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Enhanced Hg Removal from Aqueous Streams by Sulfurized Activated Carbon Products: Equilibrium and Kinetic Studies

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Abstract

The removal of Hg from contaminated aquatic media is of major importance, taking into consideration the highly toxic character of the element. One of the most promising water treatment technologies is adsorption by low cost adsorbents, such as activated carbon produced by agricultural byproducts. In this study, activated carbon in granular form (GAC) was produced using pistachio shells from Aegina Island (Greece). Two main GAC products have been synthesized. The first one was chemically activated using ZnCl2. The second one was further treated with Na2S in order to introduce S atoms on the functional groups. The effectiveness of synthesized GAC products for Hg removal was evaluated by conducting batch equilibrium and kinetic experiments. It was found that sulfurization was able to increase by a factor of more than 2 the adsorptive capacity of activated carbon. Namely the maximum adsorption capacity was 73 mg/g for the simple GAC and increased up to 166 mg/g for the S-modified product. The kinetics of adsorption was described with almost equivalent precision using the pseudo-first and the pseudo-second order models, a behavior which is often observed in adsorption experiments, depending on the experimental conditions. The value of activation energy EA was found to be negative (− 18.8 kJ/mol) in the case of simple GAC and positive (8.27 kJ/mol), in the case of S-modified GAC, suggesting that Hg adsorption on the modified carbon follows a different mechanism, closer to chemisorption processes.

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References

  • Abdelouahab-Reddam, Z., Wahby, A., Mail, E., Silvestre-Albero, R. J., Rodríguez-Reinos, F., & Sepúlveda-Escribano, S. (2014). Activated carbons impregnated with Na2S and H2SO4: Texture, surface chemistry and application to mercury removal from aqueous solutions. Adsorption Science & Technology, 32, 101–115.

    CAS  Google Scholar 

  • Abdullah, N. S., Sharifuddin, S. S., & Hussin, M. H. (2018). Study on adsorption of mercury from aqueous solution on activated carbons prepared from palm kernel shell. In International Conference on Material Science and Engineering III 783 (pp. 109–114).

    Google Scholar 

  • Aljeboree, M., Alshirifi, A., & Alkaim, A. F. (2017). Kinetics and equilibrium study for the adsorption of textile dyes on coconut shell activated carbon. Arabian Journal of Chemistry, 10, S3381–S3393.

    CAS  Google Scholar 

  • Anoop Krishnan, K., & Anirudhan, T. S. (2002). Removal of mercury (II) from aqueous solutions and chlor-alkali industry effluent by steam activated and sulphurised activated carbons prepared from bagasse pith: Kinetics and equilibrium studies. Journal of Hazardous Materials, 92, 161–183.

    CAS  Google Scholar 

  • Asasian, N., & Kaghazchi, T. (2015). Sulfurized activated carbons and their mercury adsorption/desorption behavior in aqueous phase. Environmental Science & Technology, 12, 2511–2522.

    CAS  Google Scholar 

  • Asasian-Kolur, N., Sharifian, S., Kavand, M., & Kaghazchi, T. (2019). Batch and fixed-bed mode mercury uptake by a modified adsorbent. Chemical Engineering Communications.

  • Azizian, S. (2004). Kinetic models of sorption: A theoretical analysis. Journal of Colloid and Interface Science, 276, 47–52.

    CAS  Google Scholar 

  • Baeyens, R., Ebinghous, R., & Vasilev, O. (1996). Global and regional mercury cycles: Sources. Fluxes and Mass Balances: Kluwer Academic Publishers.

    Google Scholar 

  • Barrett, E. P., Joyner, L. C., & Halenda, P. H. (1951). The determination of pore volume and area distributions in porous substances. I. Computations from Nitrogen Isotherms. Journal of the American Chemical Society, 73, 373–380.

    CAS  Google Scholar 

  • Barron-Zambrano, J., Laborie, S., Viers, P., Rakib, M., & Durand, G. (2004). Mercury removal and recovery from aqueous solutions by coupled complexation–ultrafiltration and electrolysis. Journal Membrane Science, 229(1–2), 179–186.

    CAS  Google Scholar 

  • Bartzas, G., & Komnitsas, K. (2017). Life cycle analysis of pistachio production in Greece. Science of the Total Environment, 595, 13–24.

    CAS  Google Scholar 

  • Budinova, T., Petrov, N., Parra, J., & Baloutzov, V. (2008). Use of an activated carbon from antibiotic waste for the removal of Hg (II) from aqueous solution. Journal of Environmental Management, 88, 165–172.

