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Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interface
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Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interface
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Journal Article
Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interface
2025
Overview
Photo-oxidation of methane (CH
4
) using hydrogen peroxide (H
2
O
2
) synthesized in situ from air and water under sunlight offers an attractive route for producing green methanol while storing intermittent solar energy. However, in commonly used aqueous-phase systems, photocatalysis efficiency is severely limited due to the ultralow availability of CH
4
gas and H
2
O
2
intermediate at the flooded interface. Here, we report an atomically modified metal-organic framework (MOF) membrane nanoreactor that promotes direct CH
4
photo-oxidation to methanol at the gas-solid interface in a reticular open framework. We show that the domino synergy between colocalized single-atom palladium and iron on MOF nodes enables efficient generation and in situ utilization of H
2
O
2
in the absence of liquid water, thus circumventing H
2
O
2
dilution. Meanwhile, the “breathable” MOF membrane, optimized by solar-driven interfacial water management, provides high-flux channels to facilitate efficient gas diffusion and rapid methanol desorption and transfer. As a result, we demonstrate over 210 hours of continuous photosynthesis of 0.25 M methanol with unity selectivity, achieving an exceptional methanol productivity of 14.4 millimoles per gram of catalyst per hour.
The photooxidation of CH
4
to CH
3
OH is limited by the availability of reactants at flooded interfaces. Now the authors report a modified metal organic framework nanoreactor to promote the direct photooxidation of CH4 to CH
3
OH at the gas-solid interface.
