Role of ReOx in Re-modified Rh/ZrO2 and Ir/ZrO2 catalysts in glycerol hydrogenolysis：Insights from first-principles study

doi:10.1016/S1872-2067(12)60626-3

Abstract

Abstract:

The thermodynamics of glycerol hydrogenolysis to produce 1,2-propanediol (1,2-PDO) and 1,3-propanediol (1,3-PDO) over Ru/ZrO₂, Rh/ZrO₂, ReO_x-Rh/ZrO₂, and ReO_x-Ir/ZrO₂ were studied using density functional theory calculations, with a special focus on the mechanism controlling the activity and selectivity of the reactions. It is found that the decomposition of glycerol on Ru/ZrO₂ and Rh/ZrO₂ proceeds through a dehydration-hydrogenation mechanism. The formation of 1,2-PDO is thermodynamically favored, and the activity of the Ru-based catalyst is higher than that of the Rh-based one. In contrast, a direct hydrogenolysis mechanism is proposed for the Re-modified Rh and Ir catalysts, in which a dissociated H atom on the Rh(Ir) metal surface attacks the C-O bond neighboring the alkoxide species on the ReO_x cluster. In the presence of ReO_x-Rh/ZrO₂, the modified catalyst favors the production of 1,2-PDO, and 1,3-PDO production becomes competitive. However, the ReO_x-Ir/ZrO₂ catalyst significantly improves 1,3-PDO selectivity. The direct hydrogenolysis pathway, as opposed to the indirect hydrogenolysis mechanism for monometallic catalysts, may be the key to the high 1,3-PDO selectivity on the modified catalysts, where the hydroxylated Re group facilitates the formation of terminal alkoxide species rather than secondary alkoxides. Steric effects are important in preferential terminal alkoxide formation on the ReO_x-Ir/ZrO₂ catalysts because of the growth of large Ir-Re clusters, resulting in high selectivity for 1,3-PDO.

Key words: Density functional theory, Glycerol hydrogenolysis, Propanediol, Re-modified, Metal catalyst, Thermodynamics

Jing Guan, Xiufang Chen, Gongming Peng, Xicheng Wang, Quan Cao, Zhenggang Lan, Xindong Mu. Role of ReO_x in Re-modified Rh/ZrO₂ and Ir/ZrO₂ catalysts in glycerol hydrogenolysis：Insights from first-principles study[J]. Chinese Journal of Catalysis, 2013, 34(9): 1656-1666.

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Role of ReO_x in Re-modified Rh/ZrO₂ and Ir/ZrO₂ catalysts in glycerol hydrogenolysis：Insights from first-principles study

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