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Frontiers of Environmental Science & Engineering

Front. Environ. Sci. Eng.    2020, Vol. 14 Issue (4) : 68     https://doi.org/10.1007/s11783-020-1247-8
RESEARCH ARTICLE
In situ synthesis of FeS/Carbon fibers for the effective removal of Cr(VI) in aqueous solution
Rongrong Zhang, Daohao Li, Jin Sun, Yuqian Cui(), Yuanyuan Sun()
School of Environmental Science and Engineering, Collaborative Innovation Center for Marine Biomass Fiber, Materials and Textiles of Shandong Province, Qingdao University, Qingdao 266071, China
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Abstract

• FeS/carbon fibers were in situ synthesized with Fe-carrageenan hydrogel fiber.

• The double helix structure of carrageenan is used to load and disperse Fe.

• Pyrolyzing sulfate groups enriched carrageenan-Fe could easily generate FeS.

• The adsorption mechanisms include reduction and complexation reaction.

Iron sulfide (FeS) nanoparticles (termed FSNs) have attracted much attention for the removal of pollutants due to their high efficiency and low cost, and because they are environmentally friendly. However, issues of agglomeration, transformation, and the loss of active components limit their application. Therefore, this study investigates in situ synthesized FeS/carbon fibers with an Fe-carrageenan biomass as a precursor and nontoxic sulfur source to ascertain the removal efficiency of the fibers. The enrichment of sulfate groups as well as the double-helix structure in ι-carrageenan-Fe could effectively avoid the aggregation and loss of FSNs in practical applications. The obtained FeS/carbon fibers were used to control a Cr(VI) polluted solution, and exhibited a relatively high removal capacity (81.62 mg/g). The main mechanisms included the reduction of FeS, electrostatic adsorption of carbon fibers, and Cr(III)-Fe(III) complexation reaction. The pseudo-second-order kinetic model and Langmuir adsorption model both provided a good fit of the reaction process; hence, the removal process was mainly controlled by chemical adsorption, specifically monolayer adsorption on a uniform surface. Furthermore, co-existing anions, column, and regeneration experiments indicated that the FeS/carbon fibers are a promising remediation material for practical application.

