本文選題：生物油 + 苯酚��； 參考：《西安石油大學(xué)》2017年碩士論文

【摘要】：以NiCl2、Cu(NO3)2、Ce(NO3)3為原料,KBH4為還原劑,采用浸漬法和化學(xué)還原法制備了負(fù)載型和非負(fù)載型Ni-Cu-Ce-B催化劑。以生物油中主要的含氧模型化合物苯酚加氫制備環(huán)己酮為反應(yīng)體系,利用固定床反應(yīng)器催化劑評(píng)價(jià)裝置,設(shè)計(jì)了三水平三因素正交實(shí)驗(yàn),考察了銅鎳比、鈰鎳比、負(fù)載量對(duì)催化劑活性和選擇性的影響,確定出最佳的催化劑制備條件。通過(guò)設(shè)計(jì)三水平五因素正交實(shí)驗(yàn),考察了反應(yīng)溫度、反應(yīng)壓力、液時(shí)空速、氫氣/苯酚體積比對(duì)反應(yīng)活性和選擇性的影響,確定出最佳的反應(yīng)條件。最后,分別考察了催化劑重復(fù)使用次數(shù)、儲(chǔ)存時(shí)間、助劑、載體對(duì)催化劑活性和選擇性的影響,并研究了助劑Cu、Ce在Ni-B/γ-Al2O3催化劑表面的作用機(jī)理。實(shí)驗(yàn)結(jié)果表明,最佳的催化劑制備條件為:銅鎳物質(zhì)的量比0.3,鈰鎳物質(zhì)的量比0.2,負(fù)載量30%。最佳的反應(yīng)條件為:反應(yīng)溫度150℃、反應(yīng)壓力1.0 MPa、反應(yīng)時(shí)間1.5 h、液時(shí)空速2.0 h-1、氫氣/苯酚體積比50/1。在最佳的催化劑制備和反應(yīng)條件下,催化劑的活性為47.39%,催化劑選擇性可達(dá)29.37%。所制備的Ni-Cu-Ce-B為非晶態(tài)納米級(jí)催化劑,活性組分分散良好。加入助劑Cu和Ce后,Ni-B/γ-Al2O3催化劑的熱穩(wěn)定性加強(qiáng),比表面積增大,活性和選擇性有所提高。催化劑儲(chǔ)存一段時(shí)間后仍保持了較好的活性和選擇性。Cu向Ni的電子轉(zhuǎn)移效應(yīng)和Ce對(duì)于催化劑堿性的提高都有利于增大催化劑的選擇性。
[Abstract]:Supported and unsupported Ni-Cu-Ce-B catalysts were prepared by impregnation method and chemical reduction method using NiCl2Cu CuNO 3H 3 as raw material KBH4 as reducing agent. Cyclohexanone was prepared by hydrogenation of phenol, one of the main oxygen-containing model compounds in bio-oil, as a reaction system. The three-level and three-factor orthogonal experiment was designed by using a fixed-bed reactor catalyst evaluation apparatus. The copper-nickel ratio and cerium / nickel ratio were investigated. The effect of loading amount on the activity and selectivity of the catalyst was studied, and the optimum preparation conditions were determined. The effects of reaction temperature, reaction pressure, liquid space-time velocity and the volume ratio of hydrogen to phenol on the activity and selectivity of the reaction were investigated by designing a three-level and five-factor orthogonal experiment, and the optimum reaction conditions were determined. Finally, the effects of reusing times, storage time, auxiliaries and supports on the activity and selectivity of Ni-B/ 緯 -Al 2O 3 catalyst were investigated, and the mechanism of the effect of CuCe on the surface of Ni-B/ 緯 -Al 2O 3 catalyst was studied. The experimental results show that the optimum preparation conditions are as follows: the ratio of copper to nickel is 0.3, the ratio of cerium to nickel is 0.2, and the loading amount is 30. The optimum reaction conditions are as follows: reaction temperature 150 鈩，

本文編號(hào)：1810265