对炭化土壤(RCS)进行球磨处理以激发其环境催化组分,并将所得炭化土壤(RBCS)用于活化过一硫酸盐(PMS)氧化处理有机废水.结果表明,当RBCS投加量为2g/L,PMS投加量为1.5g/L时,苯胺(AN,100mg/L)的去除率达到99.9%.与RCS相比,球磨处理显著提高了材料的PMS活化性能.猝灭实验和EPR测试表明,RBCS/PMS体系中存在SO·-4、·OH、1O2和环境永久性自由基(EPFRs).电化学实验表明,RBCS/PMS体系中还存在电子转移机制.球磨使炭化土壤表面暴露了更多的金属氧化物和含氧官能团,激活PMS产生活性氧攻击AN,石墨化碳和EPFRs则通过加速直接电子转移降解AN.研究结果为RCS提供一个环境友好的增值转化策略与处理方法,预期具有较好的应用前景.
Abstract
Pyrolysis is an important process for efficient remediation of petroleum-contaminated soil (PCS), but how to reuse the obtained carbonized soil (RCS) has not received enough attention. In this study, RCS was treated by ball milling to activate its environmental catalytic components, and the obtained carbonized soil (RBCS) was used to activate peroxymonosulfate (PMS) oxidation to treat organic wastewater. The results showed that when the dosage of RBCS was 2g/L and the dosage of PMS was 1.5g/L, the removal rate of aniline (AN, 100mg/L) reached 99.9 %. Compared with RCS, ball milling treatment significantly improved the activation performance of RBCS for PMS oxidation. Quenching experiments and EPR tests showed that SO·-4、·OH、1O2 and environmental permanent free radicals (EPFRs) existed in the RBCS/PMS system. Electrochemical experiments show that there is also an electron transfer mechanism in the RBCS/PMS system. Ball milling exposes more metal oxides, amorphous carbon and oxygen-containing groups on the surface of carbonized soil. Metal oxides and oxygen-containing groups can activate PMS to produce reactive oxygen species to attack AN, while graphitized carbon and EPFRs may promote PMS oxidation by accelerating direct electron transfer to degrade AN. This study provides an environmentally friendly, value-added transformation strategy and treatment method for RCS, which is expected to have a good application prospect.
关键词
石油污染土壤 /
热解 /
球磨 /
过硫酸盐 /
活化
Key words
petroleum-contaminated soil /
pyrolysis /
ball milling /
peroxymonosulfate /
activation
{{custom_sec.title}}
{{custom_sec.title}}
{{custom_sec.content}}
参考文献
[1] Zhuo W, Yi W, Yang L, et al. Biochar-based materials as remediation strategy in petroleum hydrocarbon-contaminated soil and water: Performances, mechanisms, and environmental impact [J]. Journal of Environmental Sciences, 2024,138:350-372.
[2] Wang H, Lv Y, Bao J, et al. Petroleum-contaminated soil bioremediation and microbial community succession induced by application of co-pyrolysis biochar amendment: An investigation of performances and mechanisms [J]. Journal of Hazardous Materials, 2024,466.
[3] Lan J, Wen F, Ren Y, et al. An overview of bioelectrokinetic and bioelectrochemical remediation of petroleum-contaminated soils [J]. Environmental Science and Ecotechnology, 2023,16.
[4] Cagnetta G, Huang J, Yu G. Remediation of petroleum-contaminated soil and simultaneous recovery of oil by fast pyrolysis [J]. Environmental science & technology, 2018,52(9):5330-5338.
[5] Xiao Z, Guo S, Cheng F, et al. Effects of mineral species and petroleum components on thermal desorption behavior of petroleum-contaminated soil [J]. Chemosphere, 2022,307.
[6] Li D, Xu W, Mu Y, et al. Remediation of petroleum-contaminated soil and simultaneous recovery of oil by fast pyrolysis [J]. Environmental Science & Technology, 2018,52(9):5330-5338.
[7] Wang S, Cheng F, Shao Z, et al. Effects of thermal desorption on ecotoxicological characteristics of heavy petroleum-contaminated soil [J]. Science of The Total Environment, 2023,857.
[8] Wang M, Xie X, Wu C. Ball milling enhances pyrolytic remediation of petroleum-contaminated soil and reuse as adsorptive/catalytic materials for wastewater treatment [J]. Journal of Water Process Engineering, 2024,58.
