Since aluminium is one of the most widely available elements in Earth’s crust, developing rechargeable aluminium batteries offers an ideal opportunity to deliver cells with high energy-to-price ratios. Nevertheless, finding appropriate host electrodes for insertion of aluminium (complex) ions remains a fundamental challenge. Here, we demonstrate a strategy for designing active materials for rechargeable aluminium batteries. This strategy entails the use of redox-active triangular phenanthrenequinone-based macrocycles, which form layered superstructures resulting in the reversible insertion and extraction of a cationic aluminium complex. This architecture exhibits an outstanding electrochemical performance with a reversible capacity of 110 mA h g–1 along with a superior cyclability of up to 5,000 cycles. Furthermore, electrodes composed of these macrocycles blended with graphite flakes result in higher specific capacity, electronic conductivity and areal loading. These findings constitute a major advance in the design of rechargeable aluminium batteries and represent a good starting point for addressing affordable large-scale energy storage.

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This research was conducted as part of the Joint Center of Excellence in Integrated Nanosystems at King Abdulaziz City for Science and Technology (KACST) and Northwestern University (NU). The authors acknowledge both KACST and NU for their financial support of this research. The Integrated Molecular Structure Education and Research Center (IMSERC) at NU is acknowledged for the use of its facilities. J.W.C. acknowledges support by National Research Foundation of Korea (NRF) grants funded by the Korea government (MEST) (NRF-2018R1A2A1A19023146, NRF-2017M1A2A2044477 and NRF-2018M1A2A2063340) and the Energy Efficiency and Resources Core Technology Programme of the Korea Institute of Energy Technology Evaluation and Planning (KETEP), which is granted financial resources from the Ministry of Trade, Industry and Energy, Republic of Korea (20152020104870).

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Author notes

    • Dong Jun Kim

    Present address: School of Chemistry, University of New South Wales, Sydney, New South Wales, Australia

  1. These authors contributed equally: Dong Jun Kim, Dong-Joo Yoo.


  1. Department of Chemistry, Northwestern University, Evanston, IL, USA

    • Dong Jun Kim
    • , Michael T. Otley
    • , Cristian Pezzato
    • , Magdalena Owczarek
    •  & J. Fraser Stoddart
  2. School of Chemical and Biological Engineering and Institute of Chemical Processes, Seoul National University, Seoul, Republic of Korea

    • Dong-Joo Yoo
    •  & Jang Wook Choi
  3. Department of Chemical and Biological Engineering, Northwestern University, Evanston, IL, USA

    • Aleksandrs Prokofjevs
  4. Graduate School of Energy, Environment, Water, and Sustainability (EEWS), Korea Advanced Institute of Science and Technology (KAIST), Daejeon, Republic of Korea

    • Seung Jong Lee
  5. Institute for Molecular Design and Synthesis, Tianjin University, Tianjin, P. R. China

    • J. Fraser Stoddart


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D.J.K. and D.-J.Y. designed and performed experimental work. D.J.K., M.T.O., A.P. and M.O. worked on synthesis and characterisation of active materials. D.-J.Y. measured ALB performance. D.-J.Y. and S.J.L. conducted ex-situ analysis of active materials. D.J.K., A.P., D.-J.Y., J.W.C. and J.F.S. wrote the manuscript. J.W.C. and J.F.S. directed this work. All authors discussed the results and commented on the manuscript.

Competing interests

The authors declare no competing interests.

Corresponding authors

Correspondence to Jang Wook Choi or J. Fraser Stoddart.

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