Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 5, Issue 11, Pages 5023-5036Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5cy00934k
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Funding
- National Energy Technology Laboratory under RES [DE-FE0004000]
- Department of Energy, National Energy Technology Laboratory, an agency of the United States Government
- AECOM Energy & Construction, Inc.
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The effectiveness of hydrogen-permselective palladium membrane reactors for non-oxidative methane dehydroaromatization (MDA) over 4 wt% Mo/HZSM-5 catalysts was investigated as a function of weight hourly space velocity (WHSV) at 700 degrees C and atmospheric pressure. CH4 conversion and aromatic product yield decrease with increasing WHSV from 750 to 9000 cm(3) g(cat)(-1) h(-1). C6H6 is the main C-containing product at and below 3000 cm(3) g(cat)(-1) h(-1) whereas C2H4 dominates the C-product distribution at higher WHSVs. Due to selective removal of H-2 from the reaction products in catalytic membrane reactors, C6H6 yield is significantly improved over the whole WHSV range compared to those obtained in fixed-bed reactors. H-2 recovery is strongly influenced by WHSV as it decreases from 48.3% at 750 cm(3) g(cat)(-1) h(-1) to 6.8% at 9000 cm(3) g(cat)(-1) h(-1). There exists a trade-off between catalytic activity and H-2 recovery, which results in the maximum enhancement (similar to 360%) in C6H6 yield at 3000 cm(3) g(cat)(-1) h(-1). At this intermediate space velocity, the largest concentration of H-2 is found in the retentate stream and helps alleviate coke accumulation particularly on HZSM-5. Carbon is deposited on the inner surface of the membrane reactor portion in contact with the catalyst bed and transports to the outer surface, thus causing H-2 permeability to decrease over the 15 h reaction period.
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