甘 露,閻 寧,張永明 (上海師范大學(xué)生命與環(huán)境科學(xué)學(xué)院,上海 200234)
紫外輻射與生物膜同步耦合降解喹啉
甘 露,閻 寧,張永明*(上海師范大學(xué)生命與環(huán)境科學(xué)學(xué)院,上海 200234)
紫外輻射光解與生物降解同步耦合的氣升式內(nèi)循環(huán)反應(yīng)器用于喹啉的降解.實(shí)驗(yàn)過(guò)程中分別采用單獨(dú)紫外光解、單獨(dú)生物降解和紫外光解與生物降解同步耦合的方法對(duì)喹啉進(jìn)行降解.結(jié)果表明,喹啉在紫外光解與生物降解同步耦合的作用下,其降解速率明顯提高.喹啉降解動(dòng)力學(xué)分析結(jié)果表明,喹啉的生物降解可以用有抑制性的 Haldane模型描述.相比生物降解過(guò)程,單獨(dú)紫外光解對(duì)喹啉的降解速率可以忽略,但將紫外輻射與生物降解耦合在一起后,可以提高喹啉的最大降解速率近1倍并減小抑制常數(shù)36%,同時(shí)還可以提高喹啉的礦化程度.
喹啉;生物降解;紫外光解;生物膜;反應(yīng)器
喹啉是一種重要的精細(xì)化工原料,主要用于合成醫(yī)藥、染料、農(nóng)藥和多種化學(xué)助劑,因此每年都有大量喹啉進(jìn)入環(huán)境系統(tǒng)中[1-2].喹啉又稱氮雜萘,分子式為C9H7N,是吡啶與苯并聯(lián)的化合物,且有兩種方式,分別成為喹啉和異喹啉,存在于煤焦油和骨焦油中.喹啉及其衍生物進(jìn)入環(huán)境后會(huì)對(duì)動(dòng)植物生長(zhǎng)發(fā)育產(chǎn)生不良反應(yīng), 有致癌、致畸、致突變性[3-4],且在較高級(jí)的生物體中有通過(guò)食物積累的可能性,對(duì)地表水和地下水環(huán)境系統(tǒng)有較大的威脅,所以對(duì)喹啉降解的研究日益受到重視[5-6].
大量文獻(xiàn)表明喹啉及其衍生物可以被生物降解,并且已經(jīng)鑒定出了大量的喹啉及其衍生物的降解菌[7-12],通過(guò)篩選所得的菌種在喹啉的生物降解效果上得到了強(qiáng)化,但也有文章有提到,單獨(dú)的生物方法耗時(shí)較長(zhǎng),耐沖擊負(fù)荷的能力也不強(qiáng)[13-14].目前喹啉及其衍生物的生物降解研究有4種類(lèi)型:好氧降解、厭氧降解、缺氧降解和共基質(zhì)降解[15].鑒于喹啉對(duì)微生物具有抑制作用,通常單獨(dú)的生物降解其效率較低.國(guó)內(nèi)外的不少學(xué)者采用了一些物化及高級(jí)氧化方法技術(shù)對(duì)喹啉及其衍生物進(jìn)行處理,較為傳統(tǒng)的物化及高級(jí)氧化方法主要有:混凝法、吸附法等,以及催化氧化、電化降解、濕式氧化、光催化氧化、臭氧氧化、超臨界水氧化等高級(jí)氧化技術(shù)[16-21].其中紫外輻射光解或光催化是相對(duì)簡(jiǎn)單、易于操作的高級(jí)氧化方法.但若單獨(dú)依賴紫外輻射將喹啉完全降解為二氧化碳和水,效率較低,且不經(jīng)濟(jì).將紫外輻射光解與生物降解耦合在一起,通過(guò)兩者的協(xié)同作用,提高喹啉的降解效率.當(dāng)將紫外輻射與生物降解結(jié)合后,喹啉中的C—C、C—N鍵吸收紫外光的能量而斷裂,使有機(jī)物逐漸降解,從而有利于生物降解,最后以CO2的形式離開(kāi)體系[22].以往將紫外輻射光解或光催化與生物降解的耦合處理難降解有機(jī)廢水方面,大多采用分步耦合的方法進(jìn)行處理,即將光解或光催化與生物降解分別在2個(gè)單元里分步進(jìn)行[23-29].這存在一個(gè)最佳控制的問(wèn)題,即光解或光催化時(shí)間過(guò)長(zhǎng),則總的效率下降;而時(shí)間過(guò)短則不利于后續(xù)的生物降解.為此,將光解或光催化與生物降解結(jié)合在一個(gè)單元里處理難降解有機(jī)物,則可以大大提高處理效率[30-31].本研究采用氣升式內(nèi)循環(huán)紫外光解與生物降解耦合反應(yīng)器,通過(guò)該反應(yīng)器將紫外輻射光解與生物降解有效地組合為一體,試圖實(shí)現(xiàn)高效降解喹啉.分別采用間歇和連續(xù)兩種方式,考查不同濃度的喹啉在單獨(dú)紫外光解、單獨(dú)生物降解以及紫外光結(jié)合生物降解過(guò)程中的降解規(guī)律.
