Pt(1) enhanced C-H activation synergistic with Pt(n) catalysis for glycerol cascade oxidation to glyceric acid

Pt(1)增强的CH活化与Pt(n)催化协同作用,促进甘油级联氧化生成甘油酸

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Abstract

The selective oxidation of glycerol to glyceric acid, an important value-added reaction from polyols, is a typical cascade catalytic process. It is still of great challenge to simultaneously achieve high glycerol activity and glyceric acid selectivity, suffering from either deep oxidation and C-C cleavage or poor oxidation efficiency from glyceraldehyde to glyceric acid. Herein, this work, inspired by nature, proposes a cascade synergistic catalysis strategy by atomic and low-coordinated cluster Pt on well-defined Cu-CuZrO(x), which involves enhanced C-H activation on atomic Pt(1) and O-H activation on cluster Pt(n) in the oxidation of glycerol to glyceraldehyde, and cluster Pt(n) for C=O activation followed by O-H insertion and atomic Pt(1) for C-H activation in the tandem oxidation of glyceraldehyde to glyceric acid. The enhanced C-H activation in the cascade process by atomic Pt(1) is revealed to be essential for the high glycerol activity (90.0±0.1%) and the glyceric acid selectivity (80.2±0.2%).

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