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Stoichiometric methane conversion to ethane using photochemical looping at ambient temperature

Author

Listed:
  • Xiang Yu

    (UMR 8181 – UCCS – Unité de Catalyse et Chimie du Solide)

  • Vladimir L. Zholobenko

    (Keele University)

  • Simona Moldovan

    (CNRS, Université Normandie and INSA Rouen Avenue de l’Université-BP12)

  • Di Hu

    (UMR 8181 – UCCS – Unité de Catalyse et Chimie du Solide)

  • Dan Wu

    (UMR 8181 – UCCS – Unité de Catalyse et Chimie du Solide)

  • Vitaly V. Ordomsky

    (UMR 8181 – UCCS – Unité de Catalyse et Chimie du Solide)

  • Andrei Y. Khodakov

    (UMR 8181 – UCCS – Unité de Catalyse et Chimie du Solide)

Abstract

Methane activation and utilization are among the major challenges of modern science. Methane is potentially an important feedstock for manufacturing value-added fuels and chemicals. However, most known processes require excessive operating temperatures and exhibit insufficient selectivity. Here, we demonstrate a photochemical looping strategy for highly selective stoichiometric conversion of methane to ethane at ambient temperature over silver–heteropolyacid–titania nanocomposites. The process involves a stoichiometric reaction of methane with highly dispersed cationic silver under illumination, which results in the formation of methyl radicals. Recombination of the generated methyl radicals leads to the selective, and almost quantitative, formation of ethane. Cationic silver species are simultaneously reduced to metallic silver. The silver–heteropolyacid–titania nanocomposites can be reversibly regenerated in air under illumination at ambient temperature. The photochemical looping process achieves a methane coupling selectivity of over 90%, a quantitative yield of ethane of over 9%, high quantum efficiency (3.5% at 362 nm) and excellent stability.

Suggested Citation

  • Xiang Yu & Vladimir L. Zholobenko & Simona Moldovan & Di Hu & Dan Wu & Vitaly V. Ordomsky & Andrei Y. Khodakov, 2020. "Stoichiometric methane conversion to ethane using photochemical looping at ambient temperature," Nature Energy, Nature, vol. 5(7), pages 511-519, July.
  • Handle: RePEc:nat:natene:v:5:y:2020:i:7:d:10.1038_s41560-020-0616-7
    DOI: 10.1038/s41560-020-0616-7
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    Citations

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    Cited by:

    1. Xiyi Li & Chao Li & Youxun Xu & Qiong Liu & Mounib Bahri & Liquan Zhang & Nigel D. Browning & Alexander J. Cowan & Junwang Tang, 2023. "Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts," Nature Energy, Nature, vol. 8(9), pages 1013-1022, September.
    2. 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.
    3. 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.
    4. Huizhen Zhang & Pengfei Sun & Xiaozhen Fei & Xuejiao Wu & Zongyi Huang & Wanfu Zhong & Qiaobin Gong & Yanping Zheng & Qinghong Zhang & Shunji Xie & Gang Fu & Ye Wang, 2024. "Unusual facet and co-catalyst effects in TiO2-based photocatalytic coupling of methane," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    5. Chao Wang & Youxun Xu & Lunqiao Xiong & Xiyi Li & Enqi Chen & Tina Jingyan Miao & Tianyu Zhang & Yang Lan & Junwang Tang, 2024. "Selective oxidation of methane to C2+ products over Au-CeO2 by photon-phonon co-driven catalysis," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    6. Michael High & Clemens F. Patzschke & Liya Zheng & Dewang Zeng & Oriol Gavalda-Diaz & Nan Ding & Ka Ho Horace Chien & Zili Zhang & George E. Wilson & Andrey V. Berenov & Stephen J. Skinner & Kyra L. S, 2022. "Precursor engineering of hydrotalcite-derived redox sorbents for reversible and stable thermochemical oxygen storage," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    7. Siyang Nie & Liang Wu & Qinghua Zhang & Yunwei Huang & Qingda Liu & Xun Wang, 2024. "High-entropy-perovskite subnanowires for photoelectrocatalytic coupling of methane to acetic acid," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    8. Chunyang Dong & Yinghao Wang & Ziqi Deng & Wenchao Wang & Maya Marinova & Karima Tayeb & Jean-Charles Morin & Melanie Dubois & Martine Trentesaux & Yury G. Kolyagin & My Nghe Tran & Vlad Martin-Diacon, 2024. "Photocatalytic dihydroxylation of light olefins to glycols by water," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    9. Wenqing Zhang & Cenfeng Fu & Jingxiang Low & Delong Duan & Jun Ma & Wenbin Jiang & Yihong Chen & Hengjie Liu & Zeming Qi & Ran Long & Yingfang Yao & Xiaobao Li & Hui Zhang & Zhi Liu & Jinlong Yang & Z, 2022. "High-performance photocatalytic nonoxidative conversion of methane to ethane and hydrogen by heteroatoms-engineered TiO2," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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