Keywords Carrageenan      FeS      Double-helix structure      Hexavalent chromium     
Corresponding Author(s): Yuqian Cui,Yuanyuan Sun   
Issue Date: 20 April 2020
 Cite this article:   
Rongrong Zhang,Daohao Li,Jin Sun, et al. In situ synthesis of FeS/Carbon fibers for the effective removal of Cr(VI) in aqueous solution[J]. Front. Environ. Sci. Eng., 2020, 14(4): 68.
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http://journal.hep.com.cn/fese/EN/10.1007/s11783-020-1247-8
http://journal.hep.com.cn/fese/EN/Y2020/V14/I4/68
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Rongrong Zhang
Daohao Li
Jin Sun
Yuqian Cui
Yuanyuan Sun
Fig.1  Scanning electron microscope (SEM) and energy-dispersive X-ray spectroscopy (EDS) mappings for different materials (A-C: FeS-700, FeS-800, FeS-900; D-F:the magnified figures of FeS-700, FeS-800, FeS-900; G: the elements mapping of FeS-900 after reaction).
Fig.2  Nitrogen adsorption/desorption isotherms (A), pore size distribution (B), X-ray diffraction (XRD) (C) and magnetization hysteresis of FeS-700, FeS-800 and FeS-900 (D).
Sample Surface area (m2/g) Pore volume (cm3/g) Smicro/Stoal
(%)
Vmicro/Vtoal (%) Dp(nm)
SBET SExt Smicro Vtoal Vmicro
FeS-700 282.88 14.17 268.71 0.1738 0.1439 94.99 82.79 2.5647
FeS-800 329.96 25.13 304.83 0.1973 0.1658 84.03 92.38 2.4864
FeS-900 368.99 35.28 333.71 0.2359 0.1869 79.23 90.44 2.6765
Tab.1  Physical properties of different samples
Fig.3  The effect of reaction time (A), pseudo-first-order fitting (B), pseudo-second-order fitting (C), the effect of initial concentration (D), Langmuir (E) and Freundlich adsorption isotherms (F) of Cr(VI) for different samples.
Sample Pseudo-first-order Pseudo-second-order
Qe (mg/g) k1 (h–1) R2 Qe (mg/g) k2 (h–1) R2
FeS-700 19.94 0.292 0.664 20.06 0.263 0.980
FeS-800 59.85 0.343 0.956 60.12 0.083 0.998
FeS-900 80.03 0.565 0.848 80.25 0.126 0.998
Tab.2  Fitting result of kinetic models for different samples
Sample Langmuir Freundlich
Qe (mg/g) KL(L/mg) R2 Kf (mg1–nLn/g) n R2
FeS-700 25.11 0.038 0.986 2.200 2.596 0.945
FeS-800 68.23 0.015 0.999 4.120 2.124 0.962
FeS-900 81.62 0.012 0.999 1.632 1.669 0.934
Tab.3  Fitting result of adsorption isotherms for different samples.
Fig.4  Effect of pH (A), pH change after reaction (B), competitive anions (C) and regeneration study (D) of the adsorption of Cr(VI) for different samples.
Fig.5  Effect of different operating conditions on the breakthrough curves for Cr(VI) removal by FeS/carbon fibers using a fixed-bed column. Effect of the adsorbents type (A), height of adsorbents (B) and initial Cr(VI) concentration (C) and flow rate (D) on Cr(VI) removal.
Fig.6  X-ray photoelectron spectroscopy (XPS) spectrum of FeS-900 before and after adsorption.
1 Z Ai, Y Cheng, L Zhang, J Qiu (2008). Efficient removal of Cr(VI) from aqueous solution with Fe@Fe2O3 core-shell nanowires. Environmental Science & Technology, 42(18): 6955–6960
https://doi.org/10.1021/es800962m pmid: 18853815
2 M M Alghamdi, A A El-Zahhar, A M Idris, T O Said, T Sahlabji, A El Nemr (2019). Synthesis, characterization, and application of a novel polymeric-bentonite-magnetite composite resin for water softening. Separation and Purification Technology, 224: 356–365
https://doi.org/10.1016/j.seppur.2019.05.037
3 A Argüelles, F Barbés, J I Espeso, C Garcia-Mateo (2019). Cryogenic study of the magnetic and thermal stability of retained austenite in nanostructured bainite. Science and Technology of Advanced Materials, 20(1): 673–687
https://doi.org/10.1080/14686996.2019.1625722 pmid: 31275459
4 C E Barrera-Diaz, V Lugo-Lugo, B Bilyeu (2012). A review of chemical, electrochemical and biological methods for aqueous Cr(VI) reduction. Journal of Hazardous Materials, 1–12: 223–224
5 M Bhaumik, A Maity, V V Srinivasu, M S Onyango (2012). Removal of hexavalent chromium from aqueous solution using polypyrrole-polyaniline nanofibers. Chemical Engineering Journal, 181–182: 323–333
