NH_4~+对镁改性生物炭除磷效果的影响
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摘要
为提高人工湿地收割植物利用率并探讨水体中氨氮对镁改性生物炭(magnesium modified biochar,MBC)除磷效果的影响,本文以人工湿地植物芦苇为原料,引入金属镁离子对其改性,制备MBC,并以未改性生物炭(biochar,BC)为对照,通过批量摇床实验,研究了不同氮磷摩尔比(0、5、10)和初始磷浓度(100～500 mg·L-1)条件下,MBC、BC、BC与金属镁离子(BC+Mg~(2+))、Mg~(2+)这4种处理方式对磷酸盐的去除效果.结果表明,4种处理方式对磷的去除量排序为MBC>>BC+Mg~(2+)≈Mg~(2+)> BC,溶液中NH+4的存在促进MBC吸附除磷,氮磷摩尔比越大,初始磷浓度越高,MBC的磷吸附能力越强. XRD图谱分析结果表明,在MBC、BC+Mg~(2+)、Mg~(2+)这3种处理方式中,当氮磷摩尔比为5、10时,NH+4与溶液中的Mg~(2+)和PO3-4发生沉淀反应,生成鸟粪石(MgNH4PO4·6H2O),促进磷的去除.本研究利用人工湿地废弃生物质对富含氨氮和磷酸盐的溶液进行处理,确定了氨氮对水体中磷酸盐去除的促进作用,达到了回收利用、以废治废的目的,为水体富营养化治理提供了新的理论依据和数据支持.
The effect of ammonia-nitrogen in water on phosphorus removal by magnesium modified biochar( MBC) was developed to increase the utilization of wetland plants. The crystal structures were measured by X-ray powder diffraction( XRD). MBC was prepared using reed as the biomass feedstock,which was modified with magnesium chloride. The raw biochar( BC) was prepared as a control.The removal of phosphate from solution using four different methods,i. e. MBC,BC,BC,and MgCl2 solutions( BC + Mg~(2+)) and MgCl2 solutions( Mg~(2+)),under different nitrogen to phosphorus molar ratios and initial phosphorus concentrations was investigated in batch experiments. The results demonstrated that the phosphorus removal efficiency of the four treatment methods,which followed the order of MBC>>BC + Mg~(2+)≈Mg~(2+)> BC. NH+4 in the solution,promoted phosphorus removal by MBC. In addition,the larger the ratio of nitrogen to phosphorus and the higher the initial phosphorus concentration,the stronger the phosphorus removal capacity of MBC was. In the three treatments with MBC,BC + Mg~(2+),and Mg~(2+),the XRD analysis showed that NH+4 reacted with Mg~(2+)and PO3-4 in the solution to form MgNH4 PO4·6 H2 O at N∶ P = 5 or 10,promoting the removal of phosphorus. For recycling purposes,waste biomass from constructed wetlands could be used to produce MBC and treat polluted water rich in ammonium and phosphate. Moreover,the ammonium-nitrogen promotes the phosphate removal by MBC. The results from this study provide a new theoretical basis and data support for the treatment of water eutrophication.
The effect of ammonia-nitrogen in water on phosphorus removal by magnesium modified biochar( MBC) was developed to increase the utilization of wetland plants. The crystal structures were measured by X-ray powder diffraction( XRD). MBC was prepared using reed as the biomass feedstock,which was modified with magnesium chloride. The raw biochar( BC) was prepared as a control.The removal of phosphate from solution using four different methods,i. e. MBC,BC,BC,and MgCl2 solutions( BC + Mg~(2+)) and MgCl2 solutions( Mg~(2+)),under different nitrogen to phosphorus molar ratios and initial phosphorus concentrations was investigated in batch experiments. The results demonstrated that the phosphorus removal efficiency of the four treatment methods,which followed the order of MBC>>BC + Mg~(2+)≈Mg~(2+)> BC. NH+4 in the solution,promoted phosphorus removal by MBC. In addition,the larger the ratio of nitrogen to phosphorus and the higher the initial phosphorus concentration,the stronger the phosphorus removal capacity of MBC was. In the three treatments with MBC,BC + Mg~(2+),and Mg~(2+),the XRD analysis showed that NH+4 reacted with Mg~(2+)and PO3-4 in the solution to form MgNH4 PO4·6 H2 O at N∶ P = 5 or 10,promoting the removal of phosphorus. For recycling purposes,waste biomass from constructed wetlands could be used to produce MBC and treat polluted water rich in ammonium and phosphate. Moreover,the ammonium-nitrogen promotes the phosphate removal by MBC. The results from this study provide a new theoretical basis and data support for the treatment of water eutrophication.
