Abstract
The sludge-based activated carbons (SACs) were prepared by sewage sludge and corn straw and modified by ferric nitrate. The H2S removal performance and the desulfurization mechanism of the modified SAC were studied. Results showed that breakthrough sulfur capacity and saturation sulfur capacity of the SAC prepared by recommended modification were 27.209 mg/g and 48.098 mg/g, which were as 4.68 times and 7.02 times larger as those before modification, respectively. Additionally, results showed that the desulfurization products of unmodified SAC were mainly sulfur, while that of modified SAC were mainly sulfate. These results indicated that ferric nitrate modification changed the way of hydrogen sulfide removal by SAC: the desulfurization process of unmodified SAC can be expressed as S2− → S0 → S4+ → S6+, and the oxidative active component was dominated by O*, while that of modified SAC can be expressed as S2− → S0 → S6+, and the oxidative active components are both Fe3+ and O*.
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References
Ahmad W, Sethupathi S, Kanadasan G, Iberahim N (2020) Selectivity of SO2 and H2S removal by ethanol-treated calcined eggshell at low temperature. Environ Sci Pollut Res 27:22065–22080. https://doi.org/10.1007/s11356-020-08671-x
Bagreev A, Bandosz TJ (2002) H2S Adsorption/Oxidation on Materials Obtained Using Sulfuric Acid Activation of Sewage Sludge-Derived Fertilizer. J Colloid Interface Sci 252(1):188–194. https://doi.org/10.1006/jcis.2002.8419
Bagreev A, Bashkova S, Locke DC, Bandosz TJ (2001) Sewage sludge-derived materials as efficient adsorbents for removal of hydrogen sulfide. Environ Sci Technol 35(7):1537–1543. https://doi.org/10.1021/es001678h
Bandosz TJ (2002) On the adsorption/oxidation of hydrogen sulfide on activated carbons at ambient temperatures. J Colloid Interface Sci 246(1):1–20. https://doi.org/10.1006/jcis.2001.7952
Bandosz TJ, Karin B (2006) Municipal sludge-industrial sludge composite desulfurization adsorbents: synergy enhancing the catalytic properties. Environ Sci Technol 40(10):3378–3383. https://doi.org/10.1021/es052272d
Bandosz TJ, Block KA (2006) Removal of hydrogen sulfide on composite sewage sludge-industrial sludge-based adsorbents. Ind Eng Chem Res 45:3666–3672. https://doi.org/10.1021/ie0514152
Chen Y, Lai X (2014) Preparation and performance evaluation of iron oxide/activated carbon supported hydrogen sulfide scavenger. Ind Catal 22:680–682. https://doi.org/10.3969/j.issn.1008-1143.2014.09.007
Chen Q, Wang J, Liu X, Zhao X, Qiao W, Long D, Ling L (2011) Alkaline carbon nanotubes as effective catalysts for H2S oxidation. Carbon 49(12):3773–3780. https://doi.org/10.1016/j.carbon.2011.05.011
Chen Q-J (2012) H2S and CO2 removal by carbon based porous materials with control structures. Dissertation. East China University of Science and Technology, Shanghai (in Chinese)
Elena S, Miguel CN, Maria B, Nuno L, Isabel E, Isabel F (2019) New adsorbents from maize cob wastes and anaerobic digestate for H2S removal from biogas. Waste Manag 94:136–145. https://doi.org/10.1016/j.wasman.2019.05.048
Eniola JO, Kumar R, Barakat MA (2019) Adsorptive removal of antibiotics from water over natural and modified adsorbents. Environ Sci Pollut Res 26:34775–34788. https://doi.org/10.1007/s11356-019-06641-6
Farooq M, Almustapha MN, Imran M, Saeed MA, Andresen JM (2018) In-situ regeneration of activated carbon with electric potential swing desorption (EPSD) for the H2S removal from biogas. Bioresour Technol 249:125–131. https://doi.org/10.1016/j.biortech.2017.09.198
Gao Q, Zhang J-Y, Qiu J-H, Zhao Y-C (2007) A Study of High-temperature Corrosion Characteristics of Coal-fired Utility Boilers. J Eng Therm Energ Power 22(3):292–296. https://doi.org/10.3969/j.issn.1001-2060.2007.03.015. (in Chinese)
