The overarching goal of this project is to develop a significantly process-intensified technology for methane dehydrogenation to aromatic (i.e., benzene) (MDA) in highly compacted microchannel protonic ceramic membrane reactors (HCM-PCMRs) by integrating multiple functions of single-atom catalysis, electrocatalysis, membrane catalysis, membrane separation, and advanced manufacturing.

Clemson University, Clemson, SC 29634

Collaborators
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN 37830
 

The current technologies for natural gas to liquid (GTL) are facing significant challenges: 1) the deployment and intermittent operation at isolated sites often lack convenient access to electricity, make-up water, and other required services; and 2) the GTL technologies (e.g., indirect catalytic conversion of methane to liquid chemicals via synthesis gas) are confirmed to be complicated, inefficient, and environment unfriendly (enormous CO₂ emission), requiring large economies of scale to compete in existing commodity markets, and relying on extensive supporting infrastructure to be available.  This three-year project will be conducted by a multidisciplinary team consisting of researchers from Clemson University and Oak Ridge National Laboratory, to develop a significantly process-intensified technology for methane dehydrogenation to aromatic in highly compacted microchannel protonic ceramic membrane reactors.
 

The major benefits of the proposed technology, as compared with state-of-art industrial GTL technology, are: 1) highly intensified process: highly compacted catalytic membrane reactors; 2) long term stability: less coke problem because of single-atom catalyst and small amount oxygen ion; 3) high benzene yield at a lower temperature: single-atom catalyst, membrane separation, and membrane catalysis; 4) high volumetric performance: microchannel design; 5) isolated operation: co-production of electricity or hydrogen; 6) flexible and cost-effective manufacturing: integrated additive manufacturing and laser process.

• Tested theoretical energy requirement of MDA in electrocatalytic protonic ceramic membrane reactors. 
• Reproducible, high-quality, tubular PCMRs with the targeted area (>10cm² ) and peak power density (300mW/cm² at 650°C) were fabricated successfully by an Integrated Additive Manufacturing and Laser Processing (I-AMLP) technique. The PCMRs are ready for long-term testing of fuel cell performance.
• Completed a long-term test of tubular PCMRs in the fuel cell mode. The successful test lasted for more than 250h. 
• Manufactured interdigital microchannel PCMRs with channel width around 200μm-300μm and fully dense membranes. 
• Developed the testing reactor for running MDA using tubular single-cell with packed catalyst powders. 
• Directly compared fixed-bed type reactor (FBR, black) with co-ionic membrane reactor. Found a catalyst for converting methane to benzene at a low reaction temperature but also demonstrated the effectiveness of the co-ionic membrane reactor. 
   

$1,000,000

$250,000

NETL — Anthony Zammerilli (anthony.zammerilli@netl.doe.gov or 304-285-4641)
Clemson University — Joshua Tong (jianhut@clemson.edu or 864-656-4954)