引文
[1]茹改霞.富营养化水体除磷技术的研究进展[J].广东化工,2017,44(23):100,114.Ru G X. Research progresses of phosphorus removal technologies of eutrophic water[J]. Guangdong Chemical Industry,2017,44(23):100,114.
[2] Conley D J,Paerl H W,Howarth R W,et al. Controlling eutrophication:nitrogen and phosphorus[J]. Science,2009,323(5917):1014-1015.
[3] Takaya C A,Fletcher L A,Singh S,et al. Phosphate and ammonium sorption capacity of biochar and hydrochar from different wastes[J]. Chemosphere,2016,145:518-527.
[4] Zhao F L,Yang W D,Zeng Z,et al. Nutrient removal efficiency and biomass production of different bioenergy plants in hypereutrophic water[J]. Biomass and Bioenergy,2012,42:212-218.
[5] Dodds W K,Bouska W W,Eitzmann J L,et al. Eutrophication of U. S. freshwaters:analysis of potential economic damages[J].Environmental Science&Technology, 2009, 43(1):12-19.
[6] Cai R, Wang X, Ji X H, et al. Phosphate reclaim from simulated and real eutrophic water by magnetic biochar derived from water hyacinth[J]. Journal of Environmental Management,2017,187:212-219.
[7] Ma Z H, Li Q, Yue Q Y, et al. Adsorption removal of ammonium and phosphate from water by fertilizer controlled release agent prepared from wheat straw[J]. Chemical Engineering Journal,2011,171(3):1209-1217.
[8] Singh B P,Cowie A L,Smernik R J. Biochar carbon stability in a clayey soil as a function of feedstock and pyrolysis temperature[J]. Environmental Science&Technology,2012,46(21):11770-11778.
[9] Tan X F,Liu Y G,Zeng G M,et al. Application of biochar for the removal of pollutants from aqueous solutions[J].Chemosphere,2015,125:70-85.
[10] Chen L,Chen X L,Zhou C H,et al. Environmental-friendly montmorillonite-biochar composites:facile production and tunable adsorption-release of ammonium and phosphate[J]. Journal of Cleaner Production,2017,156:648-659.
[11] Yao Y,Gao B,Chen J J,et al. Engineered biochar reclaiming phosphate from aqueous solutions:mechanisms and potential application as a slow-release fertilizer[J]. Environmental Science&Technology,2013,47(15):8700-8708.
[12] Zhang M,Gao B,Yao Y,et al. Synthesis of porous Mg Obiochar nanocomposites for removal of phosphate and nitrate from aqueous solutions[J]. Chemical Engineering Journal,2012,210:26-32.
[13]赵立,吴雷,杨永哲.多级潮汐流人工湿地对污泥厌氧消化液中氨氮及有机物的去除特征[J].环境工程学报,2016,10(7):3687-3693.Zhao L,Wu L,Yang Y Z. Characteristic of ammoniacal nitrogen and organic matter removal from supernatant of anaerobic digested sludge using a multi-stage tidal-flow constructed wetland[J].Chinese Journal of Environmental Engineering,2016,10(7):3687-3693.
[14] Cui X Q,Hao H L,He Z L,et al. Pyrolysis of wetland biomass waste:Potential for carbon sequestration and water remediation[J]. Journal of Environmental Management,2016,173:95-104.
[15] Cui X Q,Hao H L,Zhang C K,et al. Capacity and mechanisms of ammonium and cadmium sorption on different wetland-plant derived biochars[J]. Science of the Total Environment,2016,539:566-575.
[16] Chen B L,Chen Z M,Lv S F. A novel magnetic biochar efficiently sorbs organic pollutants and phosphate[J].Bioresource Technology,2011,102(2):716-723.
[17]孟庆瑞,崔心红,朱义,等.载氧化镁水生植物生物炭的特性表征及对水中磷的吸附[J].环境科学学报,2017,37(8):2960-2967.Meng Q R,Cui X H,Zhu Y,et al. Characterization of Mg Oloaded aquatic plants biochar and its adsorption capacity of phosphorus in aqueous solution[J]. Acta Scientiae Circumstantiae,2017,37(8):2960-2967.
[18] Gong Y P,Ni Z Y,Xiong Z Z,et al. Phosphate and ammonium adsorption of the modified biochar based on Phragmites australis after phytoremediation[J]. Environmental Science and Pollution Research,2017,24(9):8326-8335.
[19] Cui X Q,Dai X,Khan K Y,et al. Removal of phosphate from aqueous solution using magnesium-alginate/chitosan modified biochar microspheres derived from Thalia dealbata[J].Bioresource Technology,2016,218:1123-1132.
