改性花生壳吸附剂对阴离子染料的吸附作用
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摘要
以天然花生壳为原料,选用环氧氯丙烷作为醚化剂,再接枝二乙烯三胺得到改性花生壳。用扫描电镜等手段进行改性花生壳的表征,同时研究其对两种阴离子染料酸性橙(AO)和活性艳蓝(KN-R)的吸附去除情况。在系统研究初始pH、吸附剂投加量、初始染料浓度和吸附时间对吸附效率影响的基础上,通过吸附等温线和吸附动力学模型解析改性花生壳对阴离子染料的吸附机理。结果表明,改性后的花生壳孔道增多,且胺基成功地接枝到改性花生壳上。当AO和KN-R初始浓度为200 mg/L,改性花生壳投加量为0.5 g/L,溶液pH值为2时,吸附120 min后,改性花生壳对AO和KN-R的吸附容量分别为273.3 mg/g和313.6 mg/g。吸附符合Langmuir吸附等温模型和准二级动力学模型,通过计算确定改性花生壳对AO和KN-R的理论吸附容量与试验结果一致。该吸附剂原料广泛、制备方法简单,在染料废水去除方面具有良好的应用前景。
Modified peanut shell was prepared, using epichlorohydrin as etherifying agent, then grafting with diethylenetriamine. The characterizations of modified peanut shell were performed by scanning electron microscopy, etc. The potential for removal of two kinds of anionic dyes of acid orange(AO) and reactive brilliant blue(KN-R) by modified peanut shell was investigated. The influences of the initial pH, adsorbent dosage, initial dye concentration and adsorption time on the adsorption effect by modified peanut shell were evaluated. The adsorption mechanism of dye removal by modified peanut shell was explored by the adsorption isotherm and adsorption kinetics models. The main results showed that after modification, the pore channel was increased and the amine was successfully grafted on the surface of modified peanut shell. When the initial concentration of AO and KN-R was 200 mg/L, the dosage of modified peanut shells was 0.5 g/L and the solution pH value was 2, the adsorption capacity of modified peanut shells on AO and KN-R could reach 273.3 mg/g and 313.6 mg/g, respectively, after 120 minutes of adsorption. The adsorption process could be well simulated by the Langmuir adsorption isotherm and the pseudo second order kinetic models. The theoretical adsorption capacity of modified peanut shell to AO and KN-R was consistent with the experimental results. Since the adsorbent has a wide range of raw materials and a simple preparation method, it has a good application prospect in the removal of dye wastewater.
Modified peanut shell was prepared, using epichlorohydrin as etherifying agent, then grafting with diethylenetriamine. The characterizations of modified peanut shell were performed by scanning electron microscopy, etc. The potential for removal of two kinds of anionic dyes of acid orange(AO) and reactive brilliant blue(KN-R) by modified peanut shell was investigated. The influences of the initial pH, adsorbent dosage, initial dye concentration and adsorption time on the adsorption effect by modified peanut shell were evaluated. The adsorption mechanism of dye removal by modified peanut shell was explored by the adsorption isotherm and adsorption kinetics models. The main results showed that after modification, the pore channel was increased and the amine was successfully grafted on the surface of modified peanut shell. When the initial concentration of AO and KN-R was 200 mg/L, the dosage of modified peanut shells was 0.5 g/L and the solution pH value was 2, the adsorption capacity of modified peanut shells on AO and KN-R could reach 273.3 mg/g and 313.6 mg/g, respectively, after 120 minutes of adsorption. The adsorption process could be well simulated by the Langmuir adsorption isotherm and the pseudo second order kinetic models. The theoretical adsorption capacity of modified peanut shell to AO and KN-R was consistent with the experimental results. Since the adsorbent has a wide range of raw materials and a simple preparation method, it has a good application prospect in the removal of dye wastewater.
引文
[1] GUPTA V K, SUHAS. Application of low-cost adsorbents for dye removal——A review[J]. Journal of Environmental Management, 2009, 90(8):2313-2342.
[2] CRINI G. Non-conventional low-cost adsorbents for dye removal: A review[J]. Bioresource Technology, 2006, 97(9):1061-1085.
[3] NGULUBE T, GUMBO J R, MASINDI V, et al. An update on synthetic dyes adsorption onto clay based minerals: A state-of-art review[J]. Journal of Environmental Management, 2017, 191:35-57.
[4] MENG X, LIU Z, DENG C, et al. Microporous nano-MgO/diatomite ceramic membrane with high positive surface charge for tetracycline removal[J]. Journal of Hazardous Materials, 2016, 320(8):495-503.
[5] 董殿波. 印染废水处理技术研究进展[J]. 染料与染色, 2015,52(4):56-62.
