铁锰氧化物/生物炭复合材料对水中硝酸根的吸附特性
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摘要
热解经过氯化铁和高锰酸钾浸渍的小麦秸秆,制备铁锰金属氧化物/生物炭复合材料,用以去除水中硝酸根.通过X射线光电子能谱和扫描电镜分析,发现复合材料表面形成了Fe(Ⅲ)/Mn(Ⅳ)二元金属氧化物颗粒.制备优化结果表明,复合材料比表面积可达153.116 m2·g-1,零电荷点可达9.76.同时,还调查了固液比、溶液初始pH值和共存阴离子等因素的影响.研究发现,复合材料在溶液pH值1.00~9.05时对NO-3的去除率维持在75.40%~78.70%,且以配位交换为主要吸附机制.共存阴离子对吸附NO-3竞争吸附的影响顺序为:Cl->SO2-4>PO3-4.等温吸附实验数据符合Langmuir方程,且最大吸附量为37.361 3 mg·g-1.吸附动力学分析发现,吸附过程遵循二级动力学方程,且以化学吸附为主.热动力学分析表明,吸附过程为自发吸热过程.上述结果说明铁锰氧化物/生物炭复合材料对于去除水中NO-3具有潜在价值.
In this study,we synthesized Fe/Mn bimetallic oxide coated biochar sorbents by pyrolysis of wheat straw impregnated with ferric chloride and potassium permanganate and investigated their potential to adsorb nitrate in water. X-ray photoelectron spectroscopy and scanning electron microscopy analysis suggests that Fe(Ⅲ)/Mn(Ⅳ) bimetallic oxide particles emerge on the sorbents. The optimized sorbent could achieve a specific surface area of 153. 116 m2·g-1 and a point of zero charge of 9. 76. Batch nitrate adsorption experiments were carried out to investigate the influence of various factors,such as sorbent dosage,initial solution pH,and co-existing anions. Results show that the sorbent maintained a high adsorption capacity of 75. 40%-78. 70% over a wide range of pH from 1. 00 to9. 05,and the sorption mechanism was interpreted as ligand exchange. The effects of co-existing anions on the nitrate sorption followed the decreasing order of Cl-> SO2-4> PO3-4. Furthermore,the adsorption isotherms were well described by the Langmuir model,and the sorbent could exhibit a quite competitively high capacity of 37. 361 3 mg·g-1 for nitrate removal. In addition,the accordance of sorption kinetics with the pseudo-second order model implied that the sorption could be a multi-stage controlled chemical process. In addition,the thermodynamic parameters suggested that the sorption reaction could be a spontaneous and endothermic process. The results demonstrated that the Fe/Mn bimetallic oxide coated biochar could serve as a promising agent for nitrate removal from water.
In this study,we synthesized Fe/Mn bimetallic oxide coated biochar sorbents by pyrolysis of wheat straw impregnated with ferric chloride and potassium permanganate and investigated their potential to adsorb nitrate in water. X-ray photoelectron spectroscopy and scanning electron microscopy analysis suggests that Fe(Ⅲ)/Mn(Ⅳ) bimetallic oxide particles emerge on the sorbents. The optimized sorbent could achieve a specific surface area of 153. 116 m2·g-1 and a point of zero charge of 9. 76. Batch nitrate adsorption experiments were carried out to investigate the influence of various factors,such as sorbent dosage,initial solution pH,and co-existing anions. Results show that the sorbent maintained a high adsorption capacity of 75. 40%-78. 70% over a wide range of pH from 1. 00 to9. 05,and the sorption mechanism was interpreted as ligand exchange. The effects of co-existing anions on the nitrate sorption followed the decreasing order of Cl-> SO2-4> PO3-4. Furthermore,the adsorption isotherms were well described by the Langmuir model,and the sorbent could exhibit a quite competitively high capacity of 37. 361 3 mg·g-1 for nitrate removal. In addition,the accordance of sorption kinetics with the pseudo-second order model implied that the sorption could be a multi-stage controlled chemical process. In addition,the thermodynamic parameters suggested that the sorption reaction could be a spontaneous and endothermic process. The results demonstrated that the Fe/Mn bimetallic oxide coated biochar could serve as a promising agent for nitrate removal from water.
