石墨烯負(fù)載銅、金催化乙酰丙酸和對硝基苯甲醛加氫的研究
發(fā)布時間:2018-05-23 17:22
本文選題:石墨烯 + 金負(fù)載石墨烯; 參考:《大連理工大學(xué)》2016年碩士論文
【摘要】:石墨烯是碳原子通過sp2雜化以六元環(huán)形式平鋪而成的二維蜂窩狀碳納米材料。由于石墨烯具有高比表面積,良好的電子傳導(dǎo)性和導(dǎo)熱性,其在催化領(lǐng)域的應(yīng)用得到越來越多重視。本文以晶化石墨為原料,采用改進(jìn)的Hummer法進(jìn)行氧化、剝離得到氧化石墨烯,還原后即得到石墨烯;將銅、金元素分別負(fù)載于石墨烯上,制備相應(yīng)的催化劑;對負(fù)載方法進(jìn)行探索;并將其應(yīng)用于不飽和化合物選擇性催化加氫反應(yīng)中。本文第一部分采用沉淀法制備Cu/rGO,以氧化石墨烯為前體,以氫氧化鈉為沉淀劑將銅負(fù)載于氧化石墨烯表面,利用過量的氫氧化鈉高溫回流對氧化石墨烯進(jìn)行一次還原,水熱還原法進(jìn)行二次還原。探索各種制備因素對催化劑活性的影響。將該催化劑應(yīng)用于乙酰丙酸催化加氫反應(yīng),在溫度為120℃,起始壓力2 MPa條件下,反應(yīng)2 h,產(chǎn)物γ-戊內(nèi)酯的選擇性達(dá)到100%。本文第二部分制備金石墨烯催化劑,將金溶膠與氧化石墨烯膠體混合后,在溫度為110℃,起始壓力3.5 MPa條件下進(jìn)行氫氣氣氛下水熱還原制備金石墨烯催化劑。探索各種制備因素對催化劑活性的影響。將還原好的催化劑進(jìn)行洗滌后,應(yīng)用于對硝基苯甲醛選擇性催化加氫反應(yīng)。在反應(yīng)溫度120℃,起始壓力2 MPa,底物濃度為0.15moL/L,反應(yīng)時間為2 h時,轉(zhuǎn)化率達(dá)到100%時,對硝基苯甲醛選擇性最高可以達(dá)到94.3%。
[Abstract]:Graphene is a two-dimensional honeycomb carbon nanomaterial composed of carbon atoms flattened in the form of six-member rings by sp2 hybridization. Because of its high specific surface area, good electronic conductivity and thermal conductivity, graphene has attracted more and more attention in the field of catalysis. In this paper, graphene oxide was obtained by the modified Hummer method, which was oxidized by crystalline graphite, and then the graphene was obtained after reduction, and the corresponding catalysts were prepared by loading copper and gold elements on graphene, respectively. The loading method was explored and applied to the selective catalytic hydrogenation of unsaturated compounds. In the first part of this paper, Cu / rGOA was prepared by precipitation method. With graphene oxide as precursor and sodium hydroxide as precipitant, copper was loaded on the surface of graphene oxide, and the graphene oxide was reduced by reflux of excess sodium hydroxide at high temperature. The secondary reduction was carried out by hydrothermal reduction. The effects of various preparation factors on the activity of the catalyst were explored. The catalyst was applied to the hydrogenation of levulinic acid. Under the conditions of 120 鈩,
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