本文選題：合成氣 + 鈷改性��； 參考：《華東理工大學(xué)》2017年碩士論文

【摘要】：乙醇作為一種重要的基礎(chǔ)化工原料,在化工及其他領(lǐng)域都有著廣泛的用途。作為煤化工的一部分,合成氣化工的發(fā)展對(duì)于煤炭資源的潔凈應(yīng)用意義重大。采用共沉淀、浸漬法及兩者相結(jié)合的方法制備了催化劑,研究了在改性甲醇合成催化劑和改性費(fèi)托合成催化劑上CO加氫制混合醇的催化活性。通過低溫N2吸附-脫附、X射線衍射(XRD)、CO程序升溫脫附(CO-TPD)、程序升溫還原(H2-TPR)和X射線光電子能譜分析(XPS)等手段對(duì)催化劑進(jìn)行表征。通過篩選,確定了以Cu為活性組分的改性低溫甲醇合成催化劑體系。載體考察結(jié)果表明,堿性載體MgO較Al2O3、ZrO_2、SiO_2更有利于乙醇的合成,適宜的Cu/Mg摩爾比為1。對(duì)于Cu/MgO催化劑,較其他金屬助劑而言,Mn具有更強(qiáng)的鏈增長(zhǎng)能力以及C_(2+)醇收率。表征結(jié)果顯示,Mn的加入增大了 Cu/MgO催化劑的比表面積,使Cu、Mg物種更加分散,為催化反應(yīng)提供了更多的活性位,同時(shí)也增加了催化劑表面堿性位數(shù)量并增強(qiáng)了其強(qiáng)度。在Mn/Cu比為0.3時(shí),總醇中C2H5OH/C1OH由0.08增至0.31,C2H5OH 時(shí)空收率由 2.69 g(kgcat·h)-1 增至 5.65 g(kgcat·h)-1。Mn/Cu/MgO催化劑上C_(2+)OH合成能力有限,Co的加入形成Co2Mg、MnCo2O4相,有利于Cu、Mn及Mg物種的分散,為C_(2+)OH的生成提供了更多活性位。適量Co的加入有助于提高催化劑對(duì)總醇中C_(2+)OH的選擇性。對(duì)于Co0.3/Mn/Cu/MgO催化劑,在260℃,3.0MPa,2000mL(gcat·h)-1,V(H2)/V(CO)=2.0 的條件下,C_(2+)OH/C1OH 比值由未加Co時(shí)的0.31增至3.12,C_(2+)OH的時(shí)空收率則由15.83 g·(kgcat·h)-1增至50.32 g·(Kgcat·h)-1。討論了 Co-Cu基催化劑上混合醇的合成機(jī)理,該過程中Co的插碳效應(yīng)對(duì)混合醇的選擇性起著重要作用,但同時(shí)也提高了烴類產(chǎn)物的選擇性。
[Abstract]:As an important basic chemical raw material, ethanol is widely used in chemical and other fields. As a part of coal chemical industry, the development of synthetic gas chemical industry is of great significance for the clean application of coal resources. The catalyst is prepared by means of co precipitation, impregnation and the combination of the two methods, and the synthesis of modified methanol is studied. The catalytic activity of mixed alcohols from CO hydrogenation on the catalyst and modified Fisher synthesis catalyst was characterized by low temperature N2 adsorption desorption, X ray diffraction (XRD), CO programmed temperature desorption (CO-TPD), temperature programmed reduction (H2-TPR) and X ray photoelectron spectroscopy (XPS). The modification of Cu was selected to determine the modification of active components by Cu. The results show that the basic carrier MgO is more beneficial to the synthesis of ethanol than that of Al2O3, ZrO_2 and SiO_2. The suitable Cu/Mg molar ratio is 1. for Cu/MgO catalyst and Mn has stronger chain growth ability and C_ (2+) alcohol yield than the other metal additives. The characterization results show that Mn addition increases Cu/Mg. The specific surface area of the O catalyst makes the Cu, Mg species more dispersed, provides more active sites for the catalytic reaction, and increases the surface alkalinity of the catalyst and strengthens its strength. At the Mn/Cu ratio of 0.3, the C2H5OH/C1OH in total alcohol increases from 0.08 to 0.31, and the time and space yield of C2H5OH is increased from 2.69 g (kgcat h) -1 to 5.65 g (kgcat. The synthesis ability of C_ (2+) OH on MgO catalyst is limited, and Co is added to form Co2Mg, MnCo2O4 phase, which is beneficial to the dispersion of Cu, Mn and Mg species, which provides more active sites for the production of C_ 2+. 2) under the condition of /V (CO) =2.0, the ratio of C_ (2+) OH/C1OH increased from 0.31 without Co to 3.12, and the time and space yield of C_ (2+) OH increased from 15.83 g (kgcat.) to 50.32. The selectivity of hydrocarbon products is higher.

【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)】：TQ223.122;TQ426

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本文編號(hào)：1804191