生物质炭负载硫化纳米零价铁活化过硫酸盐降解土壤中典型恶臭苯系物的规律与机制
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土壤与农业可持续发展国家重点实验室(南京土壤研究所)

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国家重点研发计划项目(2020YFC1808601)资助


Mechanism of Degradation of Typical Malodorous Benzene Congeners in Soil by Activated Persulfate with Sulfidized Nano-zero-valent Iron Loaded on Biochar
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Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences

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Supported by the National Key Research and Development Program of China(No. 2020YFC1808601)

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    摘要:

    纳米零价铁(nZVI)以及硫化纳米零价铁(S-nZVI)活化过硫酸盐(PS)降解土壤中的有机污染物是目前场地原位氧化修复技术的研究热点之一。苯系物(BTEX)是石化污染场地中典型的恶臭污染物,实现BTEX的高效去除并探究其降解机理有着重要的环境意义。本研究建立了以生物质炭负载硫化纳米零价铁(S-nZVI@BC)为活化剂的过硫酸盐氧化体系,探究不同条件下BTEX的降解效果,并与其他材料催化PS降解体系的效果进行了比较。同时基于化学探针实验、电子顺磁共振实验(EPR)及吹扫捕集-气质联用法(PT-GC-MS)测定的转化产物推测BTEX可能的降解途径。结果表明,S-nZVI@BC/PS体系在pH=3、S/Fe=1/4、Fe/C=1/2、材料投加量为0.01 g•g-1、PS浓度为30 mmol•L-1时对土壤中BTEX均有着95%以上的降解效果;S-nZVI@BC/PS 体系下苯、甲苯、乙苯、邻二甲苯的降解率在2 h内分别可达到96.7%、98.5%、96.9%、98.4%;S-nZVI@BC催化体系在所研究的五种不同催化剂体系表现最佳,即催化效果表现为:PS

    Abstract:

    【Objective】The degradation of organic pollutants in soil by activated persulfate (PS) with nanoscale zero-valent iron (nZVI) or sulfidized nanoscale zero-valent iron (S-nZVI) is currently one of the research hotspots in in-situ chemical oxidation remediation technologies. Benzene, toluene, ethylbenzene, and xylene (BTEX) are typical odorous pollutants in petrochemical-contaminated sites. Thus, the discovery of remediation technologies aimed to achieve efficient removal of BTEX and the elucidation of the degradation mechanism is of great environmental significance.【Method】The study established a persulfate oxidation system using biochar-supported sulfidized nano zero-valent iron (S-nZVI@BC) as the activator, explored the degradation of BTEX under different conditions, and compared its effectiveness with other materials for PS degradation. Moreover, based on chemical probe experiments, electron paramagnetic resonance (EPR) experiments, and purge-and-trap-gas chromatography-mass spectrometry (PT-GC-MS), the degradation pathways of BTEX were indicated.【Result】The results showed that S-nZVI@BC/PS system had the best degradation efficiency on BTEX in the soil at pH = 3, S/Fe = 1/4, Fe/C = 1/2, S-nZVI@BC dosage of 0.01g•g-1soil, and PS concentration of 30 mmol•L-1. The degradation rates of benzene, toluene, ethylbenzene, and ortho-xylene in the S-nZVI@BC/PS system reached 96.7%, 98.5%, 96.9%, and 98.4% within 2 h, respectively. The S-nZVI@BC catalytic system showed the best performance among the five different catalytic systems studied in the order of PS < nZVI/PS < nZVI@BC/PS < S-nZVI/PS < S-nZVI@BC/PS. Also, S-nZVI@BC maintained good reaction activity in a wide range of pH 2-9. There were three active free radicals in the system: SO4˙-, HO˙, and O2˙-, among which SO4˙- was confirmed as the main active substance in the reaction process. Based on main free radicals and intermediates, it is indicated that BTEX may have two degradation pathways: Free radical addition and free radical hydrogen extraction reaction.【Conclusion】Sulfur modification and biochar loading effectively improved the stability of nZVI catalytic performance, and S-nZVI@BC/PS can efficiently degrade BTEX. This study provides theoretical support for the establishment of efficient degradation technology for odorous pollutants in soils.

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李炎璐,杨兴伦,卞永荣,马智勇,谷成刚,宋洋,相雷雷,王芳,蒋新.生物质炭负载硫化纳米零价铁活化过硫酸盐降解土壤中典型恶臭苯系物的规律与机制[J].土壤学报,DOI:10.11766/trxb202310240433,[待发表]
LI Yanlu, YANG Xinglun, BIAN Yongrong, MA Zhiyong, GU Chenggang, SONG Yang, XIANG Leilei, WANG Fang, JIANG Xin. Mechanism of Degradation of Typical Malodorous Benzene Congeners in Soil by Activated Persulfate with Sulfidized Nano-zero-valent Iron Loaded on Biochar[J]. Acta Pedologica Sinica, DOI:10.11766/trxb202310240433,[In Press]

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  • 收稿日期:2023-10-24
  • 最后修改日期:2023-11-29
  • 录用日期:2024-01-05
  • 在线发布日期: 2024-01-15
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