纳米片层铁锰双金属催化剂活化过

doi:10.16085/j.issn.1000-6613.2022-0001

化工进展 ›› 2022, Vol. 41 ›› Issue (10): 5661-5668.DOI: 10.16085/j.issn.1000-6613.2022-0001

纳米片层铁锰双金属催化剂活化过

薛雨微¹^,²(), 叶校圳³, 曾静³, 王永全³(), 洪俊明¹^,²()

^1.华侨大学化工学院，福建厦门 361021
^2.福建省工业废水生化处理工程技术研究中心，福建厦门 361021
^3.厦门烟草工业有限责任公司，福建厦门 361021

收稿日期:2022-01-01 修回日期:2022-03-16 出版日期:2022-10-20 发布日期:2022-10-21
通讯作者: 王永全,洪俊明
作者简介:薛雨微（1998—），女，硕士研究生，主要研究方向为水处理高级氧化。E-mail：yuwei_xue2021@126.com。
基金资助:
国家自然科学基金(51978291);福建省科技项目(2021I0030);厦门市科技计划(3502Z20226012)

Pretreatment of tobacco sugar flavoring wastewater by nano layered iron-manganese bimetallic catalysts activating peroxymonosulfate

XUE Yuwei¹^,²(), YE Xiaozhen³, ZENG Jing³, WANG Yongquan³(), HONG Junming¹^,²()

^1.College of Chemical Engineering, Huaqiao University, Xiamen 361021, Fujian, China
^2.Fujian Province Engineering Research Center of Industrial Wastewater Biochemical Treatment, Xiamen 361021, Fujian, China
^3.Xiamen Tobacco Industrial Company Limited, Xiamen 361021, Fujian, China

Received:2022-01-01 Revised:2022-03-16 Online:2022-10-20 Published:2022-10-21
Contact: WANG Yongquan, HONG Junming

摘要/Abstract

摘要：

以烟草行业糖香料废水为研究对象，首先调查了某糖香料调配中心废水的水质情况。采用共沉淀法制备纳米片层铁锰双金属催化剂激活过一硫酸盐（PMS）产生自由基对烟草糖香料废水开展预处理研究。采用透射电子显微镜（TEM）、X射线粉末衍射仪（XRD）、X射线能谱分析（EDS）和比表面积测试（BET）对催化剂进行表征。通过因素实验分析降解过程中废水的化学需氧量和氨氮降解情况，在反应时间6h、PMS浓度为4mmol/L、催化剂投加量为0.6g/L的最佳条件下，COD去除率76.5%、氨氮去除率96.3%，降解过程符合一级动力学（R²＞0.9）。降解前后水样的三维荧光和气相色谱显示，难降解物质被转化为可生物利用的有机碳源，表明这一体系作为预处理有助于提高生化段的处理效率，对高级氧化法在污水预处理中的实际应用具有良好的应用前景。

关键词: 过一硫酸盐, 催化剂活化, 糖香料废水, 化学需氧量, 纳米片层, 自由基

Abstract:

Water quality investigation were carried out on the waste water from a sugar and spice kitchen. The nano iron manganese catalyst was synthesized by co-precipitation method and utilized to activate peroxymonosulfate to produce active radicals for the degradation of sugar flavoring wastewater. The catalyst was characterized by X-ray powder diffraction (XRD), transmission electron microscopy (TEM), X-ray energy spectrometry (EDS) and Brunauer Emmett Teller (BET). Effects of different condition factors on the degradation efficiencies of COD and ammonia nitrogen were investigated. Under the optimum conditions of 6h reaction time, PMS concentration 4mmol/L and catalyst dosage 0.6g/L, the removal rates of COD and ammonia nitrogen were 76.5% and 96.3% respectively, and the degradation process followed first-order kinetics (R²>0.9). Three-dimensional fluorescence and gas chromatography analysis of the water samples before and after degradation showed that the nonbiodegradable substances were converted into bioavailable organic carbon sources, which indicated that this system as a pretreatment could help to improve the biochemical treatment efficiency and thus has a good application prospect in advanced oxidation of wastewater treatment.

Key words: peroxymonosulfate, catalyst activation, sugar flavoring wastewater, chemical oxygen demand, nano layered iron, radical

中图分类号:

薛雨微, 叶校圳, 曾静, 王永全, 洪俊明. 纳米片层铁锰双金属催化剂活化过[J]. 化工进展, 2022, 41(10): 5661-5668.

XUE Yuwei, YE Xiaozhen, ZENG Jing, WANG Yongquan, HONG Junming. Pretreatment of tobacco sugar flavoring wastewater by nano layered iron-manganese bimetallic catalysts activating peroxymonosulfate[J]. Chemical Industry and Engineering Progress, 2022, 41(10): 5661-5668.

图/表 16

表1 烟草糖香料生产线产污情况

生产线名称	名称	每月产生量/t	COD/mg·L^-1
201料液调配线	过期废料液	0.8~1	52000
	换牌清洗液	94.5	50000
	除异味换水	10	4800
	换牌清洗液	48.6	16000
303香料基调配线	换牌清洗水	32.4	19000
	除异味换水	4.5	3200
303提取线	除异味换水	2.5	1920

表2 混合水样水质情况

混合废水指标	值
COD/mg·L^-1	12240
氨氮/mg·L^-1	2246.39
pH	5.46
浊度/NTU	5.03

图1 纳米片层铁锰催化剂的XRD图

图2 纳米片层铁锰催化剂的TEM图

图3 纳米片层铁锰催化剂的EDS分析

图4 纳米片层铁锰催化剂的BET分析

图5 不同PMS浓度对COD降解效率和降解动力学的影响

表3 不同PMS初始浓度对COD降解的动力学速率常数

PMS浓度/mmol·L^-1	K/h^-1	R²
2	0.128	0.988
4	0.156	0.989
6	0.173	0.986

图6 不同PMS浓度对氨氮降解效率的影响

图7 降解过程水样的pH变化曲线

图8 不同催化剂浓度对COD降解效率和降解动力学的影响

表4 不同催化剂浓度对COD降解的动力学速率常数

催化剂浓度/g·L^-1	K/h^-1	R²
0.2	0.156	0.989
0.4	0.183	0.969
0.6	0.232	0.956

图9 不同催化剂浓度对氨氮降解效率的影响

图10 降解前后水样的气相色谱图

图11 降解前后水样的有机质三维荧光分析

图12 纳米片层铁锰催化剂可重用性实验

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纳米片层铁锰双金属催化剂活化过

Pretreatment of tobacco sugar flavoring wastewater by nano layered iron-manganese bimetallic catalysts activating peroxymonosulfate

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