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过程工程学报 ›› 2021, Vol. 21 ›› Issue (2): 193-201.DOI: 10.12034/j.issn.1009-606X.220066

• 材料工程 • 上一篇    下一篇

甲基橙在Fe0-NaA-SSFSF固定床上的催化湿式H2O2氧化

刘 剑， 黄依倪， 陈 熙， 易正戟*   

  1. 衡阳师范学院化学与材料科学学院，功能金属有机材料湖南省普通高等学校重点实验室，功能金属有机化合物湖南省重点实验室，湖南 衡阳 421008
  • 收稿日期:2020-03-01 修回日期:2020-04-26 出版日期:2021-02-22 发布日期:2021-03-01
  • 通讯作者: 易正戟 yizhengji2004@126.com
  • 基金资助:
    国家自然科学基金资助项目;湖南省教育厅科研项目;湖南省自然科学基金项目;衡阳市科技计划项目

Catalytic wet peroxide oxidation of methyl orange in a fixed bed with Fe0-NaA-SSFSF

Jian LIU, Yini HUANG, Xi CHEN, Zhengji YI*   

  1. Key Laboratory of Functional Organometallic Materials, University of Hunan Province, Key Laboratory of Functional Metal-Organic Compounds of Hunan Province, College of Chemistry and Material Science, Hengyang Normal University, Hengyang, Hunan 421008, China
  • Received:2020-03-01 Revised:2020-04-26 Online:2021-02-22 Published:2021-03-01
  • Contact: Ji zhengYi yizhengji2004@126.com

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摘要： 通过二次生长法和液相还原法制备了不锈钢纤维烧结毡复合NaA分子筛膜-纳米零价铁复合材料(Fe0-NaA-SSFSF)，研究了甲基橙在基于Fe0-NaA-SSFSF固定床上的催化湿式H2O2氧化性能，考察了不同pH值、床层高度、温度和入口浓度对甲基橙转化率、COD去除率和铁浸出浓度的影响，并测定了Fe0-NaA-SSFSF催化剂的稳定性。结果表明，当溶液pH为2.5时，甲基橙转化率在实验所测时间范围内有所波动；随pH降低至2.0，甲基橙转化率趋于稳定；继续降低pH至1.5，甲基橙转化率基本保持不变。随床层高度由0.45 cm增加至0.90 cm，甲基橙转化率基本保持不变，COD去除率由21.2%增加至85.0%；随温度由70℃降低至50℃，甲基橙转化率基本保持不变，COD去除率由85.0%降低至42.4%。随甲基橙入口浓度增加，甲基橙转化率和COD去除率变化幅度均很小。当pH=2.0、床层高度0.90 cm、温度70℃、甲基橙浓度50~200 mg/L条件下，实验所测时间范围内甲基橙转化率均大于97%，最大铁浸出浓度低于10.2 mg/L，固定床连续运转240 min后COD去除率均大于85%。催化剂被重复使用三次后，甲基橙转化率基本保持不变。

关键词: 甲基橙, 固定床, 纳米零价铁, NaA分子筛膜, 不锈钢纤维烧结毡

Abstract: Stainless steel fiber sintered felt supported Fe0-NaA molecular sieve membrane (Fe0-NaA-SSFSF) was prepared by the secondary growth and liquid-phase reduction method. The catalytic wet peroxide oxidation performance of methyl orange in a fixed bed with Fe0-NaA-SSFSF was studied. The effects of pH, bed height, temperature and inlet concentration on the conversion rate of methyl orange, COD removal rate and iron leaching concentration were investigated. The stability of Fe0-NaA-SSFSF catalyst was determined. The results showed that when the pH of the solution was 2.5, the conversion of methyl orange fluctuated in the experimental time range. With the decrease of pH to 2.0, the conversion of methyl orange tended to be stable. When the pH continued to decrease to 1.5, the conversion of methyl orange remained basically unchanged. With the increase of bed height from 0.45 cm to 0.90 cm, the conversion rate of methyl orange remained almost the same and the COD removal rate increased from 21.2% to 85.0%. With the decrease of reaction temperature from 70℃ to 50℃, the conversion rate of methyl orange remained almost unchanged and the COD removal rate decreased from 85.0% to 42.4%. Both the conversion rate of methyl orange and COD removal rate had no obvious change with the increase of inlet methyl orange concentration. Under the conditions of pH=2.0, bed height of 0.90 cm, reaction temperature of 70℃, methyl orange concentration of 50~200 mg/L, the conversion rate of methyl orange was greater than 97% in the experimental time range, the maximum iron leaching concentration was lower than 10.2 mg/L, and the COD removal rate was above 85% when the fixed bed was running continuously for 240 min. When the Fe0-NaA-SSFSF catalyst was reused three times, the conversion rate of methyl orange kept basically the same.

Key words: methyl orange, fixed bed, nanoscale zerovalent iron, NaA molecular sieve membrane, stainless steel fiber sintered felt