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Organic flexible electronics with closed-loop recycling for sustainable wearable technology

Nature Electronics volume 7, pages 39–50 (2024)Cite this article

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Abstract

Flexible organic electronics can be used to create wearable devices but the synthesis of organic electronic materials typically involves hazardous solvents, creates toxic by-products and has various other environmental and economic costs. Being able to recycle organic electronic materials and devices in an eco-friendly and economical manner is thus key for their application in sustainable wearable electronics. Here we report organic flexible electronic devices with closed-loop recycling of each component. We develop approaches to recapture and reuse organic conductors, semiconductors and gate dielectrics, and evaluate the reliability of the recycled materials. Our fabrication and recycling processes also use only eco-friendly solvents (water, anisole and acetone). We illustrate the capabilities of the approach with various recyclable organic flexible electronic devices, including electrophysiological sensing electrodes, keypads, heaters/temperature sensors, electrochemical transistors and inverters. We also develop a sustainable device cycle by reconstructing various organic flexible electronics, which are fabricated using recycled materials from different functional devices without further replenishment.

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Fig. 1: ROF electronics and recycling process.
Fig. 2: Recycling characteristics of organic components.
Fig. 3: Wearable ROF electronics.
Fig. 4: ROF a-ECT and ROF logic gate.
Fig. 5: Sustainable device cycle with closed-loop recycling of ROF electronics.

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Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.

References

  1. Nelson, J. J. M. & Schelter, E. J. Sustainable inorganic chemistry: metal separations for recycling. Inorg. Chem. 58, 979–990 (2019).

    Article  Google Scholar 

  2. Kwon, S.-J., Seo, H.-K., Ahn, S. & Lee, T.-W. Value-added recycling of inexpensive carbon sources to graphene and carbon nanotubes. Adv. Sustain. Syst. 3, 1800016 (2019).

  3. Shi, C. Q. et al. Heterogeneous integration of rigid, soft, and liquid materials for self-healable, recyclable, and reconfigurable wearable electronics. Sci. Adv. 6, eabd0202 (2020).

    Article  Google Scholar 

  4. Guo, Y. et al. Degradable and fully recyclable dynamic thermoset elastomer for 3D‐printed wearable electronics. Adv. Funct. Mater. 31, 2009799 (2020).

    Article  Google Scholar 

  5. Guo, Y. et al. A dynamically hybrid crosslinked elastomer for room‐temperature recyclable flexible electronic devices. Adv. Funct. Mater. 31, 2106281 (2021).

    Article  Google Scholar 

  6. Liu, H., Wang, L., Lin, G. & Feng, Y. Recent progress in the fabrication of flexible materials for wearable sensors. Biomater. Sci. 10, 614–632 (2022).

    Article  Google Scholar 

  7. Liu, Y. X., Wang, H. Y. & Zhu, Y. Recycling of nanowire percolation network for sustainable soft electronics. Adv. Electron. Mater. 7, 2100588 (2021).

    Article  Google Scholar 

  8. Yoo, B., Kim, Y., Han, C. J., Oh, M. S. & Kim, J. W. Recyclable patterning of silver nanowire percolated network for fabrication of flexible transparent electrode. Appl. Surf. Sci. 429, 151–157 (2018).

    Article  Google Scholar 

  9. Teng, L. et al. Liquid metal-based transient circuits for flexible and recyclable electronics. Adv. Funct. Mater. 29, 1808739 (2019).

    Article  Google Scholar 

  10. Williams, N. X., Bullard, G., Brooke, N., Therien, M. J. & Franklin, A. D. Printable and recyclable carbon electronics using crystalline nanocellulose dielectrics. Nat. Electron. 4, 261–268 (2021).

    Article  Google Scholar 

  11. Li, Y. et al. Continuous preparation of chitosan-based self-powered sensing fibers recycled from wasted materials for smart home applications. Adv. Fiber Mater. 4, 1584–1594 (2022).

    Article  Google Scholar 

  12. Sim, K. et al. Fully rubbery integrated electronics from high effective mobility intrinsically stretchable semiconductors. Sci. Adv. 5, eaav5749 (2019).

    Article  Google Scholar 

  13. Chow, P. C. Y. & Someya, T. Organic photodetectors for next-generation wearable electronics. Adv. Mater. 32, 1902045 (2020).

    Article  Google Scholar 

  14. Lee, Y. & Lee, T.-W. Organic synapses for neuromorphic electronics: from brain-inspired computing to sensorimotor nervetronics. Acc. Chem. Res. 52, 964–974 (2019).

  15. Janasz, L., Borkowski, M., Blom, P. W. M., Marszalek, T. & Pisula, W. Organic semiconductor/insulator blends for elastic field-effect transistors and sensors. Adv. Funct. Mater. 32, 2105456 (2022).

    Article  Google Scholar 

  16. Marrocchi, A., Facchetti, A., Lanari, D., Petrucci, C. & Vaccaro, L. Current methodologies for a sustainable approach to pi-conjugated organic semiconductors. Energy Environ. Sci. 9, 763–786 (2016).