氣升式內(nèi)循環(huán)光/生物一體化反應(yīng)器由石英玻璃制成,如圖1所示.反應(yīng)器中間設(shè)置一塊玻璃板,將反應(yīng)器分隔為紫外輻射光解區(qū)和生物降解區(qū).反應(yīng)器有效容積為 45mL.在距反應(yīng)器紫外輻射光解區(qū)一側(cè) 10cm是一功率為 24W,波長(zhǎng)為254nm的紫外光源.實(shí)驗(yàn)過(guò)程中,在生物降解區(qū)內(nèi)曝氣,可以驅(qū)動(dòng)液體在反應(yīng)器的光解區(qū)和生物降解區(qū)之間循環(huán)流動(dòng),使有機(jī)物不斷的經(jīng)歷光解和生物降解,從而提高其降解效率.
喹啉和分析用藥品:重鉻酸鉀、硫酸,硫酸銀均為分析純,均購(gòu)自上海國(guó)藥集團(tuán).模擬喹啉廢水是將喹啉直接稀釋到自來(lái)水中.先配制濃度為5g/L的母液置于冰箱備用,使用時(shí),根據(jù)實(shí)驗(yàn)設(shè)計(jì)要求,將濃度稀釋為100~1500mg/L.
污泥取自上海龍華水質(zhì)凈化廠的二沉池的回流污泥.馴化之前,用自來(lái)水清洗污泥,方法是將 600mL左右的污泥倒入 2L的量筒內(nèi),加入1400mL的自來(lái)水,讓污泥自由沉淀 30min后將上清液倒掉,重復(fù)上述步驟5遍,然后加入濃度為500mg/L的葡萄糖溶液,在 25~30℃條件下進(jìn)行馴化培養(yǎng),此時(shí)污泥的SV為300mL/L.培養(yǎng)初期每天更換新鮮葡萄糖溶液,在最初30d的培養(yǎng)馴化周期內(nèi),逐漸減少葡萄糖用量,直至不再加入葡萄糖,同時(shí)逐漸增加喹啉的濃度,從 50mg/L至200mg/L.30d后,待微生物適應(yīng)環(huán)境,逐漸增加喹啉的投加量,使容器內(nèi)喹啉的濃度從200mg/L逐漸增加到1000mg/L.
1.4.1 空白實(shí)驗(yàn) 在反應(yīng)器中分別裝入無(wú)生物膜的空白載體、滅活的生物膜對(duì)濃度為100mg/L、500mg/L的喹啉進(jìn)行60min的對(duì)比實(shí)驗(yàn)以了解載體、生物膜對(duì)喹啉的吸附情況.另外單純對(duì)喹啉溶液進(jìn)行曝氣,以了解喹啉在曝氣過(guò)程中的揮發(fā)情況.其中滅活生物膜是將已形成的生物膜置于溫度為100℃的恒溫箱內(nèi)1h.