Ge X-Y (2016) Microwave-assisted Modification of coal-based activated carbon and studies on PAHs adsorption properties. Dissertation. Shihezi University, Shihezi (in Chinese)
Gu L, Li C, Wen H, Zhou P, Zhang D, Zhu N, Tao H (2017) Facile synthesis of magnetic sludge-based carbons by using electro-Fenton activation and its performance in dye degradation. Bioresour Technol 241:391–396. https://doi.org/10.1016/j.biortech.2017.05.115
Gutiérrez OFJ, Aguilera PG, Ollero P (2014) Biogas desulfurization by adsorption on thermally treated sewage-sludge. Sep Purif Technol 123:200–213. https://doi.org/10.1016/j.seppur.2013.12.025
Hao W, Björnerbäck F, Trushkina Y, Bengoechea MO, Salazar AG, Barth T, Hedin N (2017) High-performance magnetic activated carbon from solid waste from lignin conversion processes. Part I: Their use as adsorbents for CO2. Energy Procedia 114:6272–6296. https://doi.org/10.1016/j.egypro.2017.08.033
He C, Giannis A, Wang JY (2013) Conversion of sewage sludge to clean solid fuel using hydrothermal carbonization: Hydrochar fuel characteristics and combustion behavior. Appl Energy 111(11):257–266. https://doi.org/10.1016/j.apenergy.2013.04.084
Hervy M, Pham MD, Gérente C, Weiss HE, Nzihou A, Villot A, Le Coq L (2018) H2S removal from syngas using wastes pyrolysis chars. Chem Eng J 334:2179–2189. https://doi.org/10.1016/j.cej.2017.11.162
Kapoor R, Ghosh P, Kumar M, Vijay V (2019) Evaluation of biogas upgrading technologies and future perspectives: a review. Environ Sci Pollut Res 26:11631–11661. https://doi.org/10.1007/s11356-019-04767-1
Kokiasmenou E, Caliri C, Kantarelou V, Germanos KA, Romano FP, Brecoulaki H (2020) Macroscopic XRF imaging in unravelling polychromy on Mycenaean wall-paintings from the Palace of Nestor at Pylos. J Archaeol Sci Rep 29:102079
Kong Y-P (2011) Study on removal of hydrogen sulfide at low-temperature by modified inferior activated carbon and regeneration. Dissertation. Ocean University of China, Qingdao (in Chinese)
Li J, Liang Z, Guo C, Mei S, Li X (2017a) Removal of Cr(VI) by sewage sludge based activated carbons impregnated with nanoscale zero-valent iron. J Nanosci Nanotechnol 17(9):6936–6941. https://doi.org/10.1166/jnn.2017.14439
Li S, Hao J, Ning P, Wang C, Li K, Tang L, Sun X, Zhang D, Mei Y, Wang Y (2017b) Preparation of CuFe nanocomposites loaded diatomite and their excellent performance in simultaneous adsorption/oxidation of hydrogen sulfide and phosphine at low temperature. Sep Purif Technol 180:23–35. https://doi.org/10.1016/j.seppur.2017.02.044
Liadi MA, Tawabini B, Shawabkeh R, Jarrah N, Oyehan TA, Shaibani A, Makkawi M (2018) Treating MTBE-contaminated water using sewage sludge-derived activated carbon. Environ Sci Pollut Res 25(29):29397–29407. https://doi.org/10.1007/s11356-018-2737-0
Liu B, Hsieh C (2018) Enhanced selective catalytic wet oxidation of H2S to S over Ce–Fe/MgO catalysts at ambient temperature. J Taiwan Inst Chem E 89:113–118. https://doi.org/10.1016/j.jtice.2018.04.023
Liu H (2017) Fabrication and modification of activated carbons from biomass in constructed wetland and their adsorption mechanisms towards heavy metal ions. Dissertation. Shan Dong University, Shan Dong (in Chinese)
Lu S, Liu Y, Feng L, Sun Z, Zhang L (2017) Characterization of ferromagnetic sludge-based activated carbon and its application in catalytic ozonation of p-chlorobenzoic acid. Environ Sci Pollut Res 25(6):1–9. https://doi.org/10.1007/s11356-017-8680-7
McCallum C, Bandosz T, McGrother S, Müller E, Gubbins K (1998) A molecular model for adsorption of water on activated carbon: comparison of simulation and experiment. Langmuir 15:533–544. https://doi.org/10.1021/la9805950
Mykola S, Bandosz TJ (2007) Tobacco waste/industrial sludge-based desulfurization adsorbents: effect of phase interactions during pyrolysis on surface activity. Environ Sci Technol 41(10):3715–3721. https://doi.org/10.1021/es0624624
