超声雾化/表面活性剂强化吸收耦合生物洗涤净化甲苯废气

doi:10.11949/0438-1157.20220590

化工学报 ›› 2022, Vol. 73 ›› Issue (10): 4692-4706.DOI: 10.11949/0438-1157.20220590

超声雾化/表面活性剂强化吸收耦合生物洗涤净化甲苯废气

侯晓松¹^,²^,³(), 刘晨星¹^,²^,³, 任爱玲¹^,²^,³, 郭斌¹^,²^,³(), 郭渊明⁴

^1.河北科技大学环境科学与工程学院，河北石家庄 050018
^2.挥发性有机物与恶臭污染防治技术国家地方联合工程研究中心，河北石家庄 050018
^3.河北省大气污染防治推广中心，河北石家庄 050018
^4.南京理工大学环境与生物工程学院，江苏南京 210094

收稿日期:2022-04-26 修回日期:2022-08-08 出版日期:2022-10-05 发布日期:2022-11-02
通讯作者: 郭斌
作者简介:侯晓松(1995—)，男，硕士研究生，15075168995@163.com
基金资助:
河北省重点研发计划项目(21373704D)

Study on purification of toluene waste gas by ultrasonic atomization/surfactants-enhanced absorption coupled with biological scrubbing

Xiaosong HOU¹^,²^,³(), Chenxing LIU¹^,²^,³, Ailing REN¹^,²^,³, Bin GUO¹^,²^,³(), Yuanming GUO⁴

^1.School of Environmental Science and Engineering, Hebei University of Science and Technology, Shijiazhuang 050018, Hebei, China
^2.National and Local Joint Engineering Research Center of Volatile Organic Compounds & Odorous Pollution Control Technology, Shijiazhuang 050018, Hebei, China
^3.Hebei Province Air Pollution and Control Promotion Center, Shijiazhuang 050018, Hebei, China
^4.School of Environmental and Bioengineering, Nanjing University of Science and Technology, Nanjing 210094, Jiangsu, China

Received:2022-04-26 Revised:2022-08-08 Online:2022-10-05 Published:2022-11-02
Contact: Bin GUO

摘要/Abstract

摘要：

为提高生物法净化疏水性VOCs的效率，构建了以微米级雾滴结合表面活性剂为特色的超声雾化/表面活性剂耦合生物洗涤器（ultrasonic atomization/surfactants-biological washing reactor，USBWR）。考察了USBWR对甲苯废气的去除能力及停运恢复性能，探讨USBWR最佳工艺条件及雾滴粒径分布，并分析系统中微生物群落结构，对比其与传统生物洗涤器（traditional biological washing reactor，TBWR）净化性能差异。结果表明：USBWR较TBWR系统有较高的甲苯去除能力和去除负荷，更适应企业非连续工况条件；在进气浓度2000 mg·m^-3、雾化量450 ml·h^-1条件下，响应曲面法优化USBWR最佳工艺条件为洗涤液pH 7.07、停留时间54.60 s、液气比0.23，USBWR去除率达97.26%；将实验室前期筛选得到的复配表面活性剂溶液（50 mg·L^-1皂角苷+500 mg·L^-1柠檬酸钠+200 mg·L^-1柠檬酸+50 mg·L^-1氯化钠）应用到超声雾化装置中，雾滴粒径均在15 μm以下，中位径为（6.911±0.326）μm，比表面积为（359.60±50.02）m²·kg^-1，雾滴小而均匀，更有利于气液充分接触；USBWR系统中主要微生物细菌门为变形杆菌门（Proteobacteria）、拟杆菌门（Bacteroidota）和绿弯菌门（Chloroflexi），与TBWR系统相比，USBWR系统促进了优势菌种变形杆菌门（Proteobacteria）的富集生长，更有利于降解甲苯废气。

关键词: 超声雾化, 复配表面活性剂, 有机化合物, 生物技术, 传质, 雾滴粒径分布, 微生物群落, 降解

Abstract:

To improve the efficiency of the biological method for the purification of hydrophobic VOCs, an ultrasonic atomization/surfactants-biological washing reactor (USBWR), featuring micron-sized droplets combined with surfactants was constructed in this study. The removal capacity and recovery performance of USBWR for toluene exhaust were investigated, the optimal process conditions and droplet size distribution of USBWR were discussed, the microbial community structure of the system was analyzed, and the difference in purification performance between USBWR and traditional biological washing reactor (TBWR) was compared. The results show that USBWR has higher toluene removal capacity and removal load than TBWR system, which is more suitable for non-continuous working conditions of enterprises. Under the conditions of inlet gas concentration of 2000 mg·m^-3 and atomization volume of 450 ml·h^-1, the best process conditions of USBWR were optimized by response surface method with washing solution pH of 7.07, residence time of 54.60 s and liquid-gas ratio of 0.23, and the removal rate of USBWR reached 97.26%. When the compound surfactant solution (50 mg·L^-1 saponin + 500 mg·L^-1 sodium citrate + 200 mg·L^-1 citric acid + 50 mg·L^-1 sodium chloride) obtained from the pre-screening laboratory was applied to the ultrasonic atomizer, the droplet size was less than 15 μm, the median diameter is (6.911±0.326) μm, the specific surface area is (359.60±50.02) m²·kg^-1, with small and uniform droplets, which is conducive to making the gas-liquid contact more adequate. The main microbial phyla in the USBWR system are Proteobacteria, Bacteroidota and Chloroflexi. Compared with the TBWR system, the USBWR system promotes the growth of the dominant bacteria Proteobacteria. The enrichment growth is more conducive to the degradation of toluene waste gas.

