本文關(guān)鍵詞：改性凹凸棒粘土的制備及其光催化降解鹽酸四環(huán)素廢水的研究　出處：《長(zhǎng)安大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 凹凸棒粘土(ATPs) 半導(dǎo)體氧化物 改性 光催化降解 抗生素廢水

【摘要】：抗生素廢水屬于難處理的工業(yè)廢水,如果大量進(jìn)入水環(huán)境系統(tǒng),將會(huì)嚴(yán)重影響人體健康和生態(tài)環(huán)境。凹凸棒粘土是一種強(qiáng)吸附性、易獲得的礦物粘土,在吸附處理抗生素廢水方面具有顯著優(yōu)勢(shì)。而TiO2、ZnO等光催化劑在處理抗生素廢水方面也取得了一定的成效,展現(xiàn)了半導(dǎo)體光催化技術(shù)在處理抗生素廢水的巨大潛能。本文旨在通過(guò)對(duì)凹凸棒粘土的改性,制備出更具降解效率的新型光催化材料,所制備的材料有Ti-ATPs、Zn/Ti-ATPs、Ni/Ti-ATPs等,其中以Zn/Ti-ATPs光催化劑性能最優(yōu)。制備的新材料既能發(fā)揮凹凸棒粘土的強(qiáng)吸附性,又能結(jié)合復(fù)合光催化劑提高光能的利用效率,使降解鹽酸四環(huán)素的能力大大提高。此外,材料的制備過(guò)程均采取浸漬-煅燒法,操作簡(jiǎn)便易于實(shí)現(xiàn),為抗生素廢水的處理研究提供新的思路。本文采用掃描電子顯微鏡(SEM)、X射線衍射儀(XRD)、紫外-可見(jiàn)漫反射吸收光譜(UV-vis)等方法對(duì)改性凹凸棒粘土的結(jié)構(gòu)、形貌和組成進(jìn)行表征,并以鹽酸四環(huán)素為目標(biāo)污染物,考察改性材料在可見(jiàn)光下的降解效果。(1)制備Ti-ATPs,改性后的凹凸棒粘土協(xié)同吸附與光催化過(guò)程,具備了良好的降解能力。UV-vis結(jié)果表明經(jīng)過(guò)Ti改性后的ATPs光催化劑光譜圖在紫外光波段吸光度有一定的提高,在可見(jiàn)光波段雖有提高但不太明顯。以鹽酸四環(huán)素為目標(biāo)污染物進(jìn)行光催化降解實(shí)驗(yàn),研究表明:在Ti含量占ATPs的40%,450℃煅燒溫度下得到的復(fù)合材料光催化降解鹽酸四環(huán)素效果最好,在300W氙燈光源(250nm~800nm)下反應(yīng)120min對(duì)鹽酸四環(huán)素的降解率達(dá)75.8%。(2)用Zn和Ti同時(shí)對(duì)凹凸棒粘土進(jìn)行改性,制備Zn/Ti-ATPs。改性后的凹凸棒粘土協(xié)同吸附與兩種半導(dǎo)體復(fù)合光催化過(guò)程,相比之前具備了更優(yōu)的降解能力。UV-Vis光譜結(jié)果表明Zn/Ti-ATPs光催化劑的光譜圖出現(xiàn)了明顯紅移現(xiàn)象,在近紫外光區(qū)和可見(jiàn)光區(qū)內(nèi)吸光度均有明顯的提升。以鹽酸四環(huán)素為目標(biāo)污染物進(jìn)行光催化降解實(shí)驗(yàn),實(shí)驗(yàn)結(jié)構(gòu)表明:在Zn/Ti金屬摩爾配比為3:1,400℃煅燒溫度下得到的復(fù)合材料光催化性能最好;在鹽酸四環(huán)素溶液pH為7,溶液初始濃度為20mg/L以及催化劑的投加量為0.4g/L時(shí),在可見(jiàn)光照射120min后,新材料Zn/Ti-ATPs對(duì)鹽酸四環(huán)素的降解率達(dá)到最高,為94.64%。Zn/Ti-ATPs復(fù)合材料相比于Ti-ATPs和Zn-ATPs均有較高的降解性能。另外,材料穩(wěn)定性較好,重復(fù)三次使用時(shí)降解率還可以達(dá)到77.42%。(3)用同種方法制備的Ni/Ti-ATPs復(fù)合材料不具備光催化活性。以鹽酸四環(huán)素為目標(biāo)污染物進(jìn)行光催化降解實(shí)驗(yàn),發(fā)現(xiàn)在不同煅燒溫度和金屬比例條件下制備的Ni/Ti-ATPs均不具備光催化能力。這是由于沒(méi)有最合適的溫度能使TiO2和NiO同時(shí)處于光催化性能最好的晶型狀態(tài),在其余溫度下兩種氧化物互相占據(jù)光催化位點(diǎn),影響光催化反應(yīng)的進(jìn)行,使得Ni/Ti-ATPs不具光催化活性,降解效率也僅僅停留在改性前粘土的吸附水平。本文對(duì)凹凸棒粘土進(jìn)行系列改性實(shí)驗(yàn)后,制備的Zn/Ti-ATPs對(duì)鹽酸四環(huán)素廢水有很高的降解效率。材料光催化活性高、性能穩(wěn)定、回收方便,對(duì)水處理領(lǐng)域的研究具有顯著的理論意義。
[Abstract]:Antibiotic wastewater is one of industrial wastewater treatment, if poured into the water system, it will seriously affect human health and ecological environment. The attapulgite clay is a kind of strong adsorption, easy to obtain the clay minerals, has a significant advantage in the treatment of antibiotic wastewater by adsorption. TiO2, ZnO photocatalyst has achieved certain results in the treatment of antibiotic wastewater, show the semiconductor photocatalytic technology has huge potential in the treatment of antibiotic wastewater. This paper is based on the modified attapulgite clay, producing new photocatalytic materials more degradation efficiency, the prepared materials are Ti-ATPs, Zn/Ti-ATPs, Ni/Ti-ATPs, and Zn/Ti-ATPs the photocatalytic performance optimal. The preparation of new materials can play a strong adsorption of attapulgite clay, and can improve the utilization efficiency of solar energy combined with the composite photocatalyst, the degradation ability of tetracycline hydrochloride Greatly improved. In addition, impregnation calcination method adopt material preparation process is simple, easy to implement, and provide a new way for the treatment of antibiotic wastewater. In this paper, using scanning electron microscopy (SEM), X ray diffraction (XRD), optical absorption spectrum UV - visible diffuse reflectance (UV-vis) structure. The method of modified attapulgite clay, morphology and composition were characterized, and the tetracycline hydrochloride as the target pollutants, study on degrading effect of modified materials under visible light. (1) preparation of Ti-ATPs modified attapulgite clay synergistic adsorption and photocatalytic process, have good degradation ability of.UV-vis results after that Ti modified ATPs photocatalyst spectra after a certain improvement in the ultraviolet absorbance in the visible light wave is improved but not obviously. The photocatalytic degradation of tetracycline hydrochloride as the target pollutant experiment, the research shows that: in T The content of I accounted for 40% of ATPs, the best effect of the Composite Photocatalytic Degradation of tetracycline hydrochloride was 450 DEG C calcination temperature, the 300W xenon light source (250nm~800nm) reaction for 120min degradation of tetracycline hydrochloride was 75.8%. (2) with Zn and Ti at the same time the attapulgite clay modification, preparation of modified Zn/Ti-ATPs. the CO adsorption of attapulgite clay and two kinds of semiconductor photocatalytic process, compared with before the degradation ability of.UV-Vis spectra showed better spectra of Zn/Ti-ATPs photocatalyst showed a red shift phenomenon in ascension has obvious absorbance near ultraviolet region and visible region. Tetracycline as target pollutants by photocatalysis the degradation experiment, experimental results show that: the photocatalytic activity of the composite is 3:1400 calcined temperature in Zn/Ti molar ratio of the metal in the best; tetracycline hydrochloride solution pH 7 Solution The liquid concentration was 20mg/L and the catalyst dosage is 0.4g/L, in 120min visible light irradiation, the new material Zn/Ti-ATPs on the degradation of tetracycline hydrochloride was highest for 94.64%.Zn/Ti-ATPs composites compared to Ti-ATPs and Zn-ATPs had a higher degradation performance. In addition, the material has good stability and repeated three times using the degradation rate can also be 77.42%. (3) Ni/Ti-ATPs composite materials with the same preparation method has no photocatalytic activity. With tetracycline hydrochloride as target pollutants photocatalytic degradation experiments, found at different calcination temperature and metal ratio under the condition of preparation of Ni/Ti-ATPs not have the photocatalytic ability. This is due to the lack of the most suitable temperature can make TiO2 and NiO in the crystalline state the best photocatalytic performance at the same time, in the temperature of two oxide photocatalytic sites occupy each other, influence of photocatalytic reaction That makes the Ni/Ti-ATPs has no photocatalytic activity. The degradation efficiency also only stay in the level of the adsorption behavior of clay. This series of experiments on the modified attapulgite clay, preparation of Zn/Ti-ATPs with high degradation efficiency of tetracycline hydrochloride wastewater. The material has high photocatalytic activity, stable performance, convenient recovery, has the theory significance to the research in the field of water treatment.

【學(xué)位授予單位】：長(zhǎng)安大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X703

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