A bipolar-redox tetraalkynylporphyrin macrocycle positive electrode with 12-electrons-transfer for high-energy aluminum-organic batteries
Yuxi Guo,
Wei Wang (),
Ke Guo,
Xiaodong Chen,
Mingyong Wang,
Zheng Huang,
Yanli Zhu (),
Weili Song and
Shuqiang Jiao ()
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Yuxi Guo: Beijing Institute of Technology
Wei Wang: University of Science and Technology Beijing
Ke Guo: Beijing Institute of Technology
Xiaodong Chen: Lanzhou University of Technology
Mingyong Wang: University of Science and Technology Beijing
Zheng Huang: University of Science and Technology Beijing
Yanli Zhu: Beijing Institute of Technology
Weili Song: Beijing Institute of Technology
Shuqiang Jiao: University of Science and Technology Beijing
Nature Communications, 2025, vol. 16, issue 1, 1-15
Abstract:
Abstract Organic electrode materials with bipolar-redox activity are a promising candidate for high-energy aluminum-ion batteries (AIBs), but face the capacity ceiling due to limited active sites and low electron transfer number. To universally address this issue, seeking for a kind of multisite bipolar organic material to achieve multielectron transfer is a prerequisite but challenging. Herein, we develop a 12-electron transfer tetraalkynylporphyrin macrocycle positive electrode with two p-type amine (‒NH‒) motifs, two n-type imine (C = N) motifs and four n-type alkynyl (C ≡ C) motifs. The bipolar 18π-electron porphyrin macrocycle can alternately bind and release AlCl4− anions at ‒NH‒ sites and AlCl2+ cations at C = N sites (oxidized from 18π to 16π or reduced from 18π to 20π), achieving four electrons transfer. Furthermore, each terminal C ≡ C site can also coordinate with two AlCl2+ cations, thereby delivering eight electrons. The designed aluminum-organic battery achieves a high capacity of up to 347 mAh g−1 (3-6 times that of conventional graphite positive electrode, 60-120 mAh g−1) and a high specific energy of 312 Wh kg−1 (up to 150% compared to cells with graphite as positive electrode) based on the mass of positive electrode materials.
Date: 2025
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DOI: 10.1038/s41467-025-58126-5
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