3种晶种对鸟粪石沉淀法去除污泥上清液氮磷的影响

doi:10.19741/j.issn.1673-4831.2021.0397

摘要/Abstract

摘要： 将剩余污泥中的固态氮和磷转变为可溶性氮和磷,是剩余污泥中氮磷处理或资源化利用的关键。该文研究了pH值对剩余污泥中氮磷的释放效果及不同晶种(蛭石、椰壳炭和石英砂)对鸟粪石沉淀法去除氮磷的影响,另外考察了单独使用晶种以及晶种与镁盐协同处理对污泥上清液氮磷的去除效果的影响。结果表明,当剩余污泥上清液的pH值由7.45上升至12时,上清液中ρ(PO₄^3--P)从15.83上升至188.20 mg·L^-1,ρ(NH₄⁺-N)由48.97上升至166.46 mg·L^-1。在镁磷摩尔比为1.2、pH值为10、搅拌时间30 min、静置30 min条件下,蛭石、椰壳炭和石英砂的投加量分别为2、2和0.5 g·(100 mL)^-1时,3种晶种对上清液中NH₄⁺-N和PO₄^3--P的去除效果均较好。3种晶种中,椰壳炭诱导鸟粪石沉淀法去除NH₄⁺-N和PO₄^3--P的效果比蛭石和石英砂好。当椰壳炭投加量为2 g·(100 mL)^-1时,上清液中PO₄^3--P和NH₄⁺-N的去除率分别为82.48%和74.98%,相比未投加晶种分别提高9.14%和13.38%。采用X射线衍射和扫描电子显微镜对沉淀产物进行分析,发现生成的沉淀主要为鸟粪石,具有较高的回收价值。

关键词: 鸟粪石, 晶种, 污泥上清液, 氮磷

Abstract: Transforming nitrogen and phosphorus in sewage sludge from solid to dissolution is the key for the treatment or resource utilization of nitrogen and phosphorus. In this paper, the effects of pH value on the release of nitrogen and phosphorus from sewage sludge, and the effects of different crystal seeds (vermiculite, coconut-shell biochar and quartz sand) on the removal of nitrogen and phosphorus by struvite precipitation were studied. In addition, the effects of only crystal seeds and the co-treatment of crystal seeds and magnesium salts on removal efficiency of nitrogen and phosphorus in the supernatant of sewage sludge were also investigated. Results show that when the pH of the supernatant increased from 7.45 to 12, the concentration of phosphate (PO₄^3--P) in the supernatant increased from 15.83 to 188.20 mg·L^-1, and ammonia nitrogen (NH₄⁺-N) increased from 48.97 to 166.46 mg·L^-1. There is better removal efficiency of NH₄⁺-N and PO₄^3--P when n(Mg):n(P)=1.2, pH=10, followed by stirring and standing both for 30 min, then adding vermiculite, coconut shell biochar and quartz sand with 2, 2 and 0.5 g·(100 mL^-1), respectively. Among the three crystal seeds, the removal efficiency of NH₄⁺-N and PO₄^3--P was higher by coconut shell biochar than those by vermiculite and quartz sand based on struvite precipitation induction. Compared to non-addition of crystal seed, when adding coconut shell biochar with 2 g·(100 mL^-1), the removal rates of PO₄^3--P and NH₄⁺-N reached to 82.48% and 74.98% and increased by 9.14% and 13.38%, respectively. The results of X-ray diffraction and scanning electron microscopy (SEM) analysis show that the precipitates are mainly struvite which has high recovery value.

Key words: struvite, seed, sludge supernatant, nitrogen and phosphorus

中图分类号:

林海芝, 李映雪, 任静雯, 徐德福. 3种晶种对鸟粪石沉淀法去除污泥上清液氮磷的影响[J]. 生态与农村环境学报, 2022, 38(8): 1084-1092.

LIN Hai-zhi, LI Ying-xue, REN Jing-wen, XU De-fu. Effect of Three Crystal Species on the Removal of Nitrogen and Phosphorus from Sludge Supernatant by Struvite Precipitation[J]. Journal of Ecology and Rural Environment, 2022, 38(8): 1084-1092.

