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Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions

Author

Listed:
  • Yu Tang

    (University of Kansas)

  • Yuting Li

    (University of Kansas)

  • Victor Fung

    (University of California)

  • De-en Jiang

    (University of California)

  • Weixin Huang

    (University of Kansas
    University of Notre Dame)

  • Shiran Zhang

    (University of Kansas
    University of Notre Dame)

  • Yasuhiro Iwasawa

    (The University of Electro-Communications)

  • Tomohiro Sakata

    (The University of Electro-Communications)

  • Luan Nguyen

    (University of Kansas
    University of Notre Dame)

  • Xiaoyan Zhang

    (University of Kansas
    Fuzhou University)

  • Anatoly I. Frenkel

    (Stony Brook University
    Division of Chemistry, Brookhaven National Laboratory)

  • Franklin (Feng) Tao

    (University of Kansas
    University of Notre Dame)

Abstract

Catalytic transformation of CH4 under a mild condition is significant for efficient utilization of shale gas under the circumstance of switching raw materials of chemical industries to shale gas. Here, we report the transformation of CH4 to acetic acid and methanol through coupling of CH4, CO and O2 on single-site Rh1O5 anchored in microporous aluminosilicates in solution at ≤150 °C. The activity of these singly dispersed precious metal sites for production of organic oxygenates can reach about 0.10 acetic acid molecules on a Rh1O5 site per second at 150 °C with a selectivity of ~70% for production of acetic acid. It is higher than the activity of free Rh cations by >1000 times. Computational studies suggest that the first C–H bond of CH4 is activated by Rh1O5 anchored on the wall of micropores of ZSM-5; the formed CH3 then couples with CO and OH, to produce acetic acid over a low activation barrier.

Suggested Citation

  • Yu Tang & Yuting Li & Victor Fung & De-en Jiang & Weixin Huang & Shiran Zhang & Yasuhiro Iwasawa & Tomohiro Sakata & Luan Nguyen & Xiaoyan Zhang & Anatoly I. Frenkel & Franklin (Feng) Tao, 2018. "Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions," Nature Communications, Nature, vol. 9(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-03235-7
    DOI: 10.1038/s41467-018-03235-7
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    Cited by:

    1. Wenqing Zhang & Dawei Xi & Yihong Chen & Aobo Chen & Yawen Jiang & Hengjie Liu & Zeyu Zhou & Hui Zhang & Zhi Liu & Ran Long & Yujie Xiong, 2023. "Light-driven flow synthesis of acetic acid from methane with chemical looping," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Xiao Sun & Xuanye Chen & Cong Fu & Qingbo Yu & Xu-Sheng Zheng & Fei Fang & Yuanxu Liu & Junfa Zhu & Wenhua Zhang & Weixin Huang, 2022. "Molecular oxygen enhances H2O2 utilization for the photocatalytic conversion of methane to liquid-phase oxygenates," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    3. Liang Shen & Minghui Zhu & Jing Xu, 2021. "Effect of micropores on the structure and CO2 methanation performance of supported Ni/SiO2 catalyst," Greenhouse Gases: Science and Technology, Blackwell Publishing, vol. 11(6), pages 1213-1221, December.
    4. Bin Li & Jiali Mu & Guifa Long & Xiangen Song & Ende Huang & Siyue Liu & Yao Wei & Fanfei Sun & Siquan Feng & Qiao Yuan & Yutong Cai & Jian Song & Wenrui Dong & Weiqing Zhang & Xueming Yang & Li Yan &, 2024. "Water-participated mild oxidation of ethane to acetaldehyde," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    5. Minjie Zhao & Chengeng Li & Daviel Gómez & Francisco Gonell & Vlad Martin Diaconescu & Laura Simonelli & Miguel Lopez Haro & Jose Juan Calvino & Debora Motta Meira & Patricia Concepción & Avelino Corm, 2023. "Low-temperature hydroformylation of ethylene by phosphorous stabilized Rh sites in a one-pot synthesized Rh-(O)-P-MFI zeolite," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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