Concerted methane fixation at ambient temperature and pressure mediated by an alcohol oxidase and Fe-ZSM-5 catalytic couple
Journal
Nature Catalysis
Journal Volume
7
Journal Issue
12
Start Page
1359
End Page
1371
ISSN
2520-1158
Date Issued
2024-12-04
Author(s)
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. (Figure presented.)
Publisher
Springer Science and Business Media LLC
Type
journal article