当前位置: X-MOL 学术Mol. Catal. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Highly efficient selective oxidation of 2-methylnaphthalene to vitamin K3 over mesoporous Al/Ti-SBA-15 catalysts: The effect of acid sites and textural property
Molecular Catalysis ( IF 3.9 ) Pub Date : 2020-08-20 , DOI: 10.1016/j.mcat.2020.111158
Yi Yu , Fanfan Li , Zhouxuan Zang , Li Xu , Guoji Liu

Catalytic oxidation of 2-methylnaphthalene to 2-methyl-1,4-naphthoquinone (vitamin K3) is a significant pathway to produce vitamin groups K. High pollution and low-productivity of the traditional method require a greener catalyst and process. In this work, Al/Ti-SBA-15 with different nSi/nAl and nSi/nTi ratios were hydrothermally prepared in mild acidic condition and tested in partial oxidation of 2-methylnaphthalene. Commercial zeolites NaY, β and ZSM-5 were applied to investigate the influence of mass transfer resistance and acidity on catalytic performance. Catalysts were characterized by XRD, N2 adsorption-desorption, TEM, NH3-TPD, FTIR and Py-FTIR. We have found that the 2-methylnaphthalene conversion and vitamin K3 selectivity depend strongly on the mesoporous structure as well as Brönsted acid concentration and strength. Irregular micropores and strong acidity will accelerate the cleavage of C = C in aromatic rings, leading to the production of phthalic anhydride. DFT calculation reveals that incorporation of aluminum in SBA-15 can reduce the energy gap, facilitating the electron transfer. And as a consequence of the substitution of Al in tetrahedral positions in SBA-15, Al-SBA-15 (10) gives the best result with 72% yield to vitamin K3. This catalyst markedly reduces the activation energy due to the modified activated center. Repeated experiments recommend that Al-SBA-15 is a steady and high-efficiency catalyst for the production of vitamin K3.



中文翻译:

介孔Al / Ti-SBA-15催化剂将2-甲基萘高效选择性氧化为维生素K 3:酸位和质构性质的影响

2-甲基萘催化氧化为2-甲基-1,4-萘醌(维生素K 3)是生产维生素K的重要途径。传统方法的高污染和低生产率要求绿色环保的催化剂和工艺。在这项工作中,在温和的酸性条件下水热制备具有不同n Si / n Al和n Si / n Ti比的Al / Ti-SBA-15,并测试了2-甲基萘的部分氧化。用商品沸石NaY,β和ZSM-5研究了传质阻力和酸度对催化性能的影响。用XRD,N 2吸附-解吸,TEM,NH 3 -TPD,FTIR和XRD对催化剂进行了表征。Py -FTIR。我们发现2-甲基萘的转化率和维生素K 3的选择性在很大程度上取决于介孔结构以及布朗斯台德酸的浓度和强度。不规则的微孔和强酸将加速C = C在芳环中的裂解,从而导致邻苯二甲酸酐的产生。DFT计算表明,在SBA-15中掺入铝可以减少能隙,从而促进电子转移。由于在SBA-15中四面体位置取代了Al,Al-SBA-15(10)可获得最佳结果,维生素K 3的收率为72%。由于修饰的活化中心,该催化剂显着降低了活化能。重复的实验建议Al-SBA-15是一种稳定高效的维生素K 3产生催化剂。

更新日期:2020-08-20
down
wechat
bug