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污水污泥水热炭活化过一硫酸盐对水热废水的降解特性和机理研究
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Abstract:
水热炭化被认为是处理污水污泥的有效方法。然而，水热废水已成为制约该方法可持续发展的瓶颈。强氧化剂过一硫酸盐(PMS)很容易通过光、电、过渡金属和碳材料等方式被激活，产生SO4？？自由基，有效处理废水中有机污染物。因此，通过水热炭化的方式制备了污泥水热炭，探究了污泥水热炭激活PMS降解水热废水的可行性，考察了水热炭化温度、水热废水初始pH和降解时间对水热废水中可溶性化学需氧量(SCOD)降解效率的影响。结果表明，HC200活化PMS降解PW160效果最好。降解时间为15分钟时，最大SCOD降解效率达到了38.1%。但水热废水初始pH对SCOD降解影响不明显。HC200可以在相对较宽的pH范围(3~9)内有效降解SCOD。水热炭脱灰实验结果表明，水热炭中铁元素会影响PMS激活。脱灰水热炭降解前后XPS分析表明，C = O官能团是活化PMS的主要官能团。因此，水热炭通过两个途径激活PMS：(1) HC200含氧官能团(C = O)活化PMS；(2) HC200中铁元素激活PMS，从而促进SCOD降解。
Hydrothermal carbonization (HTC) is considered as an effective method for sewage sludge (SS) treatment. However, process water (PW) has become a bottleneck for the sustainable development of HTC. Peroxymonosulfate (PMS) was readily activated by light, electricity, transition metals, carbon nanotubes and so on, to produce SO4？？ free radicals for the effective degradation of organic pollutants in wastewater. Therefore, sewage sludge-derived hydro char was prepared in this study to activate PMS for the degradation of PW. Effects of HTC temperature, initial pH of PW and degradation time on the degradation efficiency of soluble chemical oxygen demand (SCOD) in PW were investigated. Results showed that HC200 could activate PMS and had the best degradation effect on PW160. The maximum degradation efficiency of 38.1% was achieved at 15th minute. The pH of initial PW has little effect on SCOD degradation, and HC200 is suitable for SCOD degradation in a relatively wide pH range (3~9). Hydrochar deashing experiment showed that iron in hydrochar could activate PMS. XPS analysis of deashed hydrochar before and after degradation indicated that C = O functional group was the main functional group in activating PMS. Therefore, hydrochar activate PMS by two ways to promote the degradation of SCOD: (1) oxygen-containing functional group (C = O) in HC200; (2) iron in HC200.
| [1] | Li, K., Zhang, D., Niu, X., et al. (2022) Insights into CO2 Adsorption on KOH-Activated Biochars Derived from the Mixed Sewage Sludge and Pine Sawdust. Science of the Total Environment, 826, Article ID: 154133. https://doi.org/10.1016/j.scitotenv.2022.154133 |
| [2] | Syed-Hassan, S.S.A., Wang, Y., Hu, S., et al. (2017) Thermochemical Processing of Sewage Sludge to Energy and Fuel: Fundamentals, Challenges and Considerations. Renewable and Sustainable Energy Reviews, 80, 888-913. https://doi.org/10.1016/j.rser.2017.05.262 |
| [3] | Liu, H., Zhang, Q., Hu, H., et al. (2014) Influence of Residual Moisture on Deep Dewatered Sludge Pyrolysis. International Journal of Hydrogen Energy, 39, 1253-1261. https://doi.org/10.1016/j.ijhydene.2013.10.050 |
| [4] | Ponnusamy, V.K., Nagappan, S., Bhosale, R.R., et al. (2020) Review on Sustainable Production of Biochar through Hydrothermal Liquefaction: Physico-Chemical Properties and Applications. Bioresource Technology, 310, Article ID: 123414. https://doi.org/10.1016/j.biortech.2020.123414 |
| [5] | Wang, Z., Zhai, Y., Wang, T., et al. (2020) Effect of Temperature on the Sulfur Fate during Hydrothermal Carbonization of Sewage Sludge. Environmental Pollution, 260, Article ID: 114067. https://doi.org/10.1016/j.envpol.2020.114067 |
| [6] | Liu, H., Basar, I.A., Nzihou, A., et al. (2021) Hydrochar Derived from Municipal Sludge through Hydrothermal Processing: A Critical Review on Its Formation, Characterization, and Valorization. Water Research, 199, Article ID: 117186. https://doi.org/10.1016/j.watres.2021.117186 |
