Wei Zuojun, Lou Jiongtao, Su Chuanmin, Guo Dechao, Liu Yingxin, Deng Shuguang
Key Laboratory of Biomass Chemical Engineering of the Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, 38 Zheda Road, Xihu District, Hangzhou, 310027, P.R. China.
Research and Development Base of Catalytic Hydrogenation, College of Pharmaceutical Science, Zhejiang University of Technology, 18 Chaowang Road, Xiacheng District, Hangzhou, 310014, P.R. China.
ChemSusChem. 2017 Apr 22;10(8):1720-1732. doi: 10.1002/cssc.201601769. Epub 2017 Mar 22.
To achieve a higher activity and reusability of a Ru-based catalyst, Ru nanoparticles were embedded in N-doped mesoporous carbon through a hard-template method. The catalyst showed excellent catalytic performance (314 h turnover frequency) and recyclability (reusable five times with 3 % activity loss) for the hydrogenolysis of levulinic acid to γ-valerolactone. Compared with the mesoporous carbon without N-doping and conventional activated carbon, the introduction of N-dopant effectively improved the dispersion of Ru nanoparticles, decreased the average size of Ru nanoparticles to as small as 1.32 nm, and improved the adsorption of levulinic acid, which contributed to the increase in the activity of the catalyst. Additionally, the embedding method increased the interaction between Ru nanoparticles and carbon support in contrast with the conventional impregnation method, thus preventing the Ru nanoparticles from migration, aggregation, and leaching from the carbon surface and therefore increasing the reusability of the catalyst.
为了实现钌基催化剂更高的活性和可重复使用性,通过硬模板法将钌纳米颗粒嵌入氮掺杂的介孔碳中。该催化剂在将乙酰丙酸氢解为γ-戊内酯的反应中表现出优异的催化性能(周转频率为314 h)和可回收性(可重复使用五次,活性损失3%)。与未掺杂氮的介孔碳和传统活性炭相比,氮掺杂剂的引入有效地改善了钌纳米颗粒的分散性,将钌纳米颗粒的平均尺寸减小至1.32 nm,并提高了乙酰丙酸的吸附能力,这有助于提高催化剂的活性。此外,与传统浸渍法相比,嵌入法增加了钌纳米颗粒与碳载体之间的相互作用,从而防止钌纳米颗粒从碳表面迁移、聚集和浸出,因此提高了催化剂的可重复使用性。