU Shuxin.Recovery of sludge humic acids with alkaline pretreatment and its impact on subsequent anaerobic digestion[J].Journal of Chemical Technology&Biotechnology,2014,89(5):707-713.
[16] GARCIA-MINA J M. Stability,solubility and maximum metal binding capacity in metal-humic complexes involving humic substances extracted from peat and organic compost[J]. Organic Geochemistry,2006,37(12):1960-1972.
[17]李东阳,杨天学,吴明红,等.腐殖酸强化六氯苯厌氧降解规律及其中间产物[J].环境科学研究,2016,29(6):870-876.LI Dongyang,YANG Tianxue,WU Minghong,et al. Anaerobic degradation regulation of hexachlorobenzene and degradation products enhanced by humic acid[J]. Research of Environmental Sciences,2016,29(6):870-876.
[18]麻微微.沼气发酵复合菌系厌氧发酵特性及微生物群落结构分析[D].哈尔滨:哈尔滨工业大学,2015.
[19] BENBELKACEM H,BAYARD R,ABDELHAY A,et al. Effect of leachate injection modes on municipal solid waste degradation in anaerobic bioreactor[J]. Bioresource Technology,2010,101(14):5206-5212.
[20]李定龙,戴肖云,赵宋敏,等.pH对厨余垃圾厌氧发酵产酸的影响[J].环境科学与技术,2011,34(4):125-128.LI Dinglong,DAI Xiaoyun,ZHAO Songmin,et al. Influence of p H on acidity during anaerobic fermentation of kitchen waste[J].Environmental Science&Technology(China),2011,34(4):125-128.
[21]王艳琴,张洁,刘月娥,等.初始p H值对餐厨垃圾高温高含固率厌氧发酵产酸的影响[J].桂林理工大学学报,2016,36(3):562-566.WANG Yanqin,ZHANG Jie,LIU Yue'e,et al. Initial pH effect on volatile fatty acid production in anaerobic fermentation from highsolid food waste under thermophilic condition[J].Journal of Guilin University of Technology,2016,36(3):562-566.
[22]倪海亮,李勇,顾广发,等.污水厂污泥与餐厨垃圾共消化产甲烷特性的研究进展[J].环境工程,2014(11):113-117.NI Hailiang,LI Yong,GU Guangfa,et al. Progress in methane production characteristics of sewage sludge and food waste codigestion[J].Environmental Engineering,2014(11):113-117.
[23] YANG Tianxue,LI Yingjun,GAO Jixi,et al. Performance of dry anaerobic technology in the co-digestion of rural organic solid wastes in China[J].Energy,2015,93:2497-2502.
[24] ZHANG B,ZHANG L L,ZHANG S C,et al.The influence of p H on hydrolysis and acidogenesis of kitchen wastes in two-phase anaerobic digestion[J].Environmental Technology Letters,2005,26(3):329-339.
[25] LARA-CISNEROS G,AGUILAR-L'OPEZ R,FEMAT R. On the dynamic optimization of methane production in anaerobic digestion via extremum-seeking control approach[J]. Computers&Chemical Engineering,2015,75:49-59.
[26] DOS SANTOS A B,De MADRID M P,STAMS A J,et al.Azo dye reduction by mesophilic and thermophilic anaerobic consortia[J].Biotechnology Progress,2005,21(4):1140-1145.
[27] CERVANTES F J,BOK F A M D,DUONG-DAC T,et al.Reduction of humic substances by halorespiring,sulphate-reducing and methanogenic microorganisms[J]. Environmental Microbiology,2002,4(1):51-57.
[28] WANG Meng,LEE E,DILBECK M P,et al.Thermal pretreatment of microalgae for biomethane production:experimental studies,kinetics and energy analysis[J].Journal of Chemical Technology&Biotechnology,2016,92(2):399-407.
[29]金杰,俞志敏,吴克,等.城市食品废弃物高固体含量厌氧消化过程[J].包装与食品机械,2008,26(5):41-45.JIN Jie,YU Zhimin,WU Ke,et al. Process of high solid concentration anaerobic fermentation for the municipal biological waste[J].Packaging and Food Machinery,2008,26(5):41-45.