1.4.2 喹啉的間歇降解實(shí)驗(yàn)和連續(xù)降解實(shí)驗(yàn)分別采用單獨(dú)光解(P)、單獨(dú)生物降解(B)以及光解與生物降解同步耦合(P&B)的方法對(duì)不同濃度的喹啉進(jìn)行間歇和連續(xù)降解實(shí)驗(yàn).間歇實(shí)驗(yàn)中,通過(guò)曝氣驅(qū)動(dòng)溶液在反應(yīng)器內(nèi)循環(huán)流動(dòng),在喹啉光解時(shí),反應(yīng)器內(nèi)不裝填生物膜,開(kāi)啟紫外燈;在喹啉生物降解時(shí),反應(yīng)器內(nèi)裝入生物膜,同時(shí)關(guān)閉紫外燈;在光與生物協(xié)同降解喹啉時(shí),反應(yīng)器內(nèi)裝入生物膜的同時(shí)開(kāi)啟紫外燈對(duì)喹啉進(jìn)行降解.在連續(xù)降解實(shí)驗(yàn)中,分別針對(duì)初始濃度為 100, 500,1000mg/L的喹啉進(jìn)行連續(xù)降解,停留時(shí)間為5h.連續(xù)降解過(guò)程中,首先進(jìn)行單獨(dú)紫外光解,此時(shí)反應(yīng)器內(nèi)不加入生物膜,只開(kāi)啟紫外燈.大約150h之后,關(guān)閉紫外燈,加入生物膜,進(jìn)行單獨(dú)生物降解.300h之后,開(kāi)啟紫外燈,進(jìn)行紫外光解與生物降解同步耦合降解喹啉.實(shí)驗(yàn)中,每間隔一定的時(shí)間取樣測(cè)定喹啉的濃度之外,并測(cè)定其COD的去除情況,以了解喹啉的礦化程度.
由于喹啉屬于難降解的含氮雜環(huán)化合物,對(duì)微生物具有一定的毒性和抑制性[32].通過(guò)對(duì)喹啉降解的動(dòng)力學(xué)分析可以了解喹啉對(duì)生物膜的抑制情況.喹啉降解動(dòng)力學(xué)可以通過(guò)喹啉的初始濃度C0與其初始去除速率 V0的關(guān)系求得.對(duì)于有抑制的降解動(dòng)力學(xué)可以用Haldane模型來(lái)描述[33].
用美國(guó)產(chǎn)的Agilent 1100的高效液相色譜(配置波長(zhǎng)250nm的紫外熒光器、型號(hào)為ZORBAX SB-C18反相色譜柱)測(cè)試喹啉,流動(dòng)相為甲醇水溶液,體積比為甲醇:水(含1%醋酸) = 60:40 (V/V),流動(dòng)速率為1mL/min,檢出限在0.1mg/L以上.COD分析采用型號(hào)為 KDB—Ⅲ微波消解儀(青島科迪博電子科技有限公司)進(jìn)行消解,再用重鉻酸鉀溶液進(jìn)行滴定,以求得COD濃度.
對(duì)初始濃度分別為100mg/L和500mg/L的喹啉進(jìn)行空白對(duì)比實(shí)驗(yàn),以考察空白生物膜載體、滅活的生物膜對(duì)喹啉是否有吸附,以及喹啉在曝氣過(guò)程中的揮發(fā)情況,結(jié)果如圖2所示.結(jié)果表明,相比喹啉的生物降解,生物膜載體和滅活的生物膜對(duì)喹啉幾乎沒(méi)有吸附,同時(shí)喹啉在曝氣過(guò)程中的揮發(fā)也可以忽略.因此,在該體系內(nèi),生物膜或生物膜載體對(duì)喹啉的吸附作用很小,而后續(xù)的實(shí)驗(yàn)過(guò)程中喹啉的去除可以認(rèn)為是生物降解或光解的結(jié)果.
