生物炭负载纳米羟基磷灰石复合材料的制备及对铅离子的吸附特性
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摘要
以玉米秸秆为前体,在高温限氧条件下,将纳米羟基磷灰石(nano-HAP)负载于生物炭(BC)表面制备出了生物炭负载纳米羟基磷灰石(n HAP/BC)复合材料,并利用SEM、XRD和FTIR对其进行表征。批量吸附实验考察其对Pb~(2+)的吸附特性,研究pH、投加量、吸附时间、初始浓度及吸附温度等因素对吸附的影响。通过吸附动力学、吸附等温线和吸附热力学分析了吸附特性,通过解吸实验考察了解吸再生效应,并对吸附机制进行了探讨。结果表明:与BC相比,n HAP/BC复合材料具备更好的吸附效果,25℃时理论最大吸附量为383.75mg/g。n HAP/BC对Pb~(2+)的吸附符合拟二级动力学方程和Langmuir等温吸附模型,表明n HAP/BC对Pb~(2+)的吸附为单分子层化学吸附。热力学参数ΔG<0、ΔH>0,表明吸附是一个自发的吸热过程。n HAP/BC对Pb~(2+)的吸附机制主要包括nano-HAP的溶解-沉淀作用以及生物炭表面—OH和—COOH等含氧官能团的络合作用。n HAP/BC具有良好的循环利用能力,是一种潜在的Pb~(2+)高效吸附材料。
A novel composite material of biochar-supported nano-hydroxyapatiten(n HAP/BC) with the maize straw as the precursors was successfully fabricated by loading nano-hydroxyapatite(nano-HAP) on the surface of biochar(BC) at high temperature and in oxygen-limited atmosphere. The physicochemical properties of the n HAP/BC were characterized. Batch adsorption experiments were conducted to investigate the effect of pH values, contact time, temperature and initial Pb~(2+)concentration on the adsorption performance. The adsorption characteristics were analyzed from the aspects of kinetics, isotherms and thermodynamics, while the regeneration was investigated by desorption experiments. Following that, the adsorption mechanism was discussed. The results showed that the n HAP/BC had strong adsorption ability to Pb~(2+) with the maximum adsorption capacities of 383.75 mg/g at 25℃, which was significantly higher than that of the BC. The adsorption of Pb~(2+) onto n HAP/BC followed the pseudo-second-order kinetics equation and Langmuir isotherm, indicating that the adsorption process was a mono-molecular chemical adsorption. The ΔG was negative while the ΔH was positive, indicating a spontaneous and endothermic adsorption. The adsorption mechanism included the dissolution-precipitation of n HAP and the complexation of oxygen-containing functional groups. The n HAP/BC showed good regeneration ability, and thus is a promosing adsorption material for the efficient removal of Pb~(2+) from waste water.
A novel composite material of biochar-supported nano-hydroxyapatiten(n HAP/BC) with the maize straw as the precursors was successfully fabricated by loading nano-hydroxyapatite(nano-HAP) on the surface of biochar(BC) at high temperature and in oxygen-limited atmosphere. The physicochemical properties of the n HAP/BC were characterized. Batch adsorption experiments were conducted to investigate the effect of pH values, contact time, temperature and initial Pb~(2+)concentration on the adsorption performance. The adsorption characteristics were analyzed from the aspects of kinetics, isotherms and thermodynamics, while the regeneration was investigated by desorption experiments. Following that, the adsorption mechanism was discussed. The results showed that the n HAP/BC had strong adsorption ability to Pb~(2+) with the maximum adsorption capacities of 383.75 mg/g at 25℃, which was significantly higher than that of the BC. The adsorption of Pb~(2+) onto n HAP/BC followed the pseudo-second-order kinetics equation and Langmuir isotherm, indicating that the adsorption process was a mono-molecular chemical adsorption. The ΔG was negative while the ΔH was positive, indicating a spontaneous and endothermic adsorption. The adsorption mechanism included the dissolution-precipitation of n HAP and the complexation of oxygen-containing functional groups. The n HAP/BC showed good regeneration ability, and thus is a promosing adsorption material for the efficient removal of Pb~(2+) from waste water.
引文
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[2]OH C,HAN Y S,PARK J H,et al.Field application of selective precipitation for recovering Cu and Zn in drainage discharged from an operating mine[J].Science of the Total Environment,2016,557/558:212-220.
[3]BOHLI T,OUEDEMI A.Improvement of oxygen-containing functional groups on olive stones activated carbon by ozone and nitric acid for heavy metals removal from aqueous phase[J].Environmental Science&Pollution Research International,2016,23(16):1-10.