Ozekmekci M, Salkic G, Fellah MF (2015) Use of zeolites for the removal of H2S: a mini-review. Fuel Process Technol 139:49–60. https://doi.org/10.1016/j.fuproc.2015.08.015
Peng C, Zhai Y, Yun Z, Xu B, Wang T, Li C, Zeng G (2016) Production of char from sewage sludge employing hydrothermal carbonization: char properties, combustion behavior and thermal characteristics. Fuel 176:110–118. https://doi.org/10.1016/j.fuel.2016.02.068
Pipatmanomai S, Kaewluan S, Vitidsant T (2009) Economic assessment of biogas-to-electricity generation system with H2S removal by activated carbon in small pig farm. Appl Energy 86(5):669–674. https://doi.org/10.1016/j.apenergy.2008.07.007
Raheem A, Sikarwar VS, He J, Dastyar W, Dionysiou DD, Wang W, Zhao M (2018) Opportunities and challenges in sustainable treatment and resource reuse of sewage sludge: a review. Chem Eng J 337:616–641. https://doi.org/10.1016/j.cej.2017.12.149
Seredych M, Bandosz TJ (2006) Desulfurization of digester gas on catalytic carbonaceous adsorbents: complexity of interactions between the surface and components of the gaseous mixture. Ind Eng Chem Res 45(10):3658–3665. https://doi.org/10.1021/ie051388f
Silva TL, Ronix A, Pezoti O, Souza LS, Leandro PKT, Bedin KC, Beltrame KK, Cazetta AL, Almeida VC (2016) Mesoporous activated carbon from industrial laundry sewage sludge: adsorption studies of reactive dye Remazol Brilliant Blue R. Chem Eng J 303:467–476. https://doi.org/10.1016/j.cej.2016.06.009
Song X, Li S, Li K, Ning P, Wang C, Sun X, Wang Y (2018) Preparation of Cu-Fe composite metal oxide loaded SBA-15 and its capacity for simultaneous catalytic oxidation of hydrogen sulfide and phosphine. Microporous Mesoporous Mater 259:89–98. https://doi.org/10.1016/j.micromeso.2017.10.004
Sousa MR, Oliveira CJS, Carneiro JM, Lopes AC, Rodríguez E, Vasconcelos EAF, Holanda GBM, Landim PGC, Silva MER, Firmino PIM (2018) Evaluation of different air dosing strategies to enhance H2S removal in microaerobic systems treating low-strength wastewaters. Environ Technol 40:3724–3734. https://doi.org/10.1080/09593330.2018.1487470
Steijns M, Derks F, Verloop A, Mars P (1976) The mechanism of the catalytic oxidation of hydrogen sulfide: II. Kinetics and mechanism of hydrogen sulfide oxidation catalyzed by sulfur. J Catal 42(1):87–95. https://doi.org/10.1016/0021-9517(76)90094-4
Tasdemir HM, Yasyerli S, Yasyerli N (2015) Selective catalytic oxidation of H2S to elemental sulfur over titanium based Ti–Fe, Ti–Cr and Ti–Zr catalysts. Int J Hydrogen Energ 40(32):9989–10001. https://doi.org/10.1016/j.ijhydene.2015.06.056
Tay JH, Chen XG, Jeyaseelan S, Graham N (2001) A comparative study of anaerobically digested and undigested sewage sludges in preparation of activated carbons. Chemosphere 44(1):53–57. https://doi.org/10.1016/S0045-6535(00)00384-2
Thommes M, Kaneko K, Neimark AV, Olivier JP, Rodriguez-Reinoso F, Rouquerol J, Sing KSW (2015) Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report). Pure Appl Chem 87:1051. https://doi.org/10.1515/pac-2014-1117
Wallace R, Seredych M, Zhang P, Bandosz TJ (2014) Municipal waste conversion to hydrogen sulfide adsorbents: investigation of the synergistic effects of sewage sludge/fish waste mixture. Chem Eng J 237:88–94. https://doi.org/10.1016/j.cej.2013.10.005
Wen H, Gu L, Yu H, Qiao X, Zhang D, Ye J (2018) Radical assisted iron impregnation on preparing sewage sludge derived Fe/carbon as highly stable catalyst for heterogeneous Fenton reaction. Chem Eng J 352:837–846. https://doi.org/10.1016/j.cej.2018.07.106
Xia H, Chang X, Liu B (2017) High-temperature H2S removal performance over ordered mesoporous La-Mn-supported Al2O3-CaO sorbents. Chem Eng J 321:277–285. https://doi.org/10.1016/j.cej.2017.03.078
Xie W, Chang L-P, Yu J-L, Xie K-C (2006) Research progress of removal of H2S from coal gas by dry method. J Chem Ind Eng 09:2012–2020. https://doi.org/10.3321/j.issn:0438-1157.2006.09.002 (in Chinese)
