活性炭对苯酚的吸附及再生的研究
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摘要
使用新鲜的颗粒活性炭吸附苯酚,并采用Fenton氧化、铁炭微电解以及Fenton-微电解耦合工艺再生吸附饱和的活性炭。通过吸附效率试验、吸附等温线试验分析新鲜炭和再生炭的吸附性能和热力学特征。使用解吸附的Elovich、一级动力学、二级动力学方程表征活性炭的再生过程,研究各种活性炭再生手段的影响因素、再生过程的反应特征。
试验结果表明:新鲜活性炭具有很好的苯酚吸附性能,吸附量为9.60 mg·g~(-1),吸附是自发的放热过程,吸附量随着温度的升高而降低,吸附活化能为31.42KJ·mol~(-1),属于化学吸附。使用Fenton、微电解和Fenton-微电解耦合工艺再生的活性炭,苯酚吸附量分别为7.97 mg·g~(-1)、4.56 mg·g~(-1)和8.27 mg·g~(-1);三种工艺对活性炭的苯酚吸附量再生效率分别为82.96%、47.49%和86.13%。再生炭的吸附等温线试验表明,Fenton-微电解耦合和Fenton氧化工艺再生炭的苯酚吸附性能较好,吸附量和热力学特征比较接近新鲜活性炭,微电解再生炭的吸附性质有所改变。对各再生工艺的动力学拟合结果表明,Fenton再生主要符合解吸附的二级动力学模型,是由于苯酚解吸附到水中而被Fenton试剂氧化。微电解再生过程较复杂,符合Elovich模型。Fenton-微电解耦合再生法的Elovich模型和二级动力学模型相关性较好,说明Fenton-微电解耦合再生活性炭是一种较复杂的过程,可能涉及到微电解、Fenton反应、苯酚解吸附。
Activated carbon which was exhausted by phenol was regenerated by Fenton oxidation, iron-carbon micro-electrolysis and micro-electrolysis coupled with Fenton process. Adsorption and thermodynamic properties of fresh and regenerated carbon were analyzed by adsorption efficiency test and adsorption isotherm test, respectively. Process of regeneration was characterised by Elovich, first order kinetics and second order kinetics equation to study the affecting factors and character of regenerating reaction.
The results showed that fresh activated carbon had a good adsorption capacity for phenol. The adsorbance of fresh activated carbon was 9.60 mg·g~(-1) and the adsorption was a spontaneous exothermic process, moreover,the adsorbance decreasd with temperature increasing.The activation energy of adsorption ,which have been a chemisorption process,was 31.42KJ·mol~(-1).The adsorption capacity for phenol of activated carbon which was regenerated in the ways of Fenton, micro-electrolysis and micro-electrolysis coupled with Fenton oxidation was 7.97mg·g~(-1), 4.56 mg·g~(-1) and 8.27mg·g~(-1), respectively.Regeneration efficiency of the three kinds of process was 82.96 %, 47.49% and 86.13%.Adsorption isotherm test of regenerated carbon displayed that carbon regenerated by micro-electrolysis coupled with Fenton oxidation and Fenton oxidation process have a good adsorption capacity for phenol, whose adsorption and thermodynamic properties were closer to fresh activated carbon, and the adsorption properties of micro-electrolytic regenerative carbons had changed to some extent. Modeling results of kinetics of the regeneration process revealed that Fenton regeneration was mainly consistent with the second orde kinetics equation of desorption,because phenol was desorbed into water firstly,and then oxidated by Fenton reagent.Regeneration processes of micro-electrolysis were very complex and in accordance with Elovich model. Elovich model and second order kinetic model of regenerating process using micro-electrolysis coupled with Fenton oxidation both possessed good correlation, indicating that the process of regenerating activated carbon using micro-electrolysis coupled with Fenton oxidation was very complex, involving electrolysis, Fenton reaction and phenol desorption.
试验结果表明:新鲜活性炭具有很好的苯酚吸附性能,吸附量为9.60 mg·g~(-1),吸附是自发的放热过程,吸附量随着温度的升高而降低,吸附活化能为31.42KJ·mol~(-1),属于化学吸附。使用Fenton、微电解和Fenton-微电解耦合工艺再生的活性炭,苯酚吸附量分别为7.97 mg·g~(-1)、4.56 mg·g~(-1)和8.27 mg·g~(-1);三种工艺对活性炭的苯酚吸附量再生效率分别为82.96%、47.49%和86.13%。再生炭的吸附等温线试验表明,Fenton-微电解耦合和Fenton氧化工艺再生炭的苯酚吸附性能较好,吸附量和热力学特征比较接近新鲜活性炭,微电解再生炭的吸附性质有所改变。对各再生工艺的动力学拟合结果表明,Fenton再生主要符合解吸附的二级动力学模型,是由于苯酚解吸附到水中而被Fenton试剂氧化。微电解再生过程较复杂,符合Elovich模型。Fenton-微电解耦合再生法的Elovich模型和二级动力学模型相关性较好,说明Fenton-微电解耦合再生活性炭是一种较复杂的过程,可能涉及到微电解、Fenton反应、苯酚解吸附。
Activated carbon which was exhausted by phenol was regenerated by Fenton oxidation, iron-carbon micro-electrolysis and micro-electrolysis coupled with Fenton process. Adsorption and thermodynamic properties of fresh and regenerated carbon were analyzed by adsorption efficiency test and adsorption isotherm test, respectively. Process of regeneration was characterised by Elovich, first order kinetics and second order kinetics equation to study the affecting factors and character of regenerating reaction.