[9] Li P, Liao Y, Wang M, et al. Resource utilization of petroleum- contaminated soil to prepare persulfate activator by ferrate pretreatment and pyrolysis [J]. Journal of Cleaner Production, 2022, 337.
[10] Qiu R, Zhang P, Zhang Z, et al. The interface mechanism of ball- milled natural pyrite activating persulfate to degrade monochlorobenzene in soil: Intrinsic synergism of S and Fe species [J]. Separation and Purification Technology, 2024,341.
[11] Zhao C, Meng L, Chu H, et al. Ultrafast degradation of emerging organic pollutants via activation of peroxymonosulfate over Fe3C/ Fe@N-C-x: Singlet oxygen evolution and electron-transfer mechanisms [J]. Applied Catalysis B: Environmental, 2023,321: 122034.
[12] Kuang C, Zeng G, Zhou Y, et al. Integrating anodic sulfate activation with cathodic H2O2production/activation to generate the sulfate and hydroxyl radicals for the degradation of emerging organic contaminants [J]. Water Research, 2023,229:119464.
[13] Zhang W, Yan L, Wang Q, et al. Ball milling boosted the activation of peroxymonosulfate by biochar for tetracycline removal [J]. Journal of Environmental Chemical Engineering, 2021,9(6):106870.
[14] Zhu H, Guo A, Wang S, et al. Efficient tetracycline degradation via peroxymonosulfate activation by magnetic Co/N co-doped biochar: Emphasizing the important role of biochar graphitization [J]. Chemical Engineering Journal, 2022,450:138428.
[15] Ma Y, Lu T, Tang J, et al. One-pot hydrothermal synthesis of magnetic N-doped sludge biochar for efficient removal of tetracycline from various environmental waters [J]. Separation and Purification Technology, 2022,297:121426.
[16] Feng X, Qiu B, Sun D. Enhanced naproxen adsorption by a novel β-cyclodextrin immobilized the three-dimensional macrostructure of reduced graphene oxide and multiwall carbon nanotubes [J]. Separation and Purification Technology, 2022,290:120837.
[17] Oh W D, Lua S K, Dong Z, et al. Performance of magnetic activated carbon composite as peroxymonosulfate activator and regenerable adsorbent via sulfate radical-mediated oxidation processes [J]. Journal of Hazardous Materials, 2015,284:1-9.
[18] Xu K, Lin Q, Fan X, et al. Enhanced degradation of sulfamethoxazole by activation of peroxodisulfate with red mud modified biochar: Synergistic effect between adsorption and nonradical activation [J]. Chemical Engineering Journal, 2023,460:141578.
[19] Zhu D, Kwon S, Pignatello J J. Adsorption of single-ring organic compounds to wood charcoals prepared under different thermochemical conditions [J]. Environmental Science & Technology, 2005,39(11):3990-3998.
[20] Yang S, Li L, Xiao T, et al. Role of surface chemistry in modified ACF (activated carbon fiber)-catalyzed peroxymonosulfate oxidation [J]. Applied Surface Science, 2016,383:142-150.
[21] Song S, Liu W, Wang M, et al. Beneficial utilization of ball-milled carbon sand to activate peroxymonosulfate oxidation: Quantitation of ROS using probe-based kinetic models and mechanism insights [J]. Journal of Environmental Management, 2024,370.
[22] Peng W, Dong Y, Fu Y, et al. Non-radical reactions in persulfate-based homogeneous degradation processes: A review [J]. Chemical Engineering Journal, 2021,421:127818.
[23] Cheng X, Guo H, Zhang Y, et al. Non-photochemical production of singlet oxygen via activation of persulfate by carbon nanotubes [J]. Water Research, 2017,113:80-88.
[24] Li H, Liu Y, Jiang F, et al. Persulfate adsorption and activation by carbon structure defects provided new insights into ofloxacin degradation by biochar [J]. Science of the Total Environment, 2022, 806:150968.
[25] Li N, Li R, Duan X, et al. Correlation of active sites to generated reactive species and degradation routes of organics in peroxymonosulfate activation by Co-loaded carbon [J]. Environmental Science & Technology, 2021,55(23):16163-16174.
基金
国家自然科学基金资助项目(41772240);教育部人文社科规划基金资助项目(23YJAZH144)
PDF(2280 KB)
京公网安备 11010802030352号 