参考文献 40

[1]	陈思思,杨殿海,庞维海,等.我国剩余污泥厌氧转化的主要影响因素及影响机制研究进展[J].化工进展,2020,39(4):1511-1520.[CHEN Si-si,YANG Dian-hai,PANG Wei-hai,et al.Main Influencing Factors and Mechanisms of Anaerobic Transformation of Excess Sludge in China[J].Chemical Industry and Engineering Progress,2020,39(4):1511-1520.]
[2]	徐慧敏,秦卫华,李中林,等.双频超声改善剩余污泥的脱水性能研究[J].生态与农村环境学报,2018,34(4):380-384.[XU Hui-min,QIN Wei-hua,LI Zhong-lin,et al.Effects of Double Frequency Ultrasound Improving Dehydration Property of Waste Activated Sludge in Pretreatment[J].Journal of Ecology and Rural Environment,2018,34(4):380-384.]
[3]	宿翠霞,王龙波,李凌霄,等.城镇污水处理厂污泥处置与资源化利用[J].中国资源综合利用,2010,28(5):50-52.[SU Cui-xia,WANG Long-bo,LI Ling-xiao,et al.Sludge Handling and Reuse into Resources in Sewage Treatment Plant[J].China Resources Comprehensive Utilization,2010,28(5):50-52.]
[4]	周书征,郝丽君,兰轩花,等.污泥堆肥后处理系统初探[J].机电产品开发与创新,2013,26(1):56-58.[ZHOU Shu-zheng,HAO Li-jun,LAN Xuan-hua,et al.The Primary Study on Post-Treatment Process of Sludge Composting[J].Development&Innovation of Machinery&Electrical Products,2013,26(1):56-58.]
[5]	接伟光,彭轶,彭永臻,等.pH值对剩余污泥中氮、磷溶出及菌群组成的影响[J].中国给水排水,2014,30(17):22-25,31.[JIE Wei-guang,PENG Yi,PENG Yong-zhen,et al.Impact of pH on Dissolution of Nitrogen and Phosphorus and Community Composition of Excess Sludge[J].China Water&Wastewater,2014,30(17):22-25,31.]
[6]	DE-BASHAN L E,BASHAN Y.Recent Advances in Removing Phosphorus from Wastewater and Its Future Use as Fertilizer (1997-2003)[J].Water Research,2004,38(19):4222-4246.
[7]	吴健,平倩,李咏梅.鸟粪石结晶成粒技术回收污泥液中磷的中试研究[J].中国环境科学,2017,37(3):941-947.[WU Jian,PING Qian,LI Yong-mei.A Pilot-Scale Study on Struvite Pellet Crystallization for Phosphorus Recovery from Sludge Liquor[J].China Environmental Science,2017,37(3):941-947.]
[8]	RONTELTAP M,MAURER M,HAUSHER R R,et al.Struvite Precipitation from Urine-Influencing Factors on Particle Size[J].Water Research,2010,44(6):2038-2046.
[9]	畅萧,曾薇,王保贵,等.从剩余污泥厌氧发酵上清液中以鸟粪石形式回收磷[J].环境科学,2019,40(9):4169-4176.[CHANG Xiao,ZENG Wei,WANG Bao-gui,et al.Recovery of Phosphorus in the Form of Struvite from the Anaerobic Fermentation Supernatant of Excess Sludge[J].Environmental Science,2019,40(9):4169-4176.]
[10]	HUANG H M,YANG J,LI D.Recovery and Removal of Ammonia-Nitrogen and Phosphate from Swine Wastewater by Internal Recycling of Struvite Chlorination Product[J].Bioresource Technology,2014,172:253-259.
[11]	姚涛,蔡伟民,李龙海.磷酸铵镁法处理含氮磷废水研究进展[J].中国给水排水,2005,21(2):31-33.[YAO Tao,CAI Wei-min,LI Long-hai.Progress in the Study of Magnesium Ammonium Phosphate Process for Nitrogen-and Phosphorus-Containing Wastewater[J].China Water&Wastewater,2005,21(2):31-33.]
[12]	LE CORRE K S,VALSAMI-JONES E,HOBBS P,et al.Struvite Crystallisation and Recovery Using a Stainless Steel Structure as a Seed Material[J].Water Research,2007,41(11):2449-2456.
[13]	JANG H,KANG S H.Phosphorus Removal Using Cow Bone in Hydroxyapatite Crystallization[J].Water Research,2002,36(5):1324-1330.
[14]	商平,扈靖之,刘彦博,等.利用粉煤灰作晶种预处理垃圾渗滤液[J].天津科技大学学报,2014,29(4):67-71.[SHANG Ping,HU Jing-zhi,LIU Yan-bo,et al.Pretreatment of Landfill Leachate Using Fly Ash as Seed Crystal[J].Journal of Tianjin University of Science&Technology,2014,29(4):67-71.]
