Cu/SiO2 catalysts prepared by a convenient and efficient method using the urea hydrolysis deposition-precipitation (UHDP) technique have been proposed focusing on the effect of copper loading.The texture,structure a...Cu/SiO2 catalysts prepared by a convenient and efficient method using the urea hydrolysis deposition-precipitation (UHDP) technique have been proposed focusing on the effect of copper loading.The texture,structure and composition are systematically characterized by ICP,FTIR,N 2-physisorption,N2O chemisorption,TPR,XRD and XPS.The formation of copper phyllosilicate is observed in Cu/SiO2 catalyst by adopting UHDP method,and the amount of copper phyllosilicate is related to copper loading.It is found the structure properties and catalytic performance is profoundly affected by the amount of copper phyllosilicate.The excellent catalytic activity is attributed to the synergetic effect between Cu0 and Cu +.DMO conversion and EG selectivity are determined by the amount of Cu0 and Cu+,respectively.The proper copper loading (30 wt%) provides with the highest ratio of Cu + /Cu0,giving rise to the highest EG yield of 95% under the reaction conditions of p=2.0 MPa,T=473 K,H2/DMO=80 and LHSV=1.0h-1.展开更多
The mechanism of dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO2 catalyst was investigated by in situ Fourier transform infrared (FTIR) spectroscopy. It was found that dimethyl oxalate and methyl glyc...The mechanism of dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO2 catalyst was investigated by in situ Fourier transform infrared (FTIR) spectroscopy. It was found that dimethyl oxalate and methyl glycolate proceeded via dissociative adsorption on Cu/SiO2 catalyst, and four main intermediates, CH3OC(O)(O)C-M (1655 cm-1), M-C(O)(O)C-M (1618 cm-1), HOCH2(O)C--M (1682 cm-1) and CH3O-M (2924-2926 cm-1), were identified during the reaction. It was concluded that dimethyl oxalate hydrogenation to ethylene glycol mainly proceeded along the route: dimethyl oxalate /rightarrow CH3OC(O)(O)C-M → methyl glycolate →HOCH2(O)C-M → ethylene glycol. Finally a schematic reaction network was proposed.展开更多
The Cu/SiO2 catalyst prepared by incipient wetness method exhibited very high activity and selectivity for the vapor-phase synthesis of N-butylaniline from aniline and 1-butanol. When Cu loading was 0.70 mmol/g-SiO2 a...The Cu/SiO2 catalyst prepared by incipient wetness method exhibited very high activity and selectivity for the vapor-phase synthesis of N-butylaniline from aniline and 1-butanol. When Cu loading was 0.70 mmol/g-SiO2 and the catalyst precursor was calcined at 500 ℃, 1-butanol conversion reached 99%, and the selectivity of N-butylaniline exceeded 97%.展开更多
文摘Cu/SiO2 catalysts prepared by a convenient and efficient method using the urea hydrolysis deposition-precipitation (UHDP) technique have been proposed focusing on the effect of copper loading.The texture,structure and composition are systematically characterized by ICP,FTIR,N 2-physisorption,N2O chemisorption,TPR,XRD and XPS.The formation of copper phyllosilicate is observed in Cu/SiO2 catalyst by adopting UHDP method,and the amount of copper phyllosilicate is related to copper loading.It is found the structure properties and catalytic performance is profoundly affected by the amount of copper phyllosilicate.The excellent catalytic activity is attributed to the synergetic effect between Cu0 and Cu +.DMO conversion and EG selectivity are determined by the amount of Cu0 and Cu+,respectively.The proper copper loading (30 wt%) provides with the highest ratio of Cu + /Cu0,giving rise to the highest EG yield of 95% under the reaction conditions of p=2.0 MPa,T=473 K,H2/DMO=80 and LHSV=1.0h-1.
文摘The mechanism of dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO2 catalyst was investigated by in situ Fourier transform infrared (FTIR) spectroscopy. It was found that dimethyl oxalate and methyl glycolate proceeded via dissociative adsorption on Cu/SiO2 catalyst, and four main intermediates, CH3OC(O)(O)C-M (1655 cm-1), M-C(O)(O)C-M (1618 cm-1), HOCH2(O)C--M (1682 cm-1) and CH3O-M (2924-2926 cm-1), were identified during the reaction. It was concluded that dimethyl oxalate hydrogenation to ethylene glycol mainly proceeded along the route: dimethyl oxalate /rightarrow CH3OC(O)(O)C-M → methyl glycolate →HOCH2(O)C-M → ethylene glycol. Finally a schematic reaction network was proposed.
文摘The Cu/SiO2 catalyst prepared by incipient wetness method exhibited very high activity and selectivity for the vapor-phase synthesis of N-butylaniline from aniline and 1-butanol. When Cu loading was 0.70 mmol/g-SiO2 and the catalyst precursor was calcined at 500 ℃, 1-butanol conversion reached 99%, and the selectivity of N-butylaniline exceeded 97%.