Improving Seebeck coefficient of thermoelectrochemical cells by controlling ligand complexation at metal redox centers
Improving Seebeck coefficient of thermoelectrochemical cells by controlling ligand complexation at metal redox centers
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DOI：
10.1063/5.0052649
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发表时间：
2021-06-21
影响因子：
4
通讯作者：
Phelan, Patrick E.
中科院分区：
文献类型：
--
作者：
Gunawan, Andrey;Tarakeshwar, Pilarisetty;Phelan, Patrick E.
通过热电化学电池将废热实际转化为电能需要较高的塞贝克系数(α)来提高循环效率。Cu2+物种与溶解的多齿配体(如乙二胺四乙酸)的络合，以及对二聚平衡的控制，如1，6-二氨基己烷或1，2-二氨基乙烷，显著提高了铜/Cu2+热电化学电池的α值，最高可达185%。这导致了迄今报道的所有铜/Cu2+氧化还原体系中最高的α。系数α与熵的变化成正比(德尔塔S)。对其进行了实验测量，并与用量子化学方法得到的S增量进行了关联。这为基于分子的宏观反应解释提供了更深层次的见解。理论估计的阿尔法与实验观测到的阿尔法之间的一致性是显著的。因此，我们相信，这种协同方法使我们能够系统地扫描不同的系统，以获得具有增强的塞贝克系数的高效热电化学池。由AIP出版公司独家授权出版。
Practical conversion of waste heat into electricity via thermoelectrochemical cells requires high Seebeck coefficient (alpha) to increase cycle efficiency. The complexation of Cu2+ species with dissolved multidentate ligands, such as ethylenediaminetetraacetic acid, and the control of dimerization equilibria with bridging ligands, such as 1,6-diaminohexane or 1,2-diaminoethane, dramatically improve, by up to similar to 185%, the magnitude of the alpha of Cu/Cu2+ thermoelectrochemical cells. This results in the highest alpha for any Cu/Cu2+ redox system yet reported. The coefficient alpha is directly proportional to the change in entropy (Delta S). It was experimentally measured and correlated with Delta S obtained from quantum-chemical methods. This offers a deeper insight about a molecule-based interpretation of the macroscopic response. The agreement between the theoretically estimated and experimentally observed alpha is remarkable. Hence, we believe that this synergistic approach allows us to systematically scan different systems to obtain efficient thermoelectrochemical cells with enhanced Seebeck coefficient. Published under an exclusive license by AIP Publishing.