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<p>Poly(<i>L</i>-lactide) (PLLA) is one of the best candidates as a bio-based plastic material for circular economy because of its biodegradability, sustainability, recyclability, and good thermal and mechanical properties. The industrial production of PLLA is mainly from tin(II) 2-ethylhexanoate [Sn(Oct)<sub>2</sub>]-catalyzed ring-opening polymerization (ROP) of <i>L</i>-LA in melt and bulk conditions at high temperatures (150–200 °C). Despite the huge efforts devoted to the development of organometallics with low toxicity and many highly active catalysts under mild laboratory conditions, very few candidates can compete with Sn(Oct)<sub>2</sub> under industrially relevant conditions. Herein, we report novel zinc complexes bearing phenylimino-pyridine-phenolate ligands as efficient catalysts for <i>L</i>-LA polymerization under both mild and industrially relevant conditions, with a turnover frequency as high as 6200 h<sup>−1</sup>. The best performing catalyst competed well with Sn(Oct)<sub>2</sub> under industrial conditions and afforded colorless and semicrystalline PLLA. In addition, preliminary depolymerization experiments suggested that the new catalysts can also be used for the chemical recycling of commercial PLLA directly to <i>L</i>-LA with high selectivity under bulk and melt conditions.</p>

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Phenylimino-pyridine-phenolate Zinc Complexes for Polylactide Synthesis and Chemical Recycling to Monomers

  • 期刊论文

  • 发表日期：

    2025年1月25日

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  • Jia-Yue Li,
  • Ming-Qian Wang,
  • Zhi-Qiang Ding,
  • He He,
  • Xin-Cui Shi,
  • Bin Wang

摘要

Poly(L-lactide) (PLLA) is one of the best candidates as a bio-based plastic material for circular economy because of its biodegradability, sustainability, recyclability, and good thermal and mechanical properties. The industrial production of PLLA is mainly from tin(II) 2-ethylhexanoate [Sn(Oct)2]-catalyzed ring-opening polymerization (ROP) of L-LA in melt and bulk conditions at high temperatures (150–200 °C). Despite the huge efforts devoted to the development of organometallics with low toxicity and many highly active catalysts under mild laboratory conditions, very few candidates can compete with Sn(Oct)2 under industrially relevant conditions. Herein, we report novel zinc complexes bearing phenylimino-pyridine-phenolate ligands as efficient catalysts for L-LA polymerization under both mild and industrially relevant conditions, with a turnover frequency as high as 6200 h−1. The best performing catalyst competed well with Sn(Oct)2 under industrial conditions and afforded colorless and semicrystalline PLLA. In addition, preliminary depolymerization experiments suggested that the new catalysts can also be used for the chemical recycling of commercial PLLA directly to L-LA with high selectivity under bulk and melt conditions.