    CAS  Google Scholar 

  • Byrne, H. E., & Mazyck, D. W. (2009). Removal of trace level aqueous mercury by adsorption and photocatalysis on silica–titania composites. Journal of Hazardous Materials, 170, 915–919.

    CAS  Google Scholar 

  • Cai, J. H., & Jia, C. Q. (2010). Mercury removal from aqueous solution using coke-derived sulfur-impregnated activated carbons. Industrial & Engineering Chemistry Research, 49, 2716–2721.

    CAS  Google Scholar 

  • Chiarle, S., Ratto, M., & Rovatti, M. (2000). Mercury removal from water by ion exchange resins adsorption. Water Research, 34, 2971–2978.

    CAS  Google Scholar 

  • Cox, M., El-Shafey, E. I., Pichugin, A. A., & Appleton, Q. (2000). Removal of mercury ( II ) from aqueous solution on a carbonaceous sorbent prepared from flax shive. Journal of Chemical Technology & Biotechnology, 75, 427–435.

    CAS  Google Scholar 

  • Douven, S., Paez, C. A., & Gommes, C. J. (2015). The range of validity of sorption kinetic models. Journal of Colloid and Interface Science, 448, 437–450.

    CAS  Google Scholar 

  • Ekinci, E., Budinova, T., Yardim, T., Petrov, N., Razvigorova, M., & Minkova, V. (2002). Removal of mercury ion from aqueous solution by activated carbons obtained from biomass and coals. Fuel Processing Technology - Journal, 77–78, 437–443.

    Google Scholar 

  • El-Shafey, E. I. (2010). Removal of Zn (II) and Hg (II) from aqueous solution on a carbonaceous sorbent chemically prepared from rice husk. Journal of Hazardous Materials, 175, 319–327.

    CAS  Google Scholar 

  • EU (2020). EU mercury policy, https://ec.europa.eu/environment/chemicals/mercury/index_en.htm

  • EU Directive 98/83/EC. Drinking Water Directive.

  • Foo, K. Y., & Hameed, B. H. (2010). Insights into the modeling of adsorption isotherm systems. Chemical Engineering Journal, 156, 2–10.

    CAS  Google Scholar 

  • Hadi, P., To M.H, Hui, C. W., Lin, C., & McKay, G. (2015). Aqueous mercury adsorption by activated carbons. Water Research, 73, 37–55.

    CAS  Google Scholar 

  • Henneberry, Y. K., Tamara, E. C., Kraus, T. E., et al. (2011). Removal of inorganic mercury and methylmercury from surface waters following coagulation of dissolved organic matter with metal-based salts. Science of the Total Environment, 409, 631–637.

    CAS  Google Scholar 

  • Inbaraj, B. S., & Sulochana, N. (2006). Mercury adsorption on a carbon sorbent derived from fruit shell of Terminalia catappa. Journal of Hazardous Materials, B133, 283–290.

    Google Scholar 

  • Inbaraj, B. S., Wang, J. S., Lu, J. F., Siao, F. Y., & B.H. (2009). Chen adsorption of toxic mercury (II) by an extracellular biopolymer poly (gamma-glutamic acid). Bioresource Technology, 100, 200–207.

    CAS  Google Scholar 

  • Ioannidou, O., & Zabaniotou, A. (2006). Agricultural residues as precursors for activated carbon production—A review. Chemical Engineering Journal, 11, 1966–2005.

    Google Scholar 

  • Ismaiel, A. A., Aroua, M. K., & Yusoff, R. (2013). Palm shell activated carbon impregnated with task-specific ionic-liquids as a novel adsorbent for the removal of mercury from contaminated water. Chemical Engineering Journal, 225, 306–314.

    Google Scholar 

  • Kadirvelu K, .Kavipriya M., Karthika C., Vennilamani N., Pattabhi S. (2004). Mercury (II) adsorption by activated carbon made from sago waste. Carbon, 42,745–752.

    CAS  Google Scholar 

  • Karagianni E., Chatzitheodoridis E., Papassiopi N. (2019). Characterization of activated carbon prepared from Aegina pistachio shells for Hg removal. Proceeding of the 16th International Conference on Environmental Science and Technology, https://cest2019.gnest.org/sites/default/files/presentation_file_list/cest2019_00539_oral_paper.pf

  • Kazemi, F., Younesi, H., Ghoreyshi, A. A., Bahramifar, N., & Heidari, A. (2016). Thiol-incorporated activated carbon derived from fir wood sawdust as an efficient adsorbent for the removal of mercury ion: Batch and fixed-bed column studies. Process Safety and Environment Protection, 100, 22–35.

