Cu-Zr/SiO_(2)catalysts featured by different Cu-Zr-Si coordinations for ethanol conversion to 1,3-butadiene

Catalytic upgrading of bio-ethanol to 1,3-butadiene(1,3-BD,ETB)is a renewable and low-carbon technology for the bulk chemical production.Exploring robust catalysts and getting in-depth understanding of the relationship between the structure of catalytic sites and reaction selectivity are of great significance for ETB process applications.In this study,we constructed a robust Cu-Zr/SiO_(2) catalyst by an ammonia evaporation and post-impregnation method.Over the optimal 2%Cu-8%Zr/SiO_(2) catalyst,superior performance of 69.6%1,3-BD selectivity and 71.2%ethanol conversion were obtained.Systematic characterizations revealed that three types of Cu-Zr-Si active sites were probably constructed on the Cu-8%Zr/SiO_(2) catalysts as varying the Cu loadings from 0.5 to 20%,affording greatly different activity and selectivity in the ETB process.The 1,3-BD productivity over the(SiO)_(2)(CuO)Zr-OH sites was 8.2 and 77.2 times higher than that of(CuO)_(2)-Zr-(OSi)2 and Cu-(O)_(2)-Zr-(OSi)2 sites,respectively,attributed to the high activities and good balance among the reactions of dehydrogenation,aldol condensation,and MPVO reduction.