The selectively regulated vapour phase dehydrogenation of 1,4-butanediol to gamma-butyrolactone employing a copper-based ceria catalyst

摘要

The growing pursuit of the viable application of gamma-butyrolactone (GBL) as an industrially important product offers the possibility to use 1,4-butanediol (1,4-BDO) as a potential reactant. In this regard, different proportions of copper-based ceria catalysts (5, 10, 15, and 20CC) were synthesized using a wet impregnation method and their catalytic activities were tested for the vapour phase dehydrogenation of 1,4-BDO to GBL at temperatures from 240-300 degrees C. The synthesized copper-based ceria catalysts (5CC, 10CC, 15CC, and 20CC) were characterized using various analytical tools and the consequent results revealed that the activities of the CC catalysts were influenced by the physicochemical properties of the materials. In order to determine the influence of various supports on the catalytic activity, the addition of 10 wt% copper (Cu) to TiO2, Al2O3, ZnO, ZSM-5, and SBA-15 supports was carried out, and the respective influence on the catalytic activity was also experimentally established. The most outstanding catalytic activity was seen for the 10 wt% copper-based ceria catalyst, with a high conversion of 93% and selectivity of 98% at 240 degrees C. Factors like a high surface area, and better dispersion and basicity of active sites had a marked impact on the catalytic activity. Mechanistic analysis suggested that 1,4-BDO undergoes dehydrogenation over the copper surface to give 4-hydroxybutanal, followed by hemiacetylation and subsequent dehydrogenation to give GBL as the selective product. In terms of the stability of the catalysts, the 10 wt% copper-based ceria catalyst maintained a stable GBL selectivity of 98% for up to 7 h on-stream.