| [7] | Xu, Z.-X., Song, H., Li, P.-J., et al. (2020) Hydrothermal Carbonization of Sewage Sludge: Effect of Aqueous Phase Recycling. Chemical Engineering Journal, 387, Article ID: 123410. https://doi.org/10.1016/j.cej.2019.123410 |
| [8] | Usman, M., Ren, S., Ji, M., et al. (2020) Characterization and Biogas Production Potentials of Aqueous Phase Produced from Hydrothermal Carbonization of Biomass—Major Components and Their Binary Mixtures. Chemical Engineering Journal, 388, Article ID: 124201. https://doi.org/10.1016/j.cej.2020.124201 |
| [9] | Aragón-Brice？o, C., Ross, A.B. and Camargo-Valero, M.A. (2017) Evaluation and Comparison of Product Yields and Bio-Methane Potential in Sewage Digestate Following Hydrothermal Treatment. Applied Energy, 208, 1357-1369. https://doi.org/10.1016/j.apenergy.2017.09.019 |
| [10] | Nghiem, L.D., Sch？fer, A.I. and Elimelech, M. (2005) Pharmaceutical Retention Mechanisms by Nanofiltration Membranes. Environmental Science & Technology, 39, 7698-7705. https://doi.org/10.1021/es0507665 |
| [11] | Liu, L., Zhai, Y., Liu, X., et al. (2022) Features and Mechanisms of Sewage Sludge Hydrothermal Carbonization Aqueous Phase after Ferrous/Persulfate-Based Process: The Selective Effect of Oxidation and Coagulation. Journal of Cleaner Production, 366, Article ID: 132831. https://doi.org/10.1016/j.jclepro.2022.132831 |
| [12] | Gong, M., Feng, A., Wang, L., et al. (2022) Coupling of Hydrothermal Pretreatment and Supercritical Water Gasification of Sewage Sludge for Hydrogen Production. International Journal of Hydrogen Energy, 47, 17914-17925. https://doi.org/10.1016/j.ijhydene.2022.03.283 |
| [13] | Wang, R., Jin, Q., Ye, X., et al. (2020) Effect of Process Wastewater Recycling on the Chemical Evolution and Formation Mechanism of Hydrochar from Herbaceous Biomass during Hydrothermal Carbonization. Journal of Cleaner Production, 277, Article ID: 123281. https://doi.org/10.1016/j.jclepro.2020.123281 |
| [14] | Bagal, M.V. and Gogate, P.R. (2014) Wastewater Treatment Using Hybrid Treatment Schemes Based on Cavitation and Fenton Chemistry: A Review. Ultrasonics Sonochemistry, 21, 1-14. https://doi.org/10.1016/j.ultsonch.2013.07.009 |
| [15] | Mahdi Ahmed, M., Barbati, S., Doumenq, P., et al. (2012) Sulfate Radical Anion Oxidation of Diclofenac and Sulfamethoxazole for Water Decontamination. Chemical Engineering Journal, 197, 440-447. https://doi.org/10.1016/j.cej.2012.05.040 |
| [16] | Amor, C., Rodríguez-Chueca, J., Fernandes, J.L., et al. (2019) Winery Wastewater Treatment by Sulphate Radical Based-Advanced Oxidation Processes (SR-AOP): Thermally vs UV-Assisted Persulphate Activation. Process Safety and Environmental Protection, 122, 94-101. https://doi.org/10.1016/j.psep.2018.11.016 |
| [17] | Zhang, W., Li, X., Yang, Q., et al. (2019) Pretreatment of Landfill Leachate in Near-Neutral pH Condition by Persulfate Activated Fe-C Micro-Electrolysis System. Chemosphere, 216, 749-756. https://doi.org/10.1016/j.chemosphere.2018.10.168 |
| [18] | Luo, H., Zeng, Y., He, D., et al. (2021) Application of Iron-Based Materials in Heterogeneous Advanced Oxidation Processes for Wastewater Treatment: A Review. Chemical Engineering Journal, 407, Article ID: 127191. https://doi.org/10.1016/j.cej.2020.127191 |
| [19] | Wang, Y., Ao, Z., Sun, H., et al. (2016) Activation of Peroxymonosulfate by Carbonaceous Oxygen Groups: Experimental and Density Functional Theory Calculations. Applied Catalysis B: Environmental, 198, 295-302. https://doi.org/10.1016/j.apcatb.2016.05.075 |