圖2 喹啉的吸附、揮發(fā)及降解的對(duì)比Fig.2 Comparison adsorption and volatile with degradation of quinoline
圖3 分別在生物降解和紫外光解與生物降解協(xié)同作用下喹啉的初始去除速率與初始濃度的關(guān)系Fig.3 Relationship of initial quinoline concentration and its initial removal rates under photolysis alone, biodegradation alone and intimate coupled photolysis and biodegradation
表1 喹啉降解動(dòng)力學(xué)參數(shù)Table 1 Parameters of quinoline degradation
因此喹啉在方法B和方法P&B的降解過(guò)程中的動(dòng)力學(xué)方程可以分別用下式表示:
單獨(dú)生物降解(方法B):
紫外光解與生物降解同步耦合(方法P&B):
從圖3也可以看出,它們的擬合程度相當(dāng)高.從動(dòng)力學(xué)常數(shù)的分析可以看出,通過(guò)紫外光解與生物膜的協(xié)同作用,抑制常數(shù)降低了約36%,同時(shí)最大降解速率也提高近1倍.這說(shuō)明雖然單獨(dú)的紫外光解(P)對(duì)喹啉的降解作用相比單獨(dú)的生物降解(B)可以忽略,但紫外光解與生物膜協(xié)同作用后,即通過(guò)方法 P&B的作用,可以大大緩解喹啉對(duì)生物的抑制,同時(shí)也提高了喹啉的降解速率.
分別采用方法 P、B和 P&B對(duì)濃度為200mg/L的喹啉進(jìn)行降解,其結(jié)果如圖4所示.從圖4中可以明顯地看出,采用方法P&B時(shí),喹啉的降解速率明顯地高于其它2種方法.例如當(dāng)采用方法P&B時(shí),經(jīng)過(guò)8h后,200mg/L的喹啉已經(jīng)完全去除,而采用方法P和方法B時(shí),8h之后,喹啉的去除率分別為5%和95%.從圖4中還可以看出,喹啉在方法P&B和方法B的降解過(guò)程中,其降解趨勢(shì)十分相近,但總是慢一點(diǎn).根據(jù)動(dòng)力學(xué)分析可知,喹啉濃度為200mg/L時(shí),還沒(méi)有對(duì)生物膜產(chǎn)生抑制作用.但由于紫外輻射光解與生物降解的耦合還是提高了喹啉的降解效率.
圖4 喹啉分別在方法P、B和P&B作用下的降解規(guī)律Fig.4 Quinoline removal regularity under protocol P, B and P&B
同樣采用方法P、B和P&B 3種方法對(duì)喹啉進(jìn)行連續(xù)流降解實(shí)驗(yàn).喹啉溶液的濃度分別為100,500,1000mg/L,停留時(shí)間均為5h.各濃度的喹啉在連續(xù)流降解的情況如圖5所示.
圖5 喹啉的連續(xù)降解Fig.5 Quinoline removal in continuous flow
根據(jù)圖5的結(jié)果可以計(jì)算喹啉在3種方法處理過(guò)程中的平均體積去除負(fù)荷 (VRR).其結(jié)果如圖6所示.從圖6可以看出,采用方法P&B時(shí),喹啉的體積去除負(fù)荷明顯地高于方法B和P.其中方法B又高于方法P.但各方法中,隨著喹啉濃度的增加,體積去除負(fù)荷逐漸增大.將圖4與圖5和圖6比較,可以明顯看出,在連續(xù)流降解喹啉時(shí),喹啉的去除速率高于間歇式去除喹啉的速率.這是因?yàn)樵谶B續(xù)流過(guò)程中,喹啉降解后的中間產(chǎn)物可以及時(shí)排除反應(yīng)器,因而產(chǎn)物的抑制可大大減少.
圖6 連續(xù)流降解喹啉的體積去除負(fù)荷Fig.6 Volume removal rate of quinoline in continuous flow
對(duì)喹啉進(jìn)行降解是希望能使其得到礦化,COD是衡量喹啉礦化程度的重要指標(biāo),為此針對(duì)連續(xù)流降解喹啉過(guò)程中進(jìn)、出溶液測(cè)定其COD.喹啉所對(duì)應(yīng)的COD去除率如圖7所示.
