【摘要】：煤制油的核心技術(shù)是MTO工藝,MTO工藝的關(guān)鍵問題是高效催化劑的合成。通過查閱文獻(xiàn)資料,本文確定了采用水熱法合成SAPO-34分子篩,主要研究采用不同比例四乙基氫氧化銨和三乙胺、四乙基氫氧化銨和嗎啡啉、三乙胺和嗎啡啉復(fù)合模板劑來合成SAPO-34分子篩,以及考察不同硅鋁比對(duì)混合模板劑合成SAPO-34分子篩的影響。通過XRD、SEM、FT-IR、BET、NH3-TPD表征手段來研究合成的SAPO-34分子篩的晶粒尺寸、結(jié)構(gòu)、酸性等。采用四乙基氫氧化銨和三乙胺(2:1)、四乙基氫氧化銨和嗎啡啉(2:1)、三乙胺和嗎啡啉(2:1)來合成不同硅鋁比SAPO-34分子篩,通過MTO反應(yīng)結(jié)果可知其催化壽命在120min-480min之間隨著硅鋁比的增加而降低,低碳烯烴選擇性隨著硅鋁比的增加也降低但是變化差異很小,低碳烯烴總體選擇性基本都在80%以上最高可達(dá)90%。復(fù)合模板劑合成SAPO-34分子篩比單一模板劑合成的SAPO-34分子篩有著更長(zhǎng)的催化壽命,其中四乙基氫氧化銨和三乙胺(2:1),四乙基氫氧化銨和嗎啡啉(2:1),三乙胺和嗎啡啉(1:1)合成SAPO-34-0.2分子篩的MTO催化效果最好壽命可達(dá)420min、480min、360min,低碳烯烴總選擇性可達(dá)86.6%、89.2%、89.5%。通過GC-MS分析失活后SAPO-34分子篩孔道積碳,主要成分是萘、菲、芘類有機(jī)物,這些大分子有機(jī)物堵塞孔道使低碳烯烴無法及時(shí)擴(kuò)散出去進(jìn)一步轉(zhuǎn)化為大分子有機(jī)物,同時(shí)覆蓋催化酸性位最終導(dǎo)致催化劑的失活。
[Abstract]:The key technology of kerosene to oil is MTO process, and the key problem of MTO process is the synthesis of high efficiency catalyst. In this paper, the hydrothermal synthesis of SAPO-34 molecular sieves has been determined by consulting the literature. The main research methods are tetraethyl ammonium hydroxide and triethylamine, tetraethyl ammonium hydroxide and morpholine, and the synthesis of tetraethyl ammonium hydroxide and triethylamine, tetraethyl ammonium hydroxide and morpholine are studied in this paper. The synthesis of SAPO-34 molecular sieves with triethylamine and morpholine composite templates and the effects of different Si-Al ratios on the synthesis of SAPO-34 molecular sieves were investigated. The crystal size, structure and acidity of synthesized SAPO-34 molecular sieves were studied by XRD,SEM,FT-IR,BET,NH3-TPD characterization. Tetraethyl ammonium hydroxide and triethylamine (2:1), tetraethyl ammonium hydroxide and morpholine (2:1), triethylamine and morpholine (2:1) were used to synthesize SAPO-34 molecular sieves with different Si / Al ratios, The results of MTO show that the catalytic life of 120min-480min decreases with the increase of Si-Al ratio, and the selectivity of low-carbon olefins decreases with the increase of Si-Al ratio, but the difference is very small. The overall selectivity of low-carbon olefins is above 80% and the highest is up to 90%. The synthesis of SAPO-34 molecular sieves by composite templates has a longer catalytic life than that of SAPO-34 molecular sieves synthesized by a single template, in which tetraethyl ammonium hydroxide and triethylamine (2:1), tetraethyl ammonium hydroxide and morpholine (2:1), The MTO catalytic activity of triethylamine and morpholine (1:1) for the synthesis of SAPO-34-0.2 molecular sieves can reach 420min, 480min, 360min, the total selectivity of low carbon olefins can reach 86.6%, 89.2%, 89.5%, and the total selectivity of low carbon olefins can reach 86.6%, 89.2% and 89.5% respectively. The carbon deposition in the pores of inactivated SAPO-34 molecular sieve was analyzed by GC-MS, and the main components were naphthalene, phenanthrene and pyrene. These macromolecular organic compounds blocked the pore channels and prevented the diffusion of low carbon olefins into macromolecular organics in time. At the same time, the catalyst was deactivated by covering the acid site of the catalyst.
【學(xué)位授予單位】：中國(guó)礦業(yè)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O643.36;TQ529

【參考文獻(xiàn)】

相關(guān)期刊論文 前10條

1 李明;;國(guó)內(nèi)外乙烯供需現(xiàn)狀和發(fā)展趨勢(shì)分析[J];中國(guó)氯堿;2015年02期

2 狄春雨;李莎;李曉峰;竇濤;;采用混合模板劑制備SAPO-34分子篩及其催化性能表征[J];石油學(xué)報(bào)(石油加工);2012年S1期

3 唐宏青;;關(guān)于我國(guó)煤化工發(fā)展的三種觀點(diǎn)[J];化工設(shè)計(jì)通訊;2012年01期

4 朱杰;崔宇;陳元君;周華群;王W，

本文編號(hào)：2470802