•  
  •  
 

Corresponding Author

Jiao QU(quj100@nenu.edu.cn);
Ying LU(luy332@nenu.edu.cn)

Abstract

To study the optimal removal condition, adsorption mechanism and comparative analysis of the three typical cationic pollutants, i.e., Zn(II), anionic pollutant Cr(VI) and molecular pollutant sulfamethoxazole (SMX), using self-made upflowed electro-sorption device for adsorptions of above three pollutants by modified activated carbon fiber were researched. The activated carbon fiber (ACF) was modified by hydrochloric acid. The ACF morphology and structure before and after modification were characterized by SEM, BET and FTIR. The characterization results show that the modified ACF had fewer surface impurities than the modified surface and the gully is more obvious, the specific surface area was increased by 22%, while the micropore volume was increased by 5%, and the oxygen-containing functional groups (C-O, C=O) are significantly increased. Using the heavy metal ions (Zn(II), Cr(VI)) and the antibiotic Sulfamethoxazole (SMX) in water as the target pollutants, the adsorptions of ACF after hydrochloric acid modification on the target pollutants (static adsorption and electro-sorption) were studied. The effects of concentration, pH and applied voltage on adsorptions were investigated. The results showed that when the ACF dosage was 5 g, voltage was 1.2 V, Zn(II), Cr(VI) and SMX concentrations were 10 mg·L-1, Zn(II) solution pH was 5, the maximum adsorption capacity of Zn(II) adsorbed by ACF was 9.25 mg·g-1, which is 2.15 times of the static adsorption condition; when the pH of Cr(VI) solution was 4, the maximum adsorption amount of Cr(VI) adsorbed by ACF was 8.86 mg·g-1, which is 1.96 times of static adsorption condition; when the pH of SMX solution was 6, the maximum adsorption capacity of ACF to adsorb SMX was 8.32 mg·g-1, which is 1.84 times of static adsorption condition. The kinetic curves for the adsorptions of Zn(II), Cr(VI) and SMX by ACF were consistent with the pseudo-second-order kinetic model, and the adsorption process was chemical adsorption. The Freundlich isotherm model can better describe the adsorption characteristics of ACF on Zn(II), Cr(VI) and SMX, whose adsorption is multi-molecular layer adsorption. ACF was recycled by electrode reverse connection, whose desorption rate was fast and the desorption effect was obvious. After 4 cycles of regeneration, the removal rates of Zn(II), Cr(VI) and SMX by ACF were above 90%, and great regeneration efficiency, which can be reused in practical applications, saving resources.

Graphical Abstract

Keywords

activated carbon fiber, electro-adsorption, Zn(II), Cr(VI), sulphonamide, recycling

