Wu Minghan, Hao Siqi, Qi Linfeng, Shi Yu, Yang Wei, Bao Jingjing, Du Min, Mo Zhengyu, Sun Licheng
State Key Laboratory of Hydraulics and Mountain River Engineering, College of Water Resource & Hydropower, Sichuan University, Chengdu 610065, China.
College of Chemical Engineering, Sichuan University, Chengdu 610225, China.
ACS Appl Mater Interfaces. 2025 May 7;17(18):26775-26783. doi: 10.1021/acsami.5c03375. Epub 2025 Apr 22.
Thermogalvanic cells (TGCs) are at the forefront of effective thermoelectric conversion methods, but the practical utilization of their integrated devices is hindered by the suboptimal performance of N-type TGCs. Herein, a novel redox couple of Cu/Cu(en) is proposed to construct a liquid-state N-type TGC. The electrochemical reaction involving the Cu electrode, ethylenediamine (en), and their chelated compound Cu(en) exhibits a significant reaction entropy change, resulting in an enhanced temperature coefficient (α). We reveal that the α of the Cu/Cu(en)-based TGC reaches 1.64 mV K. Furthermore, by optimizing the concentrations of Cu, ethylenediamine, and (NH)SO in the electrolyte, both α and normalized power density can be significantly improved, achieving values of 2.12 mV K and 676 μW m K, respectively. Moreover, by constructing a P-N junction with P-type and N-type TGC, we achieve a high potential of 121 mV under a temperature gradient of 35 K. This work expands the available redox couple options for N-type TGCs and offers a new pathway for efficient thermoelectric conversion.
热电池(TGCs)处于有效热电转换方法的前沿,但N型TGCs的性能欠佳阻碍了其集成器件的实际应用。在此,提出了一种新型的Cu/Cu(en)氧化还原对来构建液态N型TGC。涉及铜电极、乙二胺(en)及其螯合物Cu(en)的电化学反应表现出显著的反应熵变,导致温度系数(α)增大。我们发现基于Cu/Cu(en)的TGC的α达到1.64 mV K。此外,通过优化电解质中铜、乙二胺和(NH)SO的浓度,α和归一化功率密度都能得到显著提高,分别达到2.12 mV K和676 μW m K。而且,通过用P型和N型TGC构建P-N结,在35 K的温度梯度下实现了121 mV的高电位。这项工作扩展了N型TGCs可用的氧化还原对选择,并为高效热电转换提供了一条新途径。