引文
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[14]王彤彤,马江波,曲东,等.两种木材生物炭对铜离子的吸附特性及其机制[J].环境科学,2017,38(5):2161-2171.Wang T T,Ma J B,Qu D,et al.Characteristics and mechanism of copper adsorption from aqueous solutions on biochar produced from sawdust and apple branch[J].Environmental Science,2017,38(5):2161-2171.
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[19]李丽,陈旭,吴丹,等.固定化改性生物质炭模拟吸附水体硝态氮潜力研究[J].农业环境科学学报,2015,34(1):137-143.Li L,Chen X,Wu D,et al.Adsorption of aqueous nitrate-N by immobilized modified biochar[J].Journal of Agro-Environment Science,2015,34(1):137-143.
[20]秦艳敏,王敦球,梁美娜,等.桑树杆活性炭/铁锰氧化物复合吸附剂的制备及其对Cr(VI)的吸附[J].环境化学,2016,35(4):783-792.Qin Y M,Wang D Q,Liang M N,et al.Preparation of mulberry stem activated carbon/Fe-Mn oxide composite sorbent and its effects on the adsorption of Cr(Ⅵ)[J].Environmental Chemistry,2016,35(4):783-792.
[21]Hu X,Ding Z H,Zimmerman A R,et al.Batch and column sorption of arsenic onto iron-impregnated biochar synthesized through hydrolysis[J].Water Research,2015,68:206-216.
[22]Wang S S,Gao B,Li Y C,et al.Manganese oxide-modified biochars:preparation,characterization,and sorption of arsenate and lead[J].Bioresource Technology,2015,181:13-17.
[23]唐登勇,黄越,胥瑞晨,等.改性芦苇生物炭对水中低浓度磷的吸附特征[J].环境科学,2016,37(6):2195-2201.Tang D Y,Huang Y,Xu R C,et al.Adsorption behavior of low concentration phosphorus from water onto modified reed biochar[J].Environmental Science,2016,37(6):2195-2201.
[24]Kenari S L D,Barbeau B.Size and zeta potential of oxidized iron and manganese in water treatment:influence of p H,ionic strength,and hardness[J].Journal of Environmental Engineering,2016,142(5):04016010.
[25]Wang S S,Gao B,Li Y C,et al.Sorption of arsenate onto magnetic iron-manganese(Fe-Mn)biochar composites[J].RSC Advance,2015,5(83):67971-67978.
[26]秦艳敏,梁美娜,王敦球,等.桑树杆生物炭/铁锰氧化物复合吸附剂的制备及其对As(Ⅴ)的吸附机理研究[J].农业环境科学学报,2016,35(7):1398-1406.Qin Y M,Liang M N,Wang D Q,et al.Preparation and arsenic adsorption and its mechanisms by mulberry stem biochar/Fe-Mn oxides composite adsorbent[J].Journal of Agro-Environment Science,2016,35(7):1398-1406.
[27]Tran H N,You S J,Hosseini-Bandegharaei A,et al.Mistakes and inconsistencies regarding adsorption of contaminants from aqueous solutions:a critical review[J].Water Research,2017,120:88-116.
[28]Goh K H,Lim T T,Dong Z L.Application of layered double hydroxides for removal of oxyanions:a review[J].Water Research,2008,42(6-7):1343-1368.
[29]Chen M,Paulson S,Kan W H,et al.Surface and bulk study of strontium-rich chromium ferrite oxide as a robust solid oxide fuel cell cathode[J].Journal of Materials Chemistry A,2015,3(45):22614-22626.
[30]Taffa D H,Hamm I,Dunkel C,et al.Electrochemical deposition of Fe2O3in the presence of organic additives:a route to enhanced photoactivity[J].RSC Advances,2015,5(125):103512-103522.