    Article  Google Scholar 

  17. Xing, L. W. & Luscombe, C. K. Advances in applying C-H functionalization and naturally sourced building blocks in organic semiconductor synthesis. J. Mater. Chem. C. 9, 16391–16409 (2021).

    Article  Google Scholar 

  18. Bi, R. et al. Synthesis of sustainable production chains for phosgene-related byproducts. J. Clean. Prod. 374, 133979 (2022).

    Article  Google Scholar 

  19. Li, C.-J. & Trost, B. M. Green chemistry for chemical synthesis. Proc. Natl Acad. Sci. USA 105, 13197–13202 (2008).

  20. Bakhiya, N. & Appel, K. E. Toxicity and carcinogenicity of furan in human diet. Arch. Toxicol. 84, 563–578 (2010).

    Article  Google Scholar 

  21. Jaladanki, C. K., Taxak, N., Varikoti, R. A. & Bharatam, P. V. Toxicity originating from thiophene containing drugs: exploring the mechanism using quantum chemical methods. Chem. Res. Toxicol. 28, 2364–2376 (2015).

    Article  Google Scholar 

  22. Celebioglu, A., Topuz, F., Yildiz, Z. I. & Uyar, T. Efficient removal of polycyclic aromatic hydrocarbons and heavy metals from water by electrospun nanofibrous polycyclodextrin membranes. ACS Omega 4, 7850–7860 (2019).

    Article  Google Scholar 

  23. Frontana-Uribe, B. A., Little, R. D., Ibanez, J. G., Palma, A. & Vasquez-Medrano, R. Organic electrosynthesis: a promising green methodology in organic chemistry. Green Chem. 12, 2099–2119 (2010).

    Article  Google Scholar 

  24. Ngai, J. H. L. et al. Design and synthesis of stable indigo polymer semiconductors for organic field-effect transistors with high fluoride sensitivity and selectivity. RSC Adv. 9, 26230–26237 (2019).

    Article  Google Scholar 

  25. Api, A. M. et al. RIFM fragrance ingredient safety assessment, anisole, CAS Registry Number 100-66-3. Food Chem. Toxicol. 159, 112680 (2022).

    Article  Google Scholar 

  26. Prat, D. et al. CHEM21 selection guide of classical- and less classical-solvents. Green. Chem. 18, 288–296 (2016).

    Article  Google Scholar 

  27. Nemani, S. K. et al. Surface modification of polymers: methods and applications. Adv. Mater. Interfaces 5, 1801247 (2018).

    Article  Google Scholar 

  28. Kim, H.-J., Sim, K., Thukral, A. & Yu, C. J. Rubbery electronics and sensors from intrinsically stretchable elastomeric composites of semiconductors and conductors. Sci. Adv. 3, e1701114 (2017).

  29. Oh, J. Y. et al. Self-seeded growth of poly(3-hexylthiophene) (P3HT) nanofibrils by a cycle of cooling and heating in solutions. Macromolecules 45, 7504–7513 (2012).

    Article  Google Scholar 

  30. Lee, Y.-Y. et al. Growth mechanism of strain-dependent morphological change in PEDOT:PSS films. Sci. Rep. 6, 25332 (2016).

  31. Chou, T.-R., Chen, S.-H., Chiang, Y.-T., Lin, Y.-T. & Chao, C.-Y. Highly conductive PEDOT:PSS film by post-treatment with dimethyl sulfoxide for ITO-free liquid crystal display. Mol. Cryst. Liq. Cryst. 612, 201–210 (2015).

  32. Zhang, S. et al. Solvent-induced changes in PEDOT:PSS films for organic electrochemical transistors. APL Mater. 3, 014911 (2015).

  33. DeLongchamp, D. M. et al. Influence of a water rinse on the structure and properties of poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) films. Langmuir 21, 11480–11483 (2005).

  34. Zhang, X., Yang, W., Zhang, H., Xie, M. & Duan, X. PEDOT:PSS: from conductive polymers to sensors. Nanotechnol. Precis. Eng. 4, 045004 (2021).

    Article  Google Scholar 

  35. Xiang, L. Y., Liu, L. Y., Zhang, F. J., Di, C. A. & Zhu, D. B. Ion-gating engineering of organic semiconductors toward multifunctional devices. Adv. Funct. Mater. 31, 2102149 (2021).

    Article  Google Scholar 

  36. Thomas, E. M. et al. X‐ray scattering reveals ion‐induced microstructural changes during electrochemical gating of poly(3‐hexylthiophene). Adv. Funct. Mater. 28, 1803687 (2018).

    Article  Google Scholar 

  37. Ye, Y.-S., Rick, J. & Hwang, B.-J. Ionic liquid polymer electrolytes. J. Mater. Chem. A 1, 2719–2743 (2013).

  38. Trung, T. Q. et al. Freestanding, fiber-based, wearable temperature sensor with tunable thermal index for healthcare monitoring. Adv. Healthc. Mater. 7, 1800074 (2018).