[30] LI Yan,TAN Wenfeng,KOOPAL L K,et al.Influence of soil humic and fulvic acid on the activity and stability of lysozyme and urease[J]. Environmental Science&Technology,2013,47(10):5050-5056.
[31]方少辉,席北斗,杨天学,等.农村混合物料干式厌氧发酵物性变化中试研究[J].环境科学研究,2012,25(9):1005-1010.FANG Shaohui,XI Beidou,YANG Tianxue,et al. Pilot study on dry-anaerobic digestion of rural organic solid waste[J].Research of Environmental Sciences,2012,25(9):1005-1010.
[32]肖天,席北斗,杨天学,等.腐殖酸强化六氯苯还原脱氯的作用规律[J].环境科学研究,2017,30(5):792-798.XIAO Tian,XI Beidou,YANG Tianxue,et al. Dechlorination of hexachlorobenzene enhanced by humic acid[J]. Research of Environmental Sciences,2017,30(5):792-798.
[33]宋佳秀,任南琪,钱东旭,等.醌呼吸影响厌氧消化产CO2/CH4及转化有毒物质的研究[J].中国环境科学,2014,34(5):1236-1241.SONG Jiaxiu,REN Nanqi,QIAN Dongxu,et al. The effect of quinone respiration on CO2/CH4production and transformation of toxic substances in anaerobic digestion[J]. China Environmental Science,2014,34(5):1236-1241.
[34]陈斌,杨天学,耿向永,等.玉米秸秆干式厌氧发酵乙酸产生规律及其对发酵的影响[J].环境科学研究,2015,28(4):647-652.CHEN Bin,YANG Tianxue,GENG Xiangyong,et al. Effects of acetic acid production on dry fermentation systems with corn stalk[J].Research of Environmental Sciences,2015,28(4):647-652.
[35] AZMAN S,KHADEM A F,PLUGGE C M,et al. Effect of humic acid on anaerobic digestion of cellulose and xylan in completely stirred tank reactors:inhibitory effect,mitigation of the inhibition and the dynamics of the microbial communities[J]. Applied Microbiology&Biotechnology,2017,101(2):889-901.
[2]姜玲玲,孙荪.我国污泥处理处置现状及发展趋势分析[J].环境卫生工程,2015,23(3):13-14.JIANG Lingling,SUN Sun. Status and development of sludge treatment and disposal in China[J]. Environment Sanitation Engineering,2015,23(3):13-14.
[3]杜婷婷,云斯宁,朱江,等.生物质废弃物厌氧发酵的研究进展[J].中国沼气,2016(2):46-52.DU Tingting,YUN Sining,ZHU Jiang,et al. Research progress of anaerobic fermentation of different biomass waste[J]. China Biogas,2016(2):46-52.
[4]于美玲,于洋,董晓莹,等.城市有机垃圾厌氧干发酵菌群与代谢产物特性研究[J].中国沼气,2015,33(6):14-18.YU Meiling,YU Yang,DONG Xiaoying,et al. Characteristics of microbial community and metabolites in municipal organic waste dry anaerobic fermentation[J].China Biogas,2015,33(6):14-18.
[5]张仙梅,云斯宁,杜玉凤,等.微晶化磷钾矿粉催化牛粪厌氧消化试验[J].农业机械学报,2016,47(5):183-190.ZHANG Xianmei,YUN Sining,DU Yufeng,et al. Application of microcrystalline phosphate or potassium powder in anaerobic digestion of cattle manure as functional catalysts[J].Transactions of the Chinese Society for Agricultural Machinery,2016,47(5):183-190.
[6] LANGERAK E P A V,BEEKMANS M M H,BEUN J J,et al.Influence of phosphate and iron on the extent of calcium carbonate precipitation during anaerobic digestion[J]. Journal of Chemical Technology&Biotechnology,2015,74(11):1030-1036.
[7] KANOUNI A E,ZERDANI I,ZAAFA S,et al.The improvement of glucose/xylose fermentation by Clostridium acetobutylicum using calcium carbonate[J]. World Journal of Microbiology&Biotechnology,1998,14(3):431-435.