[31]Li R J,Liu L F,Zhang Y H,et al.Preparation of a nano-Mn O2surface-modified reduced graphene oxide/PVDF flat sheet membrane for adsorptive removal of aqueous Ni(Ⅱ)[J].RSC Advances,2016,6(25):20542-20550.
[32]高欢,韦安磊,郑晓青,等.乙酰化小麦秸秆吸附水中六价铬[J].环境工程学报,2016,10(9):4753-4760.Gao H,Wei A L,Zheng X Q,et al.Adsorption of hexavalent chromium from aqueous solution by acetylated wheat straw[J].Chinese Journal of Environmental Engineering,2016,10(9):4753-4760.
[33]Bhatnagar A,Kumar E,SillanpM.Nitrate removal from water by nano-alumina:characterization and sorption studies[J].Chemical Engineering Journal,2010,163(3):317-323.
[34]Kanrar S,Debnath S,De P,et al.Preparation,characterization and evaluation of fluoride adsorption efficiency from water of ironaluminium oxide-graphene oxide composite material[J].Chemical Engineering Journal,2016,306:269-279.
[35]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.
[36]Wang Z,Guo H,Shen F,et al.Biochar produced from oak sawdust by Lanthanum(La)-involved pyrolysis for adsorption of ammonium(NH+4),nitrate(NO-3),and phosphate(PO3-4)[J].Chemosphere,2015,119:646-653.
[37]Xue L H,Gao B,Wan Y S,et al.High efficiency and selectivity of Mg Fe-LDH modified wheat-straw biochar in the removal of nitrate from aqueous solutions[J].Journal of the Taiwan Institute of Chemical Engineers,2016,63:312-317.
[38]Demiral H,Gündüzogˇlu G.Removal of nitrate from aqueous solutions by activated carbon prepared from sugar beet bagasse[J].Bioresource Technology,2010,101(6):1675-1680.
[39]谢超然,王兆炜,朱俊民,等.核桃青皮生物炭对重金属铅、铜的吸附特性研究[J].环境科学学报,2016,36(4):1190-1198.Xie C R,Wang Z W,Zhu J M,et al.Adsorption of lead and copper from aqueous solutions on biochar produced from walnut green husk[J].Acta Scientiae Circumstantiae,2016,36(4):1190-1198.
[2]Kamaraj R,Pandiarajan A,Jayakiruba S,et al.Kinetics,thermodynamics and isotherm modeling for removal of nitrate from liquids by facile one-pot electrosynthesized nano zinc hydroxide[J].Journal of Molecular Liquids,2016,215:204-211.
[3]张翠云,张胜,马琳娜,等.污灌区地下水硝酸盐污染来源的氮同位素示踪[J].地球科学——中国地质大学学报,2012,37(2):350-356.Zhang C Y,Zhang S,Ma L N,et al.Nitrogen isotope tracing of sources of nitrate contamination in groundwater from wastewater irrigated area[J].Earth Science-Journal of China University of Geosciences,2012,37(2):350-356.
[4]Archna,Sharma S K,Sobti R C.Nitrate removal from ground water:a review[J].Journal of Chemistry,2012,9(4):1667-1675.
[5]郑雯婧,林建伟,詹艳慧,等.锆-十六烷基三甲基氯化铵改性活性炭对水中硝酸盐和磷酸盐的吸附特性[J].环境科学,2015,36(6):2185-2194.Zheng W J,Lin J W,Zhan Y H,et al.Adsorption characteristics of nitrate and phosphate from aqueous solution on zirconium-hexadecyltrimethylammonium chloride modified activated carbon[J].Environmental Science,2015,36(6):2185-2194.
[6]王博,叶春,李法云,等.水生植物制生物炭对硝态氮的吸附规律研究[J].中国环境科学,2017,37(1):116-122.Wang B,Ye C,Li F Y,et al.Studies on adsorption of nitrate from modified hydrophyte biochars[J].China Environmental Science,2017,37(1):116-122.
