本文選題：甲烷重整制氫 + Ni-Co合金催化劑��； 參考：《南昌大學(xué)》2015年碩士論文

【摘要】：氫氣是一種綠色能源,能量密度大,燃燒后產(chǎn)物為水,不僅不會(huì)對(duì)環(huán)境造成污染,還有可能替代石化燃料解決能源危機(jī)問(wèn)題。因此,氫氣在21世紀(jì)能源舞臺(tái)上將扮演重要的角色。目前,甲烷水蒸汽重整是最有效和可行的制氫方法,且已大規(guī)模工業(yè)化。Ni基催化劑因價(jià)格低廉、儲(chǔ)量豐富且活性高,已被廣泛應(yīng)用于甲烷重整。但該類催化劑易積碳,Ni活性中心高溫下易燒結(jié),導(dǎo)致催化劑失活。因此,為降低制氫成本,促進(jìn)氫氣作為綠色能源推廣,有必要研發(fā)具有更高抗燒結(jié)能力和抗積碳性能的催化劑。本論文針對(duì)該目標(biāo)展開研究,主要結(jié)果如下:首先,使用共浸漬方法制備一系列不同Co含量的Ni-Co/γ-Al2O3雙金屬催化劑,其中Ni的質(zhì)量百分比為12%,并將其用于甲烷水蒸氣重整制氫反應(yīng)。結(jié)果表明,Co的添加雖然使得催化劑低溫活性略有降低,卻很好地提高了Ni/Al2O3催化劑的抗積碳性能和反應(yīng)穩(wěn)定性。XPS和TEM結(jié)果證明Ni和Co之間存在強(qiáng)相互作用。還原后催化劑的XRD和HAADF-STEM mapping結(jié)果提供了直接的證據(jù)表明Ni和Co之間形成了Ni-Co合金。該合金的形成可有效覆蓋部分低配位的活潑Ni中心,降低催化劑對(duì)C-H鍵的活化能力,抑制C-C鍵的形成,因而有效地抑制了催化劑在反應(yīng)過(guò)程中積碳。其次,分別合成了介孔Al-SBA-15和球形樹枝狀KCC-1載體,利用去離子水和乙二醇作為溶劑,采用浸漬法制備了7%Ni/Al-SBA-15和Ni/KCC-1等催化劑。結(jié)果表明,用乙二醇作為溶劑,結(jié)合上述兩種不同形貌介孔載體所制備的催化劑,具備很高的活性、穩(wěn)定性和優(yōu)良的抗積碳性能。XRD和TEM測(cè)試結(jié)果證明,在這些催化劑上,Ni活性組分的粒度可被孔道限域在5 nm以下,從而抑制了反應(yīng)過(guò)程中Ni的高溫?zé)Y(jié),有效地提高了催化劑的活性和抗積碳性能。
[Abstract]:Hydrogen is a kind of green energy with high energy density and water after combustion. It not only can not pollute the environment, but also can replace fossil fuels to solve the problem of energy crisis. Therefore, hydrogen will play an important role in the 21 st century energy stage. At present, steam reforming of methane is the most effective and feasible method for hydrogen production, and has been widely used in methane reforming because of its low price, rich reserves and high activity. But this kind of catalyst is easy to be sintered at high temperature, which leads to the deactivation of the catalyst. Therefore, in order to reduce the cost of hydrogen production and promote the promotion of hydrogen as a green energy, it is necessary to develop catalysts with higher sintering resistance and carbon deposition resistance. The main results are as follows: firstly, a series of Ni-Co- / 緯 -Al _ 2O _ 3 bimetallic catalysts with different Co contents were prepared by co-impregnation method, in which the mass percentage of Ni was 12%, which was used for hydrogen production by steam reforming of methane. The results showed that the low temperature activity of Ni / Al _ 2O _ 3 catalyst decreased slightly with the addition of Co, but the carbonization resistance and reaction stability of Ni / Al _ 2O _ 3 catalyst were improved. The results of XPS and TEM showed that there was a strong interaction between Ni and Co. The results of XRD and HAADF-STEM mapping showed that Ni-Co alloy was formed between Ni and Co. The formation of the alloy can effectively cover some active Ni centers with low coordination position, reduce the activation ability of the catalyst to C-H bond, and inhibit the formation of C-C bond, thus effectively restrain the carbon deposition in the reaction process of the catalyst. Secondly, mesoporous Al-SBA-15 and spherical dendritic KCC-1 support were synthesized, and 7Ni- / Al-SBA-15 and Ni- / KCC-1 catalysts were prepared by impregnation method using deionized water and ethylene glycol as solvents. The results show that the catalysts prepared by using ethylene glycol as solvent and the mesoporous carriers with different morphology have high activity, stability, and excellent resistance to carbon deposition. XRD and TEM results show that the catalysts have excellent resistance to carbon deposition. The particle size of the active component of Ni on these catalysts can be limited to 5 nm by the pore channel, which can inhibit the sintering of Ni at high temperature during the reaction, and effectively improve the activity and the resistance to carbon deposition of the catalyst.
【學(xué)位授予單位】：南昌大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：O643.36;TQ116.2

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本文編號(hào)：2091643