[8] ZHANG Wanli,XING Wanli,LI Rundong. Real-time recovery strategies for volatile fatty acid-inhibited anaerobic digestion of food waste for methane production[J]. Bioresource Technology,2018,265:82-92.
[9] YANG Yuning,LI Huan,LI Jinyi. Variation in humic and fulvic acids during thermal sludge treatment assessed by size fractionation,elementary analysis,and spectroscopic methods[J].Frontiers of Environmental Science&Engineering,2014,8(6):854-862.
[10]郝晓地,周鹏,曹亚莉.污水处理中腐殖质的来源及其演变过程[J].环境工程学报,2017,11(1):1-11.HAO Xiaodi,ZHOU Peng,CAO Yali. Origins and evolution processes of humic substances in wastewater treatment[J].Chinese Journal of Environmental Engineering,2017,11(1):1-11.
[11] AKIO I,TAKEHIKO F,KAZUO M,et al. Characterization of dissolved organic matter in effluents from wastewater treatment plants[J].Water Research,2002,36(4):859-870.
[12] POLAK J,BARTOSZEK M,SUKOWSKI W W. Comparison of some spectroscopic and physico-chemical properties of humic acids extracted from sewage sludge and bottom sediments[J]. Journal of Molecular Structure,2009,924:309-312.
[13] JASONK K,PAMELAB W,JPATRICK M.Humic acids as electron acceptors in wetland decomposition[J]. Soil Biology&Biochemistry,2009,41(7):1518-1522.
[14] YAP S D,ASTALS S,LU Y,et al. Humic acid inhibition of hydrolysis and methanogenesis with different anaerobic inocula[J].Waste Management,2018,80:130-136.
[15] LI Huan,LI Youkang,JIN Yiying,ZOU Shuxin.Recovery of sludge humic acids with alkaline pretreatment and its impact on subsequent anaerobic digestion[J].Journal of Chemical Technology&Biotechnology,2014,89(5):707-713.
[16] GARCIA-MINA J M. Stability,solubility and maximum metal binding capacity in metal-humic complexes involving humic substances extracted from peat and organic compost[J]. Organic Geochemistry,2006,37(12):1960-1972.
[17]李东阳,杨天学,吴明红,等.腐殖酸强化六氯苯厌氧降解规律及其中间产物[J].环境科学研究,2016,29(6):870-876.LI Dongyang,YANG Tianxue,WU Minghong,et al. Anaerobic degradation regulation of hexachlorobenzene and degradation products enhanced by humic acid[J]. Research of Environmental Sciences,2016,29(6):870-876.
[18]麻微微.沼气发酵复合菌系厌氧发酵特性及微生物群落结构分析[D].哈尔滨:哈尔滨工业大学,2015.
[19] BENBELKACEM H,BAYARD R,ABDELHAY A,et al. Effect of leachate injection modes on municipal solid waste degradation in anaerobic bioreactor[J]. Bioresource Technology,2010,101(14):5206-5212.
[20]李定龙,戴肖云,赵宋敏,等.pH对厨余垃圾厌氧发酵产酸的影响[J].环境科学与技术,2011,34(4):125-128.LI Dinglong,DAI Xiaoyun,ZHAO Songmin,et al. Influence of p H on acidity during anaerobic fermentation of kitchen waste[J].Environmental Science&Technology(China),2011,34(4):125-128.
[21]王艳琴,张洁,刘月娥,等.初始p H值对餐厨垃圾高温高含固率厌氧发酵产酸的影响[J].桂林理工大学学报,2016,36(3):562-566.WANG Yanqin,ZHANG Jie,LIU Yue'e,et al. Initial pH effect on volatile fatty acid production in anaerobic fermentation from highsolid food waste under thermophilic condition[J].Journal of Guilin University of Technology,2016,36(3):562-566.