[6] 任南琪, 周显娇, 郭婉茜,等. 染料废水处理技术研究进展[J]. 化工学报, 2013, 64(1):84-94.
[7] 梁婉婷, 田鹏, 张洪波. 染料废水的处理方法研究[J]. 山东化工, 2017, 46(4):152-153.
[8] 岳治杰. 染料废水处理技术现状与发展[J]. 环境科学与管理, 2012,37(7):64-67.
[9] 陈梦瑶, 王营茹, 曾伟,等. 吸附-絮凝法处理亚甲基蓝染料废水的研究[J]. 工业安全与环保, 2017, 43(1):24-28.
[10] 全姗姗, 朱玉婵, 任占海,等. 改性MCM-41分子筛对阴离子偶氮染料的吸附作用机理[J]. 化工进展, 2016, 35(1):320-326.
[11] 项小燕, 游腾钟, 袁秋兰,等. 羧基酯化改性花生壳对染料废水的吸附[J]. 应用化工, 2014, 43(3):460-464.
[12] 黄桂清, 卢丽婷, 黄怡,等. 瓜子壳和花生壳吸附去除亚甲基蓝染料的影响研究[J]. 广东化工, 2014, 41(13):34-35.
[13] 陈碧, 晁小练, 高雯雯,等. 改性花生壳对酸性橙Ⅱ的吸附影响因素及动力学研究[J]. 化学与生物工程, 2017, 34(10):44-48.
[14] 雷娟. 改性花生壳吸附亚甲基蓝的研究[J]. 太原师范学院学报(自然科学版), 2016,15(3):87-90.
[15] 李英柳, 薛彦君, 雷春生. 改性废弃生物质对直接染料的吸附研究[J]. 常州大学学报(自然科学版), 2013, 25(4):64-68.
[16] 唐婧, 范开敏. 二乙烯三胺改性花生壳纤维素对水中刚果红的吸附[J]. 环境工程学报, 2016, 10(8):4201-4205.
[17] ELKE K, LAURA S A, SCHOSSELER P. Chemical and spectroscopic characterization of algae surfaces[J]. Environmental Science & Technology, 1997, 31(31):759-764.
[18] 房文杰. 染液中染料组分的浓度分析[D]. 上海:东华大学, 2011.
[19] 于雪莲. 分光光度法在多组分染料调色中的应用[J]. 染料与染色, 2009, 6(3):39-41.
[20] WANG M, MENG G, HUANG Q. Spinach-extracted chlorophyll- a, modified peanut shell as fluorescence sensors for selective detection of Hg2+, in water[J]. Sensors & Actuators B Chemical, 2015, 26(4):237-241.
[21] HAN R, ZHANG L, SONG C, et al. Characterization of modified wheat straw, kinetic and equilibrium study about copper ion and methylene blue adsorption in batch mode[J]. Carbohydrate Polymers, 2010, 79(4):1140-1149.
[22] TARLEY C R, ARRUDA M A. Biosorption of heavy metals using rice milling by-products:Characterisation and application for removal of metals from aqueous effluents[J]. Chemosphere, 2004, 54(7):987-995.
[23] LIU Y, SUN X, LI B. Adsorption of Hg and Cd by ethylenediamine modified peanut shells[J]. Carbohydrate Polymers, 2010, 81(2):335-339.
[24] 荆煦英. 红外光谱实用指南[M]. 天津:天津科学技术出版社, 1992.
[25] JIANG X, SUN Y, LIU L, et al. Adsorption of C.I. reactive blue 19 from aqueous solutions by porous particles of the grafted chitosan[J]. Chemical Engineering Journal, 2014, 235(1):151-157.
[26] KHATAEE A R, ZAREI M, MORADKHANNEJHAD L. Application of response surface methodology for optimization of azo dye removal by oxalate catalyzed photoelectro-Fenton process using carbon nanotube-PTFE cathode[J]. Desalination, 2010, 258(1):112-119.
[27] KIM T H, PARK C, YANG J, et al. Comparison of disperse and reactive dye removals by chemical coagulation and Fenton oxidation[J]. Journal of Hazardous Materials, 2004, 112(1):95-103.
[28] GUPTA V K, JAIN R, AGARWAL S, et al. Photodegradation of hazardous dye quinoline yellow catalyzed by TiO2[J]. Journal of Colloid & Interface Science, 2012, 366(1):135-140.
[29] REHMAN M S U, MUNIR M, ASHFAQ M, et al. Adsorption of brilliant green dye from aqueous solution onto red clay[J]. Chemical Engineering Journal, 2013, 228(14):54-62.
[30] 黄文鹏, 赵雪, 安平平. 花生壳对水体中阳离子染料的吸附研究[J]. 科技创新导报, 2010,7(6):3-4.
