Abstract
In this study, an integrated two-stage system, including the in-situ catalytic microwave pyrolysis (ICMP) and subsequent catalytic wet oxidation (CWO) processes, was proposed to remove H2S released from microwave-induced pyrolysis of sewage sludge. The emission profile and H2S removal from the pyrolysis of raw sewage sludge (SS) and sewage sludge spiked with conditioner CaO (SS-CaO) were investigated. The results showed that CaO played a positive role on sulfur fixation during the pyrolysis process. It was found that SS-CaO (10 wt.%) contributed to about 35% of H2S removal at the first stage (ICMP process). Additionally, the CWO process was demonstrated to have promising potential for posttreatment of remaining H2S gas. At the Fe3+ concentration of 30 g/L, the maximum H2S removal efficiency of 94.8% was obtained for a single Fe3+/Cu2+ solution. Finally, at the pyrolysis temperature of 800 °C, 99.7% of H2S was eliminated by the integrated two-stage system meeting the discharge standard of China. Therefore, the integrated two-stage system of ICMP + CWO may provide a promising strategy to remove H2S dramatically for the biomass pyrolysis industry.
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References
Bagreev A, Bandosz TJ (2004) Efficient hydrogen sulfide adsorbents obtained by pyrolysis of sewage sludge derived fertilizer modified with spent mineral oil. Environ Sci Technol 38:345–351
Bahlake A, Farivar F, Dabir B (2016) New 3-dimensional CFD modeling of CO2 and H2S simultaneous stripping from water within PVDF hollow fiber membrane contactor. Heat Mass Transf 52:1295–1304
Bhargava SK, Tardio J, Prasad J, Föger K, Akolekar DB, Grocott SC (2006) Wet oxidation and catalytic wet oxidation. Ind Eng Chem Res 45:1221–1258
Dominguez A, Menendez J, Inguanzo M, Bernad P, Pis J (2003) Gas chromatographic–mass spectrometric study of the oil fractions produced by microwave-assisted pyrolysis of different sewage sludges. J Chromatogr A 1012:193–206
Domínguez A, Menéndez JA, Inguanzo M, Pis JJ (2005) Investigations into the characteristics of oils produced from microwave pyrolysis of sewage sludge. Fuel Process Technol 86:1007–1020
Dominguez A, Fernandez Y, Fidalgo B, Pis JJ, Menendez JA (2008) Bio-syngas production with low concentrations of CO2 and CH4 from microwave-induced pyrolysis of wet and dried sewage sludge. Chemosphere 70:397–403
Feng Y, Hu T, Wu M, Shangguan J, Fan H, Mi J (2016) Effect of microwave irradiation on the preparation of iron oxide/arenaceous clay sorbent for hot coal gas desulfurization. Fuel Process Technol 148:35–42
Hachimi A, Vilcocq L, Courson C, Kiennemann A (2014) Study of olivine supported copper sorbents performances in the desulfurization process in link with biomass gasification. Fuel Process Technol 118:254–263
Jung K-D, Joo O-S, Cho S-H, Han S-H (2003) Catalytic wet oxidation of H2S to sulfur on Fe/MgO catalyst. Appl Catal A Gen 240:235–241
Lee Y-S, Kim H-T, Yoo K-O (1995) Effect of ferric oxide on the high-temperature removal of hydrogen sulfide over ZnO-Fe2O3 mixed metal oxide sorbent. Ind Eng Chem Res 34:1181–1188
Lee E, Jung K, Joo O, Shul Y (2004) Catalytic wet oxidation of H2S to sulfur on V/MgO catalyst. Catal Lett 98:259–263
Lee E-K, Jung K-D, Shul Y-G (2007) Catalytic systems for the H2S wet oxidation at room temperature. Catal Surv Jpn 11:134–144
Liu H et al (2014) Dual role of conditioner CaO in product distributions and sulfur transformation during sewage sludge pyrolysis. Fuel 134:514–520
Liu H, Zhang Q, Xing H, Hu H, Li A, Yao H (2015a) Product distribution and sulfur behavior in sewage sludge pyrolysis: synergistic effect of Fenton peroxidation and CaO conditioning. Fuel 159:68–75
Liu S, Wei M, Qiao Y, Yang Z, Gui B, Yu Y, Xu M (2015b) Release of organic sulfur as sulfur-containing gases during low temperature pyrolysis of sewage sludge. Proc Combust Inst 35:2767–2775
