IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v16y2025i1d10.1038_s41467-025-57854-y.html
   My bibliography  Save this article

Photothermal direct methane conversion to formaldehyde at the gas-solid interface under ambient pressure

Author

Listed:
  • Yuxiong Wang

    (Zhejiang University)

  • Yaoyu Zhang

    (Nanjing Normal University)

  • Xiaoqiang Wang

    (Jiaxing University)

  • Yue Liu

    (Zhejiang University)

  • Zhongbiao Wu

    (Zhejiang University)

Abstract

Photocatalytic direct oxidation of methane to C1 oxygenates offers a green alternative to conventional energy-intensive and high-carbon-footprint multi-step processes. However, current batch-type gas–liquid–solid reaction systems under high-pressure conditions face critical challenges in real-time product separation and concentration for industrial implementation. Here, we demonstrate a continuous-flow gas–solid photothermal catalytic route for methane conversion to formaldehyde under ambient pressure, where the generated gas-phase formaldehyde can be easily collected by water absorption. The Ag single-atom modified ZnO photocatalyst achieves a formaldehyde production rate of 117.8 ± 1.7 μmol h−1 with 71.2 ± 0.8% selectivity. Meanwhile, a highly concentrated formaldehyde solution (514.2 ± 33.7 µmol mL−1, 1.54 ± 0.10 wt.%) is obtained through 12-hour water absorption, effectively overcoming the product enrichment barrier that plagues conventional batch reaction route. This study establishes a robust technological foundation for sustainable industrial-scale conversion of methane to value-added chemicals.

