High‐Rate Polymeric Redox in MXene‐Based Superlattice‐Like Heterostructure for Ammonium Ion Storage
Abstract Achieving both high redox activity and rapid ion transport is a critical and pervasive challenge in electrochemical energy storage applications. This challenge is significantly magnified when using large‐sized charge carriers, such as the sustainable ammonium ion (NH 4 + ). A self‐assembled MXene/n‐type conjugated polyelectrolyte (CPE) superlattice‐like heterostructure that enables redox‐active, fast, and reversible ammonium storage is reported. The superlattice‐like structure persists as the CPE:MXene ratio increases, accompanied by a linear increase in the interlayer spacing of MXene flakes and a greater overlap of CPEs. Concurrently, the redox activity per unit of CPE unexpectedly intensifies, a phenomenon that can be explained by the enhanced de‐solvation of ammonium due to the increased volume of 3 Å‐sized pores, as indicated by molecular dynamic simulations. At the maximum CPE mass loading (MXene:CPE ratio = 2:1), the heterostructure demonstrates the strongest polymeric redox activity with a high ammonium storage capacity of 126.1 C g −1 and a superior rate capability at 10 A g −1 . This work unveils an effective strategy for designing tunable superlattice‐like heterostructures to enhance redox activity and achieve rapid charge transfer for ions beyond lithium.
Authors
- Hongjun Liu (ORCID: https://orcid.org/0000-0003-3326-2640)
- Jaehoon Choi (ORCID: https://orcid.org/0009-0007-9974-3902)
- De‐en Jiang (ORCID: https://orcid.org/0000-0001-5167-0731)
- Marnix Wagemaker (ORCID: https://orcid.org/0000-0003-3851-1044)
- Bart Boshuizen (ORCID: https://orcid.org/0000-0002-3413-8839)
- Simon Fleischmann (ORCID: https://orcid.org/0000-0001-9475-3692)
- Guillermo Carlos Bazan (ORCID: https://orcid.org/0000-0002-2537-0310)
- Glenn Quek (ORCID: https://orcid.org/0009-0003-1254-9885)
- Ricardo Javier Vázquez (ORCID: https://orcid.org/0000-0003-3245-8123)
- Dingding Ren (ORCID: https://orcid.org/0000-0001-6829-6475)
- Xuehang Wang (ORCID: https://orcid.org/0000-0002-8984-6162)
- Bjørn‐Ove Fimland (ORCID: https://orcid.org/0000-0002-0210-4351)
- Lars J. Bannenberg (ORCID: https://orcid.org/0000-0001-8150-3694)
- Chaofan Chen (ORCID: https://orcid.org/0009-0003-1508-514X)
- Ruipeng Li (ORCID: https://orcid.org/0009-0006-5263-0671)
Institutions
- Karlsruhe Institute of Technology (DE)
- National University of Singapore (SG)
- Vanderbilt University (US)
- Brookhaven National Laboratory (US)
- Norwegian University of Science and Technology (NO)
- Indiana University Bloomington (US)
- Helmholtz-Institute Ulm (DE)
- Delft University of Technology (NL)
Publication Details
- Journal
- Advanced Energy Materials
- Published
- 2024-09-03
- DOI
- https://doi.org/10.1002/aenm.202402715
- Citations
- 13
- Primary Topic
- MXene and MAX Phase Materials
- Type
- article
- Field-Weighted Citation Impact
- 1.52
Funders
- National Science Foundation
- U.S. Department of Energy
- National University of Singapore
- Nederlandse Organisatie voor Wetenschappelijk Onderzoek
- Norges Forskningsråd
- Helmholtz Association
- Office of Science
- Office of Naval Research
- Division of Chemistry