乙醇酸
乙二醇
催化作用
乙烯
氧化还原
材料科学
产量(工程)
吸附
动力学
化学
化学工程
无机化学
光化学
有机化学
冶金
量子力学
工程类
细菌
乳酸
物理
生物
遗传学
作者
Hao Yan,Shuang Yao,Jinyao Wang,Shumin Zhao,Yinghao Sun,Mengyuan Liu,Xin Zhou,Guangyu Zhang,Xin Jin,Xiang Feng,Yibin Liu,Xiaobo Chen,De Chen,Chaohe Yang
标识
DOI:10.1016/j.apcatb.2020.119803
摘要
Rational design of desirable active sites is still a grand challenge for the efficient conversion of polyols to value-added products. Herein, we successfully constructed the Pt-Mn2O3 interfacial sites rather than Pt-MnOx solid solution to boost selective oxidation of ethylene glycol to glycolic acid under mild conditions. X-ray absorption spectroscopy and high-resolution transmission electron microscope revealed that the pre-distribution of Mn2O3 inside support unexpectedly induced the formation of Pt-Mn2O3 interfacial active sites with strong electron coupling effect, leading to an unprecedented catalytic activity (turnover frequency: 3196.9 h−1) and glycolic acid yield (86.4 %). In addition, quantitative analysis of the intrinsic active sites was performed, and a “volcano-shape” relationship was established between initial reaction rate and Pt/Mn ratio. Moreover, the structure-dependent reaction kinetics and density functional theory calculation revealed that the synergistic effect between the Mn2O3 redox cycle and Pt promotes the adsorption of ethylene glycol and the activation of CH bond, resulting in the lower activation energy of ethylene glycol oxidation. The outcome of this work offers a promising avenue for the direct construction of efficient Pt-based catalysts with desired active sites.
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