Suggested Citation

  • Yuxiong Wang & Yaoyu Zhang & Xiaoqiang Wang & Yue Liu & Zhongbiao Wu, 2025. "Photothermal direct methane conversion to formaldehyde at the gas-solid interface under ambient pressure," Nature Communications, Nature, vol. 16(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-57854-y
    DOI: 10.1038/s41467-025-57854-y
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-025-57854-y
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-025-57854-y?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Yingying Fan & Wencai Zhou & Xueying Qiu & Hongdong Li & Yuheng Jiang & Zhonghui Sun & Dongxue Han & Li Niu & Zhiyong Tang, 2021. "Selective photocatalytic oxidation of methane by quantum-sized bismuth vanadate," Nature Sustainability, Nature, vol. 4(6), pages 509-515, June.
    2. 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.
    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. 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.
    5. Xuxing Chen & Yunpeng Li & Xiaoyang Pan & David Cortie & Xintang Huang & Zhiguo Yi, 2016. "Photocatalytic oxidation of methane over silver decorated zinc oxide nanocatalysts," Nature Communications, Nature, vol. 7(1), pages 1-8, November.
    6. Yingying Fan & Yuheng Jiang & Haiting Lin & Jianan Li & Yuanjiang Xie & Anyi Chen & Siyang Li & Dongxue Han & Li Niu & Zhiyong Tang, 2024. "Insight into selectivity of photocatalytic methane oxidation to formaldehyde on tungsten trioxide," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Yingying Fan & Yuheng Jiang & Haiting Lin & Jianan Li & Yuanjiang Xie & Anyi Chen & Siyang Li & Dongxue Han & Li Niu & Zhiyong Tang, 2024. "Insight into selectivity of photocatalytic methane oxidation to formaldehyde on tungsten trioxide," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    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. Youxun Xu & Chao Wang & Xiyi Li & Lunqiao Xiong & Tianyu Zhang & Liquan Zhang & Qinghua Zhang & Lin Gu & Yang Lan & Junwang Tang, 2024. "Efficient methane oxidation to formaldehyde via photon–phonon cascade catalysis," Nature Sustainability, Nature, vol. 7(9), pages 1171-1181, September.
    4. 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.
    5. Hui Song & Kai Sun & Hengming Huang & Shangbo Ning & Shengyao Wang & Zhuan Wang & Yuxiang Weng & Yi Cui & Yifan Li & Xu-sheng Wang & Defa Wang & Lequan Liu & Zhou-jun Wang & Jinhua Ye, 2025. "Integrating photochemical and photothermal effects for selective oxidative coupling of methane into C2+ hydrocarbons with multiple active sites," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
    6. Jun Ma & Can Zhu & Keke Mao & Wenbin Jiang & Jingxiang Low & Delong Duan & Huanxin Ju & Dong Liu & Kun Wang & Yijing Zang & Shuangming Chen & Hui Zhang & Zeming Qi & Ran Long & Zhi Liu & Li Song & Yuj, 2023. "Sustainable methane utilization technology via photocatalytic halogenation with alkali halides," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    7. Shuo Wang & Chenyang Li & Yu Qi & Jiaming Zhang & Ningning Wang & Meng Liu & Boyang Zhang & Xuefen Cai & Hongbo Zhang & Su-huai Wei & Guijun Ma & Jingxiu Yang & Shanshan Chen & Fuxiang Zhang, 2025. "Etched BiVO4 photocatalyst with charge separation efficiency exceeding 90%," Nature Communications, Nature, vol. 16(1), pages 1-9, December.
    8. 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.
    9. Pu Wang & Xingyu Zhang & Run Shi & Jiaqi Zhao & Geoffrey I. N. Waterhouse & Junwang Tang & Tierui Zhang, 2024. "Photocatalytic ethylene production by oxidative dehydrogenation of ethane with dioxygen on ZnO-supported PdZn intermetallic nanoparticles," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    10. Ziyu Chen & Yutao Ye & Xiaoyi Feng & Yan Wang & Xiaowei Han & Yu Zhu & Shiqun Wu & Senyao Wang & Wenda Yang & Lingzhi Wang & Jinlong Zhang, 2023. "High-density frustrated Lewis pairs based on Lamellar Nb2O5 for photocatalytic non-oxidative methane coupling," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    11. Chengyang Feng & Shouwei Zuo & Miao Hu & Yuanfu Ren & Liwei Xia & Jun Luo & Chen Zou & Sibo Wang & Yihan Zhu & Magnus Rueping & Yu Han & Huabin Zhang, 2024. "Optimizing the reaction pathway of methane photo-oxidation over single copper sites," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    12. Mengyao Sun & Yanjun Chen & Xiaoqiang Fan & Dong Li & Jiaxin Song & Ke Yu & Zhen Zhao, 2024. "Electronic asymmetry of lattice oxygen sites in ZnO promotes the photocatalytic oxidative coupling of methane," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    13. 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.
    14. Jiwon Kim & Jae Hyung Kim & Cheoulwoo Oh & Hyewon Yun & Eunchong Lee & Hyung-Suk Oh & Jong Hyeok Park & Yun Jeong Hwang, 2023. "Electro-assisted methane oxidation to formic acid via in-situ cathodically generated H2O2 under ambient conditions," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    15. Yang, Le & Lin, Hongju & Fang, Zhihao & Yang, Yanhui & Liu, Xiaohao & Ouyang, Gangfeng, 2023. "Recent advances on methane partial oxidation toward oxygenates under mild conditions," Renewable and Sustainable Energy Reviews, Elsevier, vol. 184(C).
    16. 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.
    17. 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.
    18. 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.
    19. Mohamedali, Mohanned & Ayodele, Olumide & Ibrahim, Hussameldin, 2020. "Challenges and prospects for the photocatalytic liquefaction of methane into oxygenated hydrocarbons," Renewable and Sustainable Energy Reviews, Elsevier, vol. 131(C).
    20. Manav Chauhan & Bharti Rana & Poorvi Gupta & Rahul Kalita & Chhaya Thadhani & Kuntal Manna, 2024. "Tailored pore-confined single-site iron(III) catalyst for selective CH4 oxidation to CH3OH or CH3CO2H using O2," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-57854-y. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.