纳米磁铁矿/生物质炭催化对Fenton氧化降解苯酚的增强机理
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摘要
以生物质炭负载纳米磁铁矿(nMBC)作为催化剂,采用非均相Fenton反应体系对模拟苯酚废水进行氧化降解处理研究,确定n MBC—Fenton法处理苯酚废水的最佳工艺条件,并揭示其强化机理。实验结果表明:对于质量浓度为50 mg/L的苯酚废水,其最佳降解条件为温度为45℃,pH为3.0,H_2O_2浓度为5 mmol/L,nMBC用量为2.0 g/L。反应进行20 min后,苯酚去除率可达约100%。nMBC剂量、废水初始pH和温度等因素均对处理效果有较大影响,其中pH决定苯酚去除率,而nMBC剂量是影响降解速率的主要因素。此外,nMBC—Fenton法催化氧化降解苯酚过程符合准一级动力学反应(R~2>0.97)。
The phenol in a simulant wastewater was treated via oxidative degradation in a heterogeneous Fenton reaction system with the biochar supported nano-zero valent iron material( n MBC) as the catalyst,in oder to determine the optimal process conditions. The experimental results showed that for the phenol wastewater with the concentration of 50 mg/L,the optimum condition for the phenol degradation( i. e.,100% removed after 20 min) was temperature 45 ℃,pH = 3. 0,H_2O_2= 5 mmol/L,and n MBC dosage = 2. 0 g/L. Moreover,n MBC-Fenton method could remove phenol in a relatively short period of reaction time. Apparently,factors such as n MBC dosage,initial pH value and temperature had greater effect on the reaction. Among them,pH value determined the phenol removal rate,while n MBC dosage as one dominant factor,affecting the degradation rate. Under the abovementioned condition,the relevant phenol degradation followed the pseudo-first-order kinetics( R2>0. 97) in the heterogeneous Fenton system with the presence of nanomagnetite/biochar composites.
The phenol in a simulant wastewater was treated via oxidative degradation in a heterogeneous Fenton reaction system with the biochar supported nano-zero valent iron material( n MBC) as the catalyst,in oder to determine the optimal process conditions. The experimental results showed that for the phenol wastewater with the concentration of 50 mg/L,the optimum condition for the phenol degradation( i. e.,100% removed after 20 min) was temperature 45 ℃,pH = 3. 0,H_2O_2= 5 mmol/L,and n MBC dosage = 2. 0 g/L. Moreover,n MBC-Fenton method could remove phenol in a relatively short period of reaction time. Apparently,factors such as n MBC dosage,initial pH value and temperature had greater effect on the reaction. Among them,pH value determined the phenol removal rate,while n MBC dosage as one dominant factor,affecting the degradation rate. Under the abovementioned condition,the relevant phenol degradation followed the pseudo-first-order kinetics( R2>0. 97) in the heterogeneous Fenton system with the presence of nanomagnetite/biochar composites.
引文
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[19]王娟,杨再福.Fenton氧化在废水处理中的应用[J].环境科学与技术,2011,34(11):104-108.
[20]蒋芬芬,吴宏海,成思敏,等.针铁矿非均相Fenton法降解抗生素的研究[J].华南师范大学学报(自然科学版),2013,45(5):83-88.
[2]尹宏生,张婷,刘佳媛.UV/Fenton氧化法对苯酚氧化效果的实验研究[J].化工科技,2010,18(1):10-12.
[3]Zhang W X.Nanoscale iron particles for environmental remediation:An overview[J].Journal of Nanoparticle Research,2003,5(3/4):323-332.
[4]潘峰,尤奇中,王万峰,等.粉末炭负载纳米铁去除水中橙黄G的研究[J].科学技术与工程,2013,13(24):26-30.
[5]Ponder S M,Darab J G,Bucher J,et al.Surface chemistry andelectrochemistry of supported zerovalent iron nanoparticles in theremediation of aqueous metal contaminants[J].Chemistry of Materials,2001,13(2):479-486.
[6]Zhou Y M,Gao B,Zimmerman A R,et al.Biocharsupportedzerovalent iron for removal of various contaminants from aqueous solutions[J].Bioresource Technology,2014,152:538-542.
[7]Wu L M,Liao L B,LüG C,et al.Micro-electrolysis of Cr(Ⅵ)in the nanoscale zero-valent iron loaded activated carbon[J].Journal of Hazardous Materials,2013,254/255:277-283.
[8]刘一帆,成思敏,吴宏海,等.铁柱撑蒙脱石非均相UV/Fenton反应对模拟橙黄G染料废水的脱色机理研究[J].华南师范大学学报,2014,46(2):72-79.
[9]樊明德,袁鹏,陈天虎,等.蒙脱石载体对“核-壳”结构零价铁纳米颗粒制备及其尺寸控制的影响与机理[J].科学通报,2010,55(9):827-834.
[10]孙芳,何广平,吴宏海,等.有机配体对膨润土负载纳米零价铁还原Cr(Ⅵ)的影响[J].环境科学研究,2011,24(4):461-466.
[11]秦润华,姜炜,刘宏英,等.纳米磁性四氧化三铁的制备及表征[J].材料导报,2003(增刊1):66-68.
[12]邱星屏.四氧化三铁磁性纳米粒子的合成及表征[J].厦门大学学报(自然科学版),1999,38(5):711-715.
[13]张鑫,李鑫钢,姜斌.四氧化三铁纳米粒子合成及表征[J].化学工业与工程,2006,23(1):45-48.
[14]李亚峰,朱爱霞,姚敬博,等.UV/Fenton法处理废水中苯酚[J].沈阳建筑大学学报,2008,24(4):637-640.
[15]杨岳主,李玉平,杨道武,等.铁铜催化剂非均相Fenton降解苯酚及机制研究[J].环境科学,2013,34(7):2658-2664.
[16]Lin S H,Lo C C.Fenton process for treatment of desizing wastewater[J].Water Res,1997,31(8):2050-2056.
[17]Ramirez J H,Costa C A,Madeira L M.Experimental design to optimize the degradation of the synthetic dye OrangeⅡusing Fenton’s reagent[J].Catalysis Today,2005,107/108:68-76.
[18]Wu H H,Dou X W,Deng D Y,et al.Decolourization of the azo dye Orange G in aqueous solution via a heterogeneous Fenton-like reaction catalysed by goethite[J].Environmental Technology,2012,33(14):1545-1552.
[19]王娟,杨再福.Fenton氧化在废水处理中的应用[J].环境科学与技术,2011,34(11):104-108.
[20]蒋芬芬,吴宏海,成思敏,等.针铁矿非均相Fenton法降解抗生素的研究[J].华南师范大学学报(自然科学版),2013,45(5):83-88.