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| Preparation and application in the hydrogenation of dimethyl terephthalate of Ru@G-CS catalyst |
| Author Name | Affiliation | E-mail | | WANG Cai-Li | Key Laboratory of Biomass Chemical Engineering of Ministry of Education, Department of Chemistry, Zhejiang University, Hangzhou 310058, China | | | YE Bo-Yong | Key Laboratory of Biomass Chemical Engineering of Ministry of Education, Department of Chemistry, Zhejiang University, Hangzhou 310058, China | | | WANG Han | Zhejiang Hengyi Petrochemical Research Institute Co., Ltd., Hangzhou 311200, China | | | WANG Song-Lin | Zhejiang Hengyi Petrochemical Research Institute Co., Ltd., Hangzhou 311200, China | | | YANG Lei | Zhejiang Hengyi Petrochemical Research Institute Co., Ltd., Hangzhou 311200, China | | | HOU Zhao-Yin | Key Laboratory of Biomass Chemical Engineering of Ministry of Education, Department of Chemistry, Zhejiang University, Hangzhou 310058, China
Zhejiang Hengyi Petrochemical Research Institute Co., Ltd., Hangzhou 311200, China | zyhou@zju.edu.cn |
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| Abstract: A series of nitrogen-doped graphene-coated Ru-based catalysts (Ru@G-CS) were prepared using glucose, melamine, and RuCl3 as raw materials in a facile one-step pyrolysis method at 700℃ with a varied mass ratio of glucose/melamine in feed. The composition, structure, and surface morphology of these catalysts were characterized with powder X-ray diffraction, Raman spectroscopy, N2 adsorption-desorption, X-ray photoelectron spectroscopy, scanning electron microscope, and transmission electron microscope. Characterization results showed that nitrogen in the graphene skeleton can promote the dispersion of Ru, and there was also a strong interaction between nitrogen and loaded Ru. Ru@G-CS(1:4) catalyst (with the mass ratio of glucose/melamine in feed was 1:4) possesses the highest surface area (429 m2·g-1), biggest pore volume (0.45 cm3·g-1) and highly dispersed Ru particles (about 1 nm) that encapsulated in 1-2 layered graphene film. At the same time, the detected wRu0/wRu4 + (73.6/26.4), ID/IG (1.30) and I2D/IG (0.32) reached their maximum in Ru@G-CS(1:4). These catalysts were tested in dimethyl terephthalate (DMT) hydrogenation to 1,4-cyclohexane dimethyl dicarboxylate (DMCD) under mild conditions and compared with those traditional carriers (HZSM-5, Al2O3, MgO, ZnO) supported Ru catalysts. Ru@G-CS(1:4) exhibited high activity and stability at 160℃, 2.5 MPa H2, mDMT/mRu=833, the detected conversion of DMT reached 100% and the selectivity of DMCD remained higher than 98.5% within 4 h. The calculated turnover frequency of each Ru was 233.4 h-1. More importantly, Ru@G-CS(1:4) could maintain its performance at least in 10 cycles. It was concluded that the electron-structure synergistic effect might be the main reason for the excellent activity and stability of Ru@G-CS(1:4). |
| Keywords: dimethyl terephthalate dimethyl 1,4-cyclohexanedicarboxylate hydrogenation graphene Ru |
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| WANG Cai-Li,YE Bo-Yong,WANG Han,WANG Song-Lin,YANG Lei,HOU Zhao-Yin.Preparation and application in the hydrogenation of dimethyl terephthalate of Ru@G-CS catalyst[J].Chinese Journal of Inorganic Chemistry,2023,39(11):2091-2102. |
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