Pt1 enhanced C-H activation synergistic with Ptn catalysis for glycerol cascade oxidation to glyceric acid

作者：Zhe An, Zilong Zhang, Zeyu Huang, Hongbo Han, Binbin Song, Jian Zhang, Ping Qi, Yanru Zhu, Hongyan Song, Bin Wang, Lirong Zheng, Jing He · 发表于：Nature Communications · 年份：2022 · DOI：10.1038/s41467-022-33038-w · 被引用次数：155 · 研究领域：Catalytic Processes in Materials Science、Catalysis for Biomass Conversion、Electrocatalysts for Energy Conversion

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%).