道南渗析-零价铁耦合工艺除砷效果研究

doi:10.11949/0438-1157.20200358

摘要/Abstract

摘要：

道南渗析-零价铁耦合工艺通过在解吸液中加入零价铁，利用其腐蚀产生的吸附除砷作用，实现解吸液的同步再生，从而改善道南渗析除砷系统长期运行效果。在考察解吸液NaCl浓度对零价铁除砷性能影响的基础上确定解吸液中NaCl浓度为0.1 mol·L^-1。以该工艺对某农村含砷井水的多批次处理结果表明，在6 g·L^-1食盐溶液的解吸液中加入5 g·L^-1还原铁粉后，系统连续运行20批次，出水中砷浓度始终低于50 μg·L^-1，运行有效性远高于单一道南渗析对照组。该耦合工艺延长了解吸液使用时间，提升了道南渗析除砷装置的应用性。

关键词: 离子交换, 吸附, 再生, 零价铁, 道南渗析

Abstract:

The Donnon dialysis-zerovalent iron combined process was developed by adding zerovalent iron into the stripping solution. The arsenic adsorption by the zerovalent iron corrosion products was able to regenerate the stripping solution in situ. Therefore, the long-term arsenic removal by the Donnan dialysis system was markedly improved. In this study, the effect of NaCl concentration in the desorption solution was determined to be 0.1 mol·L^-1 based on the investigation of the effect of the NaCl concentration in the desorption solution on the arsenic removal performance of zero-valent iron. Then, the proposed Donnon dialysis-zerovalent iron combined process was used to treat arsenic containing well water for multiple batches, using stripping solution containing 6 g common salt and 5 g zerovalent iron per liter. The arsenic concentrations in the treated water was constantly below 50 μg·L^-1 for 20 batches, much lower than the performance of the single Donnan dialysis system. The coupling of Donnan dialysis with zerovalent iron prolonged the interval for the stripping solution replacement; therefore, the practical application of the Donnan dialysis household water purifier was significantly improved.

Key words: ion exchange, adsorption, regeneration, zerovalent iron, Donnan dialysis

中图分类号:

X 703

赵斌,刘念,王虹利,钱怡冉,张朝晖,王亮. 道南渗析-零价铁耦合工艺除砷效果研究[J]. 化工学报, 2020, 71(11): 5303-5308.

Bin ZHAO,Nian LIU,Hongli WANG,Yiran QIAN,Zhaohui ZHANG,Liang WANG. Arsenate removal using Donnan dialysis-zerovalent iron combined process[J]. CIESC Journal, 2020, 71(11): 5303-5308.

图/表 7

图1 “道南渗析-Fe0”实验装置照片1—料液室；2—解吸液室；3—膜；4—法兰；5—排液口；6—曝气管；7—气泵

Fig.1 Images of the “Donnan dialysis-Fe0” set-up

表1 某农村一井水水质

Table 1 Water quality of a rural well

指标	单位	数值
As	μg·L^-1	252
pH		8.09
Na⁺	mg·L^-1	151.1
Mg²⁺	mg·L^-1	22.6
Ca²⁺	mg·L^-1	26.2
Cl^-	mg·L^-1	156.8
SO₄^2-	mg·L^-1	43.2

图2 NaCl浓度对Fe0除砷动力学过程的影响

Fig.2 Effect of NaCl concentration on the kinetics of As(Ⅴ) removal by zerovalent iron

表2 Fe0除砷的动力学拟合

Table 2 Modeling of As(Ⅴ) removal kinetics by zerovalent iron

NaCl/ (mol·L^-1)	一级动力学		二级动力学		准一级动力学			准二级动力学
NaCl/ (mol·L^-1)	k₁/h^-1	r²	k₂/(L·mg^-1·h^-1)	r²	k_α/h^-1	q_As,e/(mg·g^-1)	r²	k_β/(g·mg^-1·h^-1)	q_As,e/(mg·g^-1)	r²
0	0.020	0.98	0.005	0.95	0.028	0.416	1.00	0.046	0.545	1.00
0.01	0.034	0.95	0.029	0.72	0.082	0.408	0.97	0.215	0.466	1.00
0.1	0.036	0.85	0.024	0.94	0.138	0.416	0.93	0.431	0.456	0.98
1.0	0.019	0.42	0.004	0.92	0.220	0.337	0.91	0.842	0.366	0.96

