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甲基叔丁基醚(methyl tert-butyl ether, MTBE)是一种广泛使用的汽油添加剂,分子中的叔碳原子和甲基结构,使MTBE有良好的化学稳定性。随着国内汽油消费量的快速增长,MTBE产量持续增加,在世界范围内达到了约每年20 Mt [1]。MTBE在欧美等国已经被禁止使用,但由于储油罐、输送管道及加油站汽油的意外泄露造成环境中的残留污染依然存在。因具有相对较高的溶解度(42 g·L−1, 20℃)和较低的亨利系数(5.87×10−4 atm·m−3·mol−1, 25℃)[2],在环境中易溶于水且不易被土壤颗粒吸附[3]。由于MTBE的挥发性和难降解性,其自然衰减速率较低,能够在环境中持久存在并造成水体污染[4]。MTBE是浅层地下水中排名第二的常见挥发性有机化合物[5],可明显改变水体的气味和味道[6]。美国环境保护署(Environmental Protection Agency, EPA)建议饮用水中MTBE的味觉和气味阈值分别为40 、20 µg·L−1[7]。研究表明,MTBE具有遗传毒性并对皮肤和眼睛具有刺激性,在高浓度下还有抑制神经系统的可能性[8]。此外,MTBE会引起多种类型的DNA损伤,例如单链、双链断裂等[9]。由于MTBE污染的普遍性及潜在毒性,EPA在2000年将其划分为危害健康的物质[10],又在2002年通过了于2006年实施禁用MTBE的议案[11]。随着对MTBE毒性认识的深入,我国提出了在2020年禁用MTBE的环境规划[12]。尽管囿于技术发展水平实施该规划尚有较大难度,但治理环境中潜在的MTBE污染已是目前一大重要课题。
MTBE的分子结构:
基于MTBE对环境产生的污染及对人体健康造成的危害,研究人员对其降解技术进行了大量研究。常见的处理方法包括空气汽提、物理吸附、高级氧化及生物降解[5]。Vignola等[13-14]利用原位可渗透性反应墙修复被MTBE和烃类污染的地下水,经过约100 d的处理将MTBE的浓度降到了10 µg·L−1以下。Burbano等[15]用芬顿法处理MTBE,反应1 h后降解率达到了约99%。Salanitro等[16]培养的混合菌种BC-1是最早报道的能够降解MTBE的微生物。自此,通过研究发现了更多能以MTBE作为唯一碳源和能源进行利用,或通过共代谢方式将其降解的混合菌群和单一菌株[17-18]。
尽管已经证实上述处理方法均能在一定程度上降解MTBE,但每种单独的修复技术都存在固有的缺点。其中,空气汽提法在去除较低浓度的MTBE时会消耗大量的空气流,需要搭配尾气处理装置以净化被污染的空气流,技术成本较高[5]。吸附技术会受到吸附容量的限制,且反应后MTBE仍存在于吸附剂中会产生二次污染,存在废吸附剂的处理问题。此外,地下水中的天然有机物会产生竞争吸附作用而降低处理效果[19]。高级氧化法的成本较高,会产生毒性更大的副产物,易造成二次污染[20]。对于生物处理,MTBE分子结构中的醚键及叔丁基使其具有较低的生物降解性[21]。且该方法需要投放微生物会影响当地的微生物生态,并会受到环境中温度、pH、营养物质浓度等因素的限制,在原位修复中仍有较多问题亟待解决[22]。
为了克服上述修复技术单独使用时各自的局限性,研究人员开始探索将不同的技术联合应用,通过协同效应以提高降解效率。目前,已发表有大量的相关研究详细介绍不同类型的联合修复技术。基于吸附技术具有工艺控制和操作简单;高级氧化技术处理效率高;生物降解法不会产生二次污染的特点,本文选择以上3种处理技术,总结并概述了在这3种处理方法之中应用不同的联合修复技术去除水中MTBE污染的反应机理及应用,表1归纳了各技术的优缺点。
典型联合处理技术去除甲基叔丁基醚污染的研究进展
Research progress on typical combined treatment technologies for removal of methyl tert-butyl ether
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摘要: 甲基叔丁基醚(MTBE)作为汽油添加剂的广泛使用造成了世界范围内的环境污染。考虑到其毒性及高水溶性、抗降解性等,会在环境中造成持久性污染。因此,开发高效便捷的处理技术已刻不容缓。单一的降解方法存在不同的局限性,而将不同处理技术联合应用,取长补短,能够克服各方法单独应用时固有的问题,促进协同效应,提高甲基叔丁基醚的降解率。基于物理吸附、高级氧化、生物降解技术各自的优点,文章总结了近年来应用上述3种方法的联合处理技术的研究进展,阐述了处理效果和作用机理,同时对未来的研究方向提出展望。Abstract: The extensive use of methyl tert-butyl ether (MTBE) as a gasoline additive has resulted in widespread distribution of this compound in the environment. Due to its potential toxicity, high solubility and recalcitrance to degradation, the distribution of MTBE in the environment may lead to persistent pollution. Thus, the development of technology to eliminate MTBE contamination has become a priority. The existing single treatment technique has various limitations. However, the combined application of different processes could avoid the limitations and promote synergistic effects of single technique, resulting in the increasing of MTBE degrading rates. Based on the above description, this article summarizes the recently development and mechanism of combined techniques, including physical adsorption method, advanced oxidation method, and biodegradation method. The prospects for future research have also been proposed.
