Giant gateable thermoelectric conversion by tuning the ion linkage interactions in covalent organic framework membranes

Shijie Yin, Jianguo Li, Zhuozhi Lai, Qing-Wei Meng, Weipeng Xian, Zhifeng Dai, Sai Wang, Li Zhang (), Yubing Xiong (), Shengqian Ma and Qi Sun ()
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Shijie Yin: Zhejiang Sci-Tech University
Jianguo Li: Zhejiang Sci-Tech University
Zhuozhi Lai: Zhejiang University
Qing-Wei Meng: Zhejiang University
Weipeng Xian: Zhejiang University
Zhifeng Dai: Zhejiang Sci-Tech University
Sai Wang: Zhejiang University
Li Zhang: Zhejiang Sci-Tech University
Yubing Xiong: Zhejiang Sci-Tech University
Shengqian Ma: University of North Texas
Qi Sun: Zhejiang University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Efficient energy conversion using ions as carriers necessitates membranes that sustain high permselectivity in high salinity conditions, which presents a significant challenge. This study addresses the issue by manipulating the linkages in covalent-organic-framework membranes, altering the distribution of electrostatic potentials and thereby influencing the short-range interactions between ions and membranes. We show that a charge-neutral covalent-organic-framework membrane with β-ketoenamine linkages achieves record permselectivity in high salinity environments. Additionally, the membrane retains its permselectivity under temperature gradients, providing a method for converting low-grade waste heat into electrical energy. Experiments reveal that with a 3 M KCl solution and a 50 K temperature difference, the membrane generates an output power density of 5.70 W m−2. Furthermore, guided by a short-range ionic screening mechanism, the membrane exhibits adaptable permselectivity, allowing reversible and controllable operations by finely adjusting charge polarity and magnitude on the membrane’s channel surfaces via ion adsorption. Notably, treatment with K3PO4 solutions significantly enhances permselectivity, resulting in a giant output power density of 20.22 W m−2, a 3.6-fold increase over the untreated membrane, setting a benchmark for converting low-grade heat into electrical energy.

Date: 2024
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DOI: 10.1038/s41467-024-52487-z

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