[20] Chen Q C,Qin J L,Cheng Z W,et al. Synthesis of a stable magnesium-impregnated biochar and its reduction of phosphorus leaching from soil[J]. Chemosphere,2018,199:402-408.
[21]刘铁军.表面活性剂对高浓度氨氮废水缓冲体系中氨氮迁移影响的研究[D].武汉:武汉科技大学,2012.Liu T J. Study on effects of surfactants on ammonia nitrogen mass transfer in buffer system of high concentrations of ammonia nitrogen wastewater[D]. Wuhan:Wuhan University of Science and Technology,2012.
[22] Li R H,Wang J J,Zhou B Y,et al. Simultaneous capture removal of phosphate,ammonium and organic substances by Mg O impregnated biochar and its potential use in swine wastewater treatment[J]. Journal of Cleaner Production,2017,147:96-107.
[23] Yin Q Q,Wang R K,Zhao Z H. Application of Mg-Al-modified biochar for simultaneous removal of ammonium, nitrate, and phosphate from eutrophic water[J]. Journal of Cleaner Production,2018,176:230-240.
[24] Fang C,Zhang T,Li P,et al. Phosphorus recovery from biogas fermentation liquid by Ca-Mg loaded biochar[J]. Journal of Environmental Sciences,2015,29(3):106-114.
[25] Zhang J S,Wang Q Q. Sustainable mechanisms of biochar derived from brewers'spent grain and sewage sludge for ammonianitrogen capture[J]. Journal of Cleaner Production,2016,112:3927-3934.
[26]李际会.改性生物炭吸附硝酸盐和磷酸盐研究[D].北京:中国农业科学院,2012.Li J H. Adsorption of nitrate and phosphate by modified biochar[D]. Beijing:Chinese Academy of Agricultural Sciences,2012.
[27] Yao Y,Gao B,Inyang M,et al. Removal of phosphate from aqueous solution by biochar derived from anaerobically digested sugar beet tailings[J]. Journal of Hazardous Materials,2011,190(1-3):501-507.
[28] Li R H,Wang J J,Zhou B Y,et al. Recovery of phosphate from aqueous solution by magnesium oxide decorated magnetic biochar and its potential as phosphate-based fertilizer substitute[J].Bioresource Technology,2016,215:209-214.
[29]陈靖. Fe/Mg改性生物炭去除水中氮磷的研究[D].重庆:重庆大学,2015.Chen J. The study on removing ammonia nitrogen and phosphorus in water by Fe/Mg-modified bamboo charcoal[D]. Chongqing:Chongqing University,2015.
[30]赵卫,王世亮,赵荣飞.环境条件对生物炭吸附磷的影响研究进展[J].山东化工,2016,45(8):44-50.Zhao W,Wang S L,Zhao R F. Research progress on effects of environmental conditions on adsorption of phosphorus onto biochar[J]. Shandong Chemical Industry,2016,45(8):44-50.
[31] Xu K N,Lin F Y,Dou X M,et al. Recovery of ammonium and phosphate from urine as value-added fertilizer using wood waste biochar loaded with magnesium oxides[J]. Journal of Cleaner Production,2018,187:205-214.
[32]邹安华,孙体昌,邢奕,等. pH对MAP沉淀法去除废水中氨氮的影响[J].环境科学动态,2005,(4):4-6.
[33] Li R H,Wang J J,Zhou B Y,et al. Enhancing phosphate adsorption by Mg/Al layered double hydroxide functionalized biochar with different Mg/Al ratios[J]. Science of the Total Environment,2016,559:121-129.
[34]郑庆福,王志民,陈保国,等.制备生物炭的结构特征及炭化机理的XRD光谱分析[J].光谱学与光谱分析,2016,36(10):3355-3359.
[35]霍守亮,席北斗,刘鸿亮,等.磷酸铵镁沉淀法去除与回收废水中氮磷的应用研究进展[J].化工进展,2007,26(3):371-376.Huo S L,Xi B D,Liu H L,et al. Removal and recovery of nitrogen and phosphorus from wastewater by struvite crystallization[J]. Chemical Industry and Engineering Progress,2007,26(3):371-376.
[36]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 F F,Tian Q,Li F,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.
[37]艾小雨.凤眼莲生物质炭对水中磷和氮吸附研究[D].重庆:重庆大学,2013.Ai X Y. Adsorption research of phosphorate and nitrogen from wastewater using eichhornia crassipes biochars[D]. Chongqing:Chongqing University,2013.
