MnFe2O4-CR的制备及其活化PMS降解盐酸四环素
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广西大学化学化工学院 广西石化资源加工及过程强化技术重点实验室

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国家自然科学基金(31660183);广西石化资源加工及过程强化技术重点实验室主任基金(2022Z007);广西大学2022“大学生创新创业训练计划”自治区级创新训练一般项目(S202210593278)


Preparation of MnFe2O4-CR and activation of persulfate to degrade tetracycline hydrochloride
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Guangxi Key Laboratory of Petrochemical Resource Processing and Process Strengthening Technology,College of Chemistry and Chemical Engineering,Guangxi University

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    摘要:

    利用水热法将MnFe2O4负载在生物质气化炭渣(CR)得到负载型复合催化剂MnFe2O4-CR,通过SEM、XRD、XPS、BET和VSM等技术对复合催化剂进行表征,并将其用于活化过一硫酸盐(PMS)降解盐酸四环素(TC)。考察了不同反应体系、催化剂的不同复合比例、PMS用量、催化剂用量、温度、pH、阴离子(HCO3–、H2PO4–、Cl–、NO3–)和腐植酸(HA)对MnFe2O4-CR/PMS体系降解TC的影响,并探究了MnFe2O4-CR的稳定性和循环使用性,探讨了MnFe2O4-CR/PMS体系中TC可能的降解机理。结果表明,MnFe2O4与炭渣的质量比为1∶2时制备的MnFe2O4-CR催化效果良好,在30 ℃,30 mg MnFe2O4-CR催化40 mg PMS,在90 min内对100 mL质量浓度为50 mg/L自然pH的TC溶液中TC的降解率达到91.32%;MnFe2O4-CR可利用其磁性回收,经过5次循环利用,催化PMS降解TC的降解率仍能达到82.90%。表明MnFe2O4-CR具有良好的稳定性和重复使用性。自由基淬灭实验表明,MnFe2O4-CR/PMS体系中,SO4??、?OH 、1O2 和O2??是降解TC的主要活性氧物种,并提出了相应的催化降解机理。

    Abstract:

    The composite catalyst MnFe2O4-CR was prepared by hydrothermal method by loading MnFe2O4 on biomass gasification carbon residue (CR), characterized by SEM, XRD, XPS, BET and VSM, and utilized to activate permonosulfate (PMS) to degrade tetracycline hydrochloride (TC). The effects of different reaction systems, the mass ratio of MnFe2O4 to CR, dosage of PMS, dosage of catalyst, temperature, pH value, anion(HCO3–、H2PO4–、Cl–、NO3–) and humic acid (HA) on the degradation efficiency of TC in MnFe2O4-CR/PMS system were investigated. The stability and recyclability of MnFe2O4-CR were also investigated. The possible degradation mechanism of TC in MnFe2O4-CR/PMS system was investigated by free radical quencher experiments. The results showed that: When the mass ratio of MnFe2O4 to carbon residue is 1:2, the catalytic effect of MnFe2O4-CR is good. At 30 ℃, 30 mg MnFe2O4-CR catalyzes, 40 mg PMS, and the degradation efficiency of TC in TC solution with natural pH of 100 mL and 50 mg/L reaches 91.32% within 90 min. MnFe2O4-CR catalyst can be recovered by its magnetic properties. After 5 cycles, the degradation efficiency of TC degraded by PMS can still reach 82.90%, indicating that MnFe2O4-CR has good stability and reusability. Free radical quenching experiments show that SO4??, ?OH, 1O2 and O2?? are the main reactive oxygen species for TC degradation in MnFe2O4-CR/PMS system, and the corresponding catalytic degradation mechanism is proposed.

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陈丛瑾,黄丽斌,范辉,张强煦,廖金戈,陈紫霞. MnFe2O4-CR的制备及其活化PMS降解盐酸四环素[J].精细化工,2024,41(7):

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  • 收稿日期:2023-07-17
  • 最后修改日期:2023-09-13
  • 录用日期:2023-09-02
  • 在线发布日期: 2024-07-11
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