| [20] | Zhu, S., Wang, W., Xu, Y., et al. (2019) Iron Sludge-Derived Magnetic Fe0/Fe3C Catalyst for Oxidation of Ciprofloxacin via Peroxymonosulfate Activation. Chemical Engineering Journal, 365, 99-110. https://doi.org/10.1016/j.cej.2019.02.011 |
| [21] | Hu, W., Tong, W., Li, Y., et al. (2020) Hydrothermal Route-Enabled Synthesis of Sludge-Derived Carbon with Oxygen Functional Groups for Bisphenol A Degradation through Activation of Peroxymonosulfate. Journal of Hazardous Materials, 388, Article ID: 121801. https://doi.org/10.1016/j.jhazmat.2019.121801 |
| [22] | Mian, M.M., Alam, N., Ahommed, M.S., et al. (2022) Emerging Applications of Sludge Biochar-Based Catalysts for Environmental Remediation and Energy Storage: A Review. Journal of Cleaner Production, 360, Article ID: 132131. https://doi.org/10.1016/j.jclepro.2022.132131 |
| [23] | Huang, B.-C., Jiang, J., Huang, G.-X., et al. (2018) Sludge Biochar-Based Catalysts for Improved Pollutant Degradation by Activating Peroxymonosulfate. Journal of Materials Chemistry A, 6, 8978-8985. https://doi.org/10.1039/C8TA02282H |
| [24] | Zheng, X., Shen, M., Ying, Z., et al. (2022) Correlating Phosphorus Transformation with Process Water during Hydrothermal Carbonization of Sewage Sludge via Experimental Study and Mathematical Modelling. Science of the Total Environment, 807, Article ID: 150750. https://doi.org/10.1016/j.scitotenv.2021.150750 |
| [25] | Zhang, J., Zhao, X., Wang, Y., et al. (2018) Peroxymonosulfate-Enhanced Visible Light Photocatalytic Degradation of Bisphenol A by Perylene Imide-Modified g-C3N4. Applied Catalysis B: Environmental, 237, 976-985. https://doi.org/10.1016/j.apcatb.2018.06.049 |
| [26] | Donoso-Bravo, A., Pérez-Elvira, S., Aymerich, E., et al. (2011) Assessment of the Influence of Thermal Pre-Treatment Time on the Macromolecular Composition and Anaerobic Biodegradability of Sewage Sludge. Bioresource Technology, 102, 660-666. https://doi.org/10.1016/j.biortech.2010.08.035 |
| [27] | Wang, R., Wang, C., Zhao, Z., et al. (2019) Energy Recovery from High-Ash Municipal Sewage Sludge by Hydrothermal Carbonization: Fuel Characteristics of Biosolid Products. Energy, 186, Article ID: 115848. https://doi.org/10.1016/j.energy.2019.07.178 |
| [28] | Zhuang, X., Huang, Y., Song, Y., et al. (2017) The Transformation Pathways of Nitrogen in Sewage Sludge during Hydrothermal Treatment. Bioresource Technology, 245, 463-470. https://doi.org/10.1016/j.biortech.2017.08.195 |
| [29] | Chen, P., Yang, R., Pei, Y., et al. (2022) Hydrothermal Synthesis of Similar Mineral-Sourced Humic Acid from Food Waste and the Role of Protein. Science of the Total Environment, 828, Article ID: ID: 154440. https://doi.org/10.1016/j.scitotenv.2022.154440 |
| [30] | Yang, F., Zhang, S., Cheng, K., et al. (2019) A Hydrothermal Process to Turn Waste Biomass into Artificial Fulvic and Humic Acids for Soil Remediation. Science of the Total Environment, 686, 1140-1151. https://doi.org/10.1016/j.scitotenv.2019.06.045 |
| [31] | Zang, T., Wang, H., Liu, Y., et al. (2020) Fe-Doped Biochar Derived from Waste Sludge for Degradation of Rhodamine B via Enhancing Activation of Peroxymonosulfate. Chemosphere, 261, Article ID: 127616. https://doi.org/10.1016/j.chemosphere.2020.127616 |
| [32] | Jiang, S.-F., Ling, L.-L., Chen, W.-J., et al. (2019) High Efficient Removal of Bisphenol A in a Peroxymonosulfate/Iron Functionalized Biochar System: Mechanistic Elucidation and Quantification of the Contributors. Chemical Engineering Journal, 359, 572-583. https://doi.org/10.1016/j.cej.2018.11.124 |