Xin L, Li W, Wang G, Ping W, Gong X (2015) Preparation, characterization, and application of sludge with additive scrap iron-based activated carbons. Desalin Water Treat 54(4-5):1194–1203. https://doi.org/10.1080/19443994.2014.895961
Yan R, Chin T, Ng YL, Duan H, Liang DT, Tay JH (2004) Influence of surface properties on the mechanism of H2S removal by alkaline activated carbons. Environ Sci Technol 38(1):316–323. https://doi.org/10.1021/es0303992
Yi L, Jin H, Liu W, Hang S, Yao L, Li J (2018) Study on regeneration of waste powder activated carbon through pyrolysis and its adsorption capacity of phosphorus. Sci Rep 8(1):778. https://doi.org/10.1038/s41598-017-19131-x
Yuan W, Bandosz TJ (2007) Removal of hydrogen sulfide from biogas on sludge-derived adsorbents. Fuel 86:2736–2746. https://doi.org/10.1016/j.fuel.2007.03.012
Zeng F, Liao X, Hu H, Liao L (2017a) Effect of KOH activation in the desulfurization process of activated carbon prepared by sewage sludge & corn straw. J Air Waste Manage Assoc 68(12):255–264. https://doi.org/10.1080/10962247.2017.1407378
Zeng F, Liao X, Li Y, He Y, Liao L, Hu H (2017b) Preparation of sludge-straw based activated carbon and its adsorption of H2S. Acta Sci Circumst 37(11):4269–4276. https://doi.org/10.13671/j.hjkxxb.2017.0170
Zeng F, Li Y, Zhang HM, Liao L (2017c) Preparation and orthogonal optimization experiment of sludge-based activated carbon with vegetable wastes. Renew Energ Res 35(5):653–658 CNKI:SUN:NCNY.0.2017-05-004
Zeng F, Liao X, Liao L, Hu H (2018) Mechanism and performance of preparation of compositional sewage sludge & corn straw-derived activated carbon with KOH. Desalin Water Treat 108:97–105. https://doi.org/10.5004/dwt.2018.21847
Zhai Y-B (2005) Academic research on adsorbent derived from sewage sludge based on chemical activation method and its application. Dissertation. Hunan University, Hunan (in Chinese)
Zhang CS, Wang WJ, Su HJ, Wang ZB, Wang EB (2016) Desulfurization of biogas by modified activated carbon and its regeneration. Mod Chem Ind 36:59–62. https://doi.org/10.16606/j.cnki.ISSN0253-4320.2016.12.014
Zhang F, Zhang X, Hao Z, Jiang G, Yang H, Qu S (2018) Insight into the H2S selective catalytic oxidation performance on well-mixed Ce-containing rare earth catalysts derived from MgAlCe layered double hydroxides. J Hazard Mater 342:749–757. https://doi.org/10.1016/j.jhazmat.2017.09.014
Funding
This work was supported by the Natural Science Research of Jiangsu Higher Education Institutions of China (No.19KJB610012, No.18KJB610006), the Introduction Talent Scientific Research Foundation Project of Nanjing Institute of Technology (No. YKJ201934), the Science and Technology Program of Guangzhou, China (No. 201803030038), and the National Key Research and Development Plan of China (No. 2019YFC0214302).
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FZ performed the whole experiment process of this study and was a major contributor in writing the manuscript. HHu provided understanding, proposal, and guiding direction for this study. JL analyzed and interpreted the patient data regarding the pore structure and pore size distribution. ML analyzed and interpreted the patient data regarding the N2 adsorption/desorption isotherms of different ACs. HHuang analyzed and interpreted the patient data regarding the TG-DTG curves of different SACs. KD analyzed and interpreted the patient data regarding the XPS curve of SACs. All authors read and approved the final manuscript.
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Zeng, F., Hu, H., Lu, J. et al. Performance and mechanism of hydrogen sulfide removal by sludge-based activated carbons prepared by recommended modification methods. Environ Sci Pollut Res 28, 31618–31629 (2021). https://doi.org/10.1007/s11356-021-12694-3
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DOI: https://doi.org/10.1007/s11356-021-12694-3