图3 在不同NaCl浓度含砷溶液中浸泡5 d后的Fe0表面形貌

Fig.3 SEM images of zerovalent iron in solutions of different NaCl concentrations

图4 不同NaCl溶液中得到的Fe0腐蚀产物的除砷效果

Fig.4 As(Ⅴ) removal by iron corrosion products obtained from solutions of different NaCl concentrations

图5 道南渗析和道南渗析-Fe0耦合除砷工艺运行效果比较

Fig.5 Arsenic removal by Donnan dialysis and Donnan dialysis-zerovalent iron combined process

参考文献 30

1	Sarkar S, Sengupta A K, Prakash P. The Donnan membrane principle: opportunities for sustainable engineered processes and materials [J]. Environmental Science & Technology, 2010, 44(4): 1161-1166.
2	Fox S, Bruner T, Oren Y, et al. Concurrent microbial reduction of high concentrations of nitrate and perchlorate in an ion exchange membrane bioreactor [J]. Biotechnology and Bioengineering, 2016, 113(9): 1881-1891.
3	Wisniewski J A, Kabsch-Korbutowicz M, Lakomska S. Removal of bromate ions from water in the processes with ion-exchange membranes [J]. Separation and Purification Technology, 2015, 145: 75-82.
4	Lao M, Companys E, Weng L P, et al. Speciation of Zn, Fe, Ca and Mg in wine with the Donnan membrane technique [J]. Food Chemistry, 2018, 239: 1143-1150.
5	Breytus A, Hasson D, Semiat R, et al. Ion exchange membrane adsorption in Donnan dialysis [J]. Separation and Purification Technology, 2019, 226: 252-258.
6	Bjorklund G, Aaseth J, Chirumbolo S, et al. Effects of arsenic toxicity beyond epigenetic modifications [J]. Environmental Geochemistry and Health, 2018, 40(3): 955-965.
7	Tchounwou P B, Yedjou C G, Udensi U K, et al. State of the science review of the health effects of inorganic arsenic: perspectives for future research [J]. Environmental Toxicology, 2019, 34(2): 188-202.
8	Zhao B, Zhao H Z, Dockko S, et al. Arsenate removal from simulated groundwater with a Donnan dialyzer [J]. Journal of Hazardous Materials, 2012, 215: 159-165.
9	赵斌, 刘安琪, 刁法林, 等. 道南渗析除砷过程影响因素分析[J]. 化工学报, 2016, 67(6): 2456-2461.
	Zhao B, Liu A Q, Diao F L, et al. Kinetic analysis of arsenate removal by Donnan dialysis [J]. CIESC Journal, 2016, 67(6): 2456-2461.
10	Li Y M, Guo X J, Dong H Y, et al. Selenite removal from groundwater by zero-valent iron (ZVI) in combination with oxidants [J]. Chemical Engineering Journal, 2018, 345: 432-440.
11	Zhu F, Ma S Y, Liu T, et al. Green synthesis of nano zero-valent iron/Cu by green tea to remove hexavalent chromium from groundwater [J]. Journal of Cleaner Production, 2018, 174: 184-190.
12	Li Z H, Xu S Y, Xiao G H, et al. Removal of hexavalent chromium from groundwater using sodium alginate dispersed nano zero-valent iron [J]. Journal of Environmental Management, 2019, 244: 33-39.
13	Huang J Y, Yi S P, Zheng C M, et al. Persulfate activation by natural zeolite supported nanoscale zero-valent iron for trichloroethylene degradation in groundwater [J]. Science of the Total Environment, 2019, 684: 351-359.
14	Fu F L, Dionysiou D D, Liu H. The use of zero-valent iron for groundwater remediation and wastewater treatment: a review [J]. Journal of Hazardous Materials, 2014, 267: 194-205.
15	Song X J, Zhang C, Wu B D, et al. Ligand effects on arsenite removal by zero-valent iron/O₂: dissolution, corrosion, oxidation and coprecipitation [J]. Journal of Environmental Sciences, 2019, 86: 131-140.