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Key words:
- MTBE /
- combined treatment technology /
- degradation of pollutants
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表 1 各联合修复技术的优缺点
Table 1. The advantages and disadvantages of each combined technology
方法
Method优点
Advantage缺点
Disadvantage沸石吸附-芬顿氧化 提高了降解效率,可在中性环境中工作,具有回收铁资源的可能性并可避免形成含铁污泥.沸石的化学性质稳定,可选择性吸附有机物,应用范围广泛. 需要在多种因素共存的条件下进行,反应区域有限;载体吸附剂的再生效率不稳定;
对操作条件的要求较为严格.活性炭吸附-芬顿氧化 成本较低,适用于处理较大范围的污染,工艺设备可靠,且AC的负载的能力较高,吸附性能较好. 吸附-生物降解 能在更长时间内保持较高的降解效率;易于固液分离,菌株密度高,提高了菌株抗冲击负荷的能力;延长载体的使用寿命,降低运行成本;避免二次污染,具有生态友好性. 长期运行后其降解效率有所下降,需要选择合适的吸附材料并提供充足的营养物质 高级氧化-生物降解 提高了降解速率;避免产生二次污染,适用范围广泛,可处理多种有机污染物. 需要充足的氧化剂,不适合处理成分复杂的样品. 表 2 沸石的特性
Table 2. The characteristics of zeolite
沸石
Zeolite最大自由孔径
Maximum free pore diameter/nm铁含量/%
Fe content(wt)BET表面积/ (m 2 ·g −1)
BET surface area粒径/μm
Particle sizeSiO2/Al2O3 来源
ReferenceZSM5 0.56 N.D.c 330 1.0—17a 683 [46] ZSM5 0.56 0.37 265 63—200b 400 [46] ZSM5 0.56 0.03 385 4.4—7.1a 236 [46] Fe-ZSM5 0.56 2.2 370 6.4—12a 26 [46] H-ZSM5 — — 450 1—3 25 [45] H-ZSM5 — — 425 1—3 80 [45] Na-ZSM5 — — 430 1—3 25 [45] Beta 0.75 N.D. 580 5.6—15a 200 [46] Fe-Beta 0.75 1.3 600 1.0—2.1a 35 [46] Fe-Beta 0.75 3.1 600 250—630b 25 [46] H-Beta — — 680 0.2—1.0 25 [45] H-mordenite — — 480 0.2—1.2 15 [45] H-faujasite — — 780 1—3 30 [45] a通过激光衍射分析确定的下限d50—上限d90.b筛分的粒状物料.c未检出.
a Lower limit d50—upper limit d90 determined by laser diffraction analysis. b Sieved fractions of pelletized materials. c Not detected.表 3 不同铁溶液对AC修饰改性的结果
Table 3. Results of various Fe amendment to the AC
铁类型
Fe type[Fe]initial/
(g·L−1)a[Fe]add/
(mg·kg−1)b[Fe]AC/
(mg·kg−1)[Fe]final/
(mg·L−1)epH
(Post oxidation)保留率/%
Retention ratef来源
Reference硫酸铁 低 1.25 3640 5480 c — 3.1 98.9 [69] 中 2.50 6900 8740 c — 3.0 96.8 [69] 高 3.75 8750 10590 c — 2.8 90.7 [69] 氯化铁 低 1.25 3310 5150 c — 3.1 95.2 [69] 中 2.50 5780 7620 c — 3.0 90.3 [69] 高 3.75 6960 8800 c — 2.7 83.8 [69] 硝酸铁 低 1.25 3440 5180 c — 3.2 96.6 [69] 中 2.50 6850 8690 c — 2.9 96.5 [69] 高 3.75 7850 9690 c — 2.7 87.2 [69] 硫酸亚铁 低 1.25 3730 5570 c — 3.1 99.9 [69] 低 2.50 7450 9290 c — 3.0 99.9 [69] 中 3.75 11060 12900 c — 2.9 99.5 [69] 中 4.40 — 12630d 97 — 98.0 [53] 中 5.50 — 15760d 270 — 95.0 [53] 高 6.60 — 16900d 730 — 89.0 [53] 高 8.20 — 18520d 1590 — 81.0 [53] a初始溶液中的铁浓度.b引入到AC中的铁浓度.
c[Fe]AC:AC上固定的铁=引入的铁+环境中的铁([Fe]AC=1840 mg/kg(n=14);95%的置信区间为1500—2170 mg/kg).
d[Fe]AC:AC上固定的铁=引入的铁+环境中的铁([Fe]AC=1020 mg/kg(n=3).e反应后溶液中的铁浓度.
f保留百分率=(([Fe]initial-[Fe]final)/[Fe]initial)×100%.
a Fe concentration in initial aqueous. b Amended Fe concentration immobilized in the AC.
c [Fe]AC: Total Fe on AC=Fe amended+ average background([Fe]AC=1840 mg/kg(n=14);95% confidence interval,1500–2170 mg/kg).
d [Fe]AC: Total Fe on AC=Fe amended+ average background([Fe]AC=1020 mg/kg(n=3). e Fe concentration in solution after reaction.
f Values in parentheses represent percent retention= (([Fe]initial-[Fe]final)/[Fe]initial) ×100%. -
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