[31] HUI D, LU J, LI G, et al. Adsorption of methylene blue on adsorbent materials produced from cotton stalk[J]. Chemical Engineering Journal, 2011, 172(1):326-334.
[32] 岳俊杰, 石召红, 赵前飞,等. CTAB改性沸石吸附酸性橙Ⅱ的研究[J]. 天津理工大学学报, 2016, 32(2):55-60.
[33] 吴盼盼, 方婷婷, 于欢,等. 有机改性镁铝层状氢氧化物对酸性橙Ⅱ的吸附研究[J]. 环境科学学报, 2013, 33(6):1576-1584.
[34] 刘春萍, 栾晓东, 许国锋,等. 4-氨基安替比林负载硅胶对酸性橙Ⅱ的吸附性能[J]. 鲁东大学学报(自然科学版), 2011(3):245-248.
[35] GRELUK M, HUBICKI Z. Effect of basicity of anion exchangers and number and positions of sulfonic groups of acid dyes on dyes adsorption on macroporous anion exchangers with styrenic polymer matrix[J]. Chemical Engineering Journal, 2013, 215-216(2):731-739.
[36] 唐志儒, 陈一, 闻岳,等. 交联壳聚糖珠吸附活性染料的动力学研究[J]. 环境工程学报, 2012, 6(9):3007-3010.
[37] 孟佳. 三维立体石墨烯的制备及其吸附性能的研究[D]. 大连:大连工业大学, 2016.
[38] 梁俊倩, 吴锦华, 李平,等. 柚子皮吸附活性艳蓝KN-R和活性艳橙X-GN性能研究[J]. 水处理技术, 2011, 37(4):88-90.
[39] 张平, 廖柏寒, 李科林,等. 3种生物质炭对活性艳蓝KN-R的吸附[J]. 环境工程学报, 2014, 8(2):581-586.
[40] 郑帅. 高氨基多孔壳聚糖树脂的制备及其对染料吸附性能的研究[D]. 上海:东华大学, 2012.
[2] CRINI G. Non-conventional low-cost adsorbents for dye removal: A review[J]. Bioresource Technology, 2006, 97(9):1061-1085.
[3] NGULUBE T, GUMBO J R, MASINDI V, et al. An update on synthetic dyes adsorption onto clay based minerals: A state-of-art review[J]. Journal of Environmental Management, 2017, 191:35-57.
[4] MENG X, LIU Z, DENG C, et al. Microporous nano-MgO/diatomite ceramic membrane with high positive surface charge for tetracycline removal[J]. Journal of Hazardous Materials, 2016, 320(8):495-503.
[5] 董殿波. 印染废水处理技术研究进展[J]. 染料与染色, 2015,52(4):56-62.
[6] 任南琪, 周显娇, 郭婉茜,等. 染料废水处理技术研究进展[J]. 化工学报, 2013, 64(1):84-94.
[7] 梁婉婷, 田鹏, 张洪波. 染料废水的处理方法研究[J]. 山东化工, 2017, 46(4):152-153.
[8] 岳治杰. 染料废水处理技术现状与发展[J]. 环境科学与管理, 2012,37(7):64-67.
[9] 陈梦瑶, 王营茹, 曾伟,等. 吸附-絮凝法处理亚甲基蓝染料废水的研究[J]. 工业安全与环保, 2017, 43(1):24-28.
[10] 全姗姗, 朱玉婵, 任占海,等. 改性MCM-41分子筛对阴离子偶氮染料的吸附作用机理[J]. 化工进展, 2016, 35(1):320-326.
[11] 项小燕, 游腾钟, 袁秋兰,等. 羧基酯化改性花生壳对染料废水的吸附[J]. 应用化工, 2014, 43(3):460-464.
[12] 黄桂清, 卢丽婷, 黄怡,等. 瓜子壳和花生壳吸附去除亚甲基蓝染料的影响研究[J]. 广东化工, 2014, 41(13):34-35.
[13] 陈碧, 晁小练, 高雯雯,等. 改性花生壳对酸性橙Ⅱ的吸附影响因素及动力学研究[J]. 化学与生物工程, 2017, 34(10):44-48.
[14] 雷娟. 改性花生壳吸附亚甲基蓝的研究[J]. 太原师范学院学报(自然科学版), 2016,15(3):87-90.
[15] 李英柳, 薛彦君, 雷春生. 改性废弃生物质对直接染料的吸附研究[J]. 常州大学学报(自然科学版), 2013, 25(4):64-68.
[16] 唐婧, 范开敏. 二乙烯三胺改性花生壳纤维素对水中刚果红的吸附[J]. 环境工程学报, 2016, 10(8):4201-4205.