16	Du M M, Zhang Y Q, Hussain I, et al. Effect of pyrite on enhancement of zero-valent iron corrosion for arsenic removal in water: a mechanistic study [J]. Chemosphere, 2019, 233: 744-753.
17	Liang Y J, Min X B, Chai L Y, et al. Stabilization of arsenic sludge with mechanochemically modified zero valent iron [J]. Chemosphere, 2017, 168: 1142-1151.
18	Mejia-Santillan M E, Pariona N, Bravo J, et al. Physical and arsenic adsorption properties of maghemite and magnetite sub-microparticles [J]. Journal of Magnetism and Magnetic Materials, 2018, 451: 594-601.
19	Mansouri T, Golchin A, Neyestani M R. The effects of hematite nanoparticles on phytoavailability of arsenic and corn growth in contaminated soils [J]. International Journal of Environmental Science and Technology, 2017, 14(7): 1525-1534.
20	Ramirez-Muniz K, Perez-Rodriguez F, Rangel-Mendez R. Adsorption of arsenic onto an environmental friendly goethite-polyacrylamide composite [J]. Journal of Molecular Liquids, 2018, 264: 253-260.
21	Kim H, Andersson T G. Arsenic surface segregation during the molecular-beam epitaxial growth of GaAs embedded in wurtzite GaN [J]. Applied Physics Letters, 2002, 80(25): 4768-4770.
22	Dou X M, Wang G C, Zhu M Q, et al. Identification of Fe and Zr oxide phases in an iron-zirconium binary oxide and arsenate complexes adsorbed onto their surfaces [J]. Journal of Hazardous Materials, 2018, 353: 340-347.
23	Su C M, Puls R W. Arsenate and arsenite removal by zerovalent iron: effects of phosphate, silicate, carbonate, borate, sulfate, chromate, molybdate, and nitrate, relative to chloride [J]. Environmental Science & Technology, 2001, 35(22): 4562-4568.
24	Gibert O, de Pablo J, Cortina J L, et al. In situ removal of arsenic from groundwater by using permeable reactive barriers of organic matter/limestone/zero-valent iron mixtures [J]. Environmental Geochemistry and Health, 2010, 32(4): 373-378.
25	Gatcha-Bandjun N, Noubactep C, Loura B B. Mitigation of contamination in effluents by metallic iron: the role of iron corrosion products [J]. Environmental Technology & Innovation, 2017, 8: 71-83.
26	Yang Z, Xu H, Shan C, et al. Effects of brining on the corrosion of ZVI and its subsequent As(Ⅲ/Ⅴ) and Se(Ⅳ/Ⅵ) removal from water[J]. Chemosphere, 2017, 170: 251-259.
27	Liu P P, Liang Q W, Luo H J, et al. Synthesis of nano-scale zero-valent iron-reduced graphene oxide-silica nano-composites for the efficient removal of arsenic from aqueous solutions [J]. Environmental Science and Pollution Research, 2019, 26(32): 33507-33516.
28	Mercer K L, Tobiason J E. Removal of arsenic from high ionic strength solutions: effects of ionic strength, pH, and preformed versus in situ formed HFO [J]. Environmental Science & Technology, 2008, 42(10): 3797-3802.
29	Farrell J, Wang J P, O'day P, et al. Electrochemical and spectroscopic study of arsenate removal from water using zero-valent iran media [J]. Environmental Science & Technology, 2001, 35(10): 2026-2032.
30	Esfahani A R, Firouzi A F, Sayyad G, et al. Transport and retention of polymer-stabilized zero-valent iron nanoparticles in saturated porous media: effects of initial particle concentration and ionic strength [J]. Journal of Industrial and Engineering Chemistry, 2014, 20(5): 2671-2679.

