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<p>Ionic thermocells offer a compelling route for converting low-grade heat into electricity, yet their real-world deployment is hindered by performance decay under fluctuating conditions and limited synergistic pathways. Herein, we introduce polyethyleneimine as a self-limiting sacrificial additive in a K<sub>3</sub>Fe(CN)<sub>6</sub>/K<sub>4</sub>Fe(CN)<sub>6</sub> thermocell. During initial operation, only a fraction of amine groups in polyethyleneimine engages in redox with Fe(CN)<sub>6</sub><sup>3-</sup>/Fe(CN)<sub>6</sub><sup>4-</sup>, while the remaining amine groups mediate thermally induced adsorption-desorption, selective condensation, and homogeneous catalysis. These cascaded effects boost the thermopower from 1.4 mV K<sup>-1</sup> to 7.76 mV K<sup>-1</sup>. Crucially, the self-limiting nature and temperature-dependent reactivity of polyethyleneimine-Fe(CN)<sub>6</sub><sup>3-</sup> reaction not only generates solvation-perturbing species but also ensures long-term functional stability (&gt;1000 hours). A proof-of-concept panel delivers over 5 V and 7.5 mW under a 50 K temperature difference, demonstrating system scalability. This work highlights the potential of sacrificial additive engineering to enable durable and high-performance thermocells for sustainable heat-to-electricity conversion.</p>

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In-situ recomposition of polyethyleneimine additive enables a multiprocess long-lifetime thermocell

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月7日

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  • Xinya Wu,
  • Chunlin Pang,
  • Qikai Li,
  • Yu-Ting Huang,
  • Sijia Wang,
  • Chun Cheng,
  • Wei Li,
  • Chuan He,
  • Qiyu Deng,
  • Hengjia Zhu,
  • Meng Ni,
  • Yun Chi,
  • Liqiu Wang,
  • Shien-Ping Feng

摘要

Ionic thermocells offer a compelling route for converting low-grade heat into electricity, yet their real-world deployment is hindered by performance decay under fluctuating conditions and limited synergistic pathways. Herein, we introduce polyethyleneimine as a self-limiting sacrificial additive in a K3Fe(CN)6/K4Fe(CN)6 thermocell. During initial operation, only a fraction of amine groups in polyethyleneimine engages in redox with Fe(CN)63-/Fe(CN)64-, while the remaining amine groups mediate thermally induced adsorption-desorption, selective condensation, and homogeneous catalysis. These cascaded effects boost the thermopower from 1.4 mV K-1 to 7.76 mV K-1. Crucially, the self-limiting nature and temperature-dependent reactivity of polyethyleneimine-Fe(CN)63- reaction not only generates solvation-perturbing species but also ensures long-term functional stability (>1000 hours). A proof-of-concept panel delivers over 5 V and 7.5 mW under a 50 K temperature difference, demonstrating system scalability. This work highlights the potential of sacrificial additive engineering to enable durable and high-performance thermocells for sustainable heat-to-electricity conversion.