鑲嵌式釕炭催化劑的制備及芳環(huán)加氫性能
發(fā)布時(shí)間:2018-01-07 04:02
本文關(guān)鍵詞:鑲嵌式釕炭催化劑的制備及芳環(huán)加氫性能 出處:《浙江工業(yè)大學(xué)》2016年碩士論文 論文類型:學(xué)位論文
更多相關(guān)文章: 鑲嵌式催化劑 釕炭催化劑 芳環(huán)加氫 固相碾磨法
【摘要】:新型鑲嵌式釕炭催化劑具有載體與活性組分之間的相互作用力強(qiáng)、抗燒結(jié)、抗流失性好等特征,在加氫反應(yīng)中具有較好的活性及穩(wěn)定性。通過浸漬/模板法和固相研磨/模板法制備了新型鑲嵌式的介孔釕炭催化劑。用氮?dú)馕锢砦、CO化學(xué)吸附、TPR-MS、XRD、TEM、SEM等技術(shù)對(duì)催化劑進(jìn)行了表征,研究了其在甲苯、苯甲酸、對(duì)苯二甲酸二甲酯等芳環(huán)加氫反應(yīng)中的性能,取得了以下結(jié)果:1.制備了系列不同方法改性的活性炭負(fù)載的Ru/AC催化劑和浸漬模板法制備了鑲嵌式Ru-MC催化劑,考察了上述催化劑在甲苯、對(duì)苯二甲酸二甲酯及苯甲酸等不同取代基的芳環(huán)加氫反應(yīng)中的性能。在所有的芳環(huán)加氫反應(yīng)中,隨著活性炭表面含氧基團(tuán)的增加,Ru/AC催化活性增加;鑲嵌式Ru-MC催化劑的芳環(huán)加氫性能遠(yuǎn)高于負(fù)載型Ru/MC催化劑;對(duì)不同取代基的芳環(huán)加氫反應(yīng),底物的取代基位阻越大,芳環(huán)加氫越困難,催化劑的活性越低。2.用固相研磨模板法和浸漬模板法制備了鑲嵌式釕炭催化劑,和負(fù)載型的Ru/MC,Ru/AC催化劑的加氫性能做了對(duì)比。固相碾磨法模板法制備的Ru-MC-g和浸漬模板法制得Ru-MC的苯甲酸苯環(huán)加氫性能相當(dāng),但因前者制備的催化劑釕納米粒子的鑲嵌度稍高,表面暴露的釕原子比例較低,所以其TOF值最高,在120 ℃,和4.0 MPa氫氣壓力條件下,Ru-MC-g催化劑的TOF達(dá)到了2415 h~(-1),較負(fù)載型催化劑的活性提高了約6倍。3.利用固相研磨模板法,采用尿素作為氮源,制備了N摻雜的介孔炭材料,用其作載體制備了負(fù)載型Ru/MC-N催化劑。隨著制備過程中尿素添加量的增加,其載體中的N含量也增加,其負(fù)載催化劑的活性先增高后降低。
[Abstract]:The new type of inlaid ruthenium carbon catalyst has the characteristics of strong interaction between the support and active components, anti-sintering, good anti-loss, and so on. A new type of mesoporous ruthenium carbon catalyst was prepared by impregnation / template method and solid phase grinding / template method. The catalyst was characterized by TPR-MSXRDX Tem SEM and its performance in the hydrogenation of toluene, benzoic acid and dimethyl terephthalate was studied. The following results were obtained: 1. A series of modified activated carbon supported Ru/AC catalysts and impregnated Ru-MC catalysts were prepared. The above catalysts were investigated in toluene. The properties of aromatic ring hydrogenation of dimethyl terephthalate and benzoic acid were studied. The catalytic activity of Ru-r-AC increased with the increase of oxygen-containing groups on the surface of activated carbon. The hydrogenation performance of the embedded Ru-MC catalyst is much higher than that of the supported Ru/MC catalyst. For the hydrogenation of aromatic rings with different substituents, the larger the substituent resistance of the substrates is, the more difficult the hydrogenation of aromatic rings is, and the lower the activity of the catalysts is. 2. The inlaid ruthenium carbon catalysts are prepared by solid phase grinding template method and impregnation template method. And load type Ru/MC. The hydrogenation performance of Ru/AC catalyst was compared. The hydrogenation performance of Ru-MC-g prepared by solid phase milling method was comparable to that of Ru-MC prepared by impregnation template method. However, the TOF value of ruthenium nanoparticles prepared by the former was the highest at 120 鈩,
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