    CAS  Google Scholar 

  • Kokkinos, E., Soukakos, K., Kostoglou, M., & Mitrakas, M. (2018). Cadmium, mercury, and nickel adsorption by tetravalent manganese feroxyhyte: Selectivity, kinetic modeling, and thermodynamic study. Environmental Science and Pollution Research, 25, 12263–12273.

    CAS  Google Scholar 

  • Komnitsas, K., & Zaharaki, D. (2016). Morphology of modified biochar and its potential for phenol removal from aqueous solutions. Frontiers in Environmental Science, 4, 26.

    Google Scholar 

  • Komnitsas, K., Zaharaki, D., Bartzas, G., Kaliakatsou, G., & Kritikaki. (2016). A. Efficiency of pecan shells and sawdust biochar on Pb and Cu adsorption. Desalination and Water Treatment, 57, 3237–3246.

    CAS  Google Scholar 

  • Komnitsas, K., Zaharaki, D., Pyliotis, I., Vamvuka, D., & Bartzas, G. (2015). Assessment of pistachio shell biochar quality and its potential for adsorption of heavy metals. Waste and Biomass Valorization, 6, 805–816.

    CAS  Google Scholar 

  • Li, Z., Wu, L., Liu, H., Lan, H., & Qu, J. (2013). Improvement of aqueous mercury adsorption on activated coke by thiol-functionalization. Chemical Engineering Journal, 228, 925–934.

    CAS  Google Scholar 

  • Liu, M., Hou, L. A., Xi, B., Zhao, Y., & Xia, X. (2013). Synthesis, characterization, and mercury adsorption properties of hybrid mesoporous aluminosilicate sieve prepared with fly ash. Applied Surface Science, 273, 706–716.

    CAS  Google Scholar 

  • Lo, K. S. L., & Yu, Y. H. (1988). The removal of soluble mercury by cementation processes. Water Pollution Control in Asia, 441–447.

  • Lu, Y., & Shen, L. (2008). From Langmuir kinetics to first- and second-order rate equations for adsorption. Langmuir, 24(20), 11625–11630.

    Google Scholar 

  • Matlock, M. M., Howerton, B. S., & Atwood, D. A. (2002). Chemical precipitation of heavy metals from acid mine drainage. Water Research, 36, 4757–4764.

    CAS  Google Scholar 

  • Mohan, D., Gupta, V. K., Srivastava, S. K., & Chander, S. (2001). Kinetics of mercury adsorption from wastewater using activated carbon derived from fertilizer waste. Colloids and Surfaces A, 177, 169–181.

    CAS  Google Scholar 

  • Nabais, J. V., Carrott, P. J. M., & Ribeiro M.M.Let al. (2005). Mercury removal from aqueous solution and flue gas by adsorption on activated carbon fibres. Applied Surface Science, 252, 6046–6052.

    Google Scholar 

  • Oickle, A. M., Goertzen, S. L., Hopper, K. R., Abdalla, Y. O., & Andreas, H. A. (2010). Standardization of the Boehm titration: Part II. Method of agitation, effect of filtering and dilute titrant. Carbon, 48, 3313–3322.

    CAS  Google Scholar 

  • Otani, Y., Emi, H., Kanaoka, C., Uchijima, I., & Nishino, H. (1988). Removal of mercury vapor from air with sulfur-impregnated adsorbents. Environmental Science & Technology, 22, 708–711.

    CAS  Google Scholar 

  • Pacyna E., Pacyna J., Fudala J., Strzelecka-Jastrzab E., Hlawiczka S., Panasiuk D. (2006). Mercury emissions to the atmosphere from anthropogenic sources in Europe in 2000 and their scenarios until 2020 Science of the Total Environment, 370,147–156.

    Google Scholar 

  • Pitoniak E, Chang-Yu Wu, Mazyck D.W., Powers K.W., Sigmund W.(2005). Adsorption enhancement mechanisms of silica−Titania Nanocomposites for elemental mercury vapor removal. Environmental Science & Technology, 39,1269–1274.

  • Ramakrishna, T. V., Aravamudan, G., & Vijayakumar, M. (1976). Spectrophotometric determination of mercury (II) as the ternary complex with Rhodamine 6G and iodide. Analytica Chimica Acta, 84, 369–375.

    CAS  Google Scholar 

  • Rao, M. M., Reddy, D. H. K. K., Venkateswarlu, P., & Seshaiah, K. (2009). Removal of mercury from aqueous solutions using activated carbon prepared from agricultural by-product/waste. Journal of Environmental Management, 90, 634–643.

