Absorptive hydrogen scavenging for enhanced aromatics yield during non-oxidative methane dehydroaromatization on Mo/H-ZSM-5 catalysts
Type
ArticleAuthors
Kumar, AnuragSong, Kepeng
Liu, Lingmei
Han, Yu
Bhan, Aditya
KAUST Department
Advanced Membranes and Porous Materials Research CenterChemical Science Program
Nanostructured Functional Materials (NFM) laboratory
Physical Science and Engineering (PSE) Division
KAUST Grant Number
OSR Ref. 3325Online Publication Date
2018-10-30Print Publication Date
2018-11-19Date
2018-10-30Abstract
The 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.Citation
Kumar 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.Acknowledgements
We 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.Publisher
WileyJournal
Angewandte ChemieDOI
10.1002/anie.20180943310.1002/ange.201809433