期刊
CHEMICAL ENGINEERING JOURNAL
卷 426, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.130857
关键词
Structured catalyst; Intermetallic catalysis; InNi3C0.5; Dimethyl oxalate hydrogenation; Ethylene glycol
资金
- National Natural Science Foundation of China [22072043, 21773069, 21703069, 21473057]
- Key Basic Research Project [18JC1412100]
- Shanghai Municipal Science and Technology Commission
- National Key Basic Research Program [2011CB201403]
- Ministry of Science and Technology of the People's Republic of China
A high-performance InNi3C0.5/Ni-foam catalyst has been developed for the gas-phase hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG). The catalyst exhibits a high turnover frequency of 636 h(-1) and effectively activates DMO while hindering over-hydrogenation of EG to ethanol. This catalyst shows promising potential for industrial applications with full DMO conversion and high EG selectivity.
A high-performance Ni-foam-structured nano-intermetallic InNi3C0.5 catalyst is developed for the gas-phase hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG). The InNi3C0.5/Ni-foam catalyst is obtain-able by hydrothermal growth of NiC2O4 onto the Ni-foam, impregnation with In2O3 precursor, subsequent calcination and carburization in a syngas. Despite DMO cascade hydrogenation to MG, then to EG, and finally to EtOH, such catalyst hydrogenates DMO dexterously until to EG with a high turnover frequency of 636 h(-1), because the 3Ni-In and 3Ni-C sites on InNi3C0.5(1 1 1) effectively activate DMO but hinder EG over-hydrogenation to EtOH. Favorable reaction pathway on the InNi3C0.5(1 1 1) surface predicted theoretically is DMO* -> CH3OCOCO* -> CH3OCOCHO* -> CH3OCOCHOH* -> MG* -> CH3OCHOCH2OH* -> CHOCH2OH* -> HOCHCH2OH* -> EG*. Moreover, the neutral Ni-foam diminishes the formation of ethers and diols. This catalyst achieves full DMO conversion with 96-98% EG selectivity and is stable for at least 2500 h under industrial-relevant conditions, and can also hydrogenate a broad scope of carbonyl compounds to corresponding alcohols with high yields.
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