https://doi.org/10.1016/j.cej.2011.11.088
6 Y H Cao, J N Huang, Y H Li, S Qiu, J R Liu, A Khasanov, M A Khan, D P Young, F Peng, D P Cao, X F Peng, K L Hong, Z H Guo (2016). One-pot melamine derived nitrogen doped magnetic carbon nanoadsorbents with enhanced chromium removal. Carbon, 109: 640–649
https://doi.org/10.1016/j.carbon.2016.08.035
7 T Chen, L Luo, S Deng, G Shi, S Zhang, Y Zhang, O Deng, L Wang, J Zhang, L Wei (2018). Sorption of tetracycline on H3PO4 modified biochar derived from rice straw and swine manure. Bioresource Technology, 267: 431–437
https://doi.org/10.1016/j.biortech.2018.07.074 pmid: 30032057
8 J Du, J Bao, C Lu, D Werner (2016). Reductive sequestration of chromate by hierarchical FeS@Fe0 particles. Water Research, 102: 73–81
https://doi.org/10.1016/j.watres.2016.06.009 pmid: 27322748
9 W Y Du, Q Z Zhang, Y N Shang, W Wang, Q Li, Q Y Yue, B Y Gao, X Xu (2020). Sulfate saturated biosorbent-derived Co-S@NC nanoarchitecture as an efficient catalyst for peroxymonosulfate activation. Applied Catalysis B: Environmental, 262: 118302
https://doi.org/10.1016/j.apcatb.2019.118302
10 P Duan, T Ma, Y Yue, Y Li, X Zhang, Y Shang, B Gao, Q Zhang, Q Yue, X Xu (2019). Fe/Mn nanoparticles encapsulated in nitrogen-doped carbon nanotubes as a peroxymonosulfate activator for acetamiprid degradation. Environmental Science. Nano, 6(6): 1799–1811
https://doi.org/10.1039/C9EN00220K
11 P Duan, Y Qi, S Feng, X Peng, W Wang, Y Yue, Y Shang, Y Li, B Gao, X Xu (2020). Enhanced degradation of clothianidin in peroxymonosulfate/catalyst system via core-shell FeMn@N-C and phosphate surrounding. Applied Catalysis B: Environmental, 267: 118717
https://doi.org/10.1016/j.apcatb.2020.118717
12 L Fei, Q Lin, B Yuan, G Chen, P Xie, Y Li, Y Xu, S Deng, S Smirnov, H Luo (2013). Reduced graphene oxide wrapped FeS nanocomposite for lithium-ion battery anode with improved performance. ACS Applied Materials & Interfaces, 5(11): 5330–5335
https://doi.org/10.1021/am401239f pmid: 23673403
13 K Y Foo, B H Hameed (2010). Insights into the modeling of adsorption isotherm systems. Chemical Engineering Journal, 156(1): 2–10
https://doi.org/10.1016/j.cej.2009.09.013
14 M Gheju, I Balcu, G Mosoarca (2016). Removal of Cr(VI) from aqueous solutions by adsorption on MnO2. Journal of Hazardous Materials, 310: 270–277
https://doi.org/10.1016/j.jhazmat.2016.02.042 pmid: 26947189
15 Y Gong, L Gai, J Tang, J Fu, Q Wang, E Y Zeng (2017). Reduction of Cr(VI) in simulated groundwater by FeS-coated iron magnetic nanoparticles. The Science of the total environment, 595: 743–751
https://doi.org/10.1016/j.scitotenv.2017.03.282 pmid: 28407591
16 Y Han, W Yan (2016). Reductive dechlorination of trichloroethene by zero-valent iron nanoparticles: Reactivity enhancement through sulfidation treatment. Environmental Science & Technology, 50(23): 12992–13001
https://doi.org/10.1021/acs.est.6b03997 pmid: 27934264
17 X He, X H Qiu, J Y Chen (2017). Preparation of Fe(II)-Al layered double hydroxides: Application to the adsorption/reduction of chromium. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 516: 362–374
https://doi.org/10.1016/j.colsurfa.2016.12.053
18 Y S Ho (2006). Review of second-order models for adsorption systems. Journal of Hazardous Materials, 136(3): 681–689
https://doi.org/10.1016/j.jhazmat.2005.12.043 pmid: 16460877
19 J Hu, G Chen, I M C Lo (2005). Removal and recovery of Cr(VI) from wastewater by maghemite nanoparticles. Water Research, 39(18): 4528–4536
https://doi.org/10.1016/j.watres.2005.05.051 pmid: 16146639
20 S H Huang, D H Chen (2009). Rapid removal of heavy metal cations and anions from aqueous solutions by an amino-functionalized magnetic nano-adsorbent. Journal of Hazardous Materials, 163(1): 174–179
https://doi.org/10.1016/j.jhazmat.2008.06.075 pmid: 18657903
