Dispersing Metallic Platinum on Green Rust Enables Effective and Selective Hydrogenation of Carbonyl Group in Cinnamaldehyde

将金属铂分散在绿锈上可实现肉桂醛中羰基的高效选择性加氢

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Abstract

Layered double hydroxides (LDHs), a category of two-dimensional nanostructured layered materials, can be employed widely as supports, catalyst precursors, and actual catalysts in a variety of heterogeneous catalytic reactions. In this work, we reported a series of Fe-containing LDHs-supported Pt-based catalysts for base-free selective hydrogenation of cinnamaldehyde into cinnamyl alcohol. It was revealed that their catalytic performances were closely correlated to the compositions of LDH supports. Especially, highly selective hydrogenation of cinnamaldehyde could be achieved over the Fe(II)-Fe(III)-LDH (green rust, FeFe-LDH) supported Pt catalyst, with a high cinnamyl alcohol selectivity of about 92% at a conversion of 90% after a reaction of 2 h, superior to other Fe(III)-containing LDHs (e.g., NiFe-LDH, CoFe-LDH, and ZnFe-LDH) supported Pt ones. It was demonstrated that the high catalytic efficiency of Pt/FeFe-LDH mainly originated from highly electron-rich character of metallic Pt species and the presence of surface reductive Fe(2+) species, thereby being helpful for the chemisorption and activation of carbonyl group in cinnamaldehyde. Moreover, strong interactions between green rust matrix and metallic Pt species could stabilize the surface Pt nanoparticles, thereby inhibiting the metal leaching during the above reaction. The present study illustrates the validity of support control in supported Pt catalysts via tuning the compositions of LDHs, and thus the electronic structure of active metal sites and catalytic performance in the selective hydrogenation of cinnamaldehyde.

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