苯甲腈選擇性加氫制備苯甲胺的催化劑研究
發(fā)布時間:2018-02-24 23:06
本文關鍵詞: 苯甲腈 苯甲胺 催化加氫 固定床 穩(wěn)定性 出處:《上海師范大學》2016年碩士論文 論文類型:學位論文
【摘要】:苯甲胺又稱為芐胺,是一種重要的精細化工中間體和有機化工原料。隨著我國化工產業(yè)的不斷發(fā)展,苯甲胺的需求量也不斷增加。目前,國內生產的苯甲胺年產量低,主要依靠進口,苯甲胺的生產主要集中在德國、美國、日本等國家。國內的苯甲胺生產工藝落后,因此,開發(fā)高效的苯甲胺生產工藝將具有較好的市場前景。本論文在固定床反應條件下,研究了苯甲腈加氫制備苯甲胺的催化劑與反應工藝條件,開發(fā)了性能優(yōu)異的貴金屬催化劑,貴金屬含量相比于文獻大大降低,反應條件溫和,為苯甲睛加氫制備苯甲胺實現(xiàn)連續(xù)化工業(yè)生產提供了有益的理論基礎。本論文的主要研究內容與結果如下:1.篩選不同的催化劑配方,確定了由浸漬法制備的負載型Pd/γ-Al2O3催化劑是苯甲腈加氫制備苯甲胺反應的最優(yōu)催化劑。比較了活性金屬不同負載含量對反應性能的影響,優(yōu)化后活性金屬負載量為0.5 wt%,優(yōu)化了浸漬法的制備工藝條件。2.考察反應工藝條件對催化劑性能的影響,并對反應工藝條件進行了優(yōu)化,合適的反應工藝條件為:反應溫度70-90℃,反應壓1.5 MPa,氫腈比10-40,質量空速≤0.5 h-1。在該條件下,苯甲胺的收率最高可以達到88.8%。3.考察催化劑穩(wěn)定性,在優(yōu)化的反應工藝條件下,催化劑穩(wěn)定運行209 h。之后苯甲腈的轉化率降至97%以下,對失活催化劑進行了表征分析,失活催化劑不存在明顯的活性金屬組分流失,金屬Pd并未發(fā)生大量團聚。催化劑表面覆蓋了一些吸附物質,導致催化劑比表面積、孔容和孔徑均有所下降。覆蓋物是導致催化劑失活的主要原因。
[Abstract]:Benzylamine, also known as benzylamine, is an important fine chemical intermediate and organic chemical raw material. With the continuous development of chemical industry in China, the demand for benzylamine is also increasing. At present, the domestic production of benzyl amine is low. Mainly relying on imports, the production of benzomethylamine is mainly concentrated in Germany, the United States, Japan and other countries. In this paper, the catalyst and reaction conditions for the hydrogenation of benzonitrile to benzyl methylamine were studied, and the noble metal catalyst with excellent performance was developed. Compared with the literature, the content of precious metals is much lower, and the reaction conditions are mild. The main contents and results of this thesis are as follows: 1. Screening different catalyst formulations. The supported PD / 緯 -Al _ 2O _ 3 catalyst prepared by impregnation method was determined to be the best catalyst for the hydrogenation of benzonitrile to benzamide. The preparation conditions of the impregnation method were optimized. 2. The effect of reaction conditions on the performance of the catalyst was investigated, and the reaction conditions were optimized. The suitable reaction conditions were as follows: reaction temperature 70-90 鈩,
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