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Depolymerizable and recyclable luminescent polymers with high light-emitting efficiencies

Nature Sustainability volume 7, pages 1048–1056 (2024)Cite this article

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Abstract

Luminescent polymers are of great interest in a number of photonic technologies, including electroluminescence, bioimaging, medical diagnosis, bio-stimulation and security signage. Incorporating depolymerizability and recyclability into luminescent polymers is pivotal for promoting their sustainability and minimizing their environmental impacts at the end of the product lifecycle, but existing strategies often compromise the light-emitting efficiencies. Here we develop a strategy that utilizes cleavable moiety to create depolymerizable and recyclable thermally activated delayed fluorescence (TADF) polymers without compromising their high light-emitting efficiencies. The electroluminescent devices based on the TADF polymers achieved a high external quantum efficiency of up to 15.1 %. The TADF polymers can be depolymerized under either mild acidic or heating conditions, with precise control of the kinetics, and the obtained pure monomers can potentially be isolated and repolymerized for subsequent life applications. This work promotes the end-of-life environmental friendliness and circularity of luminescent materials, paving the way to a sustainable photonic industry.

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Fig. 1: Depolymerizable luminescent polymers based on TADF mechanism and cleavable chemistry.
Fig. 2: PL and EL properties of the depolymerizable TADF polymer PDKCE.
Fig. 3: The depolymerizability of PDKCE.
Fig. 4: The recyclability of the TADF moiety in PDKCE.
Fig. 5: Depolymerizable host polymer PC6E.

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Data availability

The data that support the findings of this study are available within this article and its Supplementary Information. Additional data are available from the corresponding authors upon request. Source data are provided with this paper.

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Acknowledgements

W.L., Y.W. and J.X. acknowledge the Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the US Department of Energy under contract no. DE-AC02-06CH11357. Work performed at the Center for Nanoscale Materials, a US Department of Energy Office of Science User Facility, was supported by the US DOE, Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. S.W. acknowledges the National Science Foundation CAREER award no. 2239618, and the University of Chicago Materials Research Science and Engineering Center, which is funded by the National Science Foundation under Award No. DMR-2011854. TGA–MS measurements were performed at the Materials Characterization and Imaging Facility which receives support from the MRSEC Program (NSF DMR-1720139) of the Materials Research Center at Northwestern University. P.G. acknowledges the support from the US Air Force Office of Scientific Research (grant no. FA9550-22-1-0209).

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Author notes

  1. Hyocheol Jung

    Present address: Center for Advanced Specialty Chemicals, Division of Specialty and Bio-based Chemicals Technology, Korea Research Institute of Chemical Technology, Ulsan, Republic of Korea

  2. These authors contributed equally: Wei Liu, Yukun Wu.

Authors and Affiliations

  1. Pritzker School of Molecular Engineering, The University of Chicago, Chicago, IL, USA

    Wei Liu, Cheng Zhang, Glingna Wang, Sihong Wang & Jie Xu

  2. Nanoscience and Technology Division, Argonne National Laboratory, Lemont, IL, USA

    Yukun Wu, Aikaterini Vriza, Hyocheol Jung, Benjamin T. Diroll, Richard D. Schaller, Henry Chan, Sihong Wang & Jie Xu

  3. Department of Chemistry, Purdue University, West Lafayette, IN, USA

    Yukun Wu & Jianguo Mei

  4. Applied Materials Division, Argonne National Laboratory, Lemont, IL, USA

    Shiyu Hu & Yuepeng Zhang

  5. Department of Chemical and Environmental Engineering, Yale University, New Haven, CT, USA

    Du Chen & Peijun Guo

  6. Energy Sciences Institute, Yale University, West Haven, CT, USA

    Du Chen & Peijun Guo

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Contributions

J.X. conceived the research. W.L., Y.W. and J.X. designed the experiments. A.V., C.Z. and H.C. performed the simulation. S.H. and Y.Z. helped with printing demonstrations. B.T.D. and R.D.S performed the PL transient decay measurement. C.Z. and G.W. carried out the PLQY measurement. D.C. and P.G. helped with the measurement of low-temperature FL/PH spectra. H.J. helped with initial exploratory experiments for degradable light-emitting polymer. J.M., S.W. and J.X. supervised the research. W.L., Y.W., J.M., S.W. and J.X. wrote the paper. All the authors contributed to the discussion and paper revision.

Corresponding authors

Correspondence to Jianguo Mei, Sihong Wang or Jie Xu.

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Competing interests

J.X., Y.W. and W.L. are inventors on a pending patent filed by the Argonne National Laboratory (IN-23-027). All other authors declare no competing interests.

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Nature Sustainability thanks Xiaohong Zhang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–30 and Table 1.

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Supplementary Video 1

The demonstrate of the hidden code with non-depolymerizable PDKCM serving as the code and depolymerizable PDKCE serving as the ‘disguise’.

Source data

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Liu, W., Wu, Y., Vriza, A. et al. Depolymerizable and recyclable luminescent polymers with high light-emitting efficiencies. Nat Sustain 7, 1048–1056 (2024). https://doi.org/10.1038/s41893-024-01373-z

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