Abstract
The aromatization of light alkanes (C4-C6) is an important value-added reaction. However, the yield of aromatics is always limited by the simultaneous generation of small alkanes (CH4 and C2H6) due to H/C balance. Herein, we demonstrate that the introduction of CO into light alkanes over zeolites significantly enhanced aromatic selectivity and an aromatics selectivity of 85% was achieved in the case of cyclopentane and CO coupling reaction over H-ZSM-5. Methyl-substituted cyclopentenones were observed and considered as the most important intermediates for aromatics formation. Multiple characterizations revealed the coupling mechanism: (1) CO inserts into carbenium ions to form acylium cations, (2) acylium cations react with olefins to generate unsaturated ketones, (3) unsaturated ketones cyclize to methyl-substituted cyclopentenones, (4) methyl-substituted cyclopentenones convert to monocytic aromatics. Methyl-substituted indanones were also discovered causing the generation of binuclear aromatics, such as naphthalene. Nano-sized ZSM-5 and TEOS modifications were applied to enhance the BTX selectivity.
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