含Re復(fù)合分子篩催化劑的制備及其在汽柴油加氫精制中的應(yīng)用
發(fā)布時(shí)間:2018-02-03 02:30
本文關(guān)鍵詞: 含Re催化劑 復(fù)合分子篩 汽柴油 加氫精制 加氫脫芳 出處:《遼寧大學(xué)》2016年碩士論文 論文類型:學(xué)位論文
【摘要】:最近幾年,隨著全球變暖趨勢(shì)的日益嚴(yán)重,越來越多的人們開始關(guān)注如何制造出一些對(duì)環(huán)境更為友好的燃料。汽柴油作為當(dāng)今世界最重要的化石燃料之一,因此,如何更有效的降低其中含有的對(duì)環(huán)境有毒有害的物質(zhì)的含量越發(fā)顯得迫在眉睫。本文通過對(duì)一系列的含有新型載體的負(fù)載型催化劑的合成,首先,與汽柴油的模擬物四氫化萘在自制的儀器上進(jìn)行了加氫精制脫芳反應(yīng),而后,再與汽柴油的模擬物四氫萘、噻吩、喹啉的混合物進(jìn)行了深度脫芳脫氮脫硫,深度探究了汽柴油深度加氫精制的條件。主要做了以下四方面的工作:首先,通過改變催化劑的載體與(或)活性組分的配比與(或)組成,合成了新型的負(fù)載型的復(fù)合分子篩載體催化劑Mo-Re-Co/TiO2-USY-MCM-41,考察了汽柴油脫芳模擬物四氫萘在溫度240-320℃、壓力1.5-3.5 MPa、空速1-5 h-1、氫油比300-700的條件下,四氫萘的轉(zhuǎn)換率最高可達(dá)到67.2%。其次,為了檢驗(yàn)該催化劑對(duì)汽柴油加氫脫芳脫氮脫硫的實(shí)際效果,本文利用混合模擬物進(jìn)行了深度加氫精制的反應(yīng)。在最佳載體上負(fù)載不同的活性組分后,利用正交實(shí)驗(yàn)法找出最佳工藝條件后,在溫度260℃、壓力2.5 MPa、空速5 h-1、氫油比500的條件下進(jìn)行加氫精制反應(yīng),噻吩的轉(zhuǎn)換率可達(dá)到90.1%,喹啉的轉(zhuǎn)換率為82.6%,四氫萘的轉(zhuǎn)換率最高為62.7%。然后,將已得到的兩種綜合效果最好的催化劑進(jìn)行復(fù)配結(jié)合,通過改變催化劑裝填順序的不同,進(jìn)一步探究了原料油混合模擬物中三種物質(zhì)的轉(zhuǎn)換率。最后,對(duì)合成的復(fù)合載體及催化劑通過XRD、N2吸附-脫附進(jìn)行了表征。其中,XRD表明復(fù)合載體中出現(xiàn)了新的物質(zhì)組分Na0.3 [Al6(Si,Al)8O20(OH)10]·4H2O、 H12[(AlO2)12(SiO2)36]、Ti3O5和Al2SiO5,復(fù)合載體的N2吸附-脫附表現(xiàn)出了很好的介孔結(jié)構(gòu);同時(shí),催化劑的活性金屬組分也成功的負(fù)載在了所合成的復(fù)合載體上,達(dá)到了預(yù)期所要的結(jié)果。
[Abstract]:In recent years, with the increasing trend of global warming, more and more people begin to pay attention to how to make some more environmentally friendly fuels. Gasoline and diesel as one of the most important fossil fuels in the world today. Therefore, how to reduce the content of toxic and harmful substances is more and more urgent. In this paper, the synthesis of a series of supported catalysts containing new support, first of all. The hydrogenation of naphthalene from gasoline and diesel oil was carried out in a self-made instrument, and then the mixture of tetralin, thiophene and quinoline was used for deep denitrogenation and desulphurization with the mixture of naphthalene, thiophene and quinoline, which was the mimic of gasoline and diesel oil. The conditions of deep hydrogenation of gasoline and diesel oil were studied. The following four aspects were done: firstly, by changing the ratio and / or composition of catalyst carrier and / or active component. A novel supported composite molecular sieve support catalyst Mo-Re-Co/TiO2-USY-MCM-41 was synthesized. The dearomatization analogue tetralin was investigated under the conditions of temperature 240-320 鈩,
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