Insight into the size-dependent activity in Ag/SiO 2 catalyzed hydrogenation of dimethyl oxalate to methyl glycolate

被引:0
|
作者
Li, Zhuoshi [1 ,2 ]
Hai, Yinhe [1 ]
Feng, Yibin [1 ]
Guan, Tong [1 ]
Xiao, Tiantian [1 ,2 ]
Lv, Jing [1 ,3 ]
Huang, Shouying [1 ,3 ]
Wang, Yue [1 ,2 ,3 ,4 ]
Ma, Xinbin [1 ]
机构
[1] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn, Sch Chem Engn & Technol, Key Lab Green Chem Technol,Minist Educ, Tianjin 300072, Peoples R China
[2] Int Campus Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Fuzhou 350207, Peoples R China
[3] Haihe Lab Sustainable Chem Transformat, Tianjin 300192, Peoples R China
[4] Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
基金
中国国家自然科学基金;
关键词
Dimethyl oxalate; Methyl glycolate; Hydrogenation; Size effect; Ag -based catalyst; CHEMOSELECTIVE SYNTHESIS; SELECTIVE HYDROGENATION; SILVER NANOPARTICLES; AG; PERFORMANCE; CITRATE; SILICA; CARBON; SHAPE; CO;
D O I
10.1016/j.ces.2024.120305
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Methyl glycolate (MG) is an important building block for synthesizing biodegradable material of polyglycolic acid. Hydrogenation of coal-based dimethyl oxalate (DMO) to MG is quite promising, where Ag -based catalysts exhibited excellent selectivity. Here, a series of Ag/SiO 2 -x catalysts with particle sizes of 1.4 - 13.5 nm were prepared, which showed significant structural sensitivity in DMO hydrogenation. For Ag nanoparticles of 1.4 - 2.7 nm, the turnover frequency (TOF) was linearly increased with the surface electron density of silver, but when the Ag nanoparticles further enlarged, no significant variation of TOF was observed. Combining DFT calculation and experimental results of the model catalyst, triangular nanoplate, it was deduced that the Ag (111) played a dominant role in DMO hydrogenation to MG, originating from the benefited MG desorption as well as promoted dissociation of H 2 and DMO. This understanding about Ag particle size effect may provide guidance for designing efficient catalysts for DMO hydrogenation to MG.
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页数:8
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