4.7 Article

Excess soluble alkalis to prepare highly efficient MgO with relative low surface oxygen content applied in DMC synthesis

Journal

SCIENTIFIC REPORTS
Volume 11, Issue 1, Pages -

Publisher

NATURE PORTFOLIO
DOI: 10.1038/s41598-021-00323-5

Keywords

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Funding

  1. National Key Research and Development Plan, China [2018YFB0604500]
  2. Key Task and Local Project in Science & Technology of SYUCT, China [LDB2019005]
  3. High-Level Innovation Team Overseas Training Project of Liaoning, China [2018LNGXGJWPY-ZD002]
  4. Project for Innovative Talents in Liaoning Province, China [LR2016015]

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The study found that the MgO-P-Na2CO3-3.14 catalyst synthesized by excess Na2CO3 precipitation exhibited the best activity and stability in the transesterification of ethylene carbonate with methanol, with a DMC yield as high as 69.97% and the ability to be reused seven times without deactivation. The transesterification reaction could be separated into two steps, with catalysts containing more crystalline magnesium carbonate promoting DMC yield, and those with more Mg-O pairs showing superior transesterification ability.
The activities of various MgO catalysts, which were prepared from different methods such as hydration synthesis, thermal decomposition, combustion, sol-gel and co-precipitation, were conducted in dimethyl carbonate (DMC) synthesis via transesterification of ethylene carbonate with methanol. MgO-P-Na2CO3-3.14 synthesized by the excess Na2CO3 precipitation compared the best catalytic activity and stability, which could be reused for seven times without obvious deactivation. The DMC yield was as high as 69.97% at 68 degrees C. The transesterification reaction could be separated into two steps, and the samples obtained by NaOH precipitant exhibited better ring-opening capability, while the catalysts acquired by Na2CO3 precipitant displayed superior transesterification ability. The structure-performance relationship was evaluated by multiple characterization methods. The results indicated that the as-synthesized catalyst derived from dried precursors with more crystalline magnesium carbonate was favorable for the promotion of DMC yield, and MgO-P-Na2CO3-3.14 with more Mg-O pairs, which were the active center for the transesterification of 2-hydroxyethyl methyl carbonate (HEMC) intermediate with methanol, resulted in more moderately basic sites left that was in accordance with the DMC yield variation. MgO-P-Na2CO3-3.14 with greater BET surface area and mesopore volume, relative low surface oxygen content and larger moderately basic sites amount compared the excellent activity in DMC synthesis.

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