Absorptive hydrogen scavenging for enhanced aromatics yield during non-oxidative methane dehydroaromatization on Mo/H-ZSM-5 catalysts
KAUST DepartmentAdvanced Membranes and Porous Materials Research Center
Chemical Science Program
Nanostructured Functional Materials (NFM) laboratory
Physical Science and Engineering (PSE) Division
KAUST Grant NumberOSR Ref. 3325
Online Publication Date2018-10-30
Print Publication Date2018-11-19
Permanent link to this recordhttp://hdl.handle.net/10754/628928
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AbstractThe addition of Zr metal particles to MoCx/ZSM-5 in interpellet mixtures (2:1 weight ratio) resulted in maximum single-pass methane conversion of ~27% for dehydroaromatization at 973 K - in significant excess of the equilibrium prescribed ~10% conversion at these conditions - and a concurrent 1.4 - 5.6 fold increase in aromatic product yields due to circumvention of thermodynamic equilibrium limitations by absorptive hydrogen removal by Zr while retaining the cumulative aromatic product selectivity. The absorptive function of the polyfunctional catalyst formulation can be regenerated by thermal treatment in helium flow at 973 K yielding above equilibrium methane conversion in successive regeneration cycles. Hydrogen uptake experiments demonstrate formation of bulk ZrH₁.₇₅ on hydrogen absorption by zirconium at 973 K. Cooperation between absorption and catalytic centers distinct in location and function enables circumvention of persistent thermodynamic challenges in non-oxidative methane dehydrogenation.
CitationKumar A, Song K, Liu L, Han Y, Bhan A (2018) Absorptive hydrogen scavenging for enhanced aromatics yield during non-oxidative methane dehydroaromatization on Mo/H-ZSM-5 catalysts. Angewandte Chemie International Edition. Available: http://dx.doi.org/10.1002/anie.201809433.
SponsorsWe acknowledge financial support from KAUST (OSR Ref. 3325) and Office of Basic Energy Sciences, U.S. Department of Energy (Award DE-SC0019028) and thank Dr. Seema Thakral for XRD measurements as part of Characterization Facility, University of Minnesota, which receives partial support from NSF through MRSEC program.