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<p>Organic thermoelectric generators hold great promise for powering wearable microelectronics, yet their performance is fundamentally constrained by the trade-off between electrical conductivity (<i>σ</i>) and the Seebeck coefficient (<i>S</i>). Herein, we develop a microfluidic spinning platform to fabricate PEDOT:PSS-based nonwoven fabrics with precisely engineered micro-/nanoscale physical and electronic structures, substantially enhancing thermoelectric performance. The intense shear field and in situ coagulation within microfluidic microchannels, synergized with H<sub>2</sub>SO<sub>4</sub> treatment, promotes axial orientation and coil-to-linear conformational transition of PEDOT chains, achieving multiscale structural ordering for highly efficient charge transport in the resulting fibers. A subsequent controlled NaOH‑mediated dedoping process finely tunes the Fermi level and modulates energy‑dependent scattering, yielding a final <i>σ</i> of 2038 S&#xa0;cm<sup>−1</sup> and an <i>S</i> of 29.7&#xa0;μV&#xa0;K<sup>−1</sup>. Such integrated modulation enables effective optimization of the classic <i>σ</i>-<i>S</i> trade-off, ultimately yielding a power factor of 179.8&#xa0;μW&#xa0;m<sup>−1</sup>&#xa0;K<sup>−2</sup>. Furthermore, by integrating the fabric with an electrospun PVDF-HFP radiative-cooling layer, we demonstrate a radiation-modulated fabric device capable of maintaining an in-plane temperature gradient (Δ<i>T</i> ≈ 20&#xa0;K) under natural sunlight and efficiently harvesting ambient solar-thermal energy. This study provides a versatile route for the fabrication of all-organic, flexible fabrics with high-performance thermoelectric functionality for wearable energy applications.</p>

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Microfluidic Spinning Boosting Thermoelectric Performance of PEDOT:PSS Nonwoven Fabrics

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月20日

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  • Yuhui Zhang,
  • Hui Qiu,
  • Jian Yang,
  • Pengle Cao,
  • Yu Wang,
  • An-Quan Xie,
  • Ke-Qin Zhang,
  • Xiao-Qiao Wang

摘要

Organic thermoelectric generators hold great promise for powering wearable microelectronics, yet their performance is fundamentally constrained by the trade-off between electrical conductivity (σ) and the Seebeck coefficient (S). Herein, we develop a microfluidic spinning platform to fabricate PEDOT:PSS-based nonwoven fabrics with precisely engineered micro-/nanoscale physical and electronic structures, substantially enhancing thermoelectric performance. The intense shear field and in situ coagulation within microfluidic microchannels, synergized with H2SO4 treatment, promotes axial orientation and coil-to-linear conformational transition of PEDOT chains, achieving multiscale structural ordering for highly efficient charge transport in the resulting fibers. A subsequent controlled NaOH‑mediated dedoping process finely tunes the Fermi level and modulates energy‑dependent scattering, yielding a final σ of 2038 S cm−1 and an S of 29.7 μV K−1. Such integrated modulation enables effective optimization of the classic σ-S trade-off, ultimately yielding a power factor of 179.8 μW m−1 K−2. Furthermore, by integrating the fabric with an electrospun PVDF-HFP radiative-cooling layer, we demonstrate a radiation-modulated fabric device capable of maintaining an in-plane temperature gradient (ΔT ≈ 20 K) under natural sunlight and efficiently harvesting ambient solar-thermal energy. This study provides a versatile route for the fabrication of all-organic, flexible fabrics with high-performance thermoelectric functionality for wearable energy applications.