Article ID Journal Published Year Pages File Type
227264 Journal of Industrial and Engineering Chemistry 2016 10 Pages PDF
Abstract

•The interaction between Au and Cu atoms increases the reduction activation energy of Au3+ → Au0.•The addition of 4 wt% Cu to Au/C increases the catalytic activity and the Au loading is decreased to 0.25 wt%.•Au(0.25%)Cu(4%)/C exhibits more Au3+ species than Au(0.25%)/C catalyst.

A detailed study of low-gold-content Au(0.25%)/C and Au(0.25%)Cu(4%)/C catalysts prepared via ultrasonic-assisted impregnation method is described and discussed. The addition of 4 wt% Cu to Au/C increases the initial activity and the Au loading is decreased to 0.25 wt%. Au(0.25%)Cu(4%)/C exhibits best catalytic performance with an acetylene conversion of 97.4% and the selectivity to VCM of more than 99% at a space velocity of 720 h−1 and 150 °C. The observations are rationalized in terms: (i) Au(0.25%)Cu(4%)/C exhibits relative larger specific surface area (562 m2/g) than Cu(4%)/C (385 m2/g), which provides more active sites for acetylene hydrochlorination; (ii) the reduction activation energy of Au3+ → Au0 in Au(0.25%)Cu(4%)/C (45.5 kJ/mol) is much higher than that of Au(0.25%)/C (35.6 kJ/mol), which indicates that the Au3+ species in Au(0.25%)Cu(4%)/C catalyst is more difficult to be reduced, the reduction activation energy of Cu+ → Cu0 in Au(0.25%)Cu(4%)/C (48.9 kJ/mol) is higher than that of Cu(4%)/C (43.1 kJ/mol) as a result of the electronic interaction between Au and Cu atoms; (iii) Au(0.25%)Cu(4%)/C possesses more Au3+ species (28%) than Au(0.25%)/C (16%) determined by XPS. Free-mercury low-gold-content Au(0.25%)Cu(4%)/C catalyst is environmental-friendly, making it a potentially green catalyst for acetylene hydrochlorination.

Graphical abstractA low-gold-content Au(0.25%)Cu(4%)/C catalyst was prepared via ultrasonic-assisted impregnation method for the first time and applied to acetylene hydrochlorination. Figure Catalytic performance of Au(0.25%)Cu(4%)/C and the deduced reaction mechanism for acetylene hydrochlorination over Au(0.25%)Cu(4%)/C catalyst.Figure optionsDownload full-size imageDownload as PowerPoint slide

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