氢氧化镧改性介孔稻壳生物炭除磷性能
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摘要
通过共沉淀法将氢氧化镧固定在高介孔率的稻壳生物炭上,重点研究了生物炭孔结构、溶液pH和共存物质对氢氧化镧改性介孔稻壳生物炭吸附磷酸盐的影响.结果表明,镧负载量与生物炭介孔率呈正相关,生物炭介孔率越高,对磷酸盐的吸附速率越快,镧浸出量越低.吸附过程符合伪二级动力学模型,且受颗粒内扩散控制. Langmuir模型能够较好地描述氢氧化镧改性介孔稻壳生物炭对磷酸盐的吸附过程,理论最大吸附量分别为41. 22、43. 26和45. 62 mg·g~(-1),镧利用率较高,P/La量比均大于1. 5.此外,氢氧化镧改性介孔稻壳生物炭能在pH 3～9的范围内有效吸附磷酸盐.共存物质影响实验表明,氢氧化镧改性介孔稻壳生物炭对磷酸盐表现出良好的选择吸附性,共存Ca~(2+)会强化其对磷酸盐的吸附,而共存Mg~(2+)则会抑制吸附过程.
La-modified RHBCs( La-RHBCs) were fabricated by immobilizing La( OH)3 nanoparticles on mesoporous rice husk biochars( RHBCs) using a co-precipitation method. Specifically,the effects of the pore structure of the RHBCs,solution pH,and coexisting substances on phosphate adsorption by the La-RHBCs were studied. The results showed that the La loading of the La-RHBCs was positively correlated with the mesoporosity of the RHBCs. La-modified RHBCs with higher mesoporosity hosts showed faster adsorption rates and lower leaching of La during phosphate adsorption. The adsorption process could be described by a pseudo secondorder kinetic model,and the reaction rate was controlled by intraparticle diffusion. The Langmuir isotherm model fitted the adsorption process better,and the theoretical maximum adsorption capacities were 41. 22,43. 26,and 45. 62 mg·g~(-1),respectively. The high P/La molar ratios of more than 1. 5 indicated the high utilization efficiencies of the La in the La-immobilized RHBCs. Moreover,phosphate could be effectively removed by the La-modified RHBCs over a wide pH range of 3-9. The La-modified RHBCs also exhibited good adsorption selectivity towards phosphate in the presence of coexisting anions and humic acids. Phosphate adsorption by the La-RHBCs was enhanced in the presence of Ca~(2+),while it was inhibited in the presence of Mg~(2+).
La-modified RHBCs( La-RHBCs) were fabricated by immobilizing La( OH)3 nanoparticles on mesoporous rice husk biochars( RHBCs) using a co-precipitation method. Specifically,the effects of the pore structure of the RHBCs,solution pH,and coexisting substances on phosphate adsorption by the La-RHBCs were studied. The results showed that the La loading of the La-RHBCs was positively correlated with the mesoporosity of the RHBCs. La-modified RHBCs with higher mesoporosity hosts showed faster adsorption rates and lower leaching of La during phosphate adsorption. The adsorption process could be described by a pseudo secondorder kinetic model,and the reaction rate was controlled by intraparticle diffusion. The Langmuir isotherm model fitted the adsorption process better,and the theoretical maximum adsorption capacities were 41. 22,43. 26,and 45. 62 mg·g~(-1),respectively. The high P/La molar ratios of more than 1. 5 indicated the high utilization efficiencies of the La in the La-immobilized RHBCs. Moreover,phosphate could be effectively removed by the La-modified RHBCs over a wide pH range of 3-9. The La-modified RHBCs also exhibited good adsorption selectivity towards phosphate in the presence of coexisting anions and humic acids. Phosphate adsorption by the La-RHBCs was enhanced in the presence of Ca~(2+),while it was inhibited in the presence of Mg~(2+).
引文
[1] 2017年《中国生态环境状况公报》(摘录二)[J].环境保护,2018,46(12):67-74.
[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]苗文凭,林海,卢晓君.粉煤灰吸附除磷的改性研究[J].环境工程学报,2008,2(4):502-506.Miao W P,Lin H,Lu X J. Adsorption of phosphate using modified fly ash from water solution[J]. Chinese Journal of Environmental Engineering,2008,2(4):502-506.
