【摘要】：環(huán)保法規(guī)的日益嚴(yán)格使清潔汽油成為必然,高辛烷值是清潔汽油的質(zhì)量要求,添加抗爆劑是提高汽油辛烷值最簡單、有效的方法,苯胺類烷基化衍生物是高效、低污染型汽油抗爆劑,銅基催化劑穩(wěn)定性差是制約該產(chǎn)品工業(yè)化生產(chǎn)的主要因素。本論文通過XRD、BET、H2-TPR、TG-DTG等技術(shù)手段對新鮮、失活催化劑進(jìn)行了表征,分析了催化劑的失活原因;探討了組成、沉淀溫度、沉淀pH、焙燒溫度、助劑、使用條件等對催化劑穩(wěn)定性的影響。結(jié)果表明,銅基催化劑連續(xù)運行400h后,轉(zhuǎn)化率由67.98%降至57.55%,下降了15.34%,銅聚集、燒結(jié)、積炭和中毒導(dǎo)致催化劑失活,中毒為主要失活原因。調(diào)節(jié)制備條件、添加助劑、優(yōu)化使用條件可改善銅基催化劑的穩(wěn)定性,鋁含量為10%(w)、銅鋅比為1:1(mol)、沉淀溫度為75℃、沉淀pH為8、焙燒溫度為400℃時,制得的催化劑活性組分銅分散良好、穩(wěn)定性提高,運行400h后轉(zhuǎn)化率由69.16%降至60.22%,下降了12.93%;Ce助劑的添加不僅提高了銅的分散性,也增強(qiáng)了催化劑的抗硫氯中毒性能,催化劑的穩(wěn)定性得到進(jìn)一步提高,在Ce含量為6%(w),催化劑穩(wěn)定性提高最為明顯,400h后轉(zhuǎn)化率由72.63%降至65.58%,降低了9.74%;在溫度200℃、醇胺比2:1(mol)、空速(WHSV)0.6h-1的條件下反應(yīng),催化劑在運行400h時后轉(zhuǎn)化率由73.74%降低到67.36%,下降了8.65%。銅基催化劑的活性、穩(wěn)定性均得到提高。
[Abstract]:The increasingly strict environmental laws and regulations make clean gasoline inevitable, high octane number is the quality requirement of clean gasoline, adding antiknock agent is the simplest and most effective method to improve gasoline octane number, aniline alkylation derivative is efficient, Low-pollution gasoline antiknock agent and poor stability of copper-based catalyst are the main factors restricting the industrial production of this product. In this paper, the fresh and deactivated catalysts were characterized by XRDX BETH2-TPR-TG-DTG, the reasons of deactivation of the catalysts were analyzed, and the effects of composition, precipitation temperature, pH, calcination temperature, auxiliaries and application conditions on the stability of the catalysts were discussed. The results showed that the conversion rate of Cu-based catalyst decreased from 67.98% to 57.55% after 400 h continuous operation, and decreased 15.34%. Copper aggregation, sintering, carbon deposition and poisoning resulted in deactivation of catalyst, and poisoning was the main cause of deactivation. The stability of copper-based catalysts can be improved by adjusting the preparation conditions, adding additives and optimizing the application conditions. When the Al content is 10% (w), the copper-zinc ratio is 1:1, the (mol), precipitation temperature is 75 鈩，

本文編號：2131278