用串联法在贱金属催化剂上将PET升级为CHDM

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-03-23 DOI:10.1016/j.apcata.2025.120233

Wanzhen Ren , Chuan Gang , Chen Zhao , Peng Wu , Xiaohong Li

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引用次数: 0

摘要

1,4-环己二甲醇（CHDM）是一种重要的聚酯单体，其结构单元与PET（聚对苯二甲酸乙二醇酯）相似。因此，PET可以通过串联醇解和选择性加氢直接定向合成CHDM。然而，钯或钌等贵金属催化剂的使用限制了工业应用。本研究提出了在ch3oh -1,4-二氧六环的混合溶剂中，通过三步反应将PET转化为CHDM的新工艺，无需贵金属催化剂或任何分离纯化，首先将PET甲醇分解得到对苯二甲酸二甲酯（DMT），然后将DMT在nla -40wt%催化剂上加氢生成中间产物二甲基1,4-环己二羧酸二甲酯（DMCD）。然后在Cu1Fe1Al0.5催化剂上将DMCD进一步氢解为CHDM，得到CHMD， CHDM的总收率为0.90.2 %。重要的是，由于CHDM与副产物的沸点存在显著差异，因此仅通过蒸馏就可以很容易地分离出最终产物CHDM。

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Upgrading of PET to CHDM over base metal catalysts via tandem processes

1,4-cyclohexanedimethanol (CHDM), which has similar structural units to PET (polyethylene terephthalate), is a crucial polyester monomer. Therefore, PET can be directly oriented to synthesize CHDM through tandem alcoholysis and selective hydrogenation. However, use of precious metal catalysts such as Pd or Ru catalyst limits the industrial application. Herein, we developed a new process that converts PET into CHDM in mixed solvent of CH₃OH-1,4-dioxane via tandem three-step reactions without the involvement of precious metal catalysts or any separation or purification, including the methanolysis of PET to obtain dimethyl terephthalate (DMT) first, then DMT was hydrogenated over a NiLa-40wt% catalyst to form the intermediate dimethyl 1,4-cyclohexanedicarboxylate (DMCD), followed by the further hydrogenolysis of DMCD to CHDM over a Cu₁Fe₁Al_0.5 catalyst to yield CHMD with an overall CHDM yield of .90.2 %. Importantly, the final product CHDM could be separated easily just by distillation because there is a significant difference in the boiling point of CHDM with the by-products.

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.