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

doi:10.11949/0438-1157.20220590

Abstract

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

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

CLC Number:

X 511

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.

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.

Figures/Tables 19

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

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

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

Fig.4 Effect of EBRT on toluene removal capacity

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

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

Fig.6 Effect of shutdown time on toluene removal capacity

Fig.7 System performance recovery after 24 h of shutdown

Fig.8 System performance recovery after 48 h of shutdown

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

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

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

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

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

Fig.12 Kinetic fitting of toluene degradation in bioreactor

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

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	—

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

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

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