[15]	ELSER J,BENNETT E.A Broken Biogeochemical Cycle[J].Nature,2011,478(7367):29-31.
[16]	SONG W L,LI Z P,LIU F,et al.Effective Removal of Ammonia Nitrogen from Waste Seawater Using Crystal Seed Enhanced Struvite Precipitation Technology with Response Surface Methodology for Process Optimization[J].Environmental Science and Pollution Research International,2018,25(1):628-638.
[17]	ADDAGADA L.Enhanced Phosphate Recovery Using Crystal-Seed-Enhanced Struvite Precipitation:Process Optimization with Response Surface Methodology[J].Journal of Hazardous,Toxic,and Radioactive Waste,2020,24(4):246-279.
[18]	国家环境保护总局《水和废水监测分析方法》编委会.水和废水监测分析方法[M].4版.北京:中国环境科学出版社,2002:246-279.[State Environmental Protection Administration.Methods for Monitoring and Analysis of Water and Wastewater[M].4th ed.Beijing:China Environmental Science Press,2002:246-279.]
[19]	肖本益,刘俊新.污水处理系统剩余污泥碱处理融胞效果研究[J].环境科学,2006,27(2):319-323.[XIAO Ben-yi,LIU Jun-xin.Study on Treatment of Excess Sludge under Alkaline Condition[J].Environmental Science,2006,27(2):319-323.]
[20]	ZHUK R,FU H,ZHANG J H,et al.Studies on Removal of NH4+-N from Aqueous Solution by Using the Activated Carbons Derived from Rice Husk[J].Biomass and Bioenergy,2012,43:18-25.
[21]	王金丽,孙永利,郑华清,等.基于径流污染控制的生物滞留设施填料优化研究[J].中国给水排水,2020,36(1):110-116.[WANG Jin-li,SUN Yong-li,ZHENG Hua-qing,et al.Optimization of Bioretention Facility Filler Based on Runoff Pollution Control[J].China Water&Wastewater,2020,36(1):110-116.]
[22]	曹玉成,单胜道,张妙仙,等.膨胀蛭石同步脱铵除磷的影响因素研究[J].环境科学与技术,2009(11):32-36.[CAO Yu-cheng,SHAN Sheng-dao,ZHANG Miao-xian,et al.Influence Factors for Simultaneous Removal of Ammonium and Phosphate by Expanded Vermiculite[J].Environmental Science&Technology,2009(11):32-36.]
[23]	焦赟仪,郑利兵,魏源送,等.铁氧化物对活性炭处理尿液的影响[J].环境工程学报,2020(12):3381-3390.[JIAO Yun-yi,ZHENG Li-bing,WEI Yuan-song,et al.Effect of Iron Oxides on Urine Treatment by Activated Carbon[J].Chinese Journal of Environmental Engineering,2020(12):3381-3390.]
[24]	唐想.改性蔗渣生物质炭的制备及其吸附水中氨氮的研究[D].南宁:广西大学,2018.[TANG Xiang.The Modified Biochar Preparation and Adsorption of Ammonia-Nitrogen[D].Nanning:Guangxi University,2018.]
[25]	刘凌言,陈双荣,宋雪燕,等.生物炭吸附水中磷酸盐的研究进展[J].环境工程,2020,38(11):91-97.[LIU Ling-yan,CHEN Shuang-rong,SONG Xue-yan,et al.Research Progress in Removal of Phosphate from Water by Biochar[J].Environmental Engineering,2020,38(11):91-97.]
[26]	陶飞飞,田晴,李方,等.共存杂质对磷酸铵镁结晶法回收磷的影响研究[J].环境工程学报,2011,5(11):2437-2441.[TAO Fei-fei,TIAN Qing,LI Fang,et al.Effects of Coexisting Impurities on Phosphorus Recovery in Magnesium Ammonium Phosphate Crystallization[J].Chinese Journal of Environmental Engineering,2011,5(11):2437-2441.]
[27]	胡怡,宋永会,钱锋.赤泥晶种法诱导磷酸铵镁结晶回收模拟废水中磷的可行性研究[J].环境工程学报,2013,7(1):19-25.[HU Yi,SONG Yong-hui,QIAN Feng.Feasibility Study on Phosphate Recovery as Struvite from Synthetic Wastewater by Red Mud-Seeded Crystallization[J].Chinese Journal of Environmental Engineering,2013,7(1):19-25.]
[28]	MUHMOOD A,LU J X,KADAM R,et al.Biochar Seeding Promotes Struvite Formation,but Accelerates Heavy Metal Accumulation[J].Science of the Total Environment,2019,652:623-632.