The results showed that fresh activated carbon had a good adsorption capacity for phenol. The adsorbance of fresh activated carbon was 9.60 mg·g~(-1) and the adsorption was a spontaneous exothermic process, moreover,the adsorbance decreasd with temperature increasing.The activation energy of adsorption ,which have been a chemisorption process,was 31.42KJ·mol~(-1).The adsorption capacity for phenol of activated carbon which was regenerated in the ways of Fenton, micro-electrolysis and micro-electrolysis coupled with Fenton oxidation was 7.97mg·g~(-1), 4.56 mg·g~(-1) and 8.27mg·g~(-1), respectively.Regeneration efficiency of the three kinds of process was 82.96 %, 47.49% and 86.13%.Adsorption isotherm test of regenerated carbon displayed that carbon regenerated by micro-electrolysis coupled with Fenton oxidation and Fenton oxidation process have a good adsorption capacity for phenol, whose adsorption and thermodynamic properties were closer to fresh activated carbon, and the adsorption properties of micro-electrolytic regenerative carbons had changed to some extent. Modeling results of kinetics of the regeneration process revealed that Fenton regeneration was mainly consistent with the second orde kinetics equation of desorption,because phenol was desorbed into water firstly,and then oxidated by Fenton reagent.Regeneration processes of micro-electrolysis were very complex and in accordance with Elovich model. Elovich model and second order kinetic model of regenerating process using micro-electrolysis coupled with Fenton oxidation both possessed good correlation, indicating that the process of regenerating activated carbon using micro-electrolysis coupled with Fenton oxidation was very complex, involving electrolysis, Fenton reaction and phenol desorption.
引文
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[3]Beker U,Ganbold B,Dertli H,et al.Adsorption of phenol by activated carbon:influence of activation methods and solution pH[J]. Energy Conversion and Management,2010, 51(2): 235-240
[4]赵瑞东,刘凤玲,郑寿荣,等.CO2高温活化活性炭材料对苯酚的吸附行为研究[J].环境污染与防治,2010, (10):33-36
[5]Taman H,Okazaki M.Influence of acidic surface oxides of activated carbon on gas adsorption characteristics[J]. Carbon,1996,34(6):741-746
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[7]刘军利,古可隆.高温处理对活性炭孔隙结构的影响[J].林产化学与工业,1999,19(3):37-40
[8]Anoop K A,Anirudhan T S.Uptake of heavy metals in batch systems by sulfurized steam activated carbon prepared from sugarcane bagasse pith[J]. Industrial and Engineering Chemical Research,2002,41(20):5085-5093
[9]Gang pan,Peter S.Liss.Metastable-Equilibrium Adsorption TheoryⅠ.Theoretical[J]. Jourrnal of Colloid and Interface Science,1998,201(1)71-76
[10]单绍复.活性炭的吸附原理及在环境工程中的应用[J].污染防治技术,1991,4(4):11-15
[11]Haiyun Zhou,GangLi,Xiaoxing Wang,et al. Preparation of a kind of mesoporous carbon and its performance in adsorptive desulfurization[J]. Journal of Natural Gas Chemistry,2009,18(3): 365-368
[12]陶燕,米生权,王式功,等.活性炭吸附-超临界CO2解吸附四氯乙烯的特性研究[J].环境污染与防治,2009,30(9):1-5,30
[13]王挺,蒋新.SiO2表面吸附层中钛酸丁酯的反应过程[J].无机化学学报,2009, 25(10):1805-1811
[14]崔凯,李宝元,李兴斯.非饱和土中镉离子迁移规律的实验研究[J].水动力学研究与进展:A辑,2003,18(6):725-731
[15]唐文华,刘少友,冯庆革,等.金属掺杂二氧化钛介孔材料对葛根素的吸附行为[J].过程工程学报,2010,10(4):685-690
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[18]张卫军,卢丽敏,万其中,等.基于纳米氧化铝/壳聚糖无机-有机复合纳米材料的辣根过氧化酶生物传感器[J].分析测试学报,2010,29(4):353-358
[19]丁志斌,王秀春,程宝义,等.活性炭吸附化学战剂-沙林染毒水的实验研究[J].环境污染治理技术与设备,2002,3(12):43-45
[20]刘军利.活性炭标准国际化趋同发展趋势[J].林产化工通讯,2004,38(5):30-35
[21]岳宗豪,郑经堂,曲降伟,等.活性炭再生技术研究进展[J].应用化工,2009,38(11):1667-1670
[22]林冠烽,牟大庆,程捷,等.活性炭再生技术研究进展[J].林业科学,2008,44(2):151-154
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