[7]王荣荣,赖欣,李洁,等.花生壳生物炭对硝态氮的吸附机制研究[J].农业环境科学学报,2016,35(9):1727-1734.Wang R R,Lai X,Li J,et al.Adsorption of nitrate nitrogen by peanut shell biochar[J].Journal of Agro-Environment Science,2016,35(9):1727-1734.
[8]马锋锋,赵保卫,刁静茹,等.牛粪生物炭对水中氨氮的吸附特性[J].环境科学,2015,36(5):1678-1685.Ma F F,Zhao B W,Diao J R,et al.Ammonium adsorption characteristics in aqueous solution by dairy manure biochar[J].Environmental Science,2015,36(5):1678-1685.
[9]马锋锋,赵保卫.不同热解温度制备的玉米芯生物炭对对硝基苯酚的吸附作用[J].环境科学,2017,38(2):837-844.Ma F F,Zhao B W.Sorption of p-nitrophenol by biochars of corncob prepared at different pyrolysis temperatures[J].Environmental Science,2017,38(2):837-844.
[10]Ahmad M,Rajapaksha A U,Lim J E,et al.Biochar as a sorbent for contaminant management in soil and water:a review[J].Chemosphere,2014,99(:19-33.
[11]高欢,韦安磊,郑晓青,等.小麦秸秆生物炭对水中对羟基苯甲酸乙酯的吸附特性[J].环境科学学报,2017,37(7):2667-2679.Gao H,Wei A L,Zheng X Q,et al.Adsorption characteristic of ethyl paraben from aqueous solution using wheat straw biochar[J].Acta Scientiae Circumstantiae,2017,37(7):2667-2679.
[12]Sewu D D,Boakye P,Woo S H.Highly efficient adsorption of cationic dye by biochar produced with Korean cabbage waste[J].Bioresource Technology,2017,224:206-213.
[13]Mahmoud M E,Nabil G M,El-Mallah N M,et al.Kinetics,isotherm,and thermodynamic studies of the adsorption of reactive red 195 A dye from water by modified switchgrass biochar adsorbent[J].Journal of Industrial and Engineering Chemistry,2016,37:156-167.
[14]王彤彤,马江波,曲东,等.两种木材生物炭对铜离子的吸附特性及其机制[J].环境科学,2017,38(5):2161-2171.Wang T T,Ma J B,Qu D,et al.Characteristics and mechanism of copper adsorption from aqueous solutions on biochar produced from sawdust and apple branch[J].Environmental Science,2017,38(5):2161-2171.
[15]Kalinke C,Mangrich A S,Marcolino-Junior L H,et al.Biochar prepared from castor oil cake at different temperatures:a voltammetric study applied for Pb2+,Cd2+and Cu2+ions preconcentration[J].Journal of Hazardous Materials,2016,318:526-532.
[16]Li J H,Lv G H,Bai W B,et al.Modification and use of biochar from wheat straw(Triticum aestivum L.)for nitrate and phosphate removal from water[J].Desalination and Water Treatment,2016,57(10):4681-4693.
[17]Zhu N Y,Yan T M,Qiao J,et al.Adsorption of arsenic,phosphorus and chromium by bismuth impregnated biochar:adsorption mechanism and depleted adsorbent utilization[J].Chemosphere,2016,164:32-40.
[18]Lawrinenko M,Laird D A.Anion exchange capacity of biochar[J].Green Chemistry,2015,17(9):4628-4636.
[19]李丽,陈旭,吴丹,等.固定化改性生物质炭模拟吸附水体硝态氮潜力研究[J].农业环境科学学报,2015,34(1):137-143.Li L,Chen X,Wu D,et al.Adsorption of aqueous nitrate-N by immobilized modified biochar[J].Journal of Agro-Environment Science,2015,34(1):137-143.
[20]秦艳敏,王敦球,梁美娜,等.桑树杆活性炭/铁锰氧化物复合吸附剂的制备及其对Cr(VI)的吸附[J].环境化学,2016,35(4):783-792.Qin Y M,Wang D Q,Liang M N,et al.Preparation of mulberry stem activated carbon/Fe-Mn oxide composite sorbent and its effects on the adsorption of Cr(Ⅵ)[J].Environmental Chemistry,2016,35(4):783-792.
