本文選題：生物質油 + 乙酸�。� 參考：《浙江大學》2015年碩士論文

【摘要】：生物質作為含碳的可再生資源,通過快速熱解直接得到生物質油進而加以能源化利用,是緩解能源危機和環(huán)境污染以及生物質利用的重要方向。生物質油具有較強酸性和高含水量等特點,通過減壓蒸餾的分級處理后可得到基本不含水和酸的高沸點餾分(重質組分)和富含水及少量酸、醛、酮、醇、酚等含氧有機物的低沸點餾分(輕質組分)。重質組分通過進一步催化提質可得到液體燃料,輕質組分中的含氧有機物則可通過與水重整來制氫。 重整反應的關鍵在于催化劑高效穩(wěn)定性和反應條件經濟性。因此,本論文以乙酸為生物油輕質組分模型化合物,采用常壓固定床流動態(tài)反應工藝,開展鎳基催化劑上生物油輕質組分低溫水蒸氣重整制氫研究,獲得如下主要研究結果： 采用浸漬法制備了MgO、Y-Al2O3、ZrO2和CeO2載體負載鎳的催化劑,通過考察其在乙酸低溫水蒸氣重整反應中的反應性能,獲得了乙酸在350℃的低溫常壓下轉化率接近100%、重整制氫活性高并且穩(wěn)定的Ni/CeO2催化劑。結果表明,Ni/MgO和Ni/γ-Al2O3催化劑由于Ni組分與載體相互作用很強導致其可被還原利用的金屬Ni少,不利于反應；而Ni/CeO2催化劑由于Ni與Ce02相互弱作用,易于還原,可被利用的金屬Ni多,使其具有高的重整制氫能力。因此,載體與鎳之間的相互作用程度是影響催化劑重整制氫性能的主要因素。 以鈰鋯復合氧化物為載體,通過對不同Ce/Zr比CeO2-ZrO2載體負載Ni催化劑的研究,獲得了比Ni/CeO2催化劑性能更佳的Ni/CeO2-ZrO2乙酸水蒸氣重整制氫催化劑。不同Ce/Zr比主要影響了CexZr1-xO2固溶體的結構,并對負載Ni物種的可還原度、晶粒尺寸等產生影響。改變Ni的負載量以及焙燒溫度的研究進一步表明了Ni/CeO2-ZrO2催化劑的催化性能與可還原的鎳物種的數目及其晶粒尺寸存在一定對應關系。 通過改變還原溫度、反應溫度以及反應物中乙酸含量,研究了Ni/CeO2-ZrO2催化劑的乙酸水蒸氣重整特性。結果表明,在該體系的催化劑上,乙酸的水蒸氣重整制氫存在二條途徑,在金屬Ni上可直接發(fā)生水蒸氣重整,而在載體上則通過酮基化形成丙酮再在鄰近的Ni組分上發(fā)生重整。
[Abstract]:Biomass as a carbon-bearing renewable resource, biomass oil is directly obtained by rapid pyrolysis and energy utilization, which is an important direction to alleviate the energy crisis and environmental pollution as well as biomass utilization. Biomass oil has the characteristics of strong acidity and high water content. The high boiling point fractions (heavy components) without water and acid can be obtained by the fractionation of vacuum distillation, which are rich in water, aldehydes, ketones, alcohols, etc. A low boiling point fraction (light component) of oxygenated organics, such as phenol. Liquid fuel can be obtained by further catalytic extraction of heavy components, and hydrogen can be produced by reforming hydrogen with water by reforming oxygen-containing organic compounds in light components. The key of reforming reaction lies in the high stability of catalyst and the economy of reaction conditions. Therefore, in this paper, acetic acid was used as the model compound of light component of bio-oil, and the reaction process of fixed-bed flow state was used to study the hydrogen production of light component of bio-oil by low-temperature steam reforming of bio-oil on nickel-based catalyst. The main results are as follows: MgO- Y-Al _ 2O _ 3 ZrO _ 2 and CeO2 supported nickel catalysts were prepared by impregnation method, and their reaction performance in low-temperature steam reforming of acetic acid was investigated. The Ni / CEO _ 2 catalyst with high catalytic activity and stable hydrogen production activity was obtained. The conversion of acetic acid was close to 100 at 350 鈩，

本文編號：2103914