Publication Date

2019-12-28

Online Available Date

2018-09-30

Revised Date

2018-09-20

Received Date

2018-08-23

References

[1] Xiao J J(肖静晶). Research of recovery technology of Cu and Ni from electroplating waste-water[D]. Hunan: Central South University, 2012.
[2] Mi H, Jiang Z G, Kong J. Hydrophobic poly(ionic liquid) for highly effective separation of methyl blue and chromium ions from water[J]. Polymers, 2013, 5(4): 1203-1214.
[3] Tapiero Y, Rivas B L, Sanchez J, et al. Polypropylene membranes modified with interpenetrating polymer networks for the removal of chromium ions[J]. Journal of Applied Polymer Science, 2015, 132(19): 41953-41964.
[4] Lin H(林海), Yu M L(于明利), Dong Y B(董颖博), et al. The heavy mental leaching rules and influence mechanism of different particle size of tin mining waste rock[J]. China Environmental Science(中国环境科学), 2014, 24(3): 664-671.
[5] Pasquet J, Chevalier Y, Pelletier J, et al. The contribution of zinc ions to antimicrobial activity of zinc oxide[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2014, 457(1): 263-274.
[6] Xu Y(徐颖), Wang Q(王祺), Su M(苏墨), et al. Adsorption characteristics of sulfa antibiotics in the river sediments[J]. Journal of Safety Environment(安全与环境学报), 2016, 16(2): 278-283.
[7] Wang J L, Zhou A X, Zhang Y L, et al. Research on the adsorption and migration of sulfa antibiotics in underground environment[J]. Environment Earth Science, 2016, 75(18): 1252.
[8] Zhang D, Pan B, Zhang H, et al. Contribution of different sulfamethoxazole species to their overall adsorption on functionalized carbon nanotubes[J]. Environmental Science Technology, 2010, 44(10): 3806-3811.
[9] Yang J, Zhou M H, Zhao Y Y, et al. Electro-sorption driven by microbial fuel cells to remove phenol without external power supply[J]. Bioresource Technology, 2013, 150(3): 271-277.
[10] Mekala B, Nishith V, Kumar R S, et al. Preparation of activated carbon fibers from cost effective commercial textile grade acrylic fibers[J]. Carbon Letters, 2011, 12(1): 44-47.
[11] Zhang J J(张建军), Jiang H(姜华), Fang J H(方建慧), et al. Applications of new activated carbon meterials in the electric double-layer capacitor[J]. Journal of Electrochemistry(电化学), 2004, 10(4): 464-467.
[12] Bayram E, Ayranci E. Electrochemically enhanced removal of polycyclic aromatic basic dyes from dilute aqueous solutions by activated carbon cloth electrodes[J]. Environmental Science Technology, 2010, 44(16): 6331-6336.
[13] Utrilla R J, Prados J G, Sanchez P M, et al. Removal of nitroimidazole antibiotics from aqueous solution by adsorption/bio adsorption on activated carbon[J]. Journal of Hazardous Materials, 2009, 170(1): 298-305.
[14] Ayranci E, Hoda N. Adsorption kinetics and isotherms of pesticides onto activated carbon-cloth[J]. Chemosphere, 2005, 60(11): 1600-1607.
[15] Qiang Z M, Adams C . Potentiometric determination of acid dissociation constants (pKa) for human and veterinary antibiotics[J]. Water Research, 2004, 38(12): 2874-2890.
[16] Chen L, Chen Z H, Chen D, et al. Removal of hexavalent chromium from contaminated water by ultrasound-assisted aqueous solution ball milling[J]. Journal of Environmental Sciences, 2017, 52(2): 276-283.
[17] Gao C Y(高翠英), Li Y W(李彦威). Application of successive and simultaneous determination in water heavy metal elements analysis[J]. Guangdong Chemical Industry(广东化工), 2013, 23(40): 165-167.
[18] Xu W(徐伟), Zhang H M(张慧敏), Wu Z C(吴祖成). Electrochemical treatment of heavy metals with self-electricity generation[J]. Journal of Electrochemistry(电化学), 2013, 19(4): 345-349.
[19] Fu H Q(傅宏庆), Wang Y(王颖), Zhang D(张丹), et al. Simultaneous determination of 13 sulphonamides by high performance liquid chromatography-ultraviolet (HPLC-UV)[J]. China Animal Husbandry and Veterinary Medicine(中国畜牧兽医), 2102, 39(4): 233-237.
[20] He X S(何余生), Li Z(李忠) Xi H X(奚红霞), et al. Research progress on gas-solid adsorption isotherms[J]. Ion Exchange and Adsorption(离子交换与吸附), 2004, 20(4): 376-384.
[21] Zhang Y L, Tang Y, Qiu Q, et al. Electrochemically enhanced adsorption of aluminum from sodium carbonate solution by activated carbon fibers[J]. Industrial Engineering Chemistry Research, 2013, 52(40): 14449-14455.
[22] Chen P(陈培), Liu R L(刘润龙), Zhu D(朱丹), et al. Preparation of titanium loaded activated carbon fibers and their application in aqueous Rhodamine B photocatalytic degradation[J]. Environmental Chemistry(环境化学), 2015, 34(1): 144-149.
[23] Zhang L(张亮), Zhang H M(张红梅), Wan W H(万伟华), et al. Modifications and electrochemical properties of graphite fluoride[J]. Journal of Electrochemistry(电化学), 2018, 24(4): 385-391.
[24] Luo J W, Li X, Ge C J, et al. Sorption of norfloxacin, sulfamerazine and oxytetracycline by KOH modified biochar under single and ternary systems[J]. Bioresource Technology, 2018, 263: 385-392.