[21]Hu X,Ding Z H,Zimmerman A R,et al.Batch and column sorption of arsenic onto iron-impregnated biochar synthesized through hydrolysis[J].Water Research,2015,68:206-216.
[22]Wang S S,Gao B,Li Y C,et al.Manganese oxide-modified biochars:preparation,characterization,and sorption of arsenate and lead[J].Bioresource Technology,2015,181:13-17.
[23]唐登勇,黄越,胥瑞晨,等.改性芦苇生物炭对水中低浓度磷的吸附特征[J].环境科学,2016,37(6):2195-2201.Tang D Y,Huang Y,Xu R C,et al.Adsorption behavior of low concentration phosphorus from water onto modified reed biochar[J].Environmental Science,2016,37(6):2195-2201.
[24]Kenari S L D,Barbeau B.Size and zeta potential of oxidized iron and manganese in water treatment:influence of p H,ionic strength,and hardness[J].Journal of Environmental Engineering,2016,142(5):04016010.
[25]Wang S S,Gao B,Li Y C,et al.Sorption of arsenate onto magnetic iron-manganese(Fe-Mn)biochar composites[J].RSC Advance,2015,5(83):67971-67978.
[26]秦艳敏,梁美娜,王敦球,等.桑树杆生物炭/铁锰氧化物复合吸附剂的制备及其对As(Ⅴ)的吸附机理研究[J].农业环境科学学报,2016,35(7):1398-1406.Qin Y M,Liang M N,Wang D Q,et al.Preparation and arsenic adsorption and its mechanisms by mulberry stem biochar/Fe-Mn oxides composite adsorbent[J].Journal of Agro-Environment Science,2016,35(7):1398-1406.
[27]Tran H N,You S J,Hosseini-Bandegharaei A,et al.Mistakes and inconsistencies regarding adsorption of contaminants from aqueous solutions:a critical review[J].Water Research,2017,120:88-116.
[28]Goh K H,Lim T T,Dong Z L.Application of layered double hydroxides for removal of oxyanions:a review[J].Water Research,2008,42(6-7):1343-1368.
[29]Chen M,Paulson S,Kan W H,et al.Surface and bulk study of strontium-rich chromium ferrite oxide as a robust solid oxide fuel cell cathode[J].Journal of Materials Chemistry A,2015,3(45):22614-22626.
[30]Taffa D H,Hamm I,Dunkel C,et al.Electrochemical deposition of Fe2O3in the presence of organic additives:a route to enhanced photoactivity[J].RSC Advances,2015,5(125):103512-103522.
[31]Li R J,Liu L F,Zhang Y H,et al.Preparation of a nano-Mn O2surface-modified reduced graphene oxide/PVDF flat sheet membrane for adsorptive removal of aqueous Ni(Ⅱ)[J].RSC Advances,2016,6(25):20542-20550.
[32]高欢,韦安磊,郑晓青,等.乙酰化小麦秸秆吸附水中六价铬[J].环境工程学报,2016,10(9):4753-4760.Gao H,Wei A L,Zheng X Q,et al.Adsorption of hexavalent chromium from aqueous solution by acetylated wheat straw[J].Chinese Journal of Environmental Engineering,2016,10(9):4753-4760.
[33]Bhatnagar A,Kumar E,SillanpM.Nitrate removal from water by nano-alumina:characterization and sorption studies[J].Chemical Engineering Journal,2010,163(3):317-323.
[34]Kanrar S,Debnath S,De P,et al.Preparation,characterization and evaluation of fluoride adsorption efficiency from water of ironaluminium oxide-graphene oxide composite material[J].Chemical Engineering Journal,2016,306:269-279.
[35]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.
[36]Wang Z,Guo H,Shen F,et al.Biochar produced from oak sawdust by Lanthanum(La)-involved pyrolysis for adsorption of ammonium(NH+4),nitrate(NO-3),and phosphate(PO3-4)[J].Chemosphere,2015,119:646-653.
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