Magnetically tunable selectivity in methane oxidation enabled by Fe-embedded liquid metal catalysts
As they are liquids at room temperature, gallium-based metal substrates allow catalytic metal atoms to move freely without lattice constraints, thereby facilitating the development of catalysts with reconfigurable structures. Here we design an iron-embedded liquid metal catalyst that enables reversible switching of the aggregation and electron spin of iron atoms by controlling an external magnetic field. This facilitates a reversible conversion of the primary liquid products, methyl hydroperoxide (CH<sub>3</sub>OOH) and acetic acid (CH<sub>3</sub>COOH), under ambient conditions. The catalyst achieves promising production rates (CH<sub>3</sub>OOH, 1,679.6 <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mstyle><mml:mrow><mml:mi>m</mml:mi></mml:mrow> </mml:mstyle> <mml:mstyle><mml:mrow><mml:mi>m</mml:mi></mml:mrow> </mml:mstyle> <mml:mstyle><mml:mrow><mml:mi>o</mml:mi></mml:mrow> </mml:mstyle> <mml:mstyle><mml:mrow><mml:mi>l</mml:mi></mml:mrow> </mml:mstyle> </mml:mrow> <mml:mspace></mml:mspace> <mml:msubsup> <mml:mrow> <mml:mstyle><mml:mrow><mml:mi>g</mml:mi></mml:mrow> </mml:mstyle> </mml:mrow> <mml:mrow> <mml:mstyle><mml:mrow><mml:mi>F</mml:mi></mml:mrow> </mml:mstyle> <mml:mstyle><mml:mrow><mml:mi>e</mml:mi></mml:mrow> </mml:mstyle> </mml:mrow> <mml:mrow><mml:mo>-</mml:mo> <mml:mn>1</mml:mn></mml:mrow> </mml:msubsup> <mml:mspace></mml:mspace> <mml:msup> <mml:mrow> <mml:mstyle><mml:mrow><mml:mi>h</mml:mi></mml:mrow> </mml:mstyle> </mml:mrow> <mml:mrow><mml:mo>-</mml:mo> <mml:mn>1</mml:mn></mml:mrow> </mml:msup> </mml:math> ; CH<sub>3</sub>COOH, 790.5 <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mstyle><mml:mrow><mml:mi>m</mml:mi></mml:mrow> </mml:mstyle> <mml:mstyle><mml:mrow><mml:mi>m</mml:mi></mml:mrow> </mml:mstyle> <mml:mstyle><mml:mrow><mml:mi>o</mml:mi></mml:mrow> </mml:mstyle> <mml:mstyle><mml:mrow><mml:mi>l</mml:mi></mml:mrow> </mml:mstyle> </mml:mrow> <mml:mspace></mml:mspace> <mml:msubsup> <mml:mrow> <mml:mstyle><mml:mrow><mml:mi>g</mml:mi></mml:mrow> </mml:mstyle> </mml:mrow> <mml:mrow> <mml:mstyle><mml:mrow><mml:mi>F</mml:mi></mml:mrow> </mml:mstyle> <mml:mstyle><mml:mrow><mml:mi>e</mml:mi></mml:mrow> </mml:mstyle> </mml:mrow> <mml:mrow><mml:mo>-</mml:mo> <mml:mn>1</mml:mn></mml:mrow> </mml:msubsup> <mml:mspace></mml:mspace> <mml:msup> <mml:mrow> <mml:mstyle><mml:mrow><mml:mi>h</mml:mi></mml:mrow> </mml:mstyle> </mml:mrow> <mml:mrow><mml:mo>-</mml:mo> <mml:mn>1</mml:mn></mml:mrow> </mml:msup> </mml:math> ) and high selectivities (CH<sub>3</sub>OOH, 99.9%; CH<sub>3</sub>COOH, 91.7%). In the absence of the magnetic field, iron atoms are atomically dispersed, leading to the C1 pathway without C-C bond coupling. When a magnetic field is applied, iron atoms cluster, favouring CH<sub>3</sub>COOH production in the C2 pathway. The product distribution can be finely and reversibly tuned with magnetic field intensity adjustments ranging from 0 to 500 G. Our findings highlight the potential for using an external magnetic field to precisely control catalytic pathways.
Authors
- Rui Huang (ORCID: https://orcid.org/0000-0001-5952-2936)
- Yu Mao (ORCID: https://orcid.org/0000-0002-4656-2864)
- Yuen Shing Wu (ORCID: https://orcid.org/0000-0001-9524-2843)
- Yinhe Wang (ORCID: https://orcid.org/0000-0002-6177-7345)
- Haoran Zhang (ORCID: https://orcid.org/0009-0000-5633-3179)
- Weijie Zhong (ORCID: https://orcid.org/0009-0004-2041-0987)
- Zhiwen Zhang (ORCID: https://orcid.org/0000-0002-0797-9448)
- Jun Jiang (ORCID: https://orcid.org/0000-0002-6116-5605)
- Xiaokang Liu (ORCID: https://orcid.org/0000-0001-5614-1601)
- Zhi Liu (ORCID: https://orcid.org/0000-0002-8973-6561)
- Lei Zheng (ORCID: https://orcid.org/0000-0001-6222-2344)
- Tao Yao (ORCID: https://orcid.org/0000-0001-8699-8294)
- Yu Zhang (ORCID: https://orcid.org/0009-0008-3715-1239)
- Fan Wu (ORCID: https://orcid.org/0009-0006-4064-9279)
- Lin Hu (ORCID: https://orcid.org/0000-0001-7070-7210)
- Sicong Wang (ORCID: https://orcid.org/0009-0009-6779-5112)
- Jun Cai (ORCID: https://orcid.org/0000-0002-3806-7230)
- Zhou Huang
- Yihua Ran
Institutions
- University of Science and Technology of China (CN)
- Hefei University of Technology (CN)
- Chinese Academy of Sciences (CN)
- Hefei Institutes of Physical Science (CN)
- ShanghaiTech University (CN)
- Henan Academy of Sciences (CN)
- High Magnetic Field Laboratory (CN)
- Shanghai Institute of Microsystem and Information Technology (CN)
- National Synchrotron Radiation Laboratory (CN)
Publication Details
- Journal
- Nature Nanotechnology
- Published
- 2025-11-03
- DOI
- https://doi.org/10.1038/s41565-025-02029-5
- Citations
- 5
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 1.82
Funders
- National Natural Science Foundation of China
- Chinese Academy of Sciences
- University of Science and Technology of China
- National Synchrotron Radiation Laboratory
- Natural Science Foundation of Anhui Province
- Hefei Science Center, Chinese Academy of Sciences
- Beijing Synchrotron Radiation Facility
- High Magnetic Field Laboratory, Chinese Academy of Sciences