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<p>Ionic thermoelectric (i-TE) materials have demonstrated a high thermopower in harvesting low-grade heat, emerging as superior candidates for self-powered electronics. However, coupling two i-TE effects in n-type materials is scarce, which restricts the development of high-performance systems. Herein, we uncover an overlooked thermogalvanic redox reaction between Cu<sup>2+</sup> and Cu<sup>+</sup> stabilized by Cl⁻ and quantitatively track the progressive reaction process by operando characterization. In binary polyvinyl alcohol (PVA)-CuCl<sub>2</sub> gels, an interactive i-TE coupling effect driven by ion speciation is validated, which exhibits an enhanced thermogalvanic redox as CuCl<sub>2</sub> concentrations increase while suppressing the thermodiffusion contribution. By distinguishing and quantifying coordination species, we reveal the impact of [Cu-Cl] speciation on the i-TE effect contributions. Correspondingly, a giant thermopower of −30.6 mV K<sup>-1</sup> and a remarkable power density of 0.6 mW m<sup>-2</sup> K<sup>-2</sup> are achieved, respectively, by tuning ion coordination speciation. The long-term power generation exhibits a reversible and sustainable heat-to-electricity conversion. High output voltage of 3.5 V and power of 22 µW are produced in 16-cell i-TE modules when harvesting 15 K. Our findings reveal an interactive thermo-diffusion/galvanic coupling effect based on coordination chemistry, offering a potential design principle for high-performance i-TE materials.</p>

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Modulating thermo-diffusion/galvanic coupling via ion speciation engineering enables high-performance ionic thermoelectric cells

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月31日

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  • Yuchen Li,
  • Ying-Ru Qiu,
  • Jinsha Liao,
  • Helios Y. Li,
  • Zhouyuntong Liu,
  • Yuxiang Chen,
  • Mao Yu,
  • Lizhi Xu,
  • Chang Liu,
  • Jefferson Zhe Liu,
  • Jian-Feng Li,
  • Weishu Liu,
  • Yao-Hui Wang,
  • Nicholas X. Fang

摘要

Ionic thermoelectric (i-TE) materials have demonstrated a high thermopower in harvesting low-grade heat, emerging as superior candidates for self-powered electronics. However, coupling two i-TE effects in n-type materials is scarce, which restricts the development of high-performance systems. Herein, we uncover an overlooked thermogalvanic redox reaction between Cu2+ and Cu+ stabilized by Cl⁻ and quantitatively track the progressive reaction process by operando characterization. In binary polyvinyl alcohol (PVA)-CuCl2 gels, an interactive i-TE coupling effect driven by ion speciation is validated, which exhibits an enhanced thermogalvanic redox as CuCl2 concentrations increase while suppressing the thermodiffusion contribution. By distinguishing and quantifying coordination species, we reveal the impact of [Cu-Cl] speciation on the i-TE effect contributions. Correspondingly, a giant thermopower of −30.6 mV K-1 and a remarkable power density of 0.6 mW m-2 K-2 are achieved, respectively, by tuning ion coordination speciation. The long-term power generation exhibits a reversible and sustainable heat-to-electricity conversion. High output voltage of 3.5 V and power of 22 µW are produced in 16-cell i-TE modules when harvesting 15 K. Our findings reveal an interactive thermo-diffusion/galvanic coupling effect based on coordination chemistry, offering a potential design principle for high-performance i-TE materials.