[1]	晁京伟, 许嘉兴, 李廷贤. 基于无管束蒸发换热强化策略的吸附热池的供热性能研究[J]. 化工学报, 2023, 74(S1): 302-310.
[2]	杨学金, 杨金涛, 宁平, 王访, 宋晓双, 贾丽娟, 冯嘉予. 剧毒气体PH₃的干法净化技术研究进展[J]. 化工学报, 2023, 74(9): 3742-3755.
[3]	车睿敏, 郑文秋, 王小宇, 李鑫, 许凤. 基于离子液体的纤维素均相加工研究进展[J]. 化工学报, 2023, 74(9): 3615-3627.
[4]	赵亚欣, 张雪芹, 王荣柱, 孙国, 姚善泾, 林东强. 流穿模式离子交换层析去除单抗聚集体[J]. 化工学报, 2023, 74(9): 3879-3887.
[5]	胡亚丽, 胡军勇, 马素霞, 孙禹坤, 谭学诣, 黄佳欣, 杨奉源. 逆电渗析热机新型工质开发及电化学特性研究[J]. 化工学报, 2023, 74(8): 3513-3521.
[6]	盛冰纯, 于建国, 林森. 铝基锂吸附剂分离高钠型地下卤水锂资源过程研究[J]. 化工学报, 2023, 74(8): 3375-3385.
[7]	张瑞航, 曹潘, 杨锋, 李昆, 肖朋, 邓春, 刘蓓, 孙长宇, 陈光进. ZIF-8纳米流体天然气乙烷回收工艺的产品纯度关键影响因素分析[J]. 化工学报, 2023, 74(8): 3386-3393.
[8]	高燕, 伍鹏, 尚超, 胡泽君, 陈晓东. 基于双流体喷嘴的磁性琼脂糖微球的制备及其蛋白吸附性能探究[J]. 化工学报, 2023, 74(8): 3457-3471.
[9]	陈吉, 洪泽, 雷昭, 凌强, 赵志刚, 彭陈辉, 崔平. 基于分子动力学的焦炭溶损反应及其机理研究[J]. 化工学报, 2023, 74(7): 2935-2946.
[10]	文兆伦, 李沛睿, 张忠林, 杜晓, 侯起旺, 刘叶刚, 郝晓刚, 官国清. 基于自热再生的隔壁塔深冷空分工艺设计及优化[J]. 化工学报, 2023, 74(7): 2988-2998.
[11]	王杰, 丘晓琳, 赵烨, 刘鑫洋, 韩忠强, 许雍, 蒋文瀚. 聚电解质静电沉积改性PHBV抗氧化膜的制备与性能研究[J]. 化工学报, 2023, 74(7): 3068-3078.
[12]	卫雪岩, 钱勇. 微米级铁粉燃料中低温氧化反应特性及其动力学研究[J]. 化工学报, 2023, 74(6): 2624-2638.
[13]	陈朝光, 贾玉香, 汪锰. 以低浓度废酸驱动中和渗析脱盐的模拟与验证[J]. 化工学报, 2023, 74(6): 2486-2494.
[14]	王新悦, 王俊杰, 曹思贤, 王翠, 李灵坤, 吴宏宇, 韩静, 吴昊. 玻璃内包材界面修饰对机械应力诱导的单克隆抗体聚集体形成的影响[J]. 化工学报, 2023, 74(6): 2580-2588.
[15]	陈韶云, 徐东, 陈龙, 张禹, 张远方, 尤庆亮, 胡成龙, 陈建. 单层聚苯胺微球阵列结构的制备及其吸附性能[J]. 化工学报, 2023, 74(5): 2228-2238.