【摘要】：質(zhì)子交換膜燃料電池（PEMFC）穩(wěn)定發(fā)電要求富氫氣體中CO含量低于10ppm，然而重整-變換反應(yīng)后的富氫氣體中含有約1%CO和18%CO2。CO選擇甲烷化是除去富氫氣體中CO的一種有效方法，其能量效率高、過程控制簡單，，生成物甲烷和水均對(duì)電極以及環(huán)境無毒害作用，因此近年來逐漸引起關(guān)注。 負(fù)載鎳基催化劑是CO選擇甲烷化反應(yīng)的有效催化劑，而且比貴金屬價(jià)格低廉。本工作利用NiO與MgO易形成固溶體的特點(diǎn)，首先制備了NiO-MgO固溶體，經(jīng)還原處理后得到Ni/Mg1-xNixO催化劑，然后對(duì)其進(jìn)行CO選擇甲烷化反應(yīng)活性的研究。主要的研究內(nèi)容和結(jié)果歸納如下： 1、分別采用氫氮混合氣（70%H2、30%N2）和反應(yīng)混合氣（70%H2、18CO2、11%N2、1%CO）作為還原氣體，對(duì)氧化態(tài)樣品進(jìn)行還原處理，然后測定其甲烷化反應(yīng)活性。結(jié)果表明，采用氫氮混合氣還原得到的催化劑催化活性遠(yuǎn)高于采用反應(yīng)氣還原得到的催化劑催化活性。 2、采用不同的還原溫度（500°C～800°C）對(duì)氧化態(tài)樣品進(jìn)行還原處理，然后測定其甲烷化反應(yīng)活性。結(jié)果表明，還原溫度越高，CO選擇甲烷化活性越高，800°C下還原得到的催化劑活性最高。 3、采用不同H2濃度（50%～100%）的氫氮混合氣，對(duì)氧化態(tài)樣品進(jìn)行還原處理，然后測定其甲烷化反應(yīng)活性。結(jié)果表明，當(dāng)H2濃度為85%時(shí)，催化活性最佳；當(dāng)H2濃度為50%時(shí)，催化活性明顯降低。 4、對(duì)不同Ni/Mg投料比（10%～40%）的氧化態(tài)樣品，還原后測定其甲烷化反應(yīng)活性。結(jié)果表明，Ni/Mg投料比為20%～30%的催化劑對(duì)CO選擇甲烷化反應(yīng)催化效果最好。 5、對(duì)不同溫度（400°C～800°C）焙燒得到的氧化態(tài)樣品，還原后測定其甲烷化反應(yīng)活性。結(jié)果表明，隨著焙燒溫度升高，催化活性降低，特別是800°C焙燒的樣品活性降低很明顯。
[Abstract]:The stable generation of proton exchange membrane fuel cell (PEMFC) requires that the content of CO in the hydrogen-rich gas is less than 10 ppm. However, the methanation of about 1%CO and 18%CO2.CO in the hydrogen-rich gas after reforming and transformation reaction is an effective method to remove CO from the hydrogen-rich gas. Because of its high energy efficiency, simple process control and no toxic effect of methane and water to the electrode and environment, it has attracted more and more attention in recent years. The supported nickel-based catalyst is an effective catalyst for the methanation of CO and is cheaper than the precious metal. In this work, NiO and MgO are easy to form solid solution. Firstly, NiO-MgO solid solution was prepared. After reduction, Ni/Mg1-xNixO catalyst was obtained, and then the methanation activity of CO was studied. The main research contents and results are summarized as follows: 1. Hydrogen-nitrogen mixture (70H _ 2N _ 2) and reaction gas (n _ 2) (70 H _ 2O _ (18) CO _ (2) C _ (11) N _ (2) CO) were used as reducing gas to deoxidize the oxidized samples, and then their methanation activity was determined. The results showed that the catalytic activity of the catalysts obtained by hydrogen-nitrogen mixture reduction was much higher than that by reaction gas reduction. 2. The oxidized samples were treated with different reduction temperatures (500 擄C ~ 800 擄C). Then the methanation activity was determined. The results show that the higher the reduction temperature is, the higher the methanation activity of CO is, the higher the catalytic activity is at 800 擄C. 3. The hydrogen-nitrogen mixture with different H _ 2 concentration (50 ~ 100%) is used to deoxidize the oxidized samples. Then the methanation activity was determined. The results showed that the catalytic activity was the best when the H _ 2 concentration was 85 and the catalytic activity was significantly decreased when the H _ 2 concentration was 50. 4. The methanation activity of the oxidized samples with different Ni/Mg feed ratio (10 ~ 40%) was determined after reduction. The results show that the catalyst with 20% Ni / mg ratio is the best catalyst for the selective methanation of CO. 5. The methanation activity of oxidized samples calcined at different temperatures (400 擄C, 800 擄C) is determined after reduction. The results show that the catalytic activity decreases with the increase of calcination temperature, especially the activity of the sample calcined at 800 擄C.
【學(xué)位授予單位】：北京理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：O621.25;TM911.4

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