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Updated: Jun 24, 2026

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Temperature-Driven Switching Between Block, Near-Statistical, and Gradient Copolymers Enabled by Multinuclear

Yoseph Kim1, So Han Kim1, Gue Seon Lee2

  • 1Department of Chemistry, Chungbuk National University, Cheongju, Chungbuk, Republic of Korea.

Macromolecular Rapid Communications
|June 23, 2026
PubMed
Summary
This summary is machine-generated.

A novel aluminum catalyst enables precise control over copolymer microstructure in ring-opening polymerization of ε-caprolactone (CL) and lactide (LA). This platform allows tunable synthesis of block, statistical, and gradient copolymers by adjusting temperature and monomer addition.

Keywords:
block copolymergradient copolymerlactidemicrostructure controlmultinuclear aluminum catalystring‐opening polymerizationtransesterificationε‐caprolactone

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Catalysis

Background:

  • Ring-opening copolymerization of ε-caprolactone (CL) and lactide (LA) is crucial for biodegradable polymers.
  • Controlling copolymer microstructure (sequence distribution) is challenging due to monomer reactivity differences and transesterification.
  • Existing methods often lack precise control over the final polymer architecture.

Purpose of the Study:

  • To develop a single catalytic platform for programmable synthesis of diverse CL/LA copolymer microstructures.
  • To investigate the influence of reaction conditions on copolymer sequence distribution.
  • To establish a kinetic-thermodynamic framework for sequence control in CL/LA copolymerization.

Main Methods:

  • Utilized a single tetrameric multinuclear aluminum catalyst for ring-opening polymerization.
  • Synthesized block copolymers via sequential monomer addition under insertion-dominated conditions.
  • Investigated simultaneous copolymerization at varying temperatures to modulate microstructure.

Main Results:

  • Achieved well-controlled synthesis of diblock, triblock, and multiblock CL/LA copolymers.
  • Demonstrated temperature-dependent control over copolymer microstructure, yielding near-statistical at low temperatures and gradient at high temperatures.
  • Observed reactivity ratios near unity and average sequence lengths of two for near-statistical copolymers.

Conclusions:

  • Multinuclear aluminum catalysis offers a versatile platform for accessing diverse CL/LA copolymer architectures.
  • Temperature is a key parameter to control the balance between propagation and transesterification, thus dictating copolymer microstructure.
  • This work provides a unified framework for sequence control and highlights earth-abundant aluminum catalysts for advanced polymer synthesis.