白果壳遗态Fe/C复合材料对水中磷的吸附特征
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摘要
为研究PBGC-Fe/C-G(白果壳遗态Fe/C复合材料)对水中磷的吸附特征,以PBGC-Fe/C-G为吸附剂,对吸附剂投加量、溶液体系pH、初始磷质量浓度、温度和吸附剂粒径为影响因素进行静态吸附试验分析,并结合SEM、EDS、XRD和FT-IR等手段对吸附前、后材料进行表征,以揭示PBGC-Fe/C-G的吸附除磷机制.结果表明:①当初始磷质量浓度<10 mg/L、吸附剂投加量为0. 2g/(50 mL)、溶液为酸性(pH=3)、反应温度为45℃、吸附剂粒径<0. 149 mm时,吸附效果最佳,吸附量达1. 62 mg/g.②准二级动力学模型和Freundlich吸附等温模型能较好地模拟PBGC-Fe/C-G对磷的吸附过程.③热力学结果显示,ΔG<0、ΔS>0和ΔH>0,说明PBGC-Fe/C-G对磷的吸附过程是自发、熵增的吸热过程.研究显示,PBGC-Fe/C-G吸附除磷主要通过配位作用、静电引力、等电荷离子交换和物理作用4种协同完成,其中Fe活性位与磷酸根离子的配位反应为主要的反应过程.
The specific adsorption characteristics of phosphorus on porous biomorph-genetic composite of Fe/C with ginkgo shell template (PBGC-Fe/C-G) were studied by using PBGC-Fe/C-G as an adsorbent. Static adsorption tests were carried out to study the influencing factors of the adsorbent dosage,the pH of the solution,the initial concentration of phosphorus,and the particle size. The morphological properties of PBGC-Fe/C-G before and after the adsorption were characterized by using SEM,EDS,XRD and FT-IR. The adsorption mechanisms of phosphorus on PBGC-Fe/C-G were investigated by morphological characterization of the adsorbent combined with adsorption kinetic test. The research indicated that the maximum adsorption capacity of phosphorus on PBGC-Fe/C-G was 1. 62 mg/g under the experimental conditions: phosphorus concentration < 10 mg/L,the adsorbent dosage = 0. 2 g/ (50 mL),the solution pH = 3,reaction temperature 45 ℃,the particle size of the adsorbent< 100 mesh (< 0. 149 mm). The pseudo-second-order kinetic model and Freundlich model fit the phosphate adsorption by PBGC-Fe/C-G well. The thermodynamics results of ΔG < 0,ΔS > 0 and ΔH > 0 showed that the adsorption process of PBGC-Fe/C-G for phosphorus was a spontaneous,entropy-increasing endothermic process. The research showed that phosphorus adsorption on PBGC-Fe/C-G was accomplished cooperatively by coordination reaction,electrostatic attraction,anion exchange and physical adsorption,in which the coordination reaction between the Fe active site and the phosphate ion was the main reaction process.
The specific adsorption characteristics of phosphorus on porous biomorph-genetic composite of Fe/C with ginkgo shell template (PBGC-Fe/C-G) were studied by using PBGC-Fe/C-G as an adsorbent. Static adsorption tests were carried out to study the influencing factors of the adsorbent dosage,the pH of the solution,the initial concentration of phosphorus,and the particle size. The morphological properties of PBGC-Fe/C-G before and after the adsorption were characterized by using SEM,EDS,XRD and FT-IR. The adsorption mechanisms of phosphorus on PBGC-Fe/C-G were investigated by morphological characterization of the adsorbent combined with adsorption kinetic test. The research indicated that the maximum adsorption capacity of phosphorus on PBGC-Fe/C-G was 1. 62 mg/g under the experimental conditions: phosphorus concentration < 10 mg/L,the adsorbent dosage = 0. 2 g/ (50 mL),the solution pH = 3,reaction temperature 45 ℃,the particle size of the adsorbent< 100 mesh (< 0. 149 mm). The pseudo-second-order kinetic model and Freundlich model fit the phosphate adsorption by PBGC-Fe/C-G well. The thermodynamics results of ΔG < 0,ΔS > 0 and ΔH > 0 showed that the adsorption process of PBGC-Fe/C-G for phosphorus was a spontaneous,entropy-increasing endothermic process. The research showed that phosphorus adsorption on PBGC-Fe/C-G was accomplished cooperatively by coordination reaction,electrostatic attraction,anion exchange and physical adsorption,in which the coordination reaction between the Fe active site and the phosphate ion was the main reaction process.
引文
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[6]魏泽军,谢建平,黄玉明.潜流人工湿地演变对废水中有机物、氮及磷去除的影响[J].环境科学,2012,33(11):3812-3819.WEI Zejun,XIE Jianping,HUANG Yuming.Effects of subsurface flow constructed wetland on the removal of organic matter,nitrogen and phosphorus in wastewater[J].Environmental Science,2012,33(11):3812-3819.
[7]ZHU Zongqiang,ZENG Honghu,ZHU Yinian,et al.Kinetics and thermodynamic study of phosphate adsorption on the porous biomorph-genetic composite ofα-Fe2O3Fe3O4C with eucalyptus wood microstructure[J].Separation and Purification Technology,2013,117(5):124-130.
[8]JIA Yunsheng,WANG Huoyan,ZHAO Xuesong,et al.Kinetics,isotherms and multiple mechanisms of the removal for phosphate by Cl-hydrocalumite[J].Applied Clay Science,2016,129(8):116-121.
[9]杨孟娟,林建伟,詹艳慧,等.铝和锆改性沸石对太湖底泥-水系统中溶解性磷酸盐的固定作用[J].环境科学研究,2014,27(11):1351-1359.YANG Mengjuan,LIN Jianwei,ZHAN Yanhui,et al.Immobilization of dissolved phosphates in sediment-water system of Taihu Lake by aluminum and zirconium modified zeolites[J].Research of Environmental Sciences,2014,27(11):1351-1359.