Louhichi S, Ghorbel A, Chekir H, Trabelsi N, Khemakhem S (2016) Properties of modified crude clay by iron and copper nanoparticles as potential hydrogen sulfide adsorption. Appl Clay Sci 127–128:123–128
Lu S, Chen L, Huang Q, Yang L, Du C, Li X, Yan J (2014) Decomposition of ammonia and hydrogen sulfide in simulated sludge drying waste gas by a novel non-thermal plasma. Chemosphere 117:781–785
Luque R, Menéndez JA, Arenillas A, Cot J (2012) Microwave-assisted pyrolysis of biomass feedstocks: the way forward? Energy Environ Sci 5:5481–5488
Ma Y, Chen Z, Gong H (2016) Study on selective hydrogen sulfide removal over carbon dioxide by catalytic oxidative absorption method with chelated iron as the catalyst. Renew Energy 96, part B:1119–1126
Marques RRN et al (2011) Sewage sludge based catalysts for catalytic wet air oxidation of phenol: preparation, characterisation and catalytic performance. Appl Catal B Environ 101:306–316
Menéndez JA, Domínguez A, Inguanzo M, Pis JJ (2004) Microwave pyrolysis of sewage sludge: analysis of the gas fraction. J Anal Appl Pyrolysis 71:657–667
Ros A, Montes-Moran MA, Fuente E, Nevskaia DM, Martin JM (2006) Dried sludges and sludge-based chars for H2S removal at low temperature: influence of sewage sludge characteristics. Environ Sci Technol 40:302–309
Ros A, Lillo-Rodenas MA, Canals-Batlle C, Fuente E, Montes-Moran MA, Martin MJ, Linares-Solano A (2007) A new generation of sludge-based adsorbents for H2S abatement at room temperature. Environ Sci Technol 41:4375–4381
Santos A, Yustos P, Cordero T, Gomis S, Rodríguez S, García-Ochoa F (2005) Catalytic wet oxidation of phenol on active carbon: stability, phenol conversion and mineralization. Catal Today 102–103:213–218
Shibaoka M, Ohtsuka Y, Wornat MJ, Thomas CG, Bennett AJR (1995) Application of microscopy to the investigation of brown coal pyrolysis. Fuel 74:1648–1653
Tian Y, Zuo W, Chen D (2011a) Crystallization evolution, microstructure and properties of sewage sludge-based glass-ceramics prepared by microwave heating. J Hazard Mater 196:370–379
Tian Y, Zuo W, Ren Z, Chen D (2011b) Estimation of a novel method to produce bio-oil from sewage sludge by microwave pyrolysis with the consideration of efficiency and safety. Bioresour Technol 102:2053–2061
Tian Y, Zhang J, Zuo W, Chen L, Cui Y, Tan T (2013) Nitrogen conversion in relation to NH3 and HCN during microwave pyrolysis of sewage sludge. Environ Sci Technol 47:3498–3505
Zhang J, Tong Z (2006) Study on catalytic wet oxidation of H2S into sulfur on Fe/Cu catalyst. J Nat Gas Chem 15:63–69
Zhang J, Tian Y, Cui Y, Zuo W, Tan T (2013) Key intermediates in nitrogen transformation during microwave pyrolysis of sewage sludge: a protein model compound study. Bioresour Technol 132:57–63
Zhang J, Tian Y, Zhu J, Zuo W, Yin L (2014) Characterization of nitrogen transformation during microwave-induced pyrolysis of sewage sludge. J Anal Appl Pyrolysis 105:335–341
Zhang J, Zuo W, Tian Y, Chen L, Yin L, Zhang J (2017) Sulfur transformation during microwave and conventional pyrolysis of sewage sludge. Environ Sci Technol 51:709–717
Acknowledgements
This study was supported by the Program of International S&T Cooperation (2016YFE0123400) and HIT Environment and Ecology Innovation Special Funds (HSCJ201609). The authors also appreciate the Open Project of State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology (QA201609-02), the Heilongjiang Postdoctoral Science Foundation (LBH-Z14093) and the Fundamental Research Funds for the Central Universities (HIT. NSRIF. 2015096).
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Zhang, J., Tian, Y., Yin, L. et al. Investigation on the removal of H2S from microwave pyrolysis of sewage sludge by an integrated two-stage system. Environ Sci Pollut Res 24, 19920–19926 (2017). https://doi.org/10.1007/s11356-017-9637-6
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DOI: https://doi.org/10.1007/s11356-017-9637-6