    Article  Google Scholar 

  39. Choi, S. et al. Stretchable heater using ligand-exchanged silver nanowire nanocomposite for wearable articular thermotherapy. ACS Nano 9, 6626–6633 (2015).

    Article  Google Scholar 

  40. Wang, Y.-F. et al. Fully printed PEDOT:PSS-based temperature sensor with high humidity stability for wireless healthcare monitoring. Sci. Rep. 10, 2467 (2020).

  41. Liu, H. et al. An ultrahigh linear sensitive temperature sensor based on PANI:graphene and PDMS hybrid with negative temperature compensation. ACS Nano 16, 21527–21535 (2022).

    Article  Google Scholar 

  42. Zhang, L., Di, C. A., Yu, G. & Liu, Y. Q. Solution processed organic field-effect transistors and their application in printed logic circuits. J. Mater. Chem. 20, 7059–7073 (2010).

    Article  Google Scholar 

  43. Friedlein, J. T., McLeod, R. R. & Rivnay, J. Device physics of organic electrochemical transistors. Org. Electron. 63, 398–414 (2018).

    Article  Google Scholar 

  44. Yadav, Y., Ghosh, S. K. & Singh, S. P. High-performance organic field-effect transistors gated by imidazolium-based ionic liquids. ACS Appl. Electron. Mater. 3, 1496–1504 (2021).

    Article  Google Scholar 

  45. Kim, Y.-H., Lee, E., Um, J. G., Mativenga, M. & Jang, J. Highly robust neutral plane oxide TFTs withstanding 0.25 mm bending radius for stretchable electronics. Sci. Rep. 6, 25734 (2016).

  46. Roesing, M., Howell, J. & Boucher, D. Solubility characteristics of poly(3-hexylthiophene). J. Polym. Sci. B 55, 1075–1087 (2017).

  47. Lee, K. H. et al. ‘Cut and stick’ rubbery ion gels as high capacitance gate dielectrics. Adv. Mater. 24, 4457–4462 (2012).

    Article  Google Scholar 

  48. Lee, W. et al. Nonthrombogenic, stretchable, active multielectrode array for electroanatomical mapping. Sci. Adv. 4, eaau2426 (2018).

    Article  Google Scholar 

  49. Bontapalle, S., Na, M., Park, H. & Sim, K. Fully soft organic electrochemical transistor enabling direct skin-mountable electrophysiological signal amplification. Chem. Commun. 58, 1298–1301 (2022).

    Article  Google Scholar 

  50. Han, S. G., Polyravas, A. G., Wustoni, S., Inal, S. & Malliaras, G. G. Integration of organic electrochemical transistors with implantable probes. Adv. Mater. Technol. 6, 2100763 (2021).

    Article  Google Scholar 

  51. Shahandashti, P. F., Pourkheyrollah, H., Jahanshahi, A. & Ghafoorifard, H. Highly conformable stretchable dry electrodes based on inexpensive flex substrate for long-term biopotential (EMG/ECG) monitoring. Sens. Actuator A 295, 678–686 (2019).

  52. Zhang, L. et al. Fully organic compliant dry electrodes self-adhesive to skin for long-term motion-robust epidermal biopotential monitoring. Nat. Commun. 11, 4683 (2020).

    Article  Google Scholar 

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Acknowledgements

This work was supported by the research funds (1.200090.01 and 1.230067.01) of the Ulsan National Institute of Science & Technology (UNIST) and the National Research Foundation of Korea (NRF) grant funded by the Korean Government (NRF-2021R1C1C1007714).

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Authors and Affiliations

  1. Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST), Ulsan, Republic of Korea

    Haechan Park, Sehyun Kim, Juyeong Lee, Inwoo Lee, Sujitkumar Bontapalle, Younghoon Na & Kyoseung Sim

  2. Center for Wave Energy Materials, Ulsan National Institute of Science and Technology (UNIST), Ulsan, Republic of Korea

    Kyoseung Sim

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Contributions

H.P. and K.S. conceived the concept and designed the experiments. H.P., S.K., J.L. and I.L., prepared the materials and the fabricated devices. H.P. and J.L. characterized the device performance. H.P., S.K., I.L. and Y.N. performed the analysis of the materials. S.B. assisted H.P. to develop the materials. H.P., S.K., J.L. and K.S. analysed the experimental data. H.P. and K.S. wrote the paper. All authors reviewed and revised the paper.

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Correspondence to Kyoseung Sim.

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Nature Electronics thanks Helen Tran and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Notes 1–6 and Figs. 1–44.

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Park, H., Kim, S., Lee, J. et al. Organic flexible electronics with closed-loop recycling for sustainable wearable technology. Nat Electron 7, 39–50 (2024). https://doi.org/10.1038/s41928-023-01078-9

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