Optimizing reaction paths for methanol synthesis from CO2 hydrogenation via metal-ligand cooperativity

Yizhen Chen, Hongliang Li, Wanghui Zhao, Wenbo Zhang, Jiawei Li, Wei Li, Xusheng Zheng, Wensheng Yan, Wenhua Zhang, Junfa Zhu, Rui Si () and Jie Zeng ()
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Yizhen Chen: University of Science and Technology of China
Hongliang Li: University of Science and Technology of China
Wanghui Zhao: University of Science and Technology of China
Wenbo Zhang: University of Science and Technology of China
Jiawei Li: University of Science and Technology of China
Wei Li: Chinese Academy of Sciences
Xusheng Zheng: University of Science and Technology of China
Wensheng Yan: University of Science and Technology of China
Wenhua Zhang: University of Science and Technology of China
Junfa Zhu: University of Science and Technology of China
Rui Si: Chinese Academy of Sciences
Jie Zeng: University of Science and Technology of China

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract As diversified reaction paths exist over practical catalysts towards CO2 hydrogenation, it is highly desiderated to precisely control the reaction path for developing efficient catalysts. Herein, we report that the ensemble of Pt single atoms coordinated with oxygen atoms in MIL-101 (Pt1@MIL) induces distinct reaction path to improve selective hydrogenation of CO2 into methanol. Pt1@MIL achieves the turnover frequency number of 117 h−1 in DMF under 32 bar at 150 °C, which is 5.6 times that of Ptn@MIL. Moreover, the selectivity for methanol is 90.3% over Pt1@MIL, much higher than that (13.3%) over Ptn@MIL with CO as the major product. According to mechanistic studies, CO2 is hydrogenated into HCOO* as the intermediate for Pt1@MIL, whereas COOH* serves as the intermediate for Ptn@MIL. The unique reaction path over Pt1@MIL not only lowers the activation energy for the enhanced catalytic activity, but also contributes to the high selectivity for methanol.

Date: 2019
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DOI: 10.1038/s41467-019-09918-z

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