磁性生物炭对水体中对硝基苯酚的吸附特性
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摘要
为了制备同时具备磁分离和优良吸附性能的环境友好吸附材料,以棉花秸秆为生物质原料制备生物炭(CSBC),采用共沉淀法制得磁性棉花秸秆生物炭(MCSBC).通过元素分析、SEM、XRD、XPS、FTIR和VSM等对MCSBC进行表征,研究了CSBC和MCSBC对水中对硝基苯酚(PNP)的吸附特性.结果表明,溶液pH值对CSBC和MCSBC吸附PNP的影响较大,在酸性条件下的吸附量更大.CSBC和MCSBC对PNP的吸附动力学过程可被准二级动力学模型很好地描述,吸附过程包括液膜扩散和颗粒内扩散两个阶段.Langmuir、Freundlich和Sips模型都可以很好地描述PNP在CSBC和MCSBC上的吸附行为,最大吸附量分别为44.54和48.94mg/g,MCSBC相较于CSBC对PNP的吸附具有更好的效果.热力学研究结果表明,CSBC和MCSBC对PNP的吸附过程为熵增加的自发吸热过程.再生试验结果表明,经6次吸附-解吸循环后,MCSBC对PNP的吸附容量仍能达到初始吸附量的82%.
In order to obtain environmentally friendly adsorbent with magnetic separation and excellent adsorption characteristics, biochar(CSBC) was prepared from cotton straw, and magnetic cotton straw biochar(MCSBC) was prepared by co-precipitation method. CSBC and MCSBC were characterized by SEM, XRD, XPS, FTIR, VSM, and element analysis. The adsorption characteristics of PNP in aqueous solution using CSBC and MCSBC were investigated. The results showed that the pH value of the solution had a great influence on the adsorption of PNP by CSBC and MCSBC, and the adsorption capacity was greater under acidic conditions. Adsorption process of PNP by CSBC and MCSBC can be well fitted by the pseudo-second-order kinetic model. The adsorption process includes two stages: liquid film diffusion and intra-particle diffusion. Langmuir, Freundlich, and Sips models described the adsorption behavior well. The maximum adsorption capacity of CSBC and MCSBC for PNP were 44.54 and 48.94mg/g, respectively. The adsorption capacity of MCSBC was higher than that of the CSBC. Thermodynamic parameters indicated that the adsorption process of PNP onto CSBC and MCSBC was spontaneous with increased entropy and endothermic. The regeneration studies indicated that MCSBC kept 82% of its initial PNP adsorption capacity at the sixth adsorption/desorption cycle.
In order to obtain environmentally friendly adsorbent with magnetic separation and excellent adsorption characteristics, biochar(CSBC) was prepared from cotton straw, and magnetic cotton straw biochar(MCSBC) was prepared by co-precipitation method. CSBC and MCSBC were characterized by SEM, XRD, XPS, FTIR, VSM, and element analysis. The adsorption characteristics of PNP in aqueous solution using CSBC and MCSBC were investigated. The results showed that the pH value of the solution had a great influence on the adsorption of PNP by CSBC and MCSBC, and the adsorption capacity was greater under acidic conditions. Adsorption process of PNP by CSBC and MCSBC can be well fitted by the pseudo-second-order kinetic model. The adsorption process includes two stages: liquid film diffusion and intra-particle diffusion. Langmuir, Freundlich, and Sips models described the adsorption behavior well. The maximum adsorption capacity of CSBC and MCSBC for PNP were 44.54 and 48.94mg/g, respectively. The adsorption capacity of MCSBC was higher than that of the CSBC. Thermodynamic parameters indicated that the adsorption process of PNP onto CSBC and MCSBC was spontaneous with increased entropy and endothermic. The regeneration studies indicated that MCSBC kept 82% of its initial PNP adsorption capacity at the sixth adsorption/desorption cycle.
引文
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[17]Chiou C T,Cheng J Z,Hung W-N,et al.Resolution of adsorption and partition components of organic compounds on black carbons[J].Environmental Science&Technology,2015,49(15):9116-9123.
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[19]Zhao H X,Lang Y H.Behaviors and mechanisms of CIP and OFLadsorption by magnetic biochar[J].Environmental Science,2018,39(8):3729-3735.
[20]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.
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[22]Ma Y,Zhou Q,Li A M,et al.Preparation of a novel magnetic microporous adsorbent and its adsorption behavior of p-nitrophenol and chlorotetracycline[J].Journal of Hazardous Materials,2014,266:84-93.
