化工学报 ›› 2022, Vol. 73 ›› Issue (5): 2183-2193.doi: 10.11949/0438-1157.20220006

• 能源和环境工程 • 上一篇    下一篇

Mn强化Fe/C微电解工艺条件优化及降解油墨废水机理

贾艳萍1(),丁雪1,刚健1,佟泽为2,张海丰1,张兰河1()   

  1. 1.东北电力大学化学工程学院，吉林省 吉林市 132012
    2.长春工程学院能源动力工程学院，吉林省 长春市 130012
  • 收稿日期:2022-01-04 修回日期:2022-03-27 出版日期:2022-05-05 发布日期:2022-05-24
  • 通讯作者: 张兰河 E-mail:jiayanping1111@sina.com;zhanglanhe@163.com
  • 作者简介:贾艳萍（1973—），女，博士，教授，jiayanping1111@sina.com
  • 基金资助:
    国家自然科学基金项目(51678119);吉林省科技发展计划项目(20180201016SF)

Optimization of process conditions for Mn enhanced Fe/C microelectrolysis and degradation mechanism of ink wastewater

Yanping JIA1(),Xue DING1,Jian GANG1,Zewei TONG2,Haifeng ZHANG1,Lanhe ZHANG1()   

  1. 1.School of Chemical Engineering, Northeast Electric Power University, Jilin 132012, Jilin, China
    2.School of Energy and Power Engineering, Changchun Institute of Technology, Changchun 130012, Jilin, China
  • Received:2022-01-04 Revised:2022-03-27 Published:2022-05-05 Online:2022-05-24
  • Contact: Lanhe ZHANG E-mail:jiayanping1111@sina.com;zhanglanhe@163.com

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摘要：

为了提高Fe/C微电解工艺对油墨废水的处理效率，以金属锰改变传统铁碳填料的成分，采用响应面法优化微电解工艺条件，通过三维荧光光谱、紫外可见光谱、气-质联用色谱等分析处理前后油墨废水的有机物成分及填料表面结构的变化，探究絮凝和降解机理。结果表明：在初始pH为2.79，反应时间为1.58 h，Fe/Mn质量比为3.11，填料总投加量为93.36 g/L的条件下，COD去除率达到87.9%，预测值(87.8%)与实测值相差0.1%，采用响应面法可准确预测COD去除率的变化。经Fe/Mn/C微电解工艺处理后，油墨废水Zeta电位上升，絮凝作用增强。Fe/Mn/C微电解工艺可破坏苯环及共轭双键结构，对类溶解性微生物代谢产物、类芳香族蛋白质类物质以及类腐殖酸类物质的降解效果显著，微电解过程中填料表面生成了铁、锰氧化物，部分氧化物附着在活性炭表面。

关键词: Fe/Mn/C, 微电解, 响应面, 优化, 油墨废水, 降解机理

Abstract:

In order to improve the treatment efficiency of ink wastewater using Fe/C microelectrolysis process, the compositions of conventional Fe/C fillers were changed by using metallic manganese, and the process conditions of microelectrolysis was optimized by using response surface methodology. The changes of organic matters in the wastewater and surface structure of the filler before and after the treatment of ink wastewater were analyzed by using three-dimensional fluorescence spectra, UV-Vis spectra and GC-MS, respectively. The flocculation and degradation mechanisms of ink wastewater were explored. The results showed that under the conditions of initial pH 2.79, reaction time of 1.58 h, Fe/Mn molar ratio of 3.11 and the filler dosage of 93.36 g/L, removal efficiency of COD reached 87.9%. The difference between the predicted value (87.8%) and the measured value was 0.1%. The response surface methodology could accurately predict the changes of the removal efficiency of COD. After being treated by Fe/Mn/C micro-electrolysis process, the Zeta potential of ink waste water increases, and the flocculation effect is enhanced. Fe/Mn/C microelectrolysis process could destroy the structure of benzene ring and conjugated double bonds, and it could efficiently degrade soluble microbial metabolites, aromatic protein substances and humic acids. During the microelectrolysis process, iron and manganese oxides were formed on the surface of the filler and some of the oxides adhered to the surface of the activated carbon.

Key words: Fe/Mn/C, microelectrolysis, response surface, optimization, ink wastewater, degradation mechanism

中图分类号: 

  • X 523

图1

Fe/Mn/C微电解工艺装置示意图"

图2

单因素对COD去除率的影响"

表1

响应面实验因素及水平设计"

编码因素单位水平
-101
A初始pH—234
B反应时间h11.52
CFe/Mn质量比—234
D填料总投加量g/L80100120

表2

响应面实验组次设计及实验结果"

序号变量取值COD去除率/%
ABCD
10-10-178.4
2011080.5
3100178.6
4001182.5
5010174.2
61-10079.5
7-1-10077.9
8000087.2
900-1-182.1
10101081.9
11010-183.9
12-110081.8
1310-1079.2
14-101083.0
15-10-1083.9
16000087.3
170-11080.2
180-1-1078.2
19000086.3
20001-185.3
21000087.6
22100-180.6
23000087.9
2400-1180.2
2501-1081.6
26-100180.9
27-100-184.0
280-10177.9
29110078.5

表3

COD去除率（响应值Y）模型方差分析"

变差来源平方和自由度均方和F值P值显著性
模型320.451422.8922.76<0.0001极显著
A14.39114.3914.310.0020极显著
B5.7715.775.740.0312显著
C5.3515.355.320.0370显著
D33.70133.7033.51<0.0001极显著
AB6.1516.156.110.0268显著
AC3.2413.243.220.0943不显著
AD0.3010.300.300.5921不显著
BC2.4212.422.400.1433不显著
BD20.84120.8420.720.0005极显著
CD0.2010.200.200.6605不显著
A260.04160.0459.69<0.0001极显著
B2174.371174.37173.36<0.0001极显著
C223.88123.8823.740.0002极显著
D265.74165.7465.36<0.0001极显著
残差14.08141.01
失拟项12.67101.273.590.1149不显著
误差1.4140.35
合计334.5328
标准偏差1.00相关系数0.9579
平均值81.76校正决定系数0.9158
变异系数1.23预测相关系数0.7753
压力系数75.18信噪比16.129

图3

实测值与预测值的对比"

图4

COD去除率摄动图"

图5

不同因素对COD去除率影响的响应面三维图"

图6

进出水三维荧光光谱图"

图7

油墨废水的紫外可见光谱图"

图8

反应前后铁、锰、碳的拉曼光谱图"

图9

进出水气-质联用谱图"

图10

Fe/Mn/C微电解反应机理"

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