[4]翟世民,柳荣展,郭雪松,等.污水处理厂污泥制备生物炭及应用的研究进展[J].化工进展,2016,35(s1):363-368.ZHAI S M,LIU R Z,GUO X S,et al.Researches progress and application development of sewage sludge biochar[J].Chemical Industry and Engineering Progress,2016,35(s1):363-368.
[5]余伟光,黎吉辉,王敦,等.香蕉茎秆生物炭的制备及其对铜离子的吸附特性[J].化工进展,2017,36(4):1499-1505.YU W G,LI J H,WANG D,et al.The preparation of biochar from pre-oxidation of banana stem and its adsorption of Cu2+[J].Chemical Industry Engineering Progress,2017,36(4):1499-1505.
[6]GUNATILAKE S K,CHANDRAJITH R.Desalination and water treatment removal of Pb(Ⅱ)from contaminated water using low-temperature pyrolyzed agricultural and forest waste biochars:a comparative study[J].Desalination&Water Treatment,2017,62:316-324.
[7]LIU C,YAN C,ZHOU S,et al.Fabrication of sponge biomass adsorbent through UV-induced surface-initiated polymerization for the adsorption of Ce(Ⅲ)from wastewater[J].Water Science&Technology:A Journal of the International Association on Water Pollution Research,2017,75(12):2755.
[8]SUZUKI T,OKITA M,KAKOYAMA S,et al.Preferential adsorption and surface precipitation of lead(Ⅱ)ions onto anatase in artificially contaminated Dixie clay[J].Journal of Hazardous Materials,2017,338:482.
[9]SHAHATA M M.Adsorption of some heavy metal ions by used different immobilized substances on silica gel[J].Arabian Journal of Chemistry,2011,9(6):755-763.
[10]ZHAO Y.Review of the natural,modified,and synthetic zeolites for heavy metals removal from wastewater[J].Environmental Engineering Science,2016,33(7):443-454.
[11]IBRAHIM H S,JAMIL T S,HEGAZY E Z.Application of zeolite prepared from Egyptian kaolin for the removal of heavy metals:Ⅱ.Isotherm models[J].Journal of Hazardous Materials,2010,182(1/2/3):842-847.
[12]王彬斌,林景东,万顺利,等.氧化镁基生物质炭高效去除水体中磷的特性[J].环境科学,2017,38(7):2859-2867.WANG B B,LIN J D,WAN S L,et al.Mg O-biochar for the adsorption of phosphate in water[J].Environmental Science,2017,38(7):2859-2867.
[13]UCHIMIYA M.Influence of pyrolysis temperature on biochar property and function as a heavy metal sorbent in soil[J].J.Agric.Food Chem.,2011.59(6):2501-2510.
[14]胡田田,仓龙,王玉军,等.铅和铜离子在纳米羟基磷灰石上的竞争吸附动力学研究[J].环境科学,2012,33(8):2875-2881.HU T T,CANG L,WANG Y J,et al.Competitive adsorption kinetics of aqueous Pb2+and Cu2+on Nano-HAP surfaces[J].Environmental Science,2012,33(8):2875-2881.
[15]董黎静,朱志良,仇雁翎,等.羟基磷灰石及其复合材料对重金属的吸附研究进展[J].化学通报,2013,76(5):405-410.DONG L J,ZHU Z L,QIU Y L,et al.Advance in research of heavy metals removal by hydroxyapatite and its composite[J].Chemistry,2013,76(5):405-410.
[16]SUZUKI T,HATSUSHIKA T,HAYAKAWA Y.Synthetic hydroxyapatites employed as inorganic cation-exchangers[J].J.Chem.Soc.Faraday Trans,1981,5(5):1059-1062.
[17]郭佳丽,韩颖超,徐磊,等.纳米羟基磷灰石复合材料作为污水处理吸附剂的研究进展[J].硅酸盐通报,2016,35(8):2466-2475.GUO J L,HAN Y C,XU L,et al.Nano-hydroxyapatite composite materials as adsorbents in wastewater treatment[J].Bulletin of the Chinese Ceramic Society,2016,35(8):2466-2475.
[18]DONG L J,ZHU Z L,QIU Y L,et al.Removal of lead from aqueous solution by hydroxyapatite/magnetite composite adsorbent[J].Chemical Engineering Journal,2010,165(3):827-834.
[19]YANG Z,FANG Z,TSANG P E,et al.In situ remediation and phytotoxicity assessment of lead-contaminated soil by biocharsupported n HAP[J].Journal of Environmental Management,2016,182:247.
