期刊
JOURNAL OF CATALYSIS
卷 407, 期 -, 页码 44-53出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2021.12.001
关键词
Hydrothermal treatment; Cu/SiO2; Oxygen vacancies; DFT
资金
- National Key Research and Development Program of China [2016YFB0701100]
- National Natural Science Foundation of China [21573075]
- China Postdoctoral Science Foundation [2018M640330]
The reducibility of heterogeneous Cu-based precursor greatly affects the activity and stability of the final catalysts. In this study, a crystallization inhibition strategy was developed to fabricate a reduction-resistant CuSiO3 precursor, which showed enhanced performance in methanol dehydrogenation and DMO adsorption, leading to the successful synthesis of ethylene glycol.
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. (c) 2021 Published by Elsevier Inc.
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