多孔二氧化鈦薄膜的制備及其負(fù)載鎳基甲烷化催化劑的性能研究
發(fā)布時間:2018-03-05 03:32
本文選題:多孔 切入點:二氧化鈦薄膜 出處:《太原理工大學(xué)》2017年碩士論文 論文類型:學(xué)位論文
【摘要】:微反應(yīng)器通道狹小,傳統(tǒng)催化劑在其中易團聚、堵塞。因此,將催化劑以薄膜形式負(fù)載并進行催化反應(yīng)是解決該問題的有效方法。為了研究膜狀催化劑的催化性能,本文選用制備方法較為成熟的多孔二氧化鈦薄膜負(fù)載在鋁絲基體表面,并使用浸漬法負(fù)載活性組分Ni,進行較為環(huán)保的CO甲烷化催化反應(yīng)。其中分別研究了模板劑用量、陳化時間、熱處理溫度等制備條件對多孔二氧化鈦薄膜的影響以及以該薄膜為催化劑載體制備的Ni基甲烷化膜催化劑的催化活性和穩(wěn)定性研究。主要研究結(jié)果如下:(1)采用包含溶劑揮發(fā)誘導(dǎo)自組裝的溶膠凝膠法與浸漬提拉鍍膜技術(shù),以嵌段共聚物F127為模板劑,在預(yù)處理的鋁絲基體表面制備出了多孔二氧化鈦薄膜。研究結(jié)果表明,在一定的溶膠配比(15mL乙醇、1mL去離子水、1mL鹽酸、5mL鈦酸丁酯和0.2mL乙酰丙酮)中,當(dāng)F127的用量為1.0g、陳化時間為24h、熱處理溫度為400℃時制備的多孔二氧化鈦薄膜具有均勻的多孔結(jié)構(gòu)和最佳的結(jié)構(gòu)特性,比表面積和孔容可分別達(dá)到127 m2·g-1和0.2139 cm3·g-1。(2)采用嵌段共聚物F127與P123為混合模板劑制備多孔二氧化鈦薄膜可以優(yōu)化薄膜的孔結(jié)構(gòu)、增大比表面積和孔容。其中,當(dāng)F127與P123用量為1.0g,質(zhì)量比為3:1時,制備的二氧化鈦薄膜具有更高的比表面積和孔容,可分別達(dá)到154m2·g-1和0.3031cm3·g-1。(3)通過該方法制備的二氧化鈦薄膜在300℃、400℃、500℃熱處理溫度下均呈現(xiàn)出銳鈦礦相,且模板劑的種類對其晶相不產(chǎn)生影響;在該溶膠凝膠體系中,模板劑的分解溫度約為312℃。(4)以最優(yōu)配比的混合模板劑制備的多孔二氧化鈦薄膜作為催化劑載體,使用浸漬法負(fù)載活性組分Ni,形成Ni/TiO2甲烷化膜催化劑。在質(zhì)量空速為3000 mL·g-1·h-1的條件下對催化劑的催化活性及其穩(wěn)定性進行評價。研究結(jié)果表明:多孔二氧化鈦薄膜表面成功負(fù)載活性組分Ni并制備了Ni/TiO2甲烷化膜催化劑,且還原前活性組分主要以NiO形式均勻負(fù)載在多孔薄膜表面;通過H2-TPR表征可以發(fā)現(xiàn)NiO能夠與TiO2載體產(chǎn)生了強烈的相互作用,并形成NiTiO3;在反應(yīng)溫度超過400℃條件下,CO的轉(zhuǎn)化率高于99%且其對CH4的選擇性接近80%,并且在長達(dá)60h的穩(wěn)定性評價中也具有良好的催化穩(wěn)定性。
[Abstract]:The channel of microreactor is narrow and the traditional catalyst is easy to agglomerate and clog in it. Therefore, it is an effective method to solve this problem by loading the catalyst in the form of film and performing catalytic reaction. In this paper, porous titanium dioxide thin films with mature preparation method were used to support aluminum wire substrate, and the active component Ni was loaded by impregnation method to carry out the environmentally friendly methanation of CO. The amount of template was studied. Aging time, The effect of preparation conditions such as heat treatment temperature on porous titanium dioxide film and the catalytic activity and stability of Ni based methanation film prepared with the film as catalyst carrier were studied. The main results are as follows: 1). Sol-gel method with solvent volatilization induced self-assembly and dipping Czochralski coating, Porous titanium dioxide films were prepared on the surface of pretreated aluminum wires with block copolymer F127 as template. The results showed that in a certain ratio of 15 mL ethanol to 1 mL deionized water, 1 mL butyl titanate hydrochloride and 0.2 mL acetylacetone were prepared. When the dosage of F127 is 1.0 g, the aging time is 24 h and the heat treatment temperature is 400 鈩,
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