水热法制备铁炭复合材料及其对地下水中三氯乙烯的降解性能
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国家自然科学基金项目(21876022);国家重大研发计划(2019YFC1803803)


Prepared of iron-carbon composites by hydrothermal method and degradation performance of trichloroethylene in groundwater
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    摘要:

    以蔗糖和无水三氯化铁为原料,以氨水调节溶液pH,采用水热-炭化法在不同pH下合成了系列铁炭复合材料(Fe/C pH2、Fe/C pH4、Fe/C pH6、Fe/C pH8、Fe/C pH10)。进一步将Fe/C pH10球磨为粒径分布在100~1000nm的铁碳复合材料(Fe/C pH10-Q)。考察了各个产物对三氯乙烯的吸附和降解性能。采用SEM、XRD、TG、N2吸附-脱附对不同pH下制备的产物形态和组成进行了表征。采用气相色谱(GC)和离子色谱(IC)对污染物三氯乙烯和降解产物乙烷、乙烯、氯离子进行了定量检测。结果表明,复合材料中纳米零价铁(nZVI)和生物炭共同存在,nZVI被随机分散在碳球或碳颗粒上,不发生团聚现象。随着反应液pH的增加,产物中nZVI的含量和粒径从Fe/C pH2的6.52%、20 nm增加到Fe/C pH10的36.35%、60 nm,比表面积由Fe/C pH2的369 m2/g 减小到Fe/C pH10的302 m2/g。不同pH下制得Fe/C复合材料对TCE降解速率大小顺序为:Fe/C pH10>Fe/C pH8>Fe/C pH6>Fe/C pH4>Fe/C pH2。48h的反应时间下, Fe/C pH10对TCE的去除率可接近100%。球磨不会改变Fe/C复合材料中nZVI粒径、含量和材料的反应活性。通过石英砂柱评价了Fe/C pH10-Q的传输性能,其具有良好的地下传输性能。与市售nZVI和Fe/C pH10相比,其流动性显著提高。

    Abstract:

    Iron-carbon composites(Fe/C pH2、Fe/C pH4、Fe/C pH6、Fe/C pH8、Fe/C pH10) were synthesized by hydrothermal-carbonization method using sucrose and anhydrous ferric chloride as raw materials and adjusting the pH of solution with ammonia. Fe/C pH10 was further prepared iorn-carbon composite material(Fe/C pH10-Q) with a particle size in the range of 100~1000 nm by ball milling method. The adsorption and degradation properties of product for trichloroethylene (TCE) were investigated. The morphology and composition of the products prepared at different pH were characterized by SEM, XRD, TG, N2 adsorption-desorption. Gas chromatography (GC) and ion chromatography (IC) were used for quantitative determination of TCE and degradation products (ethane, ethylene and chloride ions). The results showed that nano-zero-valent iron (nZVI) co-existed with biochar in iron-carbon composites, nZVI was randomly dispersed over carbon spheres or particles, agglomeration don’t occurred. The content and particle size of nZVI in the product increased to 36.35%、60 nm of Fe/C pH10 from 6.52%、20 nm of Fe/C pH2 as solution pH increased. The specific surface area of the product decreased to 302 m2/g of Fe/C pH10 from 369 m2/g of Fe/C pH2. The degradation rate of TCE by Fe/C composites was in the order of Fe/C pH10>Fe/C pH8>Fe/C pH6>Fe/C pH4>Fe/C pH2. The removal rate of TCE was closed to 100% by Fe/C pH10 when reaction time was 48 h. The particle size, content and reactivity of nZVI in Fe/C composites were not changed by ball milling. The transport performance of Fe/C pH10-Q was evaluated by quartz sand column, results showed that Fe/C pH10-Q had satisfactorilly underground transmission performance. Liquidity of Fe/C pH10-Q significantly increased by compared with commercial nZVI and Fe/C pH10

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占敬敬.水热法制备铁炭复合材料及其对地下水中三氯乙烯的降解性能[J].精细化工,2022,39(4):

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  • 收稿日期:2021-12-01
  • 最后修改日期:2021-12-24
  • 录用日期:2021-12-24
  • 在线发布日期: 2022-01-29
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