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不同炭質(zhì)吸附劑對(duì)多氯聯(lián)苯的長(zhǎng)時(shí)間吸附特性研究及應(yīng)用

發(fā)布時(shí)間:2018-03-17 15:09

  本文選題:炭質(zhì)吸附劑 切入點(diǎn):理化性質(zhì) 出處:《北京交通大學(xué)》2017年碩士論文 論文類型:學(xué)位論文


【摘要】:沉積物是持久性有機(jī)污染物的大儲(chǔ)庫(kù),雖然在1974年禁止生產(chǎn),但沉積物中的污染物仍然會(huì)通過釋放作用進(jìn)入到水環(huán)境中,威脅著人類的健康,所以治理沉積物污染已經(jīng)成為一個(gè)熱點(diǎn)話題。本論文應(yīng)用5種炭質(zhì)吸附劑(椰殼活性炭、木炭活性炭、原炭(未活化炭)、東海電廠灰、煤基活性炭),以多氯聯(lián)苯(PCBs)為吸附質(zhì),利用仿生被動(dòng)采樣提取及測(cè)定吸附質(zhì),研究各炭質(zhì)吸附劑的吸附動(dòng)力學(xué)及等溫曲線,探究炭質(zhì)吸附劑的吸附原理,進(jìn)而應(yīng)用其中的煤基活性炭、椰殼活性炭、果殼、原碳為修復(fù)劑,進(jìn)行實(shí)際污染沉積物(蒲河支流某河段)的治理與修復(fù)研究,為炭質(zhì)吸附劑的應(yīng)用提供理論基礎(chǔ)。研究所得結(jié)論如下:(1)煤基活性炭、木質(zhì)活性炭具有較高的比表面積,且以中孔及微孔為主,椰殼活性炭、原炭、東海電廠灰的比表面積較小,東海電廠灰以大孔為主,幾乎沒有微孔結(jié)構(gòu)。本研究中使用5種炭質(zhì)吸附劑都含有苯環(huán)及羥基基團(tuán),且所含有的官能團(tuán)類似。三維熒光圖譜顯示,研究中使用的天然有機(jī)質(zhì)(NOM)主要成分是富里酸,結(jié)合排阻色譜可以看出,其平均分子量在5000Da附近。(2)吸附動(dòng)力學(xué)研究表明:準(zhǔn)二級(jí)動(dòng)力學(xué)能夠很好的擬合5種炭質(zhì)吸附劑對(duì)PCBs的吸附動(dòng)力學(xué)過程(相關(guān)系數(shù)R20.99),說明吸附過程是一個(gè)多重而復(fù)雜的過程;研究發(fā)現(xiàn)以大孔為主的炭質(zhì)吸附劑(如:東海電廠灰、椰殼活性炭、原炭)顆粒內(nèi)擴(kuò)散方程參數(shù)k值較大,Elovich方程參數(shù)b值較大,說明表觀吸附速率快,達(dá)到平衡所需要的時(shí)間較短,快吸附到慢吸附轉(zhuǎn)換過程不明顯,其主要以表面吸附為主;以微孔和中孔為主的炭質(zhì)吸附劑(煤基活性炭、木炭)孔隙較為發(fā)達(dá),表觀吸附速率小,快吸附到慢吸附轉(zhuǎn)換顯著,說明以內(nèi)部吸附為主;NOM對(duì)炭質(zhì)吸附劑吸附性能的影響實(shí)驗(yàn)表明,NOM的存在使得孔徑不發(fā)達(dá)的炭質(zhì)吸附劑(如:東海電廠灰、椰殼活性炭、原炭)表觀吸附速率下降,快-慢吸附速率差距增大,而NOM對(duì)孔徑較發(fā)達(dá)的炭質(zhì)吸附劑(如:煤基活性炭、木炭)具有相反的作用。(3)吸附等溫曲線研究結(jié)果表明,Freundlich吸附模型能較好的模擬實(shí)驗(yàn)數(shù)據(jù)(R20.6);吸附時(shí)間為1個(gè)月及12個(gè)月,孔隙結(jié)構(gòu)較為發(fā)達(dá)的煤基活性炭和木炭活性炭的吸附量均大于其他炭質(zhì)吸附劑,但吸附1個(gè)月時(shí),這種差距不顯著,而吸附12個(gè)月時(shí)差距較大,原因是,吸附1個(gè)月時(shí),吸附并未達(dá)到平衡(吸附動(dòng)力學(xué)研究得到同樣的結(jié)論),分配系數(shù)(Kd)并不能體現(xiàn)吸附劑的實(shí)際吸附能力,吸附12個(gè)月時(shí),吸附達(dá)到平衡,此時(shí)的Kd值能夠體現(xiàn)吸附劑的實(shí)際吸附能力。短時(shí)吸附,NOM降低了 5種炭質(zhì)吸附劑對(duì)PCBs的吸附容量,尤其是對(duì)椰殼活性炭、原炭、東海電廠灰的降低幅度較大;當(dāng)吸附時(shí)間為12個(gè)月時(shí),NOM對(duì)5種炭質(zhì)吸附劑的影響均小,究其原因,短時(shí)吸附,NOM附著在炭質(zhì)吸附劑表面(尤其是以中孔和大孔為主的吸附劑),競(jìng)爭(zhēng)和堵塞作用阻礙了其對(duì)PCBs的吸附,隨著時(shí)間的延長(zhǎng),PCBs分子能夠穿越NOM,進(jìn)而進(jìn)入炭質(zhì)吸附劑的內(nèi)部孔道,NOM的影響大大降低。(4)現(xiàn)場(chǎng)試驗(yàn)表明,煤基活性炭對(duì)PCBs的治理效果最佳,治理效果順序?yàn)?煤基活性炭果殼活性炭椰殼活性炭原炭,此結(jié)果與實(shí)驗(yàn)室研究結(jié)果完全匹配。
[Abstract]:The sediments are large reservoirs of persistent organic pollutants, while banning the production in 1974, but the pollutant in sediment will still be through release into the aquatic environment, pose a threat to human health, so the control of sediment pollution has become a hot topic. This paper used 5 kinds of carbon adsorbent (coconut shell activated carbon charcoal, activated carbon, raw carbon (non activated carbon), the East China Sea power plant ash, coal based activated carbon), with polychlorinated biphenyls (PCBs) as adsorbent, using the bionic passive sampling, extraction and determination of adsorption, adsorption kinetics and isotherm of the carbonaceous adsorbent, the adsorption principle of carbon adsorbent. Then the application of coal based activated carbon, coconut shell activated carbon, shell, raw carbon as repair agent, the actual contaminated sediments (Po River tributary of a river) governance and repair research, provide a theoretical basis for the application of carbon adsorbent. The research The conclusions are as follows: (1) coal based activated carbon and wood activated carbon with high specific surface area, and the mesopores and micropores of coconut shell activated carbon, the carbon, the East China Sea power plant ash surface area is smaller, the East China Sea power plant ash to larger pores, almost no pore