Tunable Synthesis of Ethanol or Methyl Acetate via Dimethyl Oxalate Hydrogenation on Confined Iron Catalysts

Sun Yannan; Ma Qingxiang; Ge Qingjie; Sun Jian

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Tunable Synthesis of Ethanol or Methyl Acetate via Dimethyl Oxalate Hydrogenation on Confined Iron Catalysts

机译：通过在密闭铁催化剂上通过二甲酯氢化可调谐合成乙醇或乙酸甲酯

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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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来源
《ACS catalysis》 |2021年第8期|共12页
作者
Sun Yannan; Ma Qingxiang; Ge Qingjie; Sun Jian;
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作者单位

Chinese Acad Sci Dalian Inst Chem Phys Dalian Natl Lab Clean Energy Dalian 116023 Peoples R China;

Ningxia Univ State Key Lab High Efficiency Utilizat Coal &

Gre Yinchuan 750021 Ningxia Peoples R China;

Chinese Acad Sci Dalian Inst Chem Phys Dalian Natl Lab Clean Energy Dalian 116023 Peoples R China;

Chinese Acad Sci Dalian Inst Chem Phys Dalian Natl Lab Clean Energy Dalian 116023 Peoples R China;

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原文格式 PDF
正文语种 eng
中图分类物理化学（理论化学）、化学物理学;
关键词
DMO hydrogenation; ethanol; methyl acetate; confined iron catalyst; the active site;

机译：DMO氢化;乙醇;乙酸甲酯;密闭铁催化剂;活性部位;

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1. Synthesis of Methyl Glycolate by Hydrogenation of Dimethyl Oxalate over Cu-Ag/SiO2 Catalyst [J] . 天然气化学（英文版） . 2007,第001期
2. Effects of ethanol on the in situ synthesized Cu/SiC》2 catalyst: Texture, structure, and the catalytic performance in hydrogenation dimethyl oxalate to ethylene glycol [J] . Shu Rong Wang, Ling Jun Zhu, Ying Ying Zhu, 中国化学快报（英文版） . 2011,第003期
3. Catalytic activity of Cu/ZnO catalysts mediated by MgO promoter in hydrogenation of methyl acetate to ethanol [J] . Fang Zhang, Zhiyang Chen, Xudong Fang, 天然气化学（英文版） . 2021,第010期
4. Catalytic activity of Cu/ZnO catalysts mediated by MgO promoter in hydrogenation of methyl acetate to ethanol [J] . Fang Zhang, Zhiyang Chen, Xudong Fang, 能源化学：英文版 . 2021,第010期
5. Sonochemical synthesis of Zn-promoted porous MgO-supported lamellar Cu catalysts for selective hydrogenation of dimethyl oxalate to ethanol and their long-term stability [J] . Abbas Mohamed, Zhang Juan, Chen Zheng, New Journal of Chemistry . 2018,第21期

机译：Zn促进的多孔MgO负载层状Cu催化剂的多孔化学合成，用于选择性氢化草酸二甲酯与乙醇的氢化及其长期稳定性
6. Ni-containing Cu/SiO2 catalyst for the chemoselective synthesis of ethanol via hydrogenation of dimethyl oxalate [J] . Zhao Yujun, Zhao Shuo, Geng Yaochen, Catalysis Today . 2016,第Null期

机译：含镍Cu / SiO2催化剂，用于草酸二甲酯加氢化学选择性合成乙醇
7. Cu Nanoparticles Inlaid Mesoporous Al2O3 As a High-Performance Bifunctional Catalyst for Ethanol Synthesis via Dimethyl Oxalate Hydrogenation [J] . Yifeng Zhu, Xiao Kong, Xianqing Li ACS catalysis . 2014,第10期

机译：铜纳米颗粒镶嵌介孔Al2O3作为草酸二甲酯加氢合成乙醇的高性能双功能催化剂
8. SYNTHESIS OF ETHANOL BASED ON HYDROGENATION OF DIMETHYL OXALATE VIA SYNGAS ON SUPPORTED COPPER CATALYSTS [C] . Hairong Yue, Yujun Zhao, Shuo Zhao National Meeting Exhibition . 2012

机译：基于通过合成气氢化在负载铜催化剂上的二甲酯氢化的乙醇
9. Catalyst deactivation in the synthesis of methyl acetate from methyl ether using group VIII metal salts of phosphotungstic acid. [D] . Tartamella, Timothy Leonard. 1997

机译：使用磷钨酸的group族金属盐从甲醚合成乙酸甲酯时催化剂失活。
10. Hydrogenation of Ethyl Acetate to Ethanol over Ni-Based Catalysts Obtained from Ni/Al Hydrotalcite-Like Compounds [O] . Beixiao Zhang, Lu Lin, Junping Zhuang, 2010

机译：Ni / Al水滑石样化合物制得的镍基催化剂上乙酸乙酯加氢制乙醇
11. An environmentally benign and low-cost approach to synthesis of thermally stable industrial catalyst Cu/SiO2 for the hydrogenation of dimethyl oxalate to ethylene glycol [O] . Tiberiu Popa, Yulong Zhang, Erlei Jin, 2015

机译：用于合成热稳定的工业催化剂Cu / SiO2的环境良性和低成本方法，用于草酸二甲酯与乙二醇的氢化
12. Synthesis of dimethyl ether and alternative fuels in the liquid phase from coal-derived synthesis gas. Task 2.2: Definition of preferred catalyst system; Task 2.3: Process variable scans on the preferred catalyst system; Task 2.4: Life-test on the preferred catalyst system [R] . Bhatt, B. L. 1992

机译：由煤衍生的合成气合成二甲醚和液相替代燃料。任务2.2：优选催化剂体系的定义;任务2.3：在首选催化剂体系上进行过程变量扫描;任务2.4：对首选催化剂体系进行寿命测试

Tunable Synthesis of Ethanol or Methyl Acetate via Dimethyl Oxalate Hydrogenation on Confined Iron Catalysts

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