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Direct conversion of methane to formaldehyde and CO on B2O3 catalysts

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  • Jinshu Tian

    (State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University)

  • Jiangqiao Tan

    (State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University)

  • Zhaoxia Zhang

    (State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University)

  • Peijie Han

    (State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University)

  • Min Yin

    (State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University)

  • Shaolong Wan

    (State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University)

  • Jingdong Lin

    (State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University)

  • Shuai Wang

    (State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University)

  • Yong Wang

    (Washington State University)

Abstract

Direct oxidation of methane to value-added C1 chemicals (e.g. HCHO and CO) provides a promising way to utilize natural gas sources under relatively mild conditions. Such conversions remain, however, a key selectivity challenge, resulting from the facile formation of undesired fully-oxidized CO2. Here we show that B2O3-based catalysts are selective in the direct conversion of methane to HCHO and CO (~94% selectivity with a HCHO/CO ratio of ~1 at 6% conversion) and highly stable (over 100 hour time-on-stream operation) conducted in a fixed-bed reactor (550 °C, 100 kPa, space velocity 4650 mL gcat−1 h−1). Combined catalyst characterization, kinetic studies, and isotopic labeling experiments unveil that molecular O2 bonded to tri-coordinated BO3 centers on B2O3 surfaces acts as a judicious oxidant for methane activation with mitigated CO2 formation, even at high O2/CH4 ratios of the feed. These findings shed light on the great potential of designing innovative catalytic processes for the direct conversion of alkanes to fuels/chemicals.

Suggested Citation

  • Jinshu Tian & Jiangqiao Tan & Zhaoxia Zhang & Peijie Han & Min Yin & Shaolong Wan & Jingdong Lin & Shuai Wang & Yong Wang, 2020. "Direct conversion of methane to formaldehyde and CO on B2O3 catalysts," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-19517-y
    DOI: 10.1038/s41467-020-19517-y
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    Cited by:

    1. Xiyi Li & Chao Wang & Jianlong Yang & Youxun Xu & Yi Yang & Jiaguo Yu & Juan J. Delgado & Natalia Martsinovich & Xiao Sun & Xu-Sheng Zheng & Weixin Huang & Junwang Tang, 2023. "PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    2. Lei Luo & Lei Fu & Huifen Liu & Youxun Xu & Jialiang Xing & Chun-Ran Chang & Dong-Yuan Yang & Junwang Tang, 2022. "Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    3. Lei Luo & Xiaoyu Han & Keran Wang & Youxun Xu & Lunqiao Xiong & Jiani Ma & Zhengxiao Guo & Junwang Tang, 2023. "Nearly 100% selective and visible-light-driven methane conversion to formaldehyde via. single-atom Cu and Wδ+," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    4. Zhankai Liu & Ziyi Liu & Jie Fan & Wen-Duo Lu & Fan Wu & Bin Gao & Jian Sheng & Bin Qiu & Dongqi Wang & An-Hui Lu, 2023. "Auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions," Nature Communications, Nature, vol. 14(1), pages 1-9, December.

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