载磷Mg/Al/Fe-LDO的微波辅助溶剂解吸方法特性
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摘要
针对载磷Mg/Al/Fe-LDO再生利用与解吸液富集回收磷的问题,通过对比直接溶剂解吸法与微波辅助溶剂解吸法在解吸条件、吸附性能与材料层状结构恢复方面的差异,考察了微波辅助溶剂解吸方法的技术特性,并分析了其解吸机制.结果显示,与直接溶剂解吸法相比,微波辅助溶剂解吸法解吸时间由4 h缩短为10～30 min,解吸效果提高15%以上;在同等解吸效果前提下,组合解吸剂(Na_2CO_3+NaOH)浓度降低2倍;解吸剂用量减少10倍.载磷Mg/Al/Fe-LDO经微波辅助溶剂解吸-焙烧再生后,吸附性能得到较好地恢复,3次吸附-解吸-焙烧后再生率接近90%,比直接溶剂解吸-焙烧再生提高40%.由于微波能够强化溶剂离子热运动、促进离子传质与扩散过程,加快离子交换速率,有利于材料层状结构的有效恢复,因此,微波辅助溶剂解吸法能够在较低解吸剂浓度与用量条件下,实现对载磷Mg/Al/Fe-LDO的高效、快速解吸,有利于污水中磷的富集回收.
The microwave assisted solvent desorption(MASD) method was examined, compared with direct desorption, on the regeneration of Mg/Al/Fe-LDO and the recovery of phosphorus. These two methods were investigated in terms of their desorption conditions, adsorption capability, and the structure recovery of the Mg/Al/Fe-LDO material, to reveal the desorption mechanism of microwave assisted solvent desorption. The results show that by using MASD, the desorption time was reduced from 4 h to 10～30 min and the desorption efficiency improved by more than 15%. Moreover, under the similar desorption efficiency, the concentration and the usage of combined desorption agent(Na_2CO_3+NaOH) can be decreased by 2 an 10 fold, respectively. After regeneration by MASD-roasting, the adsorption capability of Mg/Al/Fe-LDO material was well recovered. The regeneration rate of such adsorbent was nearly 90% after three cycles, and is 40% higher than that of direct solvent desorption, owing that microwave can enhance the ionic thermal movement of solvents, promote the process of ion mass transfer and diffusion, and accelerate the rate of ion exchange. These advantages are conducive to the effective restoration of the layered structure of adsorbent material. Therefore, the MASD can achieve high-efficiency and rapid desorption of phosphorus from the Mg/Al/Fe-LDO with low dosage of agent, which is helpful for the enrichment and recovery of phosphorus in sewage.
The microwave assisted solvent desorption(MASD) method was examined, compared with direct desorption, on the regeneration of Mg/Al/Fe-LDO and the recovery of phosphorus. These two methods were investigated in terms of their desorption conditions, adsorption capability, and the structure recovery of the Mg/Al/Fe-LDO material, to reveal the desorption mechanism of microwave assisted solvent desorption. The results show that by using MASD, the desorption time was reduced from 4 h to 10～30 min and the desorption efficiency improved by more than 15%. Moreover, under the similar desorption efficiency, the concentration and the usage of combined desorption agent(Na_2CO_3+NaOH) can be decreased by 2 an 10 fold, respectively. After regeneration by MASD-roasting, the adsorption capability of Mg/Al/Fe-LDO material was well recovered. The regeneration rate of such adsorbent was nearly 90% after three cycles, and is 40% higher than that of direct solvent desorption, owing that microwave can enhance the ionic thermal movement of solvents, promote the process of ion mass transfer and diffusion, and accelerate the rate of ion exchange. These advantages are conducive to the effective restoration of the layered structure of adsorbent material. Therefore, the MASD can achieve high-efficiency and rapid desorption of phosphorus from the Mg/Al/Fe-LDO with low dosage of agent, which is helpful for the enrichment and recovery of phosphorus in sewage.