[17] ELKE K, LAURA S A, SCHOSSELER P. Chemical and spectroscopic characterization of algae surfaces[J]. Environmental Science & Technology, 1997, 31(31):759-764.
[18] 房文杰. 染液中染料组分的浓度分析[D]. 上海:东华大学, 2011.
[19] 于雪莲. 分光光度法在多组分染料调色中的应用[J]. 染料与染色, 2009, 6(3):39-41.
[20] WANG M, MENG G, HUANG Q. Spinach-extracted chlorophyll- a, modified peanut shell as fluorescence sensors for selective detection of Hg2+, in water[J]. Sensors & Actuators B Chemical, 2015, 26(4):237-241.
[21] HAN R, ZHANG L, SONG C, et al. Characterization of modified wheat straw, kinetic and equilibrium study about copper ion and methylene blue adsorption in batch mode[J]. Carbohydrate Polymers, 2010, 79(4):1140-1149.
[22] TARLEY C R, ARRUDA M A. Biosorption of heavy metals using rice milling by-products:Characterisation and application for removal of metals from aqueous effluents[J]. Chemosphere, 2004, 54(7):987-995.
[23] LIU Y, SUN X, LI B. Adsorption of Hg and Cd by ethylenediamine modified peanut shells[J]. Carbohydrate Polymers, 2010, 81(2):335-339.
[24] 荆煦英. 红外光谱实用指南[M]. 天津:天津科学技术出版社, 1992.
[25] JIANG X, SUN Y, LIU L, et al. Adsorption of C.I. reactive blue 19 from aqueous solutions by porous particles of the grafted chitosan[J]. Chemical Engineering Journal, 2014, 235(1):151-157.
[26] KHATAEE A R, ZAREI M, MORADKHANNEJHAD L. Application of response surface methodology for optimization of azo dye removal by oxalate catalyzed photoelectro-Fenton process using carbon nanotube-PTFE cathode[J]. Desalination, 2010, 258(1):112-119.
[27] KIM T H, PARK C, YANG J, et al. Comparison of disperse and reactive dye removals by chemical coagulation and Fenton oxidation[J]. Journal of Hazardous Materials, 2004, 112(1):95-103.
[28] GUPTA V K, JAIN R, AGARWAL S, et al. Photodegradation of hazardous dye quinoline yellow catalyzed by TiO2[J]. Journal of Colloid & Interface Science, 2012, 366(1):135-140.
[29] REHMAN M S U, MUNIR M, ASHFAQ M, et al. Adsorption of brilliant green dye from aqueous solution onto red clay[J]. Chemical Engineering Journal, 2013, 228(14):54-62.
[30] 黄文鹏, 赵雪, 安平平. 花生壳对水体中阳离子染料的吸附研究[J]. 科技创新导报, 2010,7(6):3-4.
[31] HUI D, LU J, LI G, et al. Adsorption of methylene blue on adsorbent materials produced from cotton stalk[J]. Chemical Engineering Journal, 2011, 172(1):326-334.
[32] 岳俊杰, 石召红, 赵前飞,等. CTAB改性沸石吸附酸性橙Ⅱ的研究[J]. 天津理工大学学报, 2016, 32(2):55-60.
[33] 吴盼盼, 方婷婷, 于欢,等. 有机改性镁铝层状氢氧化物对酸性橙Ⅱ的吸附研究[J]. 环境科学学报, 2013, 33(6):1576-1584.
[34] 刘春萍, 栾晓东, 许国锋,等. 4-氨基安替比林负载硅胶对酸性橙Ⅱ的吸附性能[J]. 鲁东大学学报(自然科学版), 2011(3):245-248.
[35] GRELUK M, HUBICKI Z. Effect of basicity of anion exchangers and number and positions of sulfonic groups of acid dyes on dyes adsorption on macroporous anion exchangers with styrenic polymer matrix[J]. Chemical Engineering Journal, 2013, 215-216(2):731-739.
[36] 唐志儒, 陈一, 闻岳,等. 交联壳聚糖珠吸附活性染料的动力学研究[J]. 环境工程学报, 2012, 6(9):3007-3010.
[37] 孟佳. 三维立体石墨烯的制备及其吸附性能的研究[D]. 大连:大连工业大学, 2016.
[38] 梁俊倩, 吴锦华, 李平,等. 柚子皮吸附活性艳蓝KN-R和活性艳橙X-GN性能研究[J]. 水处理技术, 2011, 37(4):88-90.
[39] 张平, 廖柏寒, 李科林,等. 3种生物质炭对活性艳蓝KN-R的吸附[J]. 环境工程学报, 2014, 8(2):581-586.
[40] 郑帅. 高氨基多孔壳聚糖树脂的制备及其对染料吸附性能的研究[D]. 上海:东华大学, 2012.