[4] Chitrakar R,Tezuka S,Sonoda A,et al. Selective adsorption of phosphate from seawater and wastewater by amorphous zirconium hydroxide[J]. Journal of Colloid and Interface Science,2006,297(2):426-433.
[5] Xie J,Wang Z,Lu S Y,et al. Removal and recovery of phosphate from water by lanthanum hydroxide materials[J].Chemical Engineering Journal,2014,254:163-170.
[6] Zhang M,Gao B,Yao Y,et al. Phosphate removal ability of biochar/Mg Al-LDH ultra-fine composites prepared by liquidphase deposition[J]. Chemosphere,2013,92(8):1042-1047.
[7] Cai P, Zheng H, Wang C, et al. Competitive adsorption characteristics of fluoride and phosphate on calcined Mg-Al-CO3layered double hydroxides[J]. Journal of Hazardous Materials,2012,213-214:100-108.
[8] Chen J G,Kong H N,Wu D Y,et al. Removal of phosphate from aqueous solution by zeolite synthesized from fly ash[J].Journal of Colloid and Interface Science,2006,300(2):491-497.
[9] Ye J,Cong X N,Zhang P Y, et al. Interaction between phosphate and acid-activated neutralized red mud during adsorption process[J]. Applied Surface Science,2015,356:128-134.
[10] Koilraj P,Sasaki K. Selective removal of phosphate using Laporous carbon composites from aqueous solutions:Batch and column studies[J]. Chemical Engineering Journal,2017,317:1059-1068.
[11] He Y H,Lin H,Dong Y B,et al. Preferable adsorption of phosphate using lanthanum-incorporated porous zeolite:characteristics and mechanism[J]. Applied Surface Science,2017,426:995-1004.
[12] Dong S X,Wang Y L,Zhao Y W,et al. La3+/La(OH)3loaded magnetic cationic hydrogel composites for phosphate removal:effect of lanthanum species and mechanistic study[J].Water Research,2017,126:433-441.
[13] Yang J,Zhou L,Zhao L Z,et al. A designed nanoporous material for phosphate removal with high efficiency[J]. Journal of Materials Chemistry,2011,21(8):2489-2494.
[14]袁宪正,潘纲,田秉晖,等.氯化镧改性黏土固化湖泊底泥中磷的研究[J].环境科学,2007,28(2):403-406.Yuan X Z,Pan G,Tian B H,et al. Study on phosphorus(P)fixation in the sediment of lake using the clays modified by La Cl3[J]. Environmental Science,2007,28(2):403-406.
[15] Liu J Y,Zhou Q,Chen J H,et al. Phosphate adsorption on hydroxyl-iron-lanthanum doped activated carbon fiber[J].Chemical Engineering Journal,2013,215-216:859-867.
[16] Zhang Y Y,Pan B C,Shan C,et al. Enhanced phosphate removal by nanosized hydrated La(III)oxide confined in crosslinked polystyrene networks[J]. Environmental Science&Technology,2016,50(3):1447-1454.
[17] Sizmur T,Fresno T,Akgül G,et al. Biochar modification to enhance sorption of inorganics from water[J]. Bioresource Technology,2017,246:34-47.
[18]李楠,单保庆,唐文忠,等.稻壳活性炭制备及其对磷的吸附[J].环境工程学报,2013,7(3):1024-1028.Li N,Shan B Q,Tang W Z,et al. Preparation of powder activated carbon by rice husks and its adsorption capacity to phosphorus[J]. Chinese Journal of Environmental Engineering,2013,7(3):1024-1028.
[19] Guo Y P,Rockstraw D A. Activated carbons prepared from rice hull by one-step phosphoric acid activation[J]. Microporous and Mesoporous Materials,2007,100(1-3):12-19.
[20] Genuino D A D,de Luna M D G,Capareda S C. Improving the surface properties of municipal solid waste-derived pyrolysis biochar by chemical and thermal activation:Optimization of process parameters and environmental application[J]. Waste Management,2018,72:255-264.
[21] Wang Z H,Shen D K,Shen F,et al. Phosphate adsorption on lanthanum loaded biochar[J]. Chemosphere,2016,150:1-7.