Key words: ultrasonic atomization, compounded surfactant, organic compounds, biotechnology, mass transfer, droplet size distribution, microbial community, degradation

中图分类号:

X 511

侯晓松, 刘晨星, 任爱玲, 郭斌, 郭渊明. 超声雾化/表面活性剂强化吸收耦合生物洗涤净化甲苯废气[J]. 化工学报, 2022, 73(10): 4692-4706.

Xiaosong HOU, Chenxing LIU, Ailing REN, Bin GUO, Yuanming GUO. Study on purification of toluene waste gas by ultrasonic atomization/surfactants-enhanced absorption coupled with biological scrubbing[J]. CIESC Journal, 2022, 73(10): 4692-4706.

图/表 19

图1 实验装置流程图1—气泵;2—空气流量计;3—甲苯流量计;4—气体发生瓶;5—恒温水浴锅;6—缓冲瓶;7—进气口;8—循环液槽;9—蠕动泵;10—超声雾化吸收装置;11—液体转子流量计;12—填料洗涤塔;13—气相色谱-质谱仪;14—填料;15—出气口;16—曝气头;17—取样口;18—尾气吸收装置

Fig.1 Flow chart of test device1—air pump; 2—air flow meter; 3—toluene flow meter; 4—gas generation bottle; 5—constant temperature water bath; 6—buffer bottle; 7—gas inlet; 8—circulation liquid tank; 9—peristaltic pump; 10—ultrasonic atomization absorption device; 11—liquid rotameter; 12—packed scrubber tower; 13—gas chromatograph-mass spectrometer; 14—packing; 15—gas outlet; 16—aeration head; 17—sampling port; 18—exhaust gas absorption device

图2 不同浓度下气相甲苯的去除率和去除负荷

Fig.2 Removal rate and removal load of gaseous toluene at different concentration

图3 pH变化对气相甲苯去除率的影响

Fig.3 Effect of pH change on removal rate of toluene in gas phase

图4 EBRT对甲苯去除负荷的影响

Fig.4 Effect of EBRT on toluene removal capacity

图5 液气比对甲苯去除负荷的影响

Fig.5 Effect of liquid-gas ratio on toluene removal capacity

表1 生物洗涤系统工况条件及运行方式

Table 1 Working conditions and operation mode of biological washing system

序号	工况条件	运行方式
1	临时停运事故	停运1 h
2	设备故障检修	停运4 h
3	生产系统故障白天检修	停运8 h
4	夜间停运阶段	停运16 h
5	生产系统全天停运检修	停运24 h
6	双休日停运	停运48 h

图6 停运时间对甲苯去除负荷的影响

Fig.6 Effect of shutdown time on toluene removal capacity

图7 停运24 h后系统性能恢复情况

Fig.7 System performance recovery after 24 h of shutdown

图8 停运48 h后系统性能恢复情况

Fig.8 System performance recovery after 48 h of shutdown

表2 实验因素编码与水平

Table 2 Coding and level of test factors

自变量	编码水平
自变量	-1	0	1
洗涤液pH（A）	6	7	8
液气比（B）	0.30	0.25	0.20
停留时间（C）	28	42	56

图9 洗涤液pH和停留时间对甲苯去除率的响应面分析

Fig.9 Response surface analysis of pH of circulating solution and EBRT on toluene removal rate

图10 液气比和停留时间对甲苯去除率的响应面分析

Fig.10 Response surface analysis of liquid-gas ratio and EBRT on toluene removal rate

图11 洗涤液pH和液气比对甲苯去除率的响应面分析

Fig.11 Response surface analysis of pH of circulating solution and liquid-gas ratio on toluene removal rate

表3 USBWR最佳工艺参数

Table 3 USBWR optimum process parameters

洗涤液pH	停留时间/s	液气比	甲苯去除率/%
洗涤液pH	停留时间/s	液气比	预测值	实际值
7.07	54.60	0.23	97.71	97.26

图12 生物反应器降解甲苯动力学拟合

Fig.12 Kinetic fitting of toluene degradation in bioreactor

表4 动力学拟合结果对比

Table 4 Comparison of kinetic fitting results

反应器	模拟方程	比降解速率k	R²	半衰期/h
USBWR	ln(c_t /c₀)= -0.1421t+0.2719	0.1421	0.9843	4.88
TBWR	ln(c_t /c₀)= -0.0834t-0.0105	0.0834	0.9662	8.31

表5 复配表面活性剂溶液在塔中不同高度的雾滴粒径分布

Table 5 Droplet size distribution of compound surfactant at different heights in the tower

距塔底距离/cm	中位径（D₅₀)/μm	体积平均径/μm	面积平均径/μm	比表面积/ (m²·kg^-1)	跨度
15	6.546	6.755	6.483	415.10	0.32
30	7.016	7.187	6.428	345.70	0.41
45	7.172	7.423	6.987	318.00	0.57
均值	6.911	7.122	6.633	359.60	—

图13 皂角苷+柠檬酸钠+柠檬酸+氯化钠在塔中不同高度雾滴粒径分布曲线

Fig.13 Droplet size distribution curve of saponin + sodium citrate + citric acid + sodium chloride at different heights in the tower

图14 TBWR和USBWR系统中微生物在门水平上的群落分析结果

Fig.14 Community analysis results of microorganisms at the phylum level in TBWR and USBWR systems

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超声雾化/表面活性剂强化吸收耦合生物洗涤净化甲苯废气

Study on purification of toluene waste gas by ultrasonic atomization/surfactants-enhanced absorption coupled with biological scrubbing

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