期刊
ACS CATALYSIS
卷 11, 期 8, 页码 4908-4919出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c00339
关键词
DMO hydrogenation; ethanol; methyl acetate; confined iron catalyst; the active site
资金
- Youth Innovation Promotion Association of Chinese Academy of Sciences [2018214]
- LiaoNing Revitalization Talents Program [XLYC1907066]
- Dalian Outstanding Young Scientific and Technological Talents Program [2018RJ06]
- Foundation of State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering [2019-KF-11]
A confined iron catalyst is designed for balanced syntheses of ethanol and methyl acetate via dimethyl oxalate (DMO) hydrogenation. The Fe@C catalyst promotes the enrichment of hydrogen to reach a tunable selectivity of ethanol and methyl acetate, providing a strategy for tuning targeted oxygenated chemicals.
Oxygenated chemicals are essential to modern industries. However, selective syntheses with controllable products are still challenging over a single heterogeneous catalyst. Herein, a confined iron catalyst is designed for balanced syntheses of ethanol and methyl acetate via dimethyl oxalate (DMO) hydrogenation. With the characteristic structure of a microsphere, the Fe@C catalyst promotes the enrichment of hydrogen to reach a tunable selectivity of ethanol (84.3%) and methyl acetate (77.9%). The highest selectivity of methyl acetate is reached at a H-2/DMO molar ratio as low as 20, which is the lowest among catalysts reported for DMO hydrogenation by now. The molecule-level mechanism of DMO hydrogenation is further investigated. It proves that Fe5C2 in Fe@C is the main active center of DMO hydrogenation and Fe3O4 promotes the conversion of the intermediate especially in a low H-2/DMO molar ratio. This work provides a strategy for tuning targeted oxygenated chemicals.
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