[38] Rosales E,Meijide J,Pazos M,et al. Challenges and recent advances in biochar as low-cost biosorbent:from batch assays to continuous-flow systems[J]. Bioresource Technology,2017,246:176-192.
[2] Conley D J,Paerl H W,Howarth R W,et al. Controlling eutrophication:nitrogen and phosphorus[J]. Science,2009,323(5917):1014-1015.
[3] Takaya C A,Fletcher L A,Singh S,et al. Phosphate and ammonium sorption capacity of biochar and hydrochar from different wastes[J]. Chemosphere,2016,145:518-527.
[4] Zhao F L,Yang W D,Zeng Z,et al. Nutrient removal efficiency and biomass production of different bioenergy plants in hypereutrophic water[J]. Biomass and Bioenergy,2012,42:212-218.
[5] Dodds W K,Bouska W W,Eitzmann J L,et al. Eutrophication of U. S. freshwaters:analysis of potential economic damages[J].Environmental Science&Technology, 2009, 43(1):12-19.
[6] Cai R, Wang X, Ji X H, et al. Phosphate reclaim from simulated and real eutrophic water by magnetic biochar derived from water hyacinth[J]. Journal of Environmental Management,2017,187:212-219.
[7] Ma Z H, Li Q, Yue Q Y, et al. Adsorption removal of ammonium and phosphate from water by fertilizer controlled release agent prepared from wheat straw[J]. Chemical Engineering Journal,2011,171(3):1209-1217.
[8] Singh B P,Cowie A L,Smernik R J. Biochar carbon stability in a clayey soil as a function of feedstock and pyrolysis temperature[J]. Environmental Science&Technology,2012,46(21):11770-11778.
[9] Tan X F,Liu Y G,Zeng G M,et al. Application of biochar for the removal of pollutants from aqueous solutions[J].Chemosphere,2015,125:70-85.
[10] Chen L,Chen X L,Zhou C H,et al. Environmental-friendly montmorillonite-biochar composites:facile production and tunable adsorption-release of ammonium and phosphate[J]. Journal of Cleaner Production,2017,156:648-659.
[11] Yao Y,Gao B,Chen J J,et al. Engineered biochar reclaiming phosphate from aqueous solutions:mechanisms and potential application as a slow-release fertilizer[J]. Environmental Science&Technology,2013,47(15):8700-8708.
[12] Zhang M,Gao B,Yao Y,et al. Synthesis of porous Mg Obiochar nanocomposites for removal of phosphate and nitrate from aqueous solutions[J]. Chemical Engineering Journal,2012,210:26-32.
[13]赵立,吴雷,杨永哲.多级潮汐流人工湿地对污泥厌氧消化液中氨氮及有机物的去除特征[J].环境工程学报,2016,10(7):3687-3693.Zhao L,Wu L,Yang Y Z. Characteristic of ammoniacal nitrogen and organic matter removal from supernatant of anaerobic digested sludge using a multi-stage tidal-flow constructed wetland[J].Chinese Journal of Environmental Engineering,2016,10(7):3687-3693.
[14] Cui X Q,Hao H L,He Z L,et al. Pyrolysis of wetland biomass waste:Potential for carbon sequestration and water remediation[J]. Journal of Environmental Management,2016,173:95-104.
[15] Cui X Q,Hao H L,Zhang C K,et al. Capacity and mechanisms of ammonium and cadmium sorption on different wetland-plant derived biochars[J]. Science of the Total Environment,2016,539:566-575.
[16] Chen B L,Chen Z M,Lv S F. A novel magnetic biochar efficiently sorbs organic pollutants and phosphate[J].Bioresource Technology,2011,102(2):716-723.
[17]孟庆瑞,崔心红,朱义,等.载氧化镁水生植物生物炭的特性表征及对水中磷的吸附[J].环境科学学报,2017,37(8):2960-2967.Meng Q R,Cui X H,Zhu Y,et al. Characterization of Mg Oloaded aquatic plants biochar and its adsorption capacity of phosphorus in aqueous solution[J]. Acta Scientiae Circumstantiae,2017,37(8):2960-2967.
[18] Gong Y P,Ni Z Y,Xiong Z Z,et al. Phosphate and ammonium adsorption of the modified biochar based on Phragmites australis after phytoremediation[J]. Environmental Science and Pollution Research,2017,24(9):8326-8335.
[19] Cui X Q,Dai X,Khan K Y,et al. Removal of phosphate from aqueous solution using magnesium-alginate/chitosan modified biochar microspheres derived from Thalia dealbata[J].Bioresource Technology,2016,218:1123-1132.