[22] Qiu H, Liang C, Yu J H, et al. Preferable phosphate sequestration by nano-La(III)(hydr)oxides modified wheat straw with excellent properties in regeneration[J]. Chemical Engineering Journal,2017,315:345-354.
[23] Yang Q, Wang X L, Luo W, et al. Effectiveness and mechanisms of phosphate adsorption on iron-modified biochars derived from waste activated sludge[J]. Bioresource Technology,2018,247:537-544.
[24] Wang J,Zhang S J,Pan B C,et al. Hydrous ferric oxide-resin nanocomposites of tunable structure for arsenite removal:effect of the host pore structure[J]. Journal of Hazardous Materials,2011,198:241-246.
[25] Yang J, Yuan P, Chen H Y, et al. Rationally designed functional macroporous materials as new adsorbents for efficient phosphorus removal[J]. Journal of Materials Chemistry,2012,22(19):9983-9990.
[26] Zhang X L, Wang Y H, Chang X F, et al. Iron oxide nanoparticles confined in mesoporous silicates for arsenic sequestration:effect of the host pore structure[J].Environmental Science:Nano,2017,4(3):679-688.
[27] Lin L,Zhai S R,Xiao Z Y,et al. Dye adsorption of mesoporous activated carbons produced from Na OH-pretreated rice husks[J].Bioresource Technology,2013,136:437-443.
[28] Le Van K,Thi T T L. Activated carbon derived from rice husk by Na OH activation and its application in supercapacitor[J].Progress in Natural Science:Materials International,2014,24(3):191-198.
[29] Shen Y F,Zhao P T,Shao Q F. Porous silica and carbon derived materials from rice husk pyrolysis char[J]. Microporous and Mesoporous Materials,2014,188:46-76.
[30] Guo Y P,Yang S F,Yu K F,et al. The preparation and mechanism studies of rice husk based porous carbon[J].Materials Chemistry and Physics,2002,74(3):320-323.
[31] Tansel B,Sager J,Rector T,et al. Significance of hydrated radius and hydration shells on ionic permeability during nanofiltration in dead end and cross flow modes[J]. Separation and Purification Technology,2006,51(1):40-47.
[32] Zhang L,Zhou Q,Liu J Y,et al. Phosphate adsorption on lanthanum hydroxide-doped activated carbon fiber[J]. Chemical Engineering Journal,2012,185-186:160-167.
[33] He Y H,Lin H,Dong Y B,et al. Simultaneous removal of ammonium and phosphate by alkaline-activated and lanthanumimpregnated zeolite[J]. Chemosphere,2016,164:387-395.
[34] Huang W Y,Li D, Liu Z Q, et al. Kinetics, isotherm,thermodynamic,and adsorption mechanism studies of La(OH)3-modified exfoliated vermiculites as highly efficient phosphate adsorbents[J]. Chemical Engineering Journal,2014,236:191-201.
[35]王宇,高宝玉,岳文文,等.改性玉米秸秆对水中磷酸根的吸附动力学研究[J].环境科学,2008,29(3):703-708.Wang Y,Gao B Y,Yue W W,et al. Adsorption kinetics of phosphate from aqueous solutions onto modified corn residue[J].Environmental Science,2008,29(3):703-708.
[36] 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.
[37] Yao W S,Millero F J. Adsorption of phosphate on manganese dioxide in seawater[J]. Environmental Science&Technology,1996,30(2):536-541.
[38] Lin J W,Zhan Y H,Wang H,et al. Effect of calcium ion on phosphate adsorption onto hydrous zirconium oxide[J]. Chemical Engineering Journal,2017,309:118-129.
[39] Atouei M T,Rahnemaie R,Kalanpa E G,et al. Competitive adsorption of magnesium and calcium with phosphate at the goethite water interface:Kinetics,equilibrium and CD-MUSIC modeling[J]. Chemical Geology,2016,437:19-29.
[40] Lin J W,Wang X X,Zhan Y H. Effect of precipitation pH and coexisting magnesium ion on phosphate adsorption onto hydrous zirconium oxide[J]. Journal of Environmental Sciences,2019,76:167-187.