21 E J Kim, J H Kim, A M Azad, Y S Chang (2011). Facile synthesis and characterization of Fe/FeS nanoparticles for environmental applications. ACS Applied Materials & Interfaces, 3(5): 1457–1462
https://doi.org/10.1021/am200016v pmid: 21520939
22 E J Kim, J H Kim, Y S Chang, D Turcio-Ortega, P G Tratnyek (2014). Effects of metal ions on the reactivity and corrosion electrochemistry of Fe/FeS nanoparticles. Environmental Science & Technology, 48(7): 4002–4011
https://doi.org/10.1021/es405622d pmid: 24579799
23 D Li, Y Sun, S Chen, J Yao, Y Zhang, Y Xia, D Yang (2018). Highly porous FeS/Carbon fibers derived from Fe-carrageenan biomass: High-capacity and durable anodes for sodium-ion batteries. ACS Applied Materials & Interfaces, 10(20): 17175–17182
https://doi.org/10.1021/acsami.8b03059 pmid: 29693371
24 H Liang, B Song, P Peng, G J Jiao, X Yan, D She (2019). Preparation of three-dimensional honeycomb carbon materials and their adsorption of Cr(VI). Chemical Engineering Journal, 367: 9–16
https://doi.org/10.1016/j.cej.2019.02.121
25 J F Liu, Z S Zhao, G B Jiang (2008). Coating Fe3O4 magnetic nanoparticles with humic acid for high efficient removal of heavy metals in water. Environmental Science & Technology, 42(18): 6949–6954
https://doi.org/10.1021/es800924c pmid: 18853814
26 H H Lyu, J C Tang, Y Huang, L S Gai, E Y Zeng, K Liber, Y Y Gong (2017). Removal of hexavalent chromium from aqueous solutions by a novel biochar supported nanoscale iron sulfide composite. Chemical Engineering Journal, 322: 516–524
https://doi.org/10.1016/j.cej.2017.04.058
27 D Mohan, C U Pittman Jr (2006). Activated carbons and low cost adsorbents for remediation of tri- and hexavalent chromium from water. Journal of Hazardous Materials, 137(2): 762–811
https://doi.org/10.1016/j.jhazmat.2006.06.060 pmid: 16904258
28 K P Raven, A Jain, R H Loeppert (1998). Arsenite and arsenate adsorption on ferrihydrite: Kinetics, equilibrium, and adsorption envelopes. Environmental Science & Technology, 32(3): 344–349
https://doi.org/10.1021/es970421p
29 N Sankararamakrishnan, A Shankhwar, D Chauhan (2019). Mechanistic insights on immobilization and decontamination of hexavalent chromium onto nano MgS/FeS doped cellulose nanofibres. Chemosphere, 228: 390–397
https://doi.org/10.1016/j.chemosphere.2019.04.166 pmid: 31048236
30 A C Scheinost, L Charlet (2008). Selenite reduction by mackinawite, magnetite and siderite: XAS characterization of nanosized redox products. Environmental Science & Technology, 42(6): 1984–1989
https://doi.org/10.1021/es071573f pmid: 18409625
31 J Wu, X B Wang, R J Zeng (2017). Reactivity enhancement of iron sulfide nanoparticles stabilized by sodium alginate: Taking Cr(VI) removal as an example. Journal of Hazardous Materials, 333: 275–284
https://doi.org/10.1016/j.jhazmat.2017.03.023 pmid: 28371713
32 J Wu, R J Zeng (2018). In situ preparation of stabilized iron sulfide nanoparticle-impregnated alginate composite for selenite remediation. Environmental Science & Technology, 52(11): 6487–6496
https://doi.org/10.1021/acs.est.7b05861 pmid: 29722535
33 Y Xu, J Chen, R Chen, P Yu, S Guo, X Wang (2019). Adsorption and reduction of chromium(VI) from aqueous solution using polypyrrole/calcium rectorite composite adsorbent. Water Research, 160: 148–157
https://doi.org/10.1016/j.watres.2019.05.055 pmid: 31136848
34 R Yang, Y Wang, M Li, Y J Hong (2014). A new carbon/ferrous sulfide/iron composite prepares by an in situ carbonization reduction method from hemp (Cannabis sativa L.) stems and its Cr(VI) removal ability. ACS Sustainable Chemistry & Engineering, 2(5): 1270–1279
https://doi.org/10.1021/sc500092z
35 S Zhou, Y Li, J Chen, Z Liu, Z Wang, P Na (2014). Enhanced Cr(VI) removal from aqueous solutions using Ni/Fe bimetallic nanoparticles: Characterization, kinetics and mechanism. RSC Advances, 4(92): 50699–50707
https://doi.org/10.1039/C4RA08754B
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