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Concerted methane fixation at ambient temperature and pressure mediated by an alcohol oxidase and Fe-ZSM-5 catalytic couple

Nature Catalysis volume 7, pages 1359–1371 (2024)Cite this article

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Abstract

Anthropogenic methane emissions, particularly from diffuse and dilute sources, pose a significant challenge for oxidation and valorization as existing methane oxidation routes rely on high temperatures or pressures. Here we report the catalytic coupling of alcohol oxidase with the iron-modified ZSM-5 (Fe-ZSM-5) zeolite catalyst, creating a tandem methanotrophic system that partially oxidizes methane at ambient temperatures and pressures. Methane reacts at Fe-ZSM-5 to produce methanol, which is then oxidized at the enzyme to formaldehyde and hydrogen peroxide. The latter subsequently reacts back at Fe-ZSM-5 and oxidizes methane in a catalytic couple. We show that methane-to-formaldehyde selectivity can exceed 90% at room temperature. The generated formaldehyde was rapidly incorporated into a growing urea polymer, with a material growth rate exceeding 5.0 mg gcat−1 h−1, which matches or exceeds the growth rates of many methanotrophic organisms. This work presents a sustainable route for methane oxidation, driven by oxygen in the air under ambient conditions, producing high-value polymers and valorizing methane emission streams.

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Fig. 1: Tandem catalysis of Fe-ZSM-5 and AOX for the partial oxidation of methane.
Fig. 2: Growing urea-formaldehyde polymer production.
Fig. 3: Characterization of urea-formaldehyde materials.
Fig. 4: Formation of TiO2/urea-formaldehyde nanocomposites.

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The data that support the findings of this study are available within the Article and its Supplementary Information or from the corresponding author upon reasonable request.

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Acknowledgements

We would like to acknowledge the support of funding from the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (Grant DE-FG02-08ER46488). SEM, TEM, ICP-OES and XPS were carried out in part through the use of MIT.nano Characterization Facilities. We thank the MIT Department of Chemistry Instrumentation Facility for the use of their NMR spectrometers. This material is based on work sponsored in part by the US Army DEVCOM ARL Army Research Office through the MIT Institute for Soldier Nanotechnologies under Cooperative Agreement number W911NF-23-2-0121. We thank Y.-M. Jo and M. Dinca for the Brunauer–Emmett–Teller measurement of the ZSM-5 catalysts. We thank R. Zhu and Y. Roman for the ultraviolet-visible measurement of the ZSM-5 catalysts.

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Author notes

  1. Yu-Ming Tu

    Present address: Department of Chemical Engineering, National Taiwan University, Taipei, Taiwan

  2. These authors contributed equally: Daniel J. Lundberg, Jimin Kim.

Authors and Affiliations

  1. Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    Daniel J. Lundberg, Jimin Kim, Yu-Ming Tu, Cody L. Ritt & Michael S. Strano

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Contributions

M.S.S. supervised the project. M.S.S. and D.J.L. conceived the idea. D.J.L. and J.K. designed and carried out the experiments. Y.-M.T. carried out the TEM and TGA analyses. C.L.R. carried out the TEM analyses and methane oxidation reactions. All authors discussed the results and wrote the manuscript.

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Correspondence to Michael S. Strano.

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Nature Catalysis thanks Damien Debecker, Richard Lewis, Feng-Shou Xiao and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Lundberg, D.J., Kim, J., Tu, YM. et al. Concerted methane fixation at ambient temperature and pressure mediated by an alcohol oxidase and Fe-ZSM-5 catalytic couple. Nat Catal 7, 1359–1371 (2024). https://doi.org/10.1038/s41929-024-01251-z

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