An N-Type Thermogalvanic Cell with a High Temperature Coefficient Based on the Cu/Cu(en)22+ Redox Couple

IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Applied Materials & Interfaces Pub Date : 2025-04-22 DOI:10.1021/acsami.5c03375
Minghan Wu, Siqi Hao, Linfeng Qi, Yu Shi, Wei Yang, Jingjing Bao, Min Du, Zhengyu Mo, Licheng Sun
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Abstract

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)22+ 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)22+ exhibits a significant reaction entropy change, resulting in an enhanced temperature coefficient (α). We reveal that the α of the Cu/Cu(en)22+-based TGC reaches 1.64 mV K–1. Furthermore, by optimizing the concentrations of Cu2+, ethylenediamine, and (NH4)2SO4 in the electrolyte, both α and normalized power density can be significantly improved, achieving values of 2.12 mV K–1 and 676 μW m–2 K–2, 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.

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基于Cu/Cu(en)22+氧化还原偶联的高温系数n型热电电池
热电电池(TGCs)是有效热电转换方法的前沿,但其集成器件的实际利用受到n型TGCs的次优性能的阻碍。本文提出了一种新的Cu/Cu(en)22+氧化还原偶对来构建液态n型TGC。Cu电极与乙二胺(en)及其螯合物Cu(en)22+的电化学反应表现出明显的反应熵变化,导致温度系数(α)升高。结果表明,Cu/Cu(en)22+基TGC的α达到1.64 mV K-1。此外,通过优化电解液中Cu2+、乙二胺和(NH4)2SO4的浓度,可以显著提高α和归一化功率密度,分别达到2.12 mV K-1和676 μW m-2 K-2。此外,通过构建p型和n型TGC的P-N结,我们在35 K的温度梯度下获得了121 mV的高电位。这项工作扩大了n型TGCs可用的氧化还原偶选择,并为高效热电转换提供了新的途径。
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来源期刊
ACS Applied Materials & Interfaces
ACS Applied Materials & Interfaces 工程技术-材料科学:综合
CiteScore
16.00
自引率
6.30%
发文量
4978
审稿时长
1.8 months
期刊介绍: ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.
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