Yu Shitao, Cao Xincheng, Liu Shiwei, Li Lu, Wu Qiong
College of Chemical Engineering, Qingdao University of Science and Technology Qingdao 266042 China
Department of Chemical & Biomolecular Engineering, University of Tennessee Knoxville 419 Dougherty Engineering Bldg. Knoxville Tennessee 37996 USA.
RSC Adv. 2018 Jul 10;8(44):24857-24865. doi: 10.1039/c8ra03806f. eCollection 2018 Jul 9.
This study presents the utilization of a binary catalyst composed of metal-loaded modified SBA-15 (M/SBA-15) and phosphotungstic acid (HPWO) for ethylene glycol (EG) production from direct catalytic conversion of cellulose. M/SBA-15 (M = Ru, Au, Pd, Pt, Rh and Ni) catalysts were prepared using the impregnation method and characterized by means of XRD, N physisorption, TEM and H-temperature-programmed reduction (H-TPR) techniques. Their catalytic performance was then studied in detail on the basis of cellulose conversion and the selectivity of polyols and EG. The results showed that the mesoporous structure of the SBA-15 sample was well maintained after the metal-loaded modification, and almost all of the selected catalysts gave about 100% conversion of cellulose. However, the selectivity for EG was greatly different. Among the various binary catalysts, the combination of Rh/SBA-15 and HPWO gave the best selectivity to EG (55.5%), whereas the worst selectivity of EG (11%) was obtained over the Au/SBA-15 and HPWO system under identical conditions. In addition to phosphotungstic acid, other W compounds were also studied in combination with the Ru/SBA-15 catalyst. The results showed that the EG selectivity depended on the W compounds as follows: HSiWO < HWO < HPWO. Therefore, the binary catalyst of Rh/SBA-15 and HPWO showed the greatest potential for EG production from direct catalytic conversion of cellulose.
本研究介绍了一种由负载金属的改性SBA - 15(M/SBA - 15)和磷钨酸(HPWO)组成的二元催化剂用于纤维素直接催化转化制备乙二醇(EG)的应用。采用浸渍法制备了M/SBA - 15(M = Ru、Au、Pd、Pt、Rh和Ni)催化剂,并通过XRD、N物理吸附、TEM和H程序升温还原(H - TPR)技术对其进行了表征。然后基于纤维素转化率以及多元醇和EG的选择性详细研究了它们的催化性能。结果表明,负载金属改性后SBA - 15样品的介孔结构得到了良好保持,并且几乎所有选定的催化剂都能使纤维素转化率达到约100%。然而,对EG的选择性差异很大。在各种二元催化剂中,Rh/SBA - 15和HPWO的组合对EG的选择性最佳(55.5%),而在相同条件下,Au/SBA - 15和HPWO体系对EG的选择性最差(11%)。除了磷钨酸外,还研究了其他W化合物与Ru/SBA - 15催化剂的组合。结果表明,EG选择性取决于W化合物,顺序如下:HSiWO < HWO < HPWO。因此,Rh/SBA - 15和HPWO的二元催化剂在纤维素直接催化转化制备EG方面显示出最大潜力。