圖7 連續(xù)降解喹啉時(shí)的COD去除率Fig.7 COD removal percentage for quinoline in continuous flow
從圖7中可以看出,采用方法P&B,對(duì)喹啉的礦化效果是最好的,而方法P和B對(duì)喹啉的礦化率均明顯低于方法 P&B.這一結(jié)果說(shuō)明紫外光的參與降低了喹啉對(duì)生物膜的抑制作用.有資料表明,在 185/254nm的紫外光的輻照下,喹啉和異喹啉發(fā)生降解的主要途徑均有兩條[34]:(1)水的裂解產(chǎn)生的羥基與苯環(huán)加成,隨后開(kāi)環(huán)降解;(2)底物發(fā)生光電離后形成的自由基與氧氣發(fā)生反應(yīng)形成過(guò)氧化物,隨后開(kāi)環(huán)降解.喹啉的好氧生物降解途徑一般有四種,其共同點(diǎn)為[35-36]:一般情況下,首先是鄰近氮原子的羥基化,該反應(yīng)之后喹啉的苯環(huán)部分轉(zhuǎn)化為二羥基衍生物,然后環(huán)開(kāi)裂.而由于反應(yīng)器的特性,喹啉在降解過(guò)程中不斷地在光解區(qū)和生物降解區(qū)之間循環(huán)流動(dòng),在兩種方式的共同作用下,上述單獨(dú)的紫外輻射光解和生物降解對(duì)喹啉的降解途徑就發(fā)生了一定的變化,兩者耦合在一起,喹啉中的C—C、C—N鍵吸收紫外光的能量而斷裂,使有機(jī)物逐漸降解,其結(jié)構(gòu)一被破壞便立即會(huì)被微生物所利用,最后以 CO2的形式離開(kāi)體系,從而提高了生物降解的礦化能力.
3.1 紫外光解對(duì)喹啉的降解作用明顯低于生物降解,但將紫外光解與生物降解進(jìn)行耦合之后,可以明顯地提高喹啉的降解速率,即耦合后的降解速率大于單獨(dú)光解與單獨(dú)生物降解之和.
3.2 喹啉的生物降解過(guò)程符合抑制型的Haldane方程,當(dāng)紫外光解與生物膜耦合之后,可以降低抑制常數(shù) 36%,提高喹啉最大降解速率48%,即提高了生物膜對(duì)喹啉的親和程度,進(jìn)而提高喹啉的降解速率.
3.3 紫外光解與生物膜耦合之后,喹啉的體積去除負(fù)荷明顯地高于單獨(dú)的生物降解和單獨(dú)的紫外光解,相應(yīng)的礦化程度也明顯提高.
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UV irradiation intimately coupling biofilm for quinoline degradation.
GAN Lu, YAN Ning, ZHANG Yong-ming*(College of Life and Environmental Science, Shanghai Normal University, Shanghai 200234, China). China Environmental Science, 2012,32(4):623~629
Internal loop photolytic biological reactor was used for quinoline degradation by means of three protocols: photolysis alone, biodegradation alone and photo-biodegradation. Experimental results indicated that quinoline removal rate was accelerated clearly under intimately coupled photolysis and biodegradation. Quinoline removal rate could be described with Haldane model as the inhibition to microorganism according to the analysis of quinoline removal kinetics. Compared with quinoline removal rate by biodegradation alone, the photolytic rates might be ignored. But the maximum quinoline removal rate was increased by one times after photolysis was intimately coupled with biodegradation for quinoline degradation, and the inhibition constant was decreased with 36%, at the same time, the quinoline mineralization degree was also increased by intimately coupled UV irradiation and biofilm.
quinoline;biodegradation;UV photolysis;biofilm;reactor
2011-07-14
國(guó)家自然科學(xué)基金項(xiàng)目(50978164,50678102);上海市基礎(chǔ)研究重點(diǎn)項(xiàng)目(11JC1409100);上海市重點(diǎn)學(xué)科建設(shè)項(xiàng)目(S30406)
* 責(zé)任作者, 教授, zhym@shnu.edu.cn
X703
A
1000-6923(2012)04-0623-07
甘 露(1987-),女,江西南昌人,上海師范大學(xué)生命與環(huán)境科學(xué)學(xué)院碩士研究生,主要從事難降解有機(jī)廢水處理技術(shù)的研究.