    CAS  Google Scholar 

  • Raposo, F., De La Rubia, M. A., & Borga, R. (2009). Methylene blue number as useful indicator to evaluate the adsorptive capacity of granular activated carbon in batch mode: Influence of adsorbate/adsorbent mass ratio and particle size. Journal of Hazardous Materials, 165, 291–299.

    CAS  Google Scholar 

  • Saha, P., & Chowdhury, S. (2011). Insight into adsorption thermodynamics. Thermodynamics, 349–465.

  • Sajjadi, S.-A., Mohammadzadeh, A., Tran, H. N., Anastopoulos, I., Dotto, G. L., & Lopičić, et al. (2018). Efficient mercury removal from wastewater by pistachio wood wastes-derived activated carbon prepared by chemical activation using a novel activating agent. Journal of Environmental Management, 223, 1001–1009.

  • Takagai, Y., Shibata, A., Kiyokawa, S., & Takase, T. (2011). Synthesis and evaluation of different thio-modified cellulose resins for the removal of mercury (II) ion from highly acidic aqueous solutions. Journal of Colloid and Interface Science, 353, 593–597.

    CAS  Google Scholar 

  • Tan, K. L., & Hameed, B. H. (2017). Insight into the adsorption kinetics models for the removal of contaminants from aqueous solutions. Journal of the Taiwan Institute of Chemical Engineers, 74, 25–48.

    CAS  Google Scholar 

  • UN Environment: 2019. Global mercury assessment.(2018). UN Environment Programme, chemicals and health. Branch Geneva, Switzerland ISBN, 978-92-807-3744-8.

  • USEPA.(1992). United States Enviromental Protection Agency, Grounl water and drinking water, National Primary drinking water legulations.https://safewater.zendesk.com/hc/en-us/articles/212076077-4-What-are-EPA-s-drinking-water-regulations-for-mercury

  • Wang, J., Deng, B., Wang, X., & Zheng, J. (2009). Adsorption of aqueous Hg (II) by sulfur-impregnated activated carbon. Environmental Engineering Science, 26, 693–1699.

    Google Scholar 

  • Yardim, M. F., Budinova, T., Ekinci, E., Petrov, N., Razvigorova, M., & Minkova, V. (2003). Removal of mercury (II) from aqueous solution by activated carbon obtained from furfural. Chemosphere, 52(5), 835–884.

    CAS  Google Scholar 

  • Yin, C. Y., Mohd, K. A., Wan, M. A., & Wan, D. (2007). Review of modifications of activated carbon for enhancing contaminant uptakes from aqueous solutions. Separation and Purification Technology, 52, 403–415.

    CAS  Google Scholar 

  • Zabihi, M., Ahmadpour, & Asl, H. (2009). Removal of mercuryfrom water by carbonaceous sorbents derived from walnut shell. Journal of Hazardous Materials, 167, 230–236.

    CAS  Google Scholar 

  • Zhang F.-S.,. Nriagu J.O., Itoh H.(2005). Mercury removal from water using activated carbons derived from organic sewage sludge Water Research, 39,389–395.

    Google Scholar 

  • Zhu, J., Deng, B., Yang, J., & Gang, D. (2009). Modifying activated carbon with hybrid ligands for enhancing aqueous mercury removal. Carbon, 47, 2014–2025.

    CAS  Google Scholar 

  • Zúñiga-Muro, N. M., Bonilla-Petriciolet, A., Mendoza-Castillo, D. I., Reynel-Ávila, H. E., Duran-Vallec, C. J., Ghallad, H., & Sellaoui, L. (2020). Recovery of grape waste for the preparation of adsorbents for water treatment: Mercury removal. Journal of Environmental Chemical Engineering, 8, 103738.

    Google Scholar 

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Funding

This research is co-financed by Greece and the European Union (European Social Fund- ESF) through the Operational Programme «Human Resources Development, Education and Lifelong Learning» in the context of the project “Strengthening Human Resources Research Potential via Doctorate Research” (MIS-5000432), implemented by the State Scholarships Foundation (Ι.Κ.Υ.).

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Correspondence to Eleftheria Karagianni.

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Karagianni, E., Xenidis, A. & Papassiopi, N. Enhanced Hg Removal from Aqueous Streams by Sulfurized Activated Carbon Products: Equilibrium and Kinetic Studies. Water Air Soil Pollut 231, 262 (2020). https://doi.org/10.1007/s11270-020-04606-x

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