K+-induced formation of granular and dense copper phyllosilicate precursor converts dimethyl oxalate to ethylene glycol in absence of H2

作者：Fang, Yuan; Sun, Hao; Ma, Bing^*; Zhao, Chen^*

来源：Journal of Catalysis, 2022, 407: 44-53.

DOI：10.1016/j.jcat.2021.12.001

• Hydrothermal treatment
• Cu/SiO2
• Oxygen vacancies
• DFT

The reducibility of heterogeneous Cu-based precursor greatly influences the activity and stability of the final catalysts because the excessive reduction to metallic Cu significantly deactivates the catalysts. Herein, we develop a crystallization inhibition strategy to fabricate the granular and densely stacked cop-per phyllosilicate precursor which possesses stronger resistance to H-2 reduction. The reduction-resistant CuSiO3 precursor contains more abundant Cu+ species and oxygen deficiencies, which was verified by O-2- TPD, TGA, O XPS and Cu XAES measurements, and is beneficial for methanol dehydrogenation and dimethyl oxalate (DMO) adsorption. A high yield of 85.4% of ethylene glycol (EG) was achieved from DMO hydrogenation at 240 degrees C, with methanol as both the solvent and hydrogen supplier. The delicately designed synthesis of specific Cu precursor with unique properties resulted in an excellent multi-functional Cu catalyst for coupled methanol dehydrogenation and DMO hydrogenation to EG.

• 单位
  复旦大学