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

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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)

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.

Suggested Citation

  • Yizhen Chen & Hongliang Li & Wanghui Zhao & Wenbo Zhang & Jiawei Li & Wei Li & Xusheng Zheng & Wensheng Yan & Wenhua Zhang & Junfa Zhu & Rui Si & Jie Zeng, 2019. "Optimizing reaction paths for methanol synthesis from CO2 hydrogenation via metal-ligand cooperativity," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-09918-z
    DOI: 10.1038/s41467-019-09918-z
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    Cited by:

    1. Tang Yang & Xinnan Mao & Ying Zhang & Xiaoping Wu & Lu Wang & Mingyu Chu & Chih-Wen Pao & Shize Yang & Yong Xu & Xiaoqing Huang, 2021. "Coordination tailoring of Cu single sites on C3N4 realizes selective CO2 hydrogenation at low temperature," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    2. Wenjin Guo & Guangfang Li & Chengbo Bai & Qiong Liu & Fengxi Chen & Rong Chen, 2024. "General synthesis and atomic arrangement identification of ordered Bi–Pd intermetallics with tunable electrocatalytic CO2 reduction selectivity," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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