Catalytic upgrading of coal pyrolysis volatiles by Ga-substituted mesoporous ZSM-5
FUEL(2020)
Abstract
Five MFI-type zeolite catalysts, which were aluminosilicate ZSM-5 (Z5), gallium-substituted silicalite-1 (Ga-S1), mesoporous ZSM-5 (MZ5), gallium-substituted mesoporous silicalite-1 (Ga-MS1) and gallium-substituted mesoporous ZSM-5 (Ga-MZ5), were hydrothermally synthesized with combined using of TPAOH and TPOAC as micropore and mesopore structure-directing agents respectively, followed by the application in the catalytic upgrading of volatiles from low-rank coal fast pyrolysis. The obtained results indicated that significant improvements with the yield of high value-added products of BTEXN (benzene, toluene, ethylbenzene, xylene and naphthalene) increased from 5.4 mg.g(-1 )to 11.9-26.4 mg.g(-1), as well as the content of light fractions ( < 300 degrees C) in coal tars increased from 51% to 65-88% were realized by using the representative MFI-type zeolite catalysts in contrast to non-catalyst pyrolysis. Moreover, the possible mechanism for catalytic upgrading over the best-performing catalyst of gallium-substituted mesoporous ZSM-5 (Ga-MZ5) with the highest yield of aromatics and effective reduction of phenols was proposed on the basis of systematic comparison of structural features and catalytic performances of various MFI-type zeolite catalysts and fundamental study of the synergetic effects dominated by acidity, ratio of Bronsted/Lewis acid sites, intra-/extra-framework gallium species and hierarchical meso-/microporosity.
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Key words
Coal volatiles,Catalytic upgrading,Mesoporous zeolite,MFI,Gallium substitution
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