引文
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Wang Y, Gao H. 2006. Compositional and structural control on anion sorption capability of layered double hydroxides (LDHs)[J]. Journal of Colloid & Interface Science, 301(1):19-26
Wang Y, Li F, Dong S, et al. 2016. A facile approach for synthesizing Fe-based layered double hydroxides with high purity and its exfoliation[J]. Journal of Colloid and Interface Science, 467:28-34
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王卫东, 郝瑞霞, 张晓娴, 等. 2017a. 高效磷吸附剂Mg/Al-LDO的制备及除磷机制[J].环境科学,38(2): 572-579
王卫东, 郝瑞霞, 朱晓霞,等. 2017b. 磷吸附剂Mg/Al-LDO的再生方法及机制[J]. 中国环境科学, 37(6):2092-2099
肖永辉, 王志刚, 刘曙照. 2011. 水体富营养化及蓝藻水华预警模型研究进展[J].环境科学与技术,34(11): 152-157
谢明勇, 陈奕. 2006. 微波辅助萃取技术研究进展[J]. 食品与生物技术学报, 25(1):105-114
Yang K, Yan L G, Yang Y M, et al. 2014. Adsorptive removal of phosphate by Mg-Al and Zn-Al layered double hydroxides: Kinetics, isotherms and mechanisms[J]. Separation & Purification Technology, 124(124):36-42
Zhang C, Yang S, Chen H, et al. 2014. Adsorption behavior and mechanism of reactive brilliant red X-3B in aqueous solution over three kinds of hydrotalcite-like LDHs[J]. Applied Surface Science, 301(10):329-337
Zhang S, Jiao Q, Wang C, et al. 2016. In situ synthesis of Mg/Fe LDO/carbon nanohelix composites as absorbing materials[J]. Journal of Alloys & Compounds, 658:505-512
Zhou J, Yang S, Yu J, et al. 2011. Novel hollow microspheres of hierarchical zinc-aluminum layered double hydroxides and their enhanced adsorption capacity for phosphate in water[J]. Journal of Hazardous Materials, 192(3):1114-1121
Zhou W, Zhang W, Chen Z. 2017. Universal biomimetic preparation and immobilization of layered double hydroxide films and adsorption behavior[J]. Applied Surface Science, 392:153-161
张成, 贾绍义. 2004. 微波萃取技术及其应用[J]. 化学工业与工程, 21(6):444-447
Cheng X, Huang X, Wang X, et al. 2009. Phosphate adsorption from sewage sludge filtrate using zinc-aluminum layered double hydroxides[J]. Journal of Hazardous Materials, 169(1/3):958
Cheng X, Huang X, Wang X, et al. 2010. Influence of calcination on the adsorptive removal of phosphate by Zn-Al layered double hydroxides from excess sludge liquor [J]. Journal of Hazardous Materials, 177(1):516-523
Drenkovatuhtan A, Mandel K, Paulus A, et al. 2013. Phosphate recovery from wastewater using engineered superparamagnetic particles modified with layered double hydroxide ion exchangers [J]. Water Research, 47(15):5670-5677
Eskilsson C S, Bj?rklund E. 2000. Analytical-scale microwave-assisted extraction[J]. Journal of Chromatography A, 902(1):227-250
Frost R L, Musumeci A W, Kloprogge J T, et al. 2010. Raman spectroscopy of hydrotalcites with phosphate in the interlayer: implications for the removal of phosphate from water[J]. Journal of Raman Spectroscopy, 37(7):733-741
Li J, Cui H, Song X, et al. 2016. Adsorption and intercalation of organic pollutants and heavy metal ions into MgAl-LDHs nanosheets with super high capacity[J]. Rsc Advances, 6:92402-92410