[23]Zheng H S,Guo W Q,Li S,et al.Adsorption of p-nitrophenols(PNP)on microalgal biochar:Analysis of high adsorption capacity and mechanism[J].Bioresource Technology,2017,244:1456-1464.
[24]席志楠,李增波,王聪颖,等.磁性生物质炭对水体中芘的去除效果研究[J].农业环境科学学报,2017,36(1):176-182.Xi Z N,Li Z B,Wang C Y,et al.The removal effect of magnetic biochar on pyrene in aqueous phase[J].Journal of Agro-Environment Science,2017,36(1):176-182.
[25]Jia Z Q,Jiang M C,Wu G R.Amino-MIL-53(Al)sandwich-structure membranes for adsorption of p-nitrophenol from aqueous solutions[J].Chemical Engineering Journal,2017,307:283-290.
[26]王志凯,张胜利,陈豪宇,等.磁性PEI功能化秸秆的制备及对Pb(Ⅱ)的吸附[J].环境科学研究,2017,30(8):1316-1324.Wang Z K,Zhang S L,Chen H Y,et al.Preparation of magnetic polyethyleneimine functionalized rice straw and its adsorption properties for Pb(Ⅱ)ions[J].Research of Environmental Sciences,2017,30(8):1316-1324.
[27]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 o f p-nitrophenol by biochars of corncob prepared at different pyrolysis temperatures[J].Environmental Science,2017,38(2):837-844.
[28]Cotoruelo L M,Marqués M D,Díaz F J,et al.Adsorbent ability of lignin-based activated carbons for the removal of p-nitrophenol from aqueous solutions[J].Chemical Engineering Journal,2012,184:176-183.
[29]Xue G H,Gao M L,Gu Z,et al.The removal of p-nitrophenol from aqueous solutions by adsorption using gemini surfactants modified montmorillonites[J].Chemical Engineering Journal,2013,218:223-231.
[2]dos Santos A,Viante M F,Pochapski D J,et al.Enhanced removal of p-nitrophenol from aqueous media by montmorillonite clay modified with a cationic surfactant[J].Journal of Hazardous Materials,2018,355:136-144.
[3]álvarez-Torrellas S,Martin-Martinez M,Gomes H T,et al.Enhancement of p-nitrophenol adsorption capacity through N2-thermal-based treatment of activated carbons[J].Applied Surface Science,2017,414:424-434.
[4]Shao L S,Huang J H.Controllable synthesis of N-vinylimidazolemodified hyper-cross-linked resins and their efficient adsorption of p-nitrophenol and o-nitrophenol[J].Journal of Colloid and Interface Science,2017,507:42-50.
[5]任爽,孟昭福,王腾,等.阳(阴)离子复配修饰两性磁性膨润土的表面特征差异及对苯酚吸附的影响[J].环境科学,2018,39(1):187-194.Ren S,Meng S F,Wang T,et al.Comparison of amphoteric-cationic and amphoteric-anionic modified magnetic bentonites:characterization and sorption capacity of phenol[J].Environmental Science,2018,39(1):187-194.
[6]Chen B L,Zhou D D,Zhu L Z.Transitional adsorption and partition of nonpolar and polar aromatic contaminants by biochars of pine needles with different pyrolytic temperatures[J].Environmental Science&Technology,2008,42(14):5137-5143.
[7]Oliveira F R,Patel A K,Jaisi D P,et al.Environmental application of biochar:Current status and perspectives[J].Bioresource Technology,2017,246:110-122.
[8]张如玉,刘海波,邹雪华,等.小麦秸秆驱动菱铁矿热解制备磁性生物质碳及其吸附Cd2+活性[J].环境科学,2017,38(8):3519-3528.Zhang R Y,Liu H B,Zou X H,et al.Preparation of magnetic biomass carbon by thermal decomposition of siderite deriven by wheat straw and its adsorption on cadmium[J].Environmental Science,2017,38(8):3519-3528.
[9]Mohan D,Sarswat A,Ok Y S,et al.Organic and inorganic contaminants removal from water with biochar,a renewable,low cost and sustainable adsorbent-a critical review[J].Bioresource Technology,2014,160:191-202.
[10]杜文琪,曹玮,周航,等.磁性生物炭对重金属污染废水处理条件优化及机理[J].环境科学学报,2018,38(2):492-500.Du W Q,Cao W,Zhou H,et al.Optimization and the mechanism treatment of heavy metals wastewater magnetic biochar[J].Acta Scientiae Circumstantiae,2018,38(2):492-500.
