Mechanochemically accessing a challenging-to-synthesize depolymerizable polymer

Tze-Gang Hsu, Shiqi Liu, Xin Guan, Seiyoung Yoon, Junfeng Zhou, Wei-Yuan Chen, Sanjay Gaire, Joshua Seylar, Hanlin Chen, Zeyu Wang, Jared Rivera, Leyao Wu, Christopher J. Ziegler, Ruel McKenzie and Junpeng Wang ()
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Tze-Gang Hsu: The University of Akron
Shiqi Liu: The University of Akron
Xin Guan: The University of Akron
Seiyoung Yoon: The University of Akron
Junfeng Zhou: The University of Akron
Wei-Yuan Chen: The University of Akron
Sanjay Gaire: The University of Akron
Joshua Seylar: The University of Akron
Hanlin Chen: The University of Akron
Zeyu Wang: The University of Akron
Jared Rivera: The University of Akron
Leyao Wu: The University of Akron
Christopher J. Ziegler: The University of Akron
Ruel McKenzie: The University of Akron
Junpeng Wang: The University of Akron

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract Polymers with low ceiling temperatures (Tc) are highly desirable as they can depolymerize under mild conditions, but they typically suffer from demanding synthetic conditions and poor stability. We envision that this challenge can be addressed by developing high-Tc polymers that can be converted into low-Tc polymers on demand. Here, we demonstrate the mechanochemical generation of a low-Tc polymer, poly(2,5-dihydrofuran) (PDHF), from an unsaturated polyether that contains cyclobutane-fused THF in each repeat unit. Upon mechanically induced cycloreversion of cyclobutane, each repeat unit generates three repeat units of PDHF. The resulting PDHF completely depolymerizes into 2,5-dihydrofuran in the presence of a ruthenium catalyst. The mechanochemical generation of the otherwise difficult-to-synthesize PDHF highlights the power of polymer mechanochemistry in accessing elusive structures. The concept of mechanochemically regulating the Tc of polymers can be applied to develop next-generation sustainable plastics.

Date: 2023
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DOI: 10.1038/s41467-023-35925-2

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