Ling F, Fang L, Lu Y, et al. 2016. A novel CoFe layered double hydroxides adsorbent: High adsorption amount for methyl orange dye and fast removal of Cr(VI)[J]. Microporous & Mesoporous Materials, 234:230-238
李如忠, 刘科峰, 钱靖, 等. 2014. 合肥市区典型景观水体氮磷污染特征及富营养化评价[J].环境科学,35(5): 1718-1726
卢凯. 2007. 微波的原理及特点[J]. 农业科技与装备, (1):61-62
Novillo C, Guaya D, Avendaňo A P, et al. 2014. Evaluation of phosphate removal capacity of Mg/Al layered double hydroxides from aqueous solutions [J]. Fuel, 138(138):72-79
潘志彬, 何敏旋, 李绍秀. 2016. 水处理吸附剂再生技术的研究进展[J]. 能源与环境, (1):92-93
Schirmer A, Drexl A. 2015. Allocation of partially renewable resources: Concept, capabilities, and applications[J]. Networks, 37(1):21-34
孙德智, 黄新瑞, 程翔,等. 2009. Zn-Al类水滑石吸附污泥脱水液中磷的研究[J]. 北京林业大学学报, 31(2):128-132
Triantafyllidis K S, Peleka E N, Komvokis V G, et al. 2010. Iron-modified hydrotalcite-like materials as highly efficient phosphate sorbents [J]. Journal of Colloid & Interface Science, 342(2):427
Ulrich A E, Malley D F, Watts P D. 2016. Lake Winnipeg Basin: Advocacy, challenges and progress for sustainable phosphorus and eutrophication control[J]. Science of the Total Environment, 542:1030-1039
Wang K, Ma J, Yao Z, et al. 2016. Synthesis and photocatalytic properties of new ternary Ni-Fe-Cr hydrotalcite-like compounds[J]. Ceramics International, 42(14):15981-15988
Wang Y, Gao H. 2006. Compositional and structural control on anion sorption capability of layered double hydroxides (LDHs)[J]. Journal of Colloid & Interface Science, 301(1):19-26
Wang Y, Li F, Dong S, et al. 2016. A facile approach for synthesizing Fe-based layered double hydroxides with high purity and its exfoliation[J]. Journal of Colloid and Interface Science, 467:28-34
万京京, 郝瑞霞, 马静雨,等. 2018. Fe(Ⅲ)掺杂Mg/Al-LDO作为氮磷吸附剂的研究[J]. 中国环境科学, (4):1295-1303
王卫东, 郝瑞霞, 张晓娴, 等. 2017a. 高效磷吸附剂Mg/Al-LDO的制备及除磷机制[J].环境科学,38(2): 572-579
王卫东, 郝瑞霞, 朱晓霞,等. 2017b. 磷吸附剂Mg/Al-LDO的再生方法及机制[J]. 中国环境科学, 37(6):2092-2099
肖永辉, 王志刚, 刘曙照. 2011. 水体富营养化及蓝藻水华预警模型研究进展[J].环境科学与技术,34(11): 152-157
谢明勇, 陈奕. 2006. 微波辅助萃取技术研究进展[J]. 食品与生物技术学报, 25(1):105-114
Yang K, Yan L G, Yang Y M, et al. 2014. Adsorptive removal of phosphate by Mg-Al and Zn-Al layered double hydroxides: Kinetics, isotherms and mechanisms[J]. Separation & Purification Technology, 124(124):36-42
Zhang C, Yang S, Chen H, et al. 2014. Adsorption behavior and mechanism of reactive brilliant red X-3B in aqueous solution over three kinds of hydrotalcite-like LDHs[J]. Applied Surface Science, 301(10):329-337
Zhang S, Jiao Q, Wang C, et al. 2016. In situ synthesis of Mg/Fe LDO/carbon nanohelix composites as absorbing materials[J]. Journal of Alloys & Compounds, 658:505-512
Zhou J, Yang S, Yu J, et al. 2011. Novel hollow microspheres of hierarchical zinc-aluminum layered double hydroxides and their enhanced adsorption capacity for phosphate in water[J]. Journal of Hazardous Materials, 192(3):1114-1121
Zhou W, Zhang W, Chen Z. 2017. Universal biomimetic preparation and immobilization of layered double hydroxide films and adsorption behavior[J]. Applied Surface Science, 392:153-161
张成, 贾绍义. 2004. 微波萃取技术及其应用[J]. 化学工业与工程, 21(6):444-447