[20] Chen Q C,Qin J L,Cheng Z W,et al. Synthesis of a stable magnesium-impregnated biochar and its reduction of phosphorus leaching from soil[J]. Chemosphere,2018,199:402-408.
[21]刘铁军.表面活性剂对高浓度氨氮废水缓冲体系中氨氮迁移影响的研究[D].武汉:武汉科技大学,2012.Liu T J. Study on effects of surfactants on ammonia nitrogen mass transfer in buffer system of high concentrations of ammonia nitrogen wastewater[D]. Wuhan:Wuhan University of Science and Technology,2012.
[22] Li R H,Wang J J,Zhou B Y,et al. Simultaneous capture removal of phosphate,ammonium and organic substances by Mg O impregnated biochar and its potential use in swine wastewater treatment[J]. Journal of Cleaner Production,2017,147:96-107.
[23] Yin Q Q,Wang R K,Zhao Z H. Application of Mg-Al-modified biochar for simultaneous removal of ammonium, nitrate, and phosphate from eutrophic water[J]. Journal of Cleaner Production,2018,176:230-240.
[24] Fang C,Zhang T,Li P,et al. Phosphorus recovery from biogas fermentation liquid by Ca-Mg loaded biochar[J]. Journal of Environmental Sciences,2015,29(3):106-114.
[25] Zhang J S,Wang Q Q. Sustainable mechanisms of biochar derived from brewers'spent grain and sewage sludge for ammonianitrogen capture[J]. Journal of Cleaner Production,2016,112:3927-3934.
[26]李际会.改性生物炭吸附硝酸盐和磷酸盐研究[D].北京:中国农业科学院,2012.Li J H. Adsorption of nitrate and phosphate by modified biochar[D]. Beijing:Chinese Academy of Agricultural Sciences,2012.
[27] Yao Y,Gao B,Inyang M,et al. Removal of phosphate from aqueous solution by biochar derived from anaerobically digested sugar beet tailings[J]. Journal of Hazardous Materials,2011,190(1-3):501-507.
[28] Li R H,Wang J J,Zhou B Y,et al. Recovery of phosphate from aqueous solution by magnesium oxide decorated magnetic biochar and its potential as phosphate-based fertilizer substitute[J].Bioresource Technology,2016,215:209-214.
[29]陈靖. Fe/Mg改性生物炭去除水中氮磷的研究[D].重庆:重庆大学,2015.Chen J. The study on removing ammonia nitrogen and phosphorus in water by Fe/Mg-modified bamboo charcoal[D]. Chongqing:Chongqing University,2015.
[30]赵卫,王世亮,赵荣飞.环境条件对生物炭吸附磷的影响研究进展[J].山东化工,2016,45(8):44-50.Zhao W,Wang S L,Zhao R F. Research progress on effects of environmental conditions on adsorption of phosphorus onto biochar[J]. Shandong Chemical Industry,2016,45(8):44-50.
[31] Xu K N,Lin F Y,Dou X M,et al. Recovery of ammonium and phosphate from urine as value-added fertilizer using wood waste biochar loaded with magnesium oxides[J]. Journal of Cleaner Production,2018,187:205-214.
[32]邹安华,孙体昌,邢奕,等. pH对MAP沉淀法去除废水中氨氮的影响[J].环境科学动态,2005,(4):4-6.
[33] Li R H,Wang J J,Zhou B Y,et al. Enhancing phosphate adsorption by Mg/Al layered double hydroxide functionalized biochar with different Mg/Al ratios[J]. Science of the Total Environment,2016,559:121-129.
[34]郑庆福,王志民,陈保国,等.制备生物炭的结构特征及炭化机理的XRD光谱分析[J].光谱学与光谱分析,2016,36(10):3355-3359.
[35]霍守亮,席北斗,刘鸿亮,等.磷酸铵镁沉淀法去除与回收废水中氮磷的应用研究进展[J].化工进展,2007,26(3):371-376.Huo S L,Xi B D,Liu H L,et al. Removal and recovery of nitrogen and phosphorus from wastewater by struvite crystallization[J]. Chemical Industry and Engineering Progress,2007,26(3):371-376.
[36]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 F F,Tian Q,Li F,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.
[37]艾小雨.凤眼莲生物质炭对水中磷和氮吸附研究[D].重庆:重庆大学,2013.Ai X Y. Adsorption research of phosphorate and nitrogen from wastewater using eichhornia crassipes biochars[D]. Chongqing:Chongqing University,2013.
[38] Rosales E,Meijide J,Pazos M,et al. Challenges and recent advances in biochar as low-cost biosorbent:from batch assays to continuous-flow systems[J]. Bioresource Technology,2017,246:176-192.
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