2024/12/23 by Hao‐Yi Huang, Bai‐Hao Ren, Min Xie +5 · 3 citations
Chemical Engineering · Chemistry · Materials Science · #Advanced Polymer Synthesis and Characterization #Biology #Carbon dioxide utilization in catalysis #Chemistry #Combinatorial chemistry #Mechanism (biology) #Organic chemistry #Philosophy #Polyhydroxyalkanoates #Polymer #Polymer chemistry #Polymerization #biodegradable polymer synthesis and properties
paper · pdf · doi:10.1002/ange.202419494
published in Angewandte Chemie 137(7) (Wiley)
openalex publication_date 2024/12/23 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
Abstract Polyhydroxyalkanoates (PHAs) have attracted broad interest as promising sustainable materials to address plastic pollution and resource scarcity. However, the chemical synthesis of stereoregular PHAs via ring‐opening polymerization (ROP) has long been an elusive endeavor. In this contribution, we exploited a robust spiro‐salen yttrium complex ( Y3 ) as the catalyst to successfully prepare syndiotactic PHAs with diverse pendent groups. Simply altering the ratio of enantiomeric catalysts allowed to access of PHAs with diverse syndiotacticity ( P r =0.5–0.99, from sticky oil to tough materials), delivering tunable thermal properties (glass transition temperature, T g from −52 to 70 °C and melting transition temperature, T m from 38 to 223 °C). A combined experimental and computational study suggested a polymeric exchange mechanism could boost the polymerization activity and control the syndioselectivity.