丙炔對(duì)Pt系催化劑上對(duì)丙烷脫氫反應(yīng)的影響
本文選題:丙烷脫氫 + 丙炔; 參考:《華東理工大學(xué)》2017年碩士論文
【摘要】:丙烷脫氫正日益成為丙烯生產(chǎn)的重要工藝,但現(xiàn)有工藝仍存在催化劑結(jié)焦失活等問題。結(jié)焦組成和機(jī)理研究將為這一問題的解決提供重要支持。丙炔是丙烷脫氫反應(yīng)中的重要中間物種,是裂解副反應(yīng)的起始物質(zhì),對(duì)結(jié)焦反應(yīng)可能也有重要影響。本研究通過將丙炔引入丙烷脫氫體系,提高脫氫過程的副反應(yīng)程度,結(jié)合熱解氣質(zhì)聯(lián)用、拉曼、紅外、元素分析、熱重分析表征結(jié)焦的性質(zhì),探索丙烷脫氫過程結(jié)焦反應(yīng)路徑。研究結(jié)果表明Pt系催化劑上丙烷脫氫反應(yīng)的結(jié)焦可分為三類:類石墨物質(zhì),多環(huán)芳烴和碳原子數(shù)連續(xù)分布的長(zhǎng)直鏈烷烴;推出了較為完整的丙烷脫氫反應(yīng)結(jié)焦路徑,發(fā)現(xiàn)丙炔對(duì)丙烷脫氫結(jié)焦反應(yīng)路徑具有重要影響,可以直接聚合環(huán)化生成多環(huán)芳烴,并進(jìn)一步脫氫生成類石墨化物質(zhì);丙炔的加入會(huì)降低Pt系催化劑上丙烷脫氫反應(yīng)的選擇性,即除了丙炔自身的結(jié)焦反應(yīng)外,還可能誘發(fā)丙烯參與結(jié)焦反應(yīng)中。因此,抑制丙烷脫氫過程的深度脫氫反應(yīng),降低催化劑表面丙炔濃度,是抑制丙烷脫氫過程結(jié)焦的有效方法。
[Abstract]:Propane dehydrogenation is increasingly becoming an important process for propylene production, but the existing processes still exist problems such as deactivation of catalyst coking. The study of coking composition and mechanism will provide important support for solving this problem. Propargyl is an important intermediate species in the dehydrogenation of propane, which is the starting material of the pyrolysis side reaction and may also have an important influence on the coking reaction. In this study, propargyl was introduced into propane dehydrogenation system to improve the side reaction degree of dehydrogenation process, combined with pyrolysis, Raman, infrared, elemental analysis, thermogravimetric analysis to characterize the properties of coking, and to explore the coking reaction path in the process of propane dehydrogenation. The results show that the coking of propane dehydrogenation over Pt catalyst can be divided into three categories: graphite-like substances, polycyclic aromatic hydrocarbons and long-chain alkanes with continuous distribution of carbon atoms, and a complete coking path for dehydrogenation of propane is derived. It is found that propargene has an important influence on the reaction path of dehydrogenation of propane and can be directly polymerized to form polycyclic aromatic hydrocarbons (PAHs) and further dehydrogenated to form graphitized substances, and that the addition of propargene reduces the selectivity of dehydrogenation of propane over Pt catalysts. Besides the coking reaction of propyne itself, propene may also be involved in the coking reaction. Therefore, it is an effective method to restrain the coking of propane dehydrogenation by inhibiting the deep dehydrogenation of propane and reducing the concentration of propane on the catalyst surface.
【學(xué)位授予單位】:華東理工大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類號(hào)】:TQ221.212;O643.36
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