[11]杨姗也,王祥学,陈中山,等.四氧化三铁基纳米材料制备及对放射性元素和重金属离子的去除[J].化学进展,2018,30(2/3):225-242.Yang S Y,Wang X X,Chen Z S,et al.Synthesis of Fe3O4-based nanomaterials and their application in the removal of radionuclides and heavy metal ions[J].Progress in Chemistry,2018,30(2/3):225-242.
[12]Reguyal F,Sarmah A K.Adsorption of sulfamethoxazole by magnetic biochar:Effects of pH,ionic strength,natural organic matter and17α-ethinylestradiol[J].Science of the Total Environment,2018,628-629:722-730.
[13]阮长平,艾可龙,逯乐慧.耐酸性的磁性纳米复合材料去除水中有机污染物[J].分析化学,2016,44(2):224-231.Ruan C P,Ai K L,Lu L H.An acid-resistant magnetic Co/C nanocomposite for adsorption and separation of organic contaminants from water[J].Chinese Journal of Analytical Chemistry,2016,44(2):224-231.
[14]Son E-B,Poo K-M,Chang J-S,et al.Heavy metal removal from aqueous solutions using engineered magnetic biochars derived from waste marine macro-algal biomass[J].Science of the Total Environment,2018,615:161-168.
[15]Du S-k,Zhu X N,Wang H,et al.High pressure assist-alkali pretreatment of cotton stalk and physiochemical characterization of biomass[J].Bioresource Technology,2013,148:494-500.
[16]Xiong S W,Zhang S Y,Wu Q M,et al.Investigation on cotton stalk and bamboo sawdust carbonization for barbecue charcoal preparation[J].Bioresource Technology,2014,152:86-92.
[17]Chiou C T,Cheng J Z,Hung W-N,et al.Resolution of adsorption and partition components of organic compounds on black carbons[J].Environmental Science&Technology,2015,49(15):9116-9123.
[18]赵华轩,郎印海.磁性生物炭对水中CIP和OFL的吸附行为和机制[J].环境科学,2018,39(8):3729-3735.
[19]Zhao H X,Lang Y H.Behaviors and mechanisms of CIP and OFLadsorption by magnetic biochar[J].Environmental Science,2018,39(8):3729-3735.
[20]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.
[21]Yang K,Jiang Y,Yang J J,et al.Correlations and adsorption mechanisms of aromatic compounds on biochars produced from various biomass at 700°C[J].Environmental Pollution,2018,233:64-70.
[22]Ma Y,Zhou Q,Li A M,et al.Preparation of a novel magnetic microporous adsorbent and its adsorption behavior of p-nitrophenol and chlorotetracycline[J].Journal of Hazardous Materials,2014,266:84-93.
[23]Zheng H S,Guo W Q,Li S,et al.Adsorption of p-nitrophenols(PNP)on microalgal biochar:Analysis of high adsorption capacity and mechanism[J].Bioresource Technology,2017,244:1456-1464.
[24]席志楠,李增波,王聪颖,等.磁性生物质炭对水体中芘的去除效果研究[J].农业环境科学学报,2017,36(1):176-182.Xi Z N,Li Z B,Wang C Y,et al.The removal effect of magnetic biochar on pyrene in aqueous phase[J].Journal of Agro-Environment Science,2017,36(1):176-182.
[25]Jia Z Q,Jiang M C,Wu G R.Amino-MIL-53(Al)sandwich-structure membranes for adsorption of p-nitrophenol from aqueous solutions[J].Chemical Engineering Journal,2017,307:283-290.
[26]王志凯,张胜利,陈豪宇,等.磁性PEI功能化秸秆的制备及对Pb(Ⅱ)的吸附[J].环境科学研究,2017,30(8):1316-1324.Wang Z K,Zhang S L,Chen H Y,et al.Preparation of magnetic polyethyleneimine functionalized rice straw and its adsorption properties for Pb(Ⅱ)ions[J].Research of Environmental Sciences,2017,30(8):1316-1324.
[27]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 o f p-nitrophenol by biochars of corncob prepared at different pyrolysis temperatures[J].Environmental Science,2017,38(2):837-844.
[28]Cotoruelo L M,Marqués M D,Díaz F J,et al.Adsorbent ability of lignin-based activated carbons for the removal of p-nitrophenol from aqueous solutions[J].Chemical Engineering Journal,2012,184:176-183.
[29]Xue G H,Gao M L,Gu Z,et al.The removal of p-nitrophenol from aqueous solutions by adsorption using gemini surfactants modified montmorillonites[J].Chemical Engineering Journal,2013,218:223-231.