| 微生物还原改性生物炭介导水中活性氧生成及其对四环素的去除 |
| 摘要点击 1170 全文点击 8 投稿时间：2025-07-20 修订日期：2025-10-31 |
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| 中文关键词 微生物 改性生物炭 介导活性氧（ROS） 电子交换容量（EEC） 四环素 |
| 英文关键词 microorganisms modified biochar reactive oxygen species （ROS） electron exchange capacity（EEC） tetracycline |
| DOI 10.13227/j.hjkx.202507260 |
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| 中文摘要 |
| 随着生物炭（BC）在环境治理领域中的应用，生物炭介导活性氧（ROS）生成及其对污染物去除的作用已成为研究热点. 以水稻秸秆生物炭为对象，选取希瓦氏菌为水土介质中微生物的代表，研究微生物厌氧条件下对生物炭的还原改性作用，探讨微生物还原改性生物炭（RBC）介导水中ROS（·OH、H2O2和O2-·）的生成能力及其对四环素的去除作用和机制. 结果表明：①微生物还原改性使得生物炭的理化性质发生显著改变. 相比于原始BC，RBC的亲水性和极性增加，芳香化程度降低，表面形貌粗糙性增加，比表面积增大了54%~63%，含氧官能团数量和碳缺陷程度显著增加，得电子容量增加了79%~92%，持久性自由基含量增加了20%~425%. ②微生物还原改性使得生物炭介导ROS生成能力显著提升. 相较于原始BC， 500℃和700℃制备的生物炭被微生物还原改性后， 其介导产生·OH和H2O2的浓度分别提高了87%~95%和68%~126%，c（O2-·）从不可检出增加到1.47~5.25 μmol·L-1. RBC增强ROS介导能力与其增加的持久性自由基、含氧官能团、晶格碳缺陷和得电子容量密切关联. ③相比原始BC， RBC对四环素的去除效率提高了139%~157%， 其中对四环素吸附量增加了35%~161%，降解量增加了154%~495%，RBC对四环素的去除以降解作用为主. ④生物炭对四环素的去除能力与其介导的3种典型ROS的生成量均呈显著正相关关系（P<0.05），3种ROS均可能参与了四环素的降解. 生物炭悬浮液中，四环素的降解路径包括脱羟基、脱氮甲基、脱酰胺、开环裂解、脱氨和脱水等反应. |
| 英文摘要 |
| With the growing application of biochar （BC） in environmental remediation， the role of BC in mediating reactive oxygen species （ROS） generation in the environment and its subsequent impact on pollutant degradation has become a research focus. Accordingly， this study selected rice straw-derived BC as the target material and Shewanella oneidensis MR-1 as representative microorganisms in aqueous-terrestrial media to investigate the reductive modification of BC by microorganisms under anaerobic conditions， while further exploring the capacity of microbial reduced biochar （RBC） to mediate the generation of ROS （·OH， H2O2， and O2-·） in aqueous environments and the corresponding performance and mechanism for tetracycline （TC） removal. The main results are as follows： ① Microbial reductive modification induced significant changes in the physicochemical properties of BC. Compared to the original BC， RBC exhibited higher hydrophilicity and polarity， lower aromatization， higher surface roughness， a 54%-63% increase in specific surface area， notable enhancements in the number of oxygen-containing functional groups （OFGs） and the degree of carbon defects， a 79%-92% rise in electron-accepting capacity， and a 20%-425% increase in the content of persistent free radicals （PFRs）. ② Microbial reductive modification also remarkably improved the capacity of BC to mediate ROS generation. As for BC prepared at 500℃ and 700℃， microbial reduction led to an 87%-95% increase in ·OH concentration and a 68%-126% increase in H2O2 concentration mediated by RBC （relative to the original BC）， with O2-· concentration notably rising from undetectable levels by the original BC to 1.47-5.25 μmol·L-1 by RBC， and this enhanced ROS-mediating capacity of RBC was closely associated with its increased PFRs， OFGs content， lattice carbon defects， and electron-accepting capacity. ③ In terms of TC removal， RBC outperformed the original BC by 139%-157% in removal efficiency， with its TC adsorption capacity increasing by 35%-161% and TC degradation capacity by 154%-495%. The total removal of TC by RBC was mainly through degradation. ④ A significant positive correlation （P<0.05） was observed between TC removal capacity of BC and the generation amounts of the three typical ROS it mediated， which indicated that all ROS may be involved in the degradation of TC in BC suspensions. TC was gradually degraded through reactions such as dehydroxylation， demethylation， deamidation， ring opening cracking， deamination， and dehydration in biochar suspensions. |