[20]刘莹.功能性纳米羟基磷灰石的制备、表征及性能研究[D].长春:吉林大学,2009.LIU Y.Preparation,characterization and properties of functional nano-hydroxyapatite[D].Changchun:Jilin University,2009.
[21]LEHMANN J D,JOSEPH S.Biochar for environmental management:science and technology[J].Science and Technology:Earthscan,2009,25(1):15801-15811.
[22]YANG Z,FANG Z,ZHENG L,et al.Remediation of lead contaminated soil by biochar-supported nano-hydroxyapatite[J].Ecotoxicology&Environmental Safety,2016,132:224-230.
[23]MOUSA S M,AMMARA N S,IBRAHIM H A.Removal of lead ions using hydroxyapatite nano-material prepared from phosphogypsum waste[J].Journal of Saudi Chemical Society,2016,20(3):357-365.
[24]WEI Q,LU J,AI H,et al.Novel method for the fabrication of multiscale structure collagen/hydroxyapatite-microsphere composites based on Ca CO3,microparticle templates[J].Materials Letters,2012,80:91-94.
[25]GUO Y P,YAO Y B,NING C Q,et al.Fabrication of mesoporous carbonated hydroxyapatite microspheres by hydrothermal method[J].Materials Letters,2011,65(14):2205-2208.
[26]AHMAD M,LEE S S,DOU X,et al.Effects of pyrolysis temperature on soybean stover-and peanut shell-derived biochar properties and TCE adsorption in water[J].Bioresource Technology,2012,118(8):536-544.
[27]杜文慧,朱维琴,潘晓慧,等.牛粪源蚓粪及其生物炭对Pb2+、Cd2+的吸附特性[J].环境科学,2017,38(5):2172-2181.DU W H,ZHU W Q,PAN X H,et al.Adsorption of Pb2+and Cd2+from aqueous solution using vermicompost derived from cow manure and its biochar[J].Environment Science,2017,38(5):2172-2181.
[28]LIAO D,WEI Z,LI X,et al.Removal of lead(Ⅱ)from aqueous solutions using carbonate hydroxyapatite extracted from eggshell waste[J].Journal of Hazardous Materials,2010,177(1/2/3):126.
[29]YAN Y,WANG Y P,SUN X,et al.Optimizing production of hydroxyapatite from alkaline residue for removal of Pb2+from wastewater[J].Applied Surface Science,2014,317:946-954.
[30]SITKO R,ZAWISZA B,MALICKA E.Modification of carbon nanotubes for preconcentration,separation and determination of trace-metal ions[J].Trac.Trends in Analytical Chemistry,2012,37(37):22-31.
[31]SENTURK H B,OZDES D,GUNDOGDU A,et al.Removal of phenol from aqueous solutions by adsorption onto organomodified Tirebolu bentonite:equilibrium,kinetic and thermodynamic study[J].Journal of Hazardous Materials,2009,172(1):353-362.
[32]RAO M M,RAMESH A,RAO G P,et al.Removal of copper and cadmium from the aqueous solutions by activated carbon derived from Ceiba pentandra hulls[J].Journal of Hazardous Materials,2006,129(1/2/3):123-129.
[33]JAVANBAKHT V,GHOREISHI S M,HABIBI N,et al.A novel magnetic chitosan/clinoptilolite/magnetite nanocomposite for highly efficient removal of Pb(Ⅱ)ions from aqueous solution[J].Powder Technology,2016,302:372-383.
[34]李瑞月,陈德,李恋卿,等.不同作物秸秆生物炭对溶液中Pb2+、Cd2+的吸附[J].农业环境科学学报,2015,34(5):1001-1008.LI R Y,CHEN D,LI L Q,et al.Adsorption of Pb 2+and Cd 2+in aqueous solution by biochars derived from different crop residues[J].Journal of Agro-Environment Science,2015,34(5):1001-1008.
[35]GOOGERDCHIAN F,MOHEB A,EMADI R.Lead sorption properties of nanohydroxyapatite-alginate composite adsorbents[J].Chemical Engineering Journal,2012,200/201/202(16):471-479.
[36]ZHUANG F,TAN R,SHEN W,et al.Monodisperse magnetic hydroxyapatite/Fe3O4 microspheres for removal of lead(Ⅱ)from aqueous solution[J].Journal of Alloys and Compounds,2015,637:531-537.
[37]黄明,李绍峰,鲁秀国,等.磁性高岭土的制备及对铅离子的吸附[J].环境工程学报,2016,10(11):6439-6445.HUANG M,LI S F,LU X G,et al.Synthesis of magnetic kaolin and adsorption of lead(Ⅱ)[J].Chinese Journal of Environmental Engineering,2016,10(11):6439-6445.
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