[29]	GUAN Q,ZENG G S,SONG J T,et al.Ultrasonic Power Combined with Seed Materials for Recovery of Phosphorus from Swine Wastewater via Struvite Crystallization Process[J].Journal of Environmental Management,2021,293:112961.
[30]	刘晨,聂锦霞,郭琳,等.晶种对磷酸铵镁法去除水中磷的影响[J].应用化工,2018,47(7):1391-1394.[LIU Chen,NIE Jin-xia,GUO Lin,et al.Effects of Seed Crystals on Phosphorus Removal by Magnesium Ammonium Phosphate Crystallization[J].Applied Chemical Industry,2018,47(7):1391-1394.]
[31]	商平,郝永俊,刘涛利,等.改性蛭石结合鸟粪石沉淀法回收垃圾渗滤液中氨氮的实验研究[J].环境工程学报,2012,6(2):523-528.[SHANG Ping,HAO Yong-jun,LIU Tao-li,et al.Research on the Process of Nitrogen of Landfill Leachate with Modified Vermiculite and Magnesium Ammonium Phosphate Precipitation[J].Chinese Journal of Environmental Engineering,2012,6(2):523-528.]
[32]	陈理想,吴平霄,杨林,等.巯基乙胺改性蛭石对水体中Ag (I)的吸附性能研究[J].中国环境科学,2015,35(4):1109-1115.[CHEN Li-xiang,WU Ping-xiao,YANG Lin,et al.Efficient Removal of Silver from Aqueous Solution with Vermiculite Modification by 2-Aminoethanethiol[J].China Environmental Science,2015,35(4):1109-1115.]
[33]	罗仙平,张艳,邓扬悟.几种常见离子交换材料在氨氮废水处理中的应用[J].有色金属科学与工程,2012,3(6):51-54,74.[LUO Xian-ping,ZHANG Yan,DENG Yang-wu.Several Common Ion Exchange Materials and Their Application in Treatment of Ammonia-Nitrogen Wastewater[J].Nonferrous Metals Science and Engineering,2012,3(6):51-54,74.]
[34]	VINH N,ZAFAR M,BEHERA S K,et al.Arsenic (Ⅲ) Removal from Aqueous Solution by Raw and Zinc-Loaded Pine Cone Biochar:Equilibrium,Kinetics,and Thermodynamics Studies[J].International Journal of Environmental Science and Technology,2015,12(4):1283-1294.
[35]	WANG Y,HU Y T,ZHAO X,et al.Comparisons of Biochar Properties from Wood Material and Crop Residues at Different Temperatures and Residence Times[J].Energy&Fuels,2013,27(10):5890-5899.
[36]	于维钊,郑经堂,何小超,等.改性活性炭对噻吩的吸附性能研究[J].离子交换与吸附,2009,25(1):52-61.[YU Wei-zhao,ZHENG Jing-tang,HE Xiao-chao,et al.Adsorption Performance of Thiophene Onto Modified Activated Carbons[J].Ion Exchange and Adsorption,2009,25(1):52-61.]
[37]	谭珍珍,张学杨,王昌松,等.椰壳炭对水中阿莫西林的吸附特性[J].江苏农业科学,2019,47(4):252-256.[TAN Zhen-zhen,ZHANG Xue-yang,WANG Chang-song,et al.Adsorption Properties of Amoxicillin in Aqueous Solution by Coconut Shell Char[J].Jiangsu Agricultural Sciences,2019,47(4):252-256.]
[38]	豆婵婵.石英砂负载壳聚糖及CTAB改性麦秸秆对甲基橙和刚果红的吸附研究[D].郑州:郑州大学,2011.[DOU Chan-chan.A Study on the Adsorption Property of Methyl Orange and Congo Red by Chitosan Immobilized on Quartz Sand and CTAB Motified Wheat Staw[D].Zhengzhou:Zhengzhou University,2011.]
[39]	褚军,薛建辉,金梅娟,等.生物炭对农业面源污染氮、磷流失的影响研究进展[J].生态与农村环境学报,2014,30(4):409-415.[CHU Jun,XUE Jian-hui,JIN Mei-juan,et al.Review of Researches on Effects of Biochar in Reducing Nitrogen and Phosphorus Losses with Agricultural NonPoint Source Pollution[J].Journal of Ecology and Rural Environment,2014,30(4):409-415.]
[40]	王健,王长秋,鲁安怀,等.鸟粪石结晶法预处理垃圾渗滤液中高浓度氨氮的研究[J].矿物学报,2010,30(1):26-32.[WANG Jian,WANG Chang-qiu,LU An-huai,et al.Removal of Ammonium-nitrogen as Struvite Crystallization from Landfill Leachate[J].Acta Mineralogica Sinica,2010,30(1):26-32.]