文献类型：期刊文献

英文题名：Glycols Production from Sorbitol Hydrogenolysis Over Hydrothermally Stable Ni Catalysts and the Mechanistic Study

作者：Zhu, Xinyu[1]; Feng, Xindi[1]; Yao, Chang[1]; Sun, Weixiao[1]; Ma, Jianbo[2,3]; Zhong, Fuzeyu[1]; Zeng, Jianrong[2,3]; Ge, Xiaohu[1]; Chen, Wenyao[1]; Qian, Gang[1]; Duan, Xuezhi[1]; Cao, Yueqiang[1]; Liu, Zhen[1]; Zhou, Xinggui[1]; Zhang, Jing[1]

机构：[1] State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China; [2] Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201204, China; [3] Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201800, China

年份：2023

外文期刊名：SSRN

收录：EI(收录号：20230430574)

语种：英文

外文关键词：Catalyst activity - Catalyst selectivity - Condensation reactions - Density functional theory - Ethylene - Ethylene glycol - Hydrogenolysis - Hydrolysis - Ketones - Leaching - Nickel oxide

摘要：Hydrogenolysis of sorbitol can produce value-added glycols (ethylene glycol and 1,2-propanediol), which are widely used as antifreezes, coolants, and monomers for polyester fibers and resins. Although Ni based catalysts have advantages in low cost, high selectivity, and high activity, they are susceptible to sintering and leaching under hydrothermal conditions, especially given that the glycols formation often require a temperature higher than 200 °C. Here, Ni on well mixed oxides (Ni/MgaAl10-aOx) derived from layered double hydroxide (LDH) precursors were successfully synthesized, and then evaluated in the aqueous phase hydrogenolysis of sorbitol at 250 °C. A total glycols yield of 43.8% was obtained at a sorbitol conversion of 97.9% using the Ni/Mg6Al4Ox. Notably, the activity of Ni/Mg6Al4Ox was maintained during the recyclability test with minimal sintering and leaching. On the contrary, the Ni/Al2O3 and Ni/MgO catalysts made by conventional co-precipitation suffered severe deactivation, sintering, and leaching. Catalyst characterization revealed the formation of highly dispersed Ni on well-mixed oxides after the reduction of NiMgAl-LDH precursor. The largely improved hydrothermal stability may be due to the enhanced metal support interactions derived from the NiMgAl-LDH precursor, as compared to the Ni/Al2O3 and Ni/MgO. Density functional theory calculations suggest that the 1,2-propanediol formation from sorbitol is likely to proceed via the dehydration of glyceraldehyde instead of dihydroxyacetone, and the rate-determining step is the formation of dihydroxyacetone and glyceraldehyde during the retro-aldol condensation of ketohexose. ? 2023, The Authors. All rights reserved.