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        硫修飾的多孔Co3O4活化過一硫酸鹽降解亞甲基藍
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        重慶理工大學 化學化工學院

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        中圖分類號:

        X131.2

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        重慶市教委科學技術研究項目(KJQN202101102),重慶理工大學科研項目(2022CX034,2022CX071,gzlcx20223170)


        Porous Co3O4 Modified with Sulfur in Activating Peroxymonosulfate for Degradation of Methylene Blue
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        College of Chemistry and Chemical Engineering,Chongqing University of Technology

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          摘要:

          以Na2S2O3為硫源,采用改進的草酸鹽-熱解法制備出系列不同硫修飾量的Co3O4多孔催化劑材料(Sx@Co3O4,x=0.25、0.5、0.75、1,x代表硫的添加比例,以Co(NO3)2?6H2O的物質的量為基準計算得到)。以亞甲基藍(MB)為降解模型,對不同催化劑活化過一硫酸鹽(PMS)的性能進行對比研究??疾炝斯に噮担ù呋瘎┯昧?、PMS濃度、反應溫度、常見陰離子種類)在Sx@Co3O4-PMS體系下對MB降解率的影響,并對催化劑的循環穩定性進行了評價。結果表明,隨著硫引入量的增加,Co3O4的催化性能逐漸升高,S1@Co3O4樣品表現出最佳的催化性能。硫元素以SO42-的形式鍵合在Co3O4的表面,Co3O4催化活性的增強是SO42-在其表面修飾引起的比表面積增大、表面氧空位含量增多以及對HSO5-的極化增強三者綜合作用的結果。在最優化反應條件下(催化劑用量0.04 g/L、PMS濃度0.6 mmol/L、反應溫度25 ℃,反應時間25 min),S1@Co3O4-PMS高級氧化體系對 500 mL 10 mg/L MB溶液的降解率高達98.35%。S1@Co3O4可通過簡單的方式回收利用,在連續4次循環使用后其對MB的降解率仍可達68.57%。電子順磁共振譜(EPR)證實,MB在S1@Co3O4-PMS體系中的降解是自由基(?SO4-、?OH和?O2-)和非自由基(1O2)共同作用的結果。

          Abstract:

          Using Na2S2O3 as sulfur source, a series of sulfur-modified porous Co3O4 catalysts with different sulfur contents were prepared by an improved oxalate-pyrolysis method (Sx@Co3O4, x=0.25, 0.5, 0.75, 1, where x represented the added ratio of sulfur and was calculated by the amount of Co(NO3)2?6H2O). Their properties for activating peroxymonosulfate (PMS) to degrade methylene blue (MB) were compared and the catalyst with the best catalytic performance was screened out. On this basis, the influences of treatment parameters including catalyst dosage, PMS concentration, reaction temperature and common anion species on MB degradation ratios under Sx@Co3O4-PMS system were investigated. Besides, the cyclic stability of catalyst was evaluated. Results showed that the performance of Co3O4 was boosted with the increase of sulfur content in the range of this study, and S1@Co3O4 exhibited the best catalytic performance. Moreover, it was confirmed that sulfur element was uniformly bonded on the surface of Co3O4 in the form of SO42-. The modification of S increased the specific surface area, oxygen vacancy content of Co3O4 and enhanced the polarization effect for HSO5-, which was considered as a key reason for improving the catalytic activity of Co3O4. Under the optimal reaction conditions: catalyst dosage of 0.04 g/L, PMS concentration of 0.6 mmol/L, reaction temperature of 25 ℃, and reaction time of 25 min, a degradation rate of 98.35% for MB (500 mL 10 mg/L) could be reached in the S1@Co3O4-PMS advanced oxidation system. S1@Co3O4 was recycled in a simple way and the degradation ratio of MB could reach 68.57% after four consecutive cycles. Furthermore, electron paramagnetic resonance spectroscopy (EPR) confirmed that the degradation of MB in S1@Co3O4-PMS system was the result of co-action of free radicals (?SO4-, ?OH and ?O2-) and non-free radicals (1O2).

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        引用本文

        沈海麗,夏強,廖小剛,李綱,田甜,李紅梅.硫修飾的多孔Co3O4活化過一硫酸鹽降解亞甲基藍[J].精細化工,2023,40(6):

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        • 收稿日期:2022-10-06
        • 最后修改日期:2023-02-04
        • 錄用日期:2023-02-09
        • 在線發布日期: 2023-05-11
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