[22]倪海亮,李勇,顾广发,等.污水厂污泥与餐厨垃圾共消化产甲烷特性的研究进展[J].环境工程,2014(11):113-117.NI Hailiang,LI Yong,GU Guangfa,et al. Progress in methane production characteristics of sewage sludge and food waste codigestion[J].Environmental Engineering,2014(11):113-117.
[23] YANG Tianxue,LI Yingjun,GAO Jixi,et al. Performance of dry anaerobic technology in the co-digestion of rural organic solid wastes in China[J].Energy,2015,93:2497-2502.
[24] ZHANG B,ZHANG L L,ZHANG S C,et al.The influence of p H on hydrolysis and acidogenesis of kitchen wastes in two-phase anaerobic digestion[J].Environmental Technology Letters,2005,26(3):329-339.
[25] LARA-CISNEROS G,AGUILAR-L'OPEZ R,FEMAT R. On the dynamic optimization of methane production in anaerobic digestion via extremum-seeking control approach[J]. Computers&Chemical Engineering,2015,75:49-59.
[26] DOS SANTOS A B,De MADRID M P,STAMS A J,et al.Azo dye reduction by mesophilic and thermophilic anaerobic consortia[J].Biotechnology Progress,2005,21(4):1140-1145.
[27] CERVANTES F J,BOK F A M D,DUONG-DAC T,et al.Reduction of humic substances by halorespiring,sulphate-reducing and methanogenic microorganisms[J]. Environmental Microbiology,2002,4(1):51-57.
[28] WANG Meng,LEE E,DILBECK M P,et al.Thermal pretreatment of microalgae for biomethane production:experimental studies,kinetics and energy analysis[J].Journal of Chemical Technology&Biotechnology,2016,92(2):399-407.
[29]金杰,俞志敏,吴克,等.城市食品废弃物高固体含量厌氧消化过程[J].包装与食品机械,2008,26(5):41-45.JIN Jie,YU Zhimin,WU Ke,et al. Process of high solid concentration anaerobic fermentation for the municipal biological waste[J].Packaging and Food Machinery,2008,26(5):41-45.
[30] LI Yan,TAN Wenfeng,KOOPAL L K,et al.Influence of soil humic and fulvic acid on the activity and stability of lysozyme and urease[J]. Environmental Science&Technology,2013,47(10):5050-5056.
[31]方少辉,席北斗,杨天学,等.农村混合物料干式厌氧发酵物性变化中试研究[J].环境科学研究,2012,25(9):1005-1010.FANG Shaohui,XI Beidou,YANG Tianxue,et al. Pilot study on dry-anaerobic digestion of rural organic solid waste[J].Research of Environmental Sciences,2012,25(9):1005-1010.
[32]肖天,席北斗,杨天学,等.腐殖酸强化六氯苯还原脱氯的作用规律[J].环境科学研究,2017,30(5):792-798.XIAO Tian,XI Beidou,YANG Tianxue,et al. Dechlorination of hexachlorobenzene enhanced by humic acid[J]. Research of Environmental Sciences,2017,30(5):792-798.
[33]宋佳秀,任南琪,钱东旭,等.醌呼吸影响厌氧消化产CO2/CH4及转化有毒物质的研究[J].中国环境科学,2014,34(5):1236-1241.SONG Jiaxiu,REN Nanqi,QIAN Dongxu,et al. The effect of quinone respiration on CO2/CH4production and transformation of toxic substances in anaerobic digestion[J]. China Environmental Science,2014,34(5):1236-1241.
[34]陈斌,杨天学,耿向永,等.玉米秸秆干式厌氧发酵乙酸产生规律及其对发酵的影响[J].环境科学研究,2015,28(4):647-652.CHEN Bin,YANG Tianxue,GENG Xiangyong,et al. Effects of acetic acid production on dry fermentation systems with corn stalk[J].Research of Environmental Sciences,2015,28(4):647-652.
[35] AZMAN S,KHADEM A F,PLUGGE C M,et al. Effect of humic acid on anaerobic digestion of cellulose and xylan in completely stirred tank reactors:inhibitory effect,mitigation of the inhibition and the dynamics of the microbial communities[J]. Applied Microbiology&Biotechnology,2017,101(2):889-901.
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