structure. This study used 5 kinds of carbon adsorbent containing phenyl and hydroxyl groups, and contains similar functional groups. Show the three-dimensional fluorescence spectra, used in the study of natural organic matter (NOM) is the main component of fulvic acid, combined exclusion chromatography can be seen, the average molecular weight in the vicinity of 5000Da. (2) the results showed that the adsorption kinetics the quasi two level dynamic can fit 5 kinds of carbon adsorption adsorption agent on PCBs (correlation coefficient R20.99), indicating that the adsorption process is a multiple and complicated process; the study found that the carbonaceous adsorbent to larger pores (such as: the East China Sea Power Plant Ash, coconut shell activated carbon, The original carbon particle diffusion equation) parameter K value is large, the parameter of Elovich equation b value is large, indicating the apparent adsorption rate, the time needed to reach equilibrium is short, fast to slow adsorption adsorption conversion process is not obvious, mainly by surface adsorption; carbon with microporous and mesoporous adsorbent (mainly coal based activated carbon, charcoal pore) is developed, the apparent adsorption rate of small, fast adsorption to slow adsorption conversion significantly, illustrated by the internal adsorption; experiments show the effect of agent NOM on adsorption performance of carbon adsorption, the presence of NOM carbonaceous adsorbent developed the aperture (such as the East China Sea power plant ash, coconut shell activated carbon, the carbon) apparent adsorption rate decreased fast slow adsorption rate gap increases, and the carbon NOM on the pore developed adsorbent (such as coal based activated carbon, charcoal) has the opposite effect. (3) adsorption isotherm results show that Freundlich adsorption model can To simulate the experimental data better (R20.6); the adsorption time was 1 months and 12 months, the adsorption amount of the more developed pore structure of coal based activated carbon and charcoal activated carbon are higher than that of other carbon adsorbent, but the adsorption at 1 months, the difference was not significant, while the adsorption of 12 month gap the reason is that, the adsorption at 1 months, the adsorption did not reach equilibrium (get the same conclusion adsorption kinetics), distribution coefficient (Kd) can not reflect the actual adsorption capacity, adsorption at 12 months, the adsorption equilibrium, the Kd value can reflect the actual adsorption capacity of absorbing agent. Short term adsorption, NOM reduced 5 carbon adsorption capacity of PCBs, especially for the coconut shell activated carbon, raw carbon, the East China Sea power plant ash is greatly reduced; when the adsorption time is 12 months, the effect of NOM on 5 kinds of carbon adsorbent are small, the reason for the short time of adsorption NOM, attached to The carbonaceous adsorbent surface (especially adsorbent to medium and large pore mainly), competition and blocking effects hindered the adsorption of PCBs, with the extension of time, PCBs molecules can pass through NOM and then enter the carbon adsorbent internal hole, the influence of NOM greatly reduced. (4) the field test show that the effect of coal based activated carbon treatment on PCBs best treatment effect order of coal based activated carbon coconut shell activated carbon raw carbon, with the result of laboratory results perfectly matched.

【學(xué)位授予單位】:北京交通大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類號(hào)】:X52;O647.3

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