[10]JIAN Chen,YAN Liangguo,YU Haiqin,et al.Efficient removal of phosphate by facile prepared magnetic diatomite and illite clay from aqueous solution[J].Chemical Engineering Journal,2016,287(3):162-172.
[11]ZHANG Ling,WAN Lihua,CHANG Ning,et al.Removal of phosphate from water by activated carbon fiber loaded with lanthanum oxide[J].Journal of Hazardous Materials,2011,190(1):848-855.
[12]何世颖,冯彦房,周玉玲,等.Fe3O4BC复合材料的制备及其吸附除磷性能[J].环境科学研究,2018,31(1):143-153.HE Shiying,FENG Yanfang,ZHOU Yuling,et al.Preparation of Fe3O4BC composites and their phosphorus removal performance[J].Research of Environmental Sciences,2018,31(1):143-153.
[13]HUANG Xiao.Intersection of isotherms for phosphate adsorption on hematite[J].Journal of Colloid&Interface Science,2004,271(2):296-307.
[14]TORRENT J,SCHWERTMANN U,BARRON V.Phosphate sorption by natural hematites[J].European Journal of Soil Science,2010,45(1):45-51.
[15]LIU C,HUANG P M.Kinetics of phosphate adsorption on iron oxides formed under the influence of citrate[J].Canadian Journal of Soil Science,2000,80(3):445-454.
[16]修瑞瑞,何世颖,宋海亮,等.改性硅藻土负载纳米零价铁去除水中硝酸盐氮[J].化工学报,2016,67(9):3888-3894.XIU Ruirui,HE Shiying,SONG Hailiang,et al.Removal of nitrate nitrogen from water by modified diatomite loaded with nano-zerovalent iron[J].CIESC Journal,2016,67(9):3888-3894.
[17]XUAN Shouhu,ZENG Suyuan,FAN Meiqiang,et al.One-step method of fabricating Fe3O4montmorillonite magnetic nanocomposites[J].Rare Metal Materials&Engineering,2010,39(4):165-168.
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[19]FARMANY A,MORTAZAVI S S,MAHDAVI H.Ultrasond-assisted synthesis of Fe3O4SiO2coreshell with enhanced adsorption capacity for diazinon removal[J].Journal of Magnetism&Magnetic Materials,2016,416(10):75-80.
[20]苏鹃,伍钧,杨刚,等.改性白果壳对水溶液中重金属镉的吸附研究[J].农业环境科学学报,2014,33(6):1218-1225.SU Juan,WU Jun,YANG Gang,et al.Adsorption of heavy metal cadmium in aqueous solution by modified ginkgo husk[J].Journal of Agro-Environment Science,2014,33(6):1218-1225.
[21]朱宗强,朱义年,韦文慧,等.一种毛竹遗态Fe2O3Fe3O4复合重金属吸附剂的制备方法:ZL201210446693.8[P].2012-11-11.
[22]国家环境保护总局.水和废水监测分析方法[M].4版.北京:中国环境科学出版社,2007.
[23]ZHU Yinian,JIANG Yanhong,ZHU Zongqiang,et al.Preparation of a porous hydroxyapatite-carbon composite with the bio-template of sugarcane top stems and its use for the Pb(Ⅱ)removal[J].Journal of Cleaner Production,2018,187(3):650-661
[24]BISWAS B K,INOUE K,GHIMIRE K N,et al.The adsorption of phosphate from an aquatic environment using metal-loaded orange waste[J].Journal of Colloid and Interface Science,2007,312(2):214-223.
[25]LI R,WANG J J,ZHOU B,et al.Enhancing phosphate adsorption by MgAl layered double hydroxide functionalized biochar with different MgAl ratios[J].Science of the Total Environment,2016,559(3):121-129.
[26]LIU Yun,SHENG Xia,DONG Yuanhua,et al.Removal of highconcentration phosphate by calcite:effect of sulfate and p H[J].Desalination,2012,289(1):66-71.
[27]徐建林,淡小敏,王程程,等.不同粒径的锑纳米颗粒在润滑油中的分散性与摩擦性能[J].材料热处理学报,2016,37(8):209-214.XU Jianlin,DAN Xiaomin,WANG Chengcheng,et al.Dispersibility and friction properties of niobium nanoparticles with different particle sizes in lubricating oils[J].Journal of Materials Processing,2016,37(8):209-214.
[28]李超,朱宗强,曹爽,等.桉树遗态结构HAPC复合材料对水中Cu(Ⅱ)的吸附特征[J].环境科学,2017,38(3):1074-1084.LI Chao,ZHU Zongqiang,CAO Shuang,et al.Adsorption characteristics of Cu(II)in Water by HAPC composites of eucalyptus structure[J].Environmental Science,2017,38(3):1074-1084.
[29]JIANG Hualin,CHEN Pinghua,LUO Shenglian,et al.Synthesis of novel nanocomposite Fe3O4ZrO2chitosan and its application for removal of nitrate and phosphate[J].Applied Surface Science,2013,284(4):942-949.
[30]BOPARAI H K,JOSEPH M,O'CARROLL D M.Kinetics and thermodynamics of cadmium ion removal by adsorption onto nano zerovalent iron particles[J].Journal of Hazardous Materials,2011,186(1):458-465.
[31]YANG Jinbei,YU Meiqiong,QIU Ting.Adsorption thermodynamics and kinetics of Cr(Ⅵ)on KIP210 resin[J].Journal of Industrial and Engineering Chemistry,2014,20(2):480-486.
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