[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]苗文凭,林海,卢晓君.粉煤灰吸附除磷的改性研究[J].环境工程学报,2008,2(4):502-506.Miao W P,Lin H,Lu X J. Adsorption of phosphate using modified fly ash from water solution[J]. Chinese Journal of Environmental Engineering,2008,2(4):502-506.
[4] Chitrakar R,Tezuka S,Sonoda A,et al. Selective adsorption of phosphate from seawater and wastewater by amorphous zirconium hydroxide[J]. Journal of Colloid and Interface Science,2006,297(2):426-433.
[5] Xie J,Wang Z,Lu S Y,et al. Removal and recovery of phosphate from water by lanthanum hydroxide materials[J].Chemical Engineering Journal,2014,254:163-170.
[6] Zhang M,Gao B,Yao Y,et al. Phosphate removal ability of biochar/Mg Al-LDH ultra-fine composites prepared by liquidphase deposition[J]. Chemosphere,2013,92(8):1042-1047.
[7] Cai P, Zheng H, Wang C, et al. Competitive adsorption characteristics of fluoride and phosphate on calcined Mg-Al-CO3layered double hydroxides[J]. Journal of Hazardous Materials,2012,213-214:100-108.
[8] Chen J G,Kong H N,Wu D Y,et al. Removal of phosphate from aqueous solution by zeolite synthesized from fly ash[J].Journal of Colloid and Interface Science,2006,300(2):491-497.
[9] Ye J,Cong X N,Zhang P Y, et al. Interaction between phosphate and acid-activated neutralized red mud during adsorption process[J]. Applied Surface Science,2015,356:128-134.
[10] Koilraj P,Sasaki K. Selective removal of phosphate using Laporous carbon composites from aqueous solutions:Batch and column studies[J]. Chemical Engineering Journal,2017,317:1059-1068.
[11] He Y H,Lin H,Dong Y B,et al. Preferable adsorption of phosphate using lanthanum-incorporated porous zeolite:characteristics and mechanism[J]. Applied Surface Science,2017,426:995-1004.
[12] Dong S X,Wang Y L,Zhao Y W,et al. La3+/La(OH)3loaded magnetic cationic hydrogel composites for phosphate removal:effect of lanthanum species and mechanistic study[J].Water Research,2017,126:433-441.
[13] Yang J,Zhou L,Zhao L Z,et al. A designed nanoporous material for phosphate removal with high efficiency[J]. Journal of Materials Chemistry,2011,21(8):2489-2494.
[14]袁宪正,潘纲,田秉晖,等.氯化镧改性黏土固化湖泊底泥中磷的研究[J].环境科学,2007,28(2):403-406.Yuan X Z,Pan G,Tian B H,et al. Study on phosphorus(P)fixation in the sediment of lake using the clays modified by La Cl3[J]. Environmental Science,2007,28(2):403-406.
[15] Liu J Y,Zhou Q,Chen J H,et al. Phosphate adsorption on hydroxyl-iron-lanthanum doped activated carbon fiber[J].Chemical Engineering Journal,2013,215-216:859-867.
[16] Zhang Y Y,Pan B C,Shan C,et al. Enhanced phosphate removal by nanosized hydrated La(III)oxide confined in crosslinked polystyrene networks[J]. Environmental Science&Technology,2016,50(3):1447-1454.
[17] Sizmur T,Fresno T,Akgül G,et al. Biochar modification to enhance sorption of inorganics from water[J]. Bioresource Technology,2017,246:34-47.
[18]李楠,单保庆,唐文忠,等.稻壳活性炭制备及其对磷的吸附[J].环境工程学报,2013,7(3):1024-1028.Li N,Shan B Q,Tang W Z,et al. Preparation of powder activated carbon by rice husks and its adsorption capacity to phosphorus[J]. Chinese Journal of Environmental Engineering,2013,7(3):1024-1028.
[19] Guo Y P,Rockstraw D A. Activated carbons prepared from rice hull by one-step phosphoric acid activation[J]. Microporous and Mesoporous Materials,2007,100(1-3):12-19.
[20] Genuino D A D,de Luna M D G,Capareda S C. Improving the surface properties of municipal solid waste-derived pyrolysis biochar by chemical and thermal activation:Optimization of process parameters and environmental application[J]. Waste Management,2018,72:255-264.