[25] Alchemic A, Conway B E. Investigation of removal of Cr(VI), Mo(VI), W(VI), V(N), and V(V) oxy-ions from industrial waste-waters by adsorption and electro-sorption at high-area carbon cloth[J]. Journal of Colloid and Interface Science, 2002, 251(2): 248-255.
[26] Yang J, Zhao Y Y, Zhang C, et al. Electrosorption driven by microbial fuel cells without electric grid energy consumption for simultaneous phenol removal and wastewater treatment[J]. Electrochemistry Communications, 2013, 34: 121-124.
[27] Yang W L, Han H X, Zhou M H, et al. Simultaneous electricity generation and tetracycline removal in continuous flow electro-sorption driven by microbial fuel cells[J]. RSC Advances, 2015, 5(61): 49513-49520.
[28] Qu G Z, Kou L Q, Wang T C, et al. Evaluation of activated carbon fiber supported nanoscale zero-valent iron for chromium(VI) removal from groundwater in a permeable reactive column[J]. Journal of Environmental Management, 2017, 201: 378-387.
[29] Zhang C L, Wang F A, Wang Y. Solubilities of sulfadiazine, sulfamethazine, sulfadimethoxine, sulfamethoxydiazine, sulfamonomethoxine, sulfamethoxazole, and sulfachloropyrazine in water from (298.15 to 333.15)K[J]. Journal of Chemical Engineering Data, 2007, 52(5): 1563-1566.
[30] Xie H H(谢欢欢), Zhou Y X(周元祥), Fan C C(范晨晨), et al. Study of the adsorption of heavy metal ions by modified activated carbon fibers[J]. Journal of Hefei University of Technology(Natural Science) (合肥工业大学学报(自然科学版)), 2016, 39(2): 256-259.
[31] Shrestha S, Son G, Lee S H, et al. Isotherm and thermodynamic studies of Zn(II) adsorption on lignite and coconut shell-based activated carbon fiber[J]. Chemosphere, 2013, 92(8): 1053-1061.
[32] Qiu B, Xu C X, Sun D Z, et al. Polyaniline coating on carbon fiber fabrics for improved hexavalent chromium removal[J]. RSC Advances, 2014, 4(56): 29855-29865.
[33] Huang L H, Zhou S J, Jin F, et al. Characterization and mechanism analysis of activated fiber felt-stabilized nanoscale zero-valent iron for the removal of Cr(VI) from aqueous solution[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2014, 447: 59-66.
[34] Qiang Z M, Adams C. Potentiometric determination of acid dissociation constants (pKa) for human and veterinary antibiotics[J]. Water Research, 2004, 38(12): 2874-2890.
[35] Li H, Zheng N, Liang N, et al. Adsorption mechanism of different organic chemicals on fluorinated carbon nanotubes[J]. Chemosphere, 2016, 154: 258-265.
[36] Wu M, Pan B, Zhang D, et al. The sorption of organic contaminants on biochars derived from sediments with high organic carbon content[J]. Chemosphere, 2013, 90(2): 782-788.
[37] Pan B, Xing B S. Adsorption mechanisms of organic chemicals on carbon nanotubes[J]. Environmental Science Technology, 2008, 42(24): 9005-9013.
[38] Wu Y Q, Xu C, Zhao Y, et al. Preparation of calcium silicate-chitosan polymer and the adsorptive removal of heavy metals in wastewater[J]. Environmental Chemistry, 2016, 35(3): 562-567.
[39] Park S J, JangY S. Pore structure and surface properties of chemically modified activated carbons for adsorption mechanism and rate of Cr(VI)[J]. Journal of Colloid and Interface Science, 2002, 249(2): 458-463.
[40] Anskjær G G, Krogh K A, Halling-Sorensen B. Dialysis experiments for assessing the pH-dependent sorption of sulfonamides to soil clay fractions[J]. Chemosphere, 2014, 95(1): 116-123.
[41] Quan X(全燮), Liu M W(刘梦薇), Wang S T(王斯坦), et al. Cylindrical electrosorption filter device using activated carbon fiber as electric adsorption material: China, 201510593323.0. [P]. 2015.
[42] Sibel T, Tamer A. Zn(II) biosorption properties of Botrytis cinerea biomass[J]. Journal of Hazardous Materials, 2006, 131(1): 137-145.
[43] Dong X L, Ma L Q, Li Y C. Characteristics and mechanisms of hexavalent chromium removal by biochar from sugar beet tailing[J]. Journal of Hazardous Materials, 2011, 190(1): 909-915.
[44] Gao J A, Pedersen J A. Adsorption of sulfonamide antimicrobial agents to clay minerals[J]. Environmental Science Technology, 2005, 39(24): 9509-9516.
[45] Li X, Zhao H, Quan X, et al. Adsorption of ionizable organic contaminants on multi-walled carbon nanotubes with different oxygen contents[J]. Journal of Hazardous Materials, 2011, 186(1): 407-415.
[46] Liu M W(刘梦薇). Electrochemical assistant adsorption of two sulfonamides on activated carbon fibers[D]. Dalian: Dalian University of Technology, 2016.
[47] Xu F C(徐芳草), Wang D D(王丹丹), Xu Q D(许庆迪), et al. Research on the treatment of low concentration wastewater containing Cu2+ by electrosorption[J]. Guangdong Chemical Industry(广东化工), 2015, 42(23): 155-157.

Share

COinS
 
 

To view the content in your browser, please download Adobe Reader or, alternately,
you may Download the file to your hard drive.

NOTE: The latest versions of Adobe Reader do not support viewing PDF files within Firefox on Mac OS and if you are using a modern (Intel) Mac, there is no official plugin for viewing PDF files within the browser window.