氧化鈰基材料的制備及光催化脫硝性能研究
發(fā)布時間:2018-05-05 09:33
本文選題:納米氧化鈰 + 石墨烯; 參考:《江蘇大學(xué)》2017年碩士論文
【摘要】:工業(yè)廢氣和汽車發(fā)動機尾氣中所含的大量氮氧化物不僅會對人體造成一次傷害,更將形成酸雨以及光化學(xué)煙霧。因此,開發(fā)高效脫硝催化劑脫除氮氧化物,遏制霧霾的產(chǎn)生,發(fā)展綠色循環(huán)經(jīng)濟,構(gòu)建環(huán)境與經(jīng)濟的協(xié)調(diào)發(fā)展已經(jīng)刻不容緩。本課題針對這一現(xiàn)狀選取富含分級多孔結(jié)構(gòu)的生物組織作為模板,利用生物大分子的誘導(dǎo)作用獲取結(jié)構(gòu)不同的仿生納米光催化材料。研究氧空位在導(dǎo)向光還原中起的關(guān)鍵作用;揭示光催化材料的微觀結(jié)構(gòu)-氧空位濃度-導(dǎo)向光還原性能三者之間的內(nèi)在關(guān)系。通過設(shè)計對比實驗,指導(dǎo)仿生納米復(fù)合光催化劑材料的設(shè)計。使用不同的生物模板及預(yù)處理方法、調(diào)控與氧化鈰納米顆粒復(fù)合的碳材料,搭建模擬光還原脫除廢氣反應(yīng)裝置,在不同溫度、不同光強、不同氣流空速下利用制得的催化材料轉(zhuǎn)化模擬工業(yè)廢氣,揭示仿生富集的分級多孔結(jié)構(gòu)對氮氧化物導(dǎo)向光還原速率及反應(yīng)產(chǎn)物的影響規(guī)律。本課題以新鮮豆芽,螺旋藻,油菜莖桿富含分級多孔結(jié)構(gòu)的組織作為生物模板制備仿生納米CeO_2/石墨烯光催化劑,在燒結(jié)溫度為800°C,煅燒速率為2°C/min條件下,仿生CeO_2/石墨烯納米催化劑精確復(fù)制了生物模板的微觀形貌特征。經(jīng)熒光顯微鏡、X射線衍射、拉曼、氮氣吸附脫吸儀、電子顯微鏡、紫外漫散射表征后可知仿油菜莖桿形貌的CeO_2/石墨烯光催化材料其孔隙結(jié)構(gòu)更為均勻,晶粒尺寸更小,精確復(fù)制了其具有的分級多孔結(jié)構(gòu),繼承了油菜莖桿模板高孔隙率,超大比表面積及易于調(diào)控的微觀形貌特征,有效地增強了所制備的納米光催化劑對可見光的捕獲能力,顯著提高了材料的光催化活性,為光催化脫硝提供了良好的催化環(huán)境。通過實驗探究出最佳光催化低溫脫除氮氧化物條件,最佳納米光催化劑的生物模板即仿油菜莖桿形貌的CeO_2/石墨烯在煅燒溫度為800°C、煅燒速率為2°C/min、催化劑填充體積為6 m L、NO濃度為600 ppm、氨氣濃度為600 ppm、氮氣為載氣、反應(yīng)溫度為140°C、空速為1000 h-1時催化劑的脫硝效率達到最高,對NO的催化脫除效率達到87%。
[Abstract]:Industrial exhaust and a large amount of nitrogen oxides in automobile engine exhaust will not only cause a damage to the human body, but also form acid rain and photochemical smog. Therefore, it is urgent to develop high efficiency denitrification catalyst to remove nitrogen oxides, to contain the production of haze, to develop green circular economy and to build a coordinated development of environment and economy. In order to solve this problem, biomimetic nano-photocatalytic materials with different structure were obtained by using biological macromolecules as template. The key role of oxygen vacancy in guided photoreduction is studied, and the relationship between microstructure, oxygen vacancy concentration and photoreduction performance of photocatalytic materials is revealed. The design of biomimetic nano-composite photocatalyst material was guided by the design and contrast experiment. Different biological templates and pretreatment methods were used to control the carbon composite with cerium oxide nanoparticles, and the simulated photoreduction and removal of waste gas reaction device was set up at different temperatures and different light intensities. The catalytic materials prepared under different airflow velocities were used to simulate industrial waste gas, which revealed the effect of bionic enrichment of porous structure on the photoreduction rate and reaction products of nitrogen oxides. In this paper, the biomimetic nanometer CeO_2/ graphene photocatalyst was prepared by using fresh bean sprouts, spirulina and rape stems as biomimetic templates, which were rich in graded porous structures. The sintering temperature was 800 擄C and the calcination rate was 2 擄C/min. The biomimetic CeO_2/ graphene nanocatalyst accurately duplicates the microscopic morphology of the biological template. X-ray diffraction, Raman, nitrogen adsorption-desorption apparatus, electron microscope and ultraviolet diffuse scattering analysis showed that the CeO_2/ graphene photocatalytic material, which mimic the morphology of rape stem, had more uniform pore structure and smaller grain size. The high porosity, large specific surface area and easy to control micromorphology of rape stem template were inherited, which effectively enhanced the ability of the prepared nano-photocatalyst to capture the visible light, so that it could accurately reproduce the hierarchical porous structure, and inherit the characteristics of high porosity, large specific surface area and easy to adjust and control the microscopic morphology of rape stem template. The photocatalytic activity of the material was improved significantly, which provided a good catalytic environment for photocatalytic denitrification. The optimum conditions of photocatalytic removal of nitrogen oxides at low temperature were investigated by experiments. The best biological template of nano-photocatalyst, CeO_2/ graphene, which mimics the morphology of rape stem, is calcined at 800 擄C, calcination rate is 2 擄C / min, the volume of catalyst filling is 600ppm, ammonia is 600ppm, nitrogen is carrier gas. When the reaction temperature is 140 擄C and the space velocity is 1000 h ~ (-1), the denitrification efficiency of the catalyst is the highest, and the catalytic removal efficiency of no is 87%.
【學(xué)位授予單位】:江蘇大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2017
【分類號】:X701;O643.36
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