[21] Wang Z H,Shen D K,Shen F,et al. Phosphate adsorption on lanthanum loaded biochar[J]. Chemosphere,2016,150:1-7.
[22] Qiu H, Liang C, Yu J H, et al. Preferable phosphate sequestration by nano-La(III)(hydr)oxides modified wheat straw with excellent properties in regeneration[J]. Chemical Engineering Journal,2017,315:345-354.
[23] Yang Q, Wang X L, Luo W, et al. Effectiveness and mechanisms of phosphate adsorption on iron-modified biochars derived from waste activated sludge[J]. Bioresource Technology,2018,247:537-544.
[24] Wang J,Zhang S J,Pan B C,et al. Hydrous ferric oxide-resin nanocomposites of tunable structure for arsenite removal:effect of the host pore structure[J]. Journal of Hazardous Materials,2011,198:241-246.
[25] Yang J, Yuan P, Chen H Y, et al. Rationally designed functional macroporous materials as new adsorbents for efficient phosphorus removal[J]. Journal of Materials Chemistry,2012,22(19):9983-9990.
[26] Zhang X L, Wang Y H, Chang X F, et al. Iron oxide nanoparticles confined in mesoporous silicates for arsenic sequestration:effect of the host pore structure[J].Environmental Science:Nano,2017,4(3):679-688.
[27] Lin L,Zhai S R,Xiao Z Y,et al. Dye adsorption of mesoporous activated carbons produced from Na OH-pretreated rice husks[J].Bioresource Technology,2013,136:437-443.
[28] Le Van K,Thi T T L. Activated carbon derived from rice husk by Na OH activation and its application in supercapacitor[J].Progress in Natural Science:Materials International,2014,24(3):191-198.
[29] Shen Y F,Zhao P T,Shao Q F. Porous silica and carbon derived materials from rice husk pyrolysis char[J]. Microporous and Mesoporous Materials,2014,188:46-76.
[30] Guo Y P,Yang S F,Yu K F,et al. The preparation and mechanism studies of rice husk based porous carbon[J].Materials Chemistry and Physics,2002,74(3):320-323.
[31] Tansel B,Sager J,Rector T,et al. Significance of hydrated radius and hydration shells on ionic permeability during nanofiltration in dead end and cross flow modes[J]. Separation and Purification Technology,2006,51(1):40-47.
[32] Zhang L,Zhou Q,Liu J Y,et al. Phosphate adsorption on lanthanum hydroxide-doped activated carbon fiber[J]. Chemical Engineering Journal,2012,185-186:160-167.
[33] He Y H,Lin H,Dong Y B,et al. Simultaneous removal of ammonium and phosphate by alkaline-activated and lanthanumimpregnated zeolite[J]. Chemosphere,2016,164:387-395.
[34] Huang W Y,Li D, Liu Z Q, et al. Kinetics, isotherm,thermodynamic,and adsorption mechanism studies of La(OH)3-modified exfoliated vermiculites as highly efficient phosphate adsorbents[J]. Chemical Engineering Journal,2014,236:191-201.
[35]王宇,高宝玉,岳文文,等.改性玉米秸秆对水中磷酸根的吸附动力学研究[J].环境科学,2008,29(3):703-708.Wang Y,Gao B Y,Yue W W,et al. Adsorption kinetics of phosphate from aqueous solutions onto modified corn residue[J].Environmental Science,2008,29(3):703-708.
[36] 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.
[37] Yao W S,Millero F J. Adsorption of phosphate on manganese dioxide in seawater[J]. Environmental Science&Technology,1996,30(2):536-541.
[38] Lin J W,Zhan Y H,Wang H,et al. Effect of calcium ion on phosphate adsorption onto hydrous zirconium oxide[J]. Chemical Engineering Journal,2017,309:118-129.
[39] Atouei M T,Rahnemaie R,Kalanpa E G,et al. Competitive adsorption of magnesium and calcium with phosphate at the goethite water interface:Kinetics,equilibrium and CD-MUSIC modeling[J]. Chemical Geology,2016,437:19-29.
[40] Lin J W,Wang X X,Zhan Y H. Effect of precipitation pH and coexisting magnesium ion on phosphate adsorption onto hydrous zirconium oxide[J]. Journal of Environmental Sciences,2019,76:167-187.
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