Performance and mechanism of hydrogen sulfide removal by sludge-based activated carbons prepared by recommended modification methods

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*.

This is a preview of subscription content, access via your institution.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Data availability

All data generated or analyzed during this study are included in this published article.

References

  1. 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

    CAS  Article  Google Scholar 

  2. 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

    CAS  Article  Google Scholar 

  3. 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

    CAS  Article  Google Scholar 

  4. 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

    CAS  Article  Google Scholar 

  5. 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

    CAS  Article  Google Scholar 

  6. 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

    CAS  Article  Google Scholar 

  7. 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

    CAS  Article  Google Scholar 

  8. 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

    CAS  Article  Google Scholar 

  9. 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)

  10. 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

    CAS  Article  Google Scholar 

  11. 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

    CAS  Article  Google Scholar 

  12. 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

    CAS  Article  Google Scholar 

  13. 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)

  14. Ge X-Y (2016) Microwave-assisted Modification of coal-based activated carbon and studies on PAHs adsorption properties. Dissertation. Shihezi University, Shihezi (in Chinese)

  15. 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

    CAS  Article  Google Scholar 

  16. 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

    CAS  Article  Google Scholar 

  17. 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

    CAS  Article  Google Scholar 

  18. 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

    CAS  Article  Google Scholar 

  19. 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

    CAS  Article  Google Scholar 

  20. 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

    CAS  Article  Google Scholar 

  21. 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

    Google Scholar 

  22. 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)

  23. 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

    CAS  Article  Google Scholar 

  24. 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

    CAS  Article  Google Scholar 

  25. 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

    CAS  Article  Google Scholar 

  26. 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

    CAS  Article  Google Scholar 

  27. 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)

  28. 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

    CAS  Article  Google Scholar 

  29. 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

    Article  Google Scholar 

  30. 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

    CAS  Article  Google Scholar 

  31. 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

    CAS  Article  Google Scholar 

  32. 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

    CAS  Article  Google Scholar 

  33. 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

    CAS  Article  Google Scholar 

  34. 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

    CAS  Article  Google Scholar 

  35. 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

    CAS  Article  Google Scholar 

  36. 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

    CAS  Article  Google Scholar 

  37. 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

    CAS  Article  Google Scholar 

  38. 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

    CAS  Article  Google Scholar 

  39. 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

    CAS  Article  Google Scholar 

  40. 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

    CAS  Article  Google Scholar 

  41. 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

    CAS  Article  Google Scholar 

  42. 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

    CAS  Article  Google Scholar 

  43. 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

    CAS  Article  Google Scholar 

  44. 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

    CAS  Article  Google Scholar 

  45. 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

    CAS  Article  Google Scholar 

  46. 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)

  47. 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

    CAS  Article  Google Scholar 

  48. 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

    CAS  Article  Google Scholar 

  49. 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

    CAS  Article  Google Scholar 

  50. 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

    CAS  Article  Google Scholar 

  51. 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

    CAS  Article  Google Scholar 

  52. 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

    CAS  Article  Google Scholar 

  53. 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

    Google Scholar 

  54. 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

    CAS  Article  Google Scholar 

  55. 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)

  56. 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

    Article  Google Scholar 

  57. 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

    CAS  Article  Google Scholar 

Download references

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).

Author information

Affiliations

Authors

Contributions

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.

Corresponding authors

Correspondence to Fan Zeng or Hui Hu.

Ethics declarations

Ethics approval and consent to participate

Not applicable

Consent for publication

Not applicable

Competing interests

The authors no competing interests.

Additional information

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Responsible Editor: Ta Yeong Wu

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

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 (2021). https://doi.org/10.1007/s11356-021-12694-3

Download citation

Keywords

  • Sewage sludge
  • Corn straw
  • Modification
  • Ferric nitrate
  • Dry desulfurization
  • Desulfurization mechanism