Trace Compounds Confined in SAPO-34 and a Probable Evolution Route of Coke in the MTO Process

SAPO-34中痕量化合物的含量及其在MTO工艺中焦炭的可能演化路径

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Abstract

Confined compounds in SAPO-34 cages are important to understand the activation and deactivation mechanisms of the methanol-to-olefin process. In this work, gas chromatography-mass spectrometry (GC-MS) chromatograms of CCl(4)-extracted samples of used SAPO-34 were denoised by subtracting signals of air compounds and stationary phase bleeding of the chromatographic column, which enhanced the identification of trace compounds. In addition to the generally noted methyl aromatics, this work also identified alkanes, cycloalkanes, alkyl (ethyl, propyl, and butyl) compounds, partially saturated compounds, and bridged compounds. These novel identified trace compounds favor the evolution route depiction of monocyclic, bicyclic, tricyclic, tetracyclic, and multicore hydrocarbons in the SAPO-34 cage. Confined compounds should grow via step-by-step alkylation, cyclization, and aromatization processes. C(2+) side chains, especially C(3+), favor the growth of rings. Alkyldihydroindenes should be key intermediates between monocyclic and bicyclic aromatics. Bridged soluble compounds